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  • 1.
    Abrahamsson, Tobias
    et al.
    Linköping University, Department of Science and Technology, Laboratory of Organic Electronics. Linköping University, Faculty of Science & Engineering.
    Vagin, Mikhail
    Linköping University, Department of Science and Technology, Laboratory of Organic Electronics. Linköping University, Faculty of Science & Engineering.
    Seitanidou, Maria S
    Linköping University, Department of Science and Technology, Laboratory of Organic Electronics. Linköping University, Faculty of Science & Engineering.
    Roy, Arghyamalya
    Linköping University, Department of Science and Technology, Laboratory of Organic Electronics. Linköping University, Faculty of Science & Engineering.
    Phopase, Jaywant
    Linköping University, Department of Science and Technology, Laboratory of Organic Electronics. Linköping University, Faculty of Science & Engineering.
    Petsagkourakis, Ioannis
    Linköping University, Department of Science and Technology, Laboratory of Organic Electronics. Linköping University, Faculty of Science & Engineering.
    Moro, Nathalie
    Linköping University, Department of Science and Technology, Laboratory of Organic Electronics. Linköping University, Faculty of Science & Engineering. Empa, Switzerland.
    Tybrandt, Klas
    Linköping University, Department of Science and Technology, Laboratory of Organic Electronics. Linköping University, Faculty of Science & Engineering.
    Crispin, Xavier
    Linköping University, Department of Science and Technology, Laboratory of Organic Electronics. Linköping University, Faculty of Science & Engineering.
    Berggren, Magnus
    Linköping University, Department of Science and Technology, Laboratory of Organic Electronics. Linköping University, Faculty of Science & Engineering.
    Simon, Daniel
    Linköping University, Department of Science and Technology, Laboratory of Organic Electronics. Linköping University, Faculty of Science & Engineering.
    Investigating the role of polymer size on ionic conductivity in free-standing hyperbranched polyelectrolyte membranes2021In: Polymer, ISSN 0032-3861, E-ISSN 1873-2291, Vol. 223, article id 123664Article in journal (Refereed)
    Abstract [en]

    Polymer-based ion exchange membranes (IEMs) are utilized for many applications such as in water desalination, energy storage, fuel cells and in electrophoretic drug delivery devices, exemplified by the organic electronic ion pump (OEIP). The bulk of current research is primarily focused on finding highly conductive and stable IEM materials. Even though great progress has been made, a lack of fundamental understanding of how specific polymer properties affect ionic transport capabilities still remains. This leads to uncertainty in how to proceed with synthetic approaches for designing better IEM materials. In this study, an investigation of the structure-property relationship between polymer size and ionic conductivity was performed by comparing a series of membranes, based on ionically charged hyperbranched polyglycerol of different polymer sizes. Observing an increase in ionic conductivity associated with increasing polymer size and greater electrolyte exclusion, indi-cating an ionic transportation phenomenon not exclusively based on membrane electrolyte uptake. These findings further our understanding of ion transport phenomena in semi-permeable membranes and indicate a strong starting point for future design and synthesis of IEM polymers to achieve broader capabilities for a variety of ion transport-based applications.

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  • 2.
    Ahmed, Fareed
    et al.
    Linköping University, Department of Science and Technology, Laboratory of Organic Electronics. Linköping University, Faculty of Science & Engineering.
    Ding, Penghui
    Linköping University, Department of Science and Technology, Laboratory of Organic Electronics. Linköping University, Faculty of Science & Engineering.
    Ail, Ujwala
    Linköping University, Department of Science and Technology, Laboratory of Organic Electronics. Linköping University, Faculty of Science & Engineering.
    Warczak, Magdalena
    Linköping University, Department of Science and Technology, Laboratory of Organic Electronics. Linköping University, Faculty of Science & Engineering.
    Grimoldi, Andrea
    Linköping University, Department of Science and Technology, Laboratory of Organic Electronics. Linköping University, Faculty of Science & Engineering.
    Ederth, Thomas
    Linköping University, Department of Physics, Chemistry and Biology, Biophysics and bioengineering. Linköping University, Faculty of Science & Engineering.
    Håkansson, Karl M. O.
    RISE Bioeconomy, Stockholm, Sweden.
    Vagin, Mikhail
    Linköping University, Department of Science and Technology, Laboratory of Organic Electronics. Linköping University, Faculty of Science & Engineering.
    Gueskine, Viktor
    Linköping University, Department of Science and Technology, Laboratory of Organic Electronics. Linköping University, Faculty of Science & Engineering.
    Berggren, Magnus
    Linköping University, Department of Science and Technology, Laboratory of Organic Electronics. Linköping University, Faculty of Science & Engineering.
    Crispin, Xavier
    Linköping University, Department of Science and Technology, Laboratory of Organic Electronics. Linköping University, Faculty of Science & Engineering.
    Manufacturing Poly(3,4-Ethylenedioxythiophene) Electrocatalytic Sheets for Large-Scale H2O2 Production2022In: Advanced Sustainable Systems, E-ISSN 2366-7486, Vol. 6, no 1, article id 2100316Article in journal (Refereed)
    Abstract [en]

    Producing thick films of conducting polymers by a low-cost manufacturing technique would enable new applications. However, removing huge solvent volume from diluted suspension or dispersion (1-3 wt%) in which conducting polymers are typically obtained is a true manufacturing challenge. In this work, a procedure is proposed to quickly remove water from the conducting polymer poly(3,4-ethylenedioxythiophene:poly(4-styrene sulfonate) (PEDOT:PSS) suspension. The PEDOT:PSS suspension is first flocculated with 1 m H2SO4 transforming PEDOT nanoparticles (approximate to 50-500 nm) into soft microparticles. A filtration process inspired by pulp dewatering in a paper machine on a wire mesh with apertures dimension between 60 mu m and 0.5 mm leads to thick free-standing films (approximate to 0.5 mm). Wire mesh clogging that hinders dewatering (known as dead-end filtration) is overcome by adding to the flocculated PEDOT: PSS dispersion carbon fibers that aggregate and form efficient water channels. Moreover, this enables fast formation of thick layers under simple atmospheric pressure filtration, thus making the process truly scalable. Thick freestanding PEDOT films thus obtained are used as electrocatalysts for efficient reduction of oxygen to hydrogen peroxide, a promising green chemical and fuel. The inhomogeneity of the films does not affect their electrochemical function.

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  • 3.
    Ajjan, Fátima
    et al.
    Linköping University, Department of Science and Technology, Laboratory of Organic Electronics. Linköping University, Faculty of Science & Engineering.
    Khan, Ziyauddin
    Linköping University, Department of Science and Technology, Laboratory of Organic Electronics. Linköping University, Faculty of Science & Engineering.
    Riera-Galindo, Sergi
    Linköping University, Department of Science and Technology, Laboratory of Organic Electronics. Linköping University, Faculty of Science & Engineering.
    Lienemann, Samuel
    Linköping University, Department of Science and Technology, Laboratory of Organic Electronics. Linköping University, Faculty of Science & Engineering.
    Vagin, Mikhail
    Linköping University, Department of Science and Technology, Laboratory of Organic Electronics. Linköping University, Faculty of Science & Engineering.
    Petsagkourakis, Ioannis
    Linköping University, Department of Science and Technology, Laboratory of Organic Electronics. Linköping University, Faculty of Science & Engineering.
    Gabrielsson, Roger
    Linköping University, Department of Science and Technology, Laboratory of Organic Electronics. Linköping University, Faculty of Science & Engineering.
    Braun, Slawomir
    Linköping University, Department of Science and Technology, Laboratory of Organic Electronics. Linköping University, Faculty of Science & Engineering.
    Fahlman, Mats
    Linköping University, Department of Science and Technology, Laboratory of Organic Electronics. Linköping University, Faculty of Science & Engineering.
    Inganäs, Olle
    Linköping University, Department of Physics, Chemistry and Biology, Biomolecular and Organic Electronics. Linköping University, Faculty of Science & Engineering.
    Berggren, Magnus
    Linköping University, Department of Science and Technology, Laboratory of Organic Electronics. Linköping University, Faculty of Science & Engineering.
    Crispin, Xavier
    Linköping University, Department of Science and Technology, Laboratory of Organic Electronics. Linköping University, Faculty of Science & Engineering.
    Doped Conjugated Polymer Enclosing a Redox Polymer: Wiring Polyquinones with Poly(3,4‐Ethylenedioxythiophene)2020In: Advanced Energy and Sustainability Research, E-ISSN 2699-9412, Vol. 1, no 2, article id 2000027Article in journal (Refereed)
    Abstract [en]

    The mass implementation of renewable energies is limited by the absence of efficient and affordable technology to store electrical energy. Thus, the development of new materials is needed to improve the performance of actual devices such as batteries or supercapacitors. Herein, the facile consecutive chemically oxidative polymerization of poly(1-amino-5-chloroanthraquinone) (PACA) and poly(3,4-ethylenedioxythiophene (PEDOT) resulting in a water dispersible material PACA-PEDOT is shown. The water-based slurry made of PACA-PEDOT nanoparticles can be processed as film coated in ambient atmosphere, a critical feature for scaling up the electrode manufacturing. The novel redox polymer electrode is a nanocomposite that withstands rapid charging (16 A g−1) and delivers high power (5000 W kg−1). At lower current density its storage capacity is high (198 mAh g−1) and displays improved cycling stability (60% after 5000 cycles). Its great electrochemical performance results from the combination of the redox reversibility of the quinone groups in PACA that allows a high amount of charge storage via Faradaic reactions and the high electronic conductivity of PEDOT to access to the redox-active sites. These promising results demonstrate the potential of PACA-PEDOT to make easily organic electrodes from a water-coating process, without toxic metals, and operating in non-flammable aqueous electrolyte for large scale pseudocapacitors. 

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  • 4.
    Ajjan, Fátima
    et al.
    Linköping University, Department of Physics, Chemistry and Biology, Biomolecular and Organic Electronics. Linköping University, Faculty of Science & Engineering.
    Vagin, Mikhail
    Linköping University, Department of Science and Technology, Laboratory of Organic Electronics. Linköping University, Faculty of Science & Engineering.
    Rebis, Tomasz
    Poznan Univ Tech, Poland.
    Ever Aguirre, Luis
    Linköping University, Department of Physics, Chemistry and Biology, Biomolecular and Organic Electronics. Linköping University, Faculty of Science & Engineering.
    Ouyang, Liangqi
    Linköping University, Department of Physics, Chemistry and Biology, Biomolecular and Organic Electronics. Linköping University, Faculty of Science & Engineering.
    Inganäs, Olle
    Linköping University, Department of Physics, Chemistry and Biology, Electronic and photonic materials. Linköping University, Faculty of Science & Engineering.
    Scalable Asymmetric Supercapacitors Based on Hybrid Organic/Biopolymer Electrodes2017In: ADVANCED SUSTAINABLE SYSTEMS, ISSN 2366-7486, Vol. 1, no 8, article id 1700054Article in journal (Refereed)
    Abstract [en]

    A trihybrid bioelectrode composed of lignin, poly(3,4-ethylenedioxythiophene) (PEDOT), and poly(aminoanthraquinone) (PAAQ) is prepared by a two-step galvanostatic electropolymerization, and characterized for supercapacitor applications. Using PEDOT/Lignin as a base layer, followed by the consecutive deposition of PAAQ, the hybrid electrode PEDOT/Lignin/PAAQ shows a high specific capacitance of 418 F g(-1) with small self-discharge. This trihybrid electrode material can be assembled into symmetric and asymmetric super-capacitors. The asymmetric supercapacitor uses PEDOT + Lignin/PAAQ as positive electrode and PEDOT/PAAQ as negative electrode, and exhibits superior electrochemical performance due to the synergistic effect of the two electrodes, which leads to a specific capacitance of 74 F g(-1). It can be reversibly cycled in the voltage range of 0-0.7 V. More than 80% capacitance is retained after 10 000 cycles. These remarkable features reveal the exciting potential of a full organic energy storage device with long cycle life.

  • 5.
    Anwar, Nargis
    et al.
    Dundalk Inst Technol, Ireland.
    Armstrong, Gordon
    Univ Limerick, Ireland.
    Laffir, Fathima
    Univ Limerick, Ireland.
    Dickinson, Calum
    Univ Limerick, Ireland.
    Vagin, Mikhail
    Linköping University, Department of Science and Technology, Physics and Electronics. Linköping University, Department of Physics, Chemistry and Biology. Linköping University, Faculty of Science & Engineering.
    McCormac, Timothy
    Dundalk Inst Technol, Ireland.
    Redox switching of polyoxometalate-doped polypyrrole films in ionic liquid media2018In: Electrochimica Acta, ISSN 0013-4686, E-ISSN 1873-3859, Vol. 265, p. 254-258Article in journal (Refereed)
    Abstract [en]

    The surface immobilization of the parent Dawson polyoxometalate (POM) as a counter-ion for the electropolymerization of polypyrrole (PPy) or as an electrode-adhered solid was utilized for voltammetric studies of the surface adhered POM in room temperature ionic liquids (RTIL). Illustrating the efficiency of intermediate stabilization, voltammetry at POM-modified electrodes in a PF6-based RTIL revealed richer redox behaviour and higher stabilization in comparison with aqueous electrolytes and with BF4-based RTIL, respectively. High stability of the POM-doped PPy towards continuous charge-discharge voltammetric redox cycles was confirmed by minor changes in film morphology observed after the cycling in RTILs. (c) 2017 Elsevier Ltd. All rights reserved.

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  • 6.
    Bamgbopa, Musbaudeen O.
    et al.
    Dubai Elect & Water Author DEWA, U Arab Emirates.
    Fetyan, Abdulmonem
    Dubai Elect & Water Author DEWA, U Arab Emirates.
    Vagin, Mikhail
    Linköping University, Department of Science and Technology, Laboratory of Organic Electronics. Linköping University, Faculty of Science & Engineering.
    Adelodun, Adedeji A.
    Fed Univ Technol Akure, Nigeria.
    Towards eco-friendly redox flow batteries with all bio-sourced cell components2022In: Journal of Energy Storage, ISSN 2352-152X, E-ISSN 2352-1538, Vol. 50, article id 104352Article, review/survey (Refereed)
    Abstract [en]

    Recent research and few pilot deployments have demonstrated promising aqueous organic redox flow battery (RFB) systems. However, the claim that these organic RFB systems are eco-friendlier energy storage than Lithium-ion batteries and aqueous inorganic metallic RFB counterparts needs reinforcement, primarily if cell components other than redox-active species are still based on unsustainable materials. This thesis of the present work presents the prospects of achieving future eco-friendly RFBs with higher consideration for sustainability by adopting significant amounts of abundant bio-sourced/based materials for all main cell components. As we highlight the promising sources of the energy materials from a review of previous studies, we infer that plant derived quinones and other organic polymers may continue to dominate the organic redox-active species space. Furthermore, a candidate methodology to accomplish porous electrodes and membranes/separators of the eco-friendly RFBs is to apply stand-alone bio-based/sourced fibrils derived from cellulose, lignin, chitin, among other materials. These materials can be combined with (un)carbonised biomass or food wastes & residues to impart conductivity, catalytic activity, and ion selectivity. We explore symmetric chemistry as an ideal system for the eco-friendly RFBs of the discourse, given interplay between the electrolyte, electrode material and membrane dictates energy efficiency and cycling stability. These strategies also need to be coupled with further improvements to achieve reliability.

    The full text will be freely available from 2024-03-03 16:15
  • 7.
    Cattelan, Mattia
    et al.
    School of Chemistry, University of Bristol, Cantocks Close, Bristol, United Kingdom.
    Vagin, Mikhail
    Linköping University, Department of Physics, Chemistry and Biology. Linköping University, Department of Science and Technology, Laboratory of Organic Electronics. Linköping University, Faculty of Science & Engineering.
    Fox, Neil A.
    School of Chemistry, University of Bristol, Cantocks Close, Bristol, United Kingdom.
    Ivanov, Ivan Gueorguiev
    Linköping University, Department of Physics, Chemistry and Biology, Semiconductor Materials. Linköping University, Faculty of Science & Engineering.
    Shtepliuk, Ivan
    Linköping University, Department of Physics, Chemistry and Biology, Semiconductor Materials. Linköping University, Faculty of Science & Engineering.
    Yakimova, Rositsa
    Linköping University, Department of Physics, Chemistry and Biology, Semiconductor Materials. Linköping University, Faculty of Science & Engineering.
    Anodization study of epitaxial graphene: insights on the oxygen evolution reaction of graphitic materials2019In: Nanotechnology, ISSN 0957-4484, E-ISSN 1361-6528, Vol. 30, no 28, article id 285701Article in journal (Refereed)
    Abstract [en]

    The photoemission electron microscopy and x-ray photoemission spectroscopy were utilized for the study of anodized epitaxial graphene (EG) on silicon carbide as a fundamental aspect of the oxygen evolution reaction on graphitic materials. The high-resolution analysis of surface morphology and composition quantified the material transformation during the anodization. We investigated the surface with lateral resolution amp;lt;150 nm, revealing significant transformations on the EG and the role of multilayer edges in increasing the film capacitance.

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  • 8.
    Che, Canyan
    et al.
    Linköping University, Department of Science and Technology, Laboratory of Organic Electronics. Linköping University, Faculty of Science & Engineering.
    Vagin, Mikhail
    Linköping University, Faculty of Science & Engineering. Linköping University, Department of Science and Technology, Laboratory of Organic Electronics. Linköping University, Department of Physics, Chemistry and Biology.
    Ail, Ujwala
    Linköping University, Department of Science and Technology, Laboratory of Organic Electronics. Linköping University, Faculty of Science & Engineering.
    Gueskine, Viktor
    Linköping University, Department of Science and Technology, Laboratory of Organic Electronics. Linköping University, Faculty of Science & Engineering.
    Phopase, Jaywant
    Linköping University, Department of Science and Technology, Laboratory of Organic Electronics. Linköping University, Faculty of Science & Engineering. Linköping University, Department of Physics, Chemistry and Biology.
    Brooke, Robert
    RISE, Norrköping, Sweden.
    Gabrielsson, Roger
    Linköping University, Department of Science and Technology, Laboratory of Organic Electronics. Linköping University, Faculty of Science & Engineering.
    Jonsson, Magnus P.
    Linköping University, Department of Science and Technology, Laboratory of Organic Electronics. Linköping University, Faculty of Science & Engineering.
    Mak, Wing Cheung
    Linköping University, Department of Physics, Chemistry and Biology, Sensor and Actuator Systems. Linköping University, Faculty of Science & Engineering.
    Berggren, Magnus
    Linköping University, Department of Science and Technology, Laboratory of Organic Electronics. Linköping University, Faculty of Science & Engineering.
    Crispin, Xavier
    Linköping University, Department of Science and Technology, Laboratory of Organic Electronics. Linköping University, Faculty of Science & Engineering.
    Twinning Lignosulfonate with a Conducting Polymer via Counter-Ion Exchange for Large-Scale Electrical Storage2019In: Advanced Sustainable Systems, ISSN 2366-7486, Vol. 3, no 9, article id 1900039Article in journal (Refereed)
    Abstract [en]

    Abstract Lignosulfonate (LS) is a large-scale surplus product of the forest and paper industries, and has primarily been utilized as a low-cost plasticizer in making concrete for the construction industry. LS is an anionic redox-active polyelectrolyte and is a promising candidate to boost the charge capacity of the positive electrode (positrode) in redox-supercapacitors. Here, the physical-chemical investigation of how this biopolymer incorporates into the conducting polymer PEDOT matrix, of the positrode, by means of counter-ion exchange is reported. Upon successful incorporation, an optimal access to redox moieties is achieved, which provides a 63% increase of the resulting stored electrical charge by reversible redox interconversion. The effects of pH, ionic strength, and concentrations, of included components, on the polymer?polymer interactions are optimized to exploit the biopolymer-associated redox currents. Further, the explored LS-conducting polymer incorporation strategy, via aqueous synthesis, is evaluated in an up-scaling effort toward large-scale electrical energy storage technology. By using an up-scaled production protocol, integration of the biopolymer within the conducting polymer matrix by counter-ion exchange is confirmed and the PEDOT-LS synthesized through optimized strategy reaches an improved charge capacity of 44.6 mAh g?1.

  • 9.
    Che, Canyan
    et al.
    Linköping University, Department of Science and Technology. Linköping University, Faculty of Science & Engineering.
    Vagin, Mikhail
    Linköping University, Department of Science and Technology, Physics and Electronics. Linköping University, Department of Physics, Chemistry and Biology. Linköping University, Faculty of Science & Engineering.
    Wijeratne, Kosala
    Linköping University, Department of Science and Technology, Physics and Electronics. Linköping University, Faculty of Science & Engineering.
    Zhao, Dan
    Linköping University, Department of Science and Technology, Physics and Electronics. Linköping University, Faculty of Science & Engineering.
    Warczak, Magdalena
    Linköping University, Department of Science and Technology, Physics and Electronics. Linköping University, Faculty of Science & Engineering.
    Jonsson, Magnus
    Linköping University, Department of Science and Technology, Physics and Electronics. Linköping University, Faculty of Science & Engineering.
    Crispin, Xavier
    Linköping University, Department of Science and Technology, Physics and Electronics. Linköping University, Faculty of Science & Engineering.
    Conducting Polymer Electrocatalysts for Proton-Coupled Electron Transfer Reactions: Toward Organic Fuel Cells with Forest Fuels2018In: Advanced Sustainable Systems, ISSN 2366-7486, Vol. 317Article in journal (Refereed)
    Abstract [en]

    Lignin is one of the most abundant biopolymers, constituting 25% of plants. The pulp and paper industries extract lignin in their process and today seek new applications for this by-product. Here, it is reported that the aromatic alcohols obtained from lignin depolymerization can be used as fuel in high power density electrical power sources. This study shows that the conducting polymer poly(3,4-ethylenedioxythiophene), fabricated from abundant ele-ments via low temperature synthesis, enables efficient, direct, and reversible chemical-to-electrical energy conversion of aromatic alcohols such as lignin residues in aqueous media. A material operation principle related to the rela-tively high molecular diffusion and ionic conductivity within the conducting polymer matrix, ensuring efficient uptake of protons in the course of proton-coupled electron transfers between organic molecules is proposed.

  • 10.
    Ghorbani Shiraz, Hamid
    et al.
    Linköping University, Department of Science and Technology, Laboratory of Organic Electronics. Linköping University, Faculty of Science & Engineering.
    Khan, Zia
    Linköping University, Department of Science and Technology, Laboratory of Organic Electronics. Linköping University, Faculty of Science & Engineering.
    Pere, Daniel
    IMRA Europe SAS, France.
    Liu, Xianjie
    Linköping University, Department of Science and Technology, Laboratory of Organic Electronics. Linköping University, Faculty of Science & Engineering.
    Coppel, Yannick
    Univ Toulouse, France.
    Fahlman, Mats
    Linköping University, Department of Science and Technology, Laboratory of Organic Electronics. Linköping University, Faculty of Science & Engineering.
    Vagin, Mikhail
    Linköping University, Department of Science and Technology, Laboratory of Organic Electronics. Linköping University, Faculty of Science & Engineering.
    Chmielowski, Radoslaw
    IMRA Europe SAS, France.
    Kahn, Myrtil L.
    Univ Toulouse, France.
    Berggren, Magnus
    Linköping University, Department of Science and Technology, Laboratory of Organic Electronics. Linköping University, Faculty of Science & Engineering.
    Crispin, Xavier
    Linköping University, Department of Science and Technology, Laboratory of Organic Electronics. Linköping University, Faculty of Science & Engineering.
    Effect of Oxygen Poisoning on the Bidirectional Hydrogen Electrocatalysis in TaS2 Nanosheets2023In: The Journal of Physical Chemistry C, ISSN 1932-7447, E-ISSN 1932-7455, Vol. 127, no 12, p. 5825-5832Article in journal (Refereed)
    Abstract [en]

    Sustainable production of hydrogen gas, a green energy carrier of high density, is possible only by electrolysis of water based on the hydrogen evolution reaction (HER). Here, we report the effect of oxygen poisoning on the efficiency of hydrogen production and the consumption by the HER and the hydrogen oxidation reaction (HOR), respectively, on the interface of platinum group metal-free electrocatalyst TaS2 in pristine form and intercalated by the organic Lewis base hexylamine. The state of the surface probed by photoelectron spectroscopy was significantly altered by both Lewis base doping and oxygen poisoning. This alteration dramatically affects the hydrogen production efficiency in the HER, while the back process by the HOR was less sensitive to the changes in the surface states of the electrocatalysts. The oxygenated and intercalated electrocatalyst shows more than 2 x 105 times lower exchange current density of the HER compared to pristine oxygenated materials.

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  • 11.
    Ghorbani Shiraz, Hamid
    et al.
    Linköping University, Department of Science and Technology, Laboratory of Organic Electronics. Linköping University, Faculty of Science & Engineering.
    Ullah Khan, Zia
    Linköping University, Department of Science and Technology, Laboratory of Organic Electronics. Linköping University, Faculty of Science & Engineering.
    Pere, Daniel
    IMRA Europe SAS, France.
    Liu, Xianjie
    Linköping University, Department of Science and Technology, Laboratory of Organic Electronics. Linköping University, Faculty of Science & Engineering.
    Coppel, Yannick
    Univ Toulouse, France.
    Fahlman, Mats
    Linköping University, Department of Science and Technology, Laboratory of Organic Electronics. Linköping University, Faculty of Science & Engineering.
    Berggren, Magnus
    Linköping University, Department of Science and Technology, Laboratory of Organic Electronics. Linköping University, Faculty of Science & Engineering.
    Chmielowski, Radoslaw
    IMRA Europe SAS, France.
    Kahn, Myrtil L.
    Univ Toulouse, France.
    Vagin, Mikhail
    Linköping University, Department of Science and Technology, Laboratory of Organic Electronics. Linköping University, Faculty of Science & Engineering.
    Crispin, Xavier
    Linköping University, Department of Science and Technology, Laboratory of Organic Electronics. Linköping University, Faculty of Science & Engineering.
    3R-TaS2 as an Intercalation-Dependent Electrified Interface for Hydrogen Reduction and Oxidation Reactions2022In: The Journal of Physical Chemistry C, ISSN 1932-7447, E-ISSN 1932-7455, Vol. 126, no 40, p. 17056-17065Article in journal (Refereed)
    Abstract [en]

    Hydrogen technology, as a future breakthrough for the energy industry, has been defined as an environmentally friendly, renewable, and high-power energy carrier. The green production of hydrogen, which mainly relies on electrocatalysts, is limited by the high cost and/ or the performance of the catalytic system. Recently, studies have been conducted in search of bifunctional electrocatalysts accelerating both the hydrogen evolution reaction (HER) and the hydrogen oxidation reaction (HOR). Herein, we report the investigation of the high efficiency bifunctional electrocatalyst TaS2 for both the HER and the HOR along with the asymmetric effect of inhibition by organic intercalation. The linear organic agent, to boost the electron donor property and to ease the process of intercalation, provides a higher interlayer gap in the tandem structure of utilized nanosheets. XRD and XPS data reveal an increase in the interlayer distance of 22%. The HER and the HOR were characterized in a Pt group metal-free electrochemical system. The pristine sample shows a low overpotential of -0.016 Vat the onset. The intercalated sample demonstrates a large shift in its performance for the HER. It is revealed that the intercalation is a potential key strategy for tuning the performance of this family of catalysts. The inhibition of the HER by intercalation is considered as the increase in the operational window of a water-based electrolyte on a negative electrode, which is relevant to technologies of electrochemical energy storage.

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  • 12.
    Ghorbani Shiraz, Hamid
    et al.
    Linköping University, Department of Science and Technology, Laboratory of Organic Electronics. Linköping University, Faculty of Science & Engineering.
    Vagin, Mikhail
    Linköping University, Department of Science and Technology, Laboratory of Organic Electronics. Linköping University, Faculty of Science & Engineering.
    Ruoko, Tero-Petri
    Linköping University, Department of Science and Technology, Laboratory of Organic Electronics. Linköping University, Faculty of Science & Engineering. Tampere Univ, Finland.
    Gueskine, Viktor
    Linköping University, Department of Science and Technology, Laboratory of Organic Electronics. Linköping University, Faculty of Science & Engineering.
    Karon, Krzysztof
    Silesian Tech Univ, Poland.
    Lapkowski, Mieczyslaw
    Silesian Tech Univ, Poland.
    Abrahamsson, Tobias
    Linköping University, Department of Science and Technology, Laboratory of Organic Electronics. Linköping University, Faculty of Science & Engineering.
    Ederth, Thomas
    Linköping University, Department of Physics, Chemistry and Biology, Biophysics and bioengineering. Linköping University, Faculty of Science & Engineering.
    Berggren, Magnus
    Linköping University, Department of Science and Technology, Laboratory of Organic Electronics. Linköping University, Faculty of Science & Engineering.
    Crispin, Xavier
    Linköping University, Department of Science and Technology, Laboratory of Organic Electronics. Linköping University, Faculty of Science & Engineering.
    Towards electrochemical hydrogen storage in liquid organic hydrogen carriers via proton-coupled electron transfers2022In: Journal of Energy Challenges and Mechanics, E-ISSN 2056-9386, Vol. 73, p. 292-300Article in journal (Refereed)
    Abstract [en]

    Green hydrogen is identified as one of the prime clean energy carriers due to its high energy density and a zero emission of CO2. A possible solution for the transport of H2 in a safe and low-cost way is in the form of liquid organic hydrogen carriers (LOHCs). As an alternative to loading LOHC with H2 via a two-step procedure involving preliminary electrolytic production of H2 and subsequent chemical hydrogenation of the LOHC, we explore here the possibility of electrochemical hydrogen storage (EHS) via conversion of proton of a proton donor into a hydrogen atom involved in covalent bonds with the LOHC (R) via a protoncoupled electron transfer (PCET) reaction: . We chose 9-fluorenone/ fluorenol (Fnone/Fnol) conversion as such a model PCET reaction. The electrochemical activation of Fnone via two sequential electron transfers was monitored with in-situ and operando spectroscopies in absence and in presence of different alcohols as proton donors of different reactivity, which enabled us to both quantify and get the mechanistic insight on PCET. The possibility of hydrogen extraction from the loaded carrier molecule was illustrated by chemical activation.

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  • 13.
    Gryszel, Maciej
    et al.
    Linköping University, Department of Science and Technology, Physics and Electronics. Linköping University, Faculty of Science & Engineering.
    Markov, Aleksandr
    Linköping University, Department of Science and Technology, Physics and Electronics. Linköping University, Faculty of Science & Engineering.
    Vagin, Mikhail
    Linköping University, Department of Science and Technology, Physics and Electronics. Linköping University, Faculty of Science & Engineering.
    Glowacki, Eric
    Linköping University, Department of Science and Technology, Physics and Electronics. Linköping University, Faculty of Science & Engineering.
    Organic heterojunction photocathodes for optimized photoelectrochemical hydrogen peroxide production2018In: Journal of Materials Chemistry A, ISSN 2050-7488, Vol. 6, no 48, p. 24709-24716Article in journal (Refereed)
    Abstract [en]

    Solar-to-chemical conversion of sunlight into hydrogen peroxide as a chemical fuel is an emerging carbon-free sustainable energy strategy. The process is based on the reduction of dissolved oxygen to hydrogen peroxide. Only limited amounts of photoelectrode materials have been successfully explored for photoelectrochemical production of hydrogen peroxide. Herein we detail approaches to produce robust organic semiconductor photocathodes for peroxide evolution. They are based on evaporated donor-acceptor heterojunctions between phthalocyanine and tetracarboxylic perylenediimide, respectively. These small molecules form nanocrystalline films with good operational stability and high surface area. We discuss critical parameters which allow fabrication of efficient devices. These photocathodes can support continuous generation of high concentrations of peroxide with faradaic efficiency remaining at around 70%. We find that an advantage of the evaporated heterojunctions is that they can be readily vertically stacked to produce tandem cells which produce higher voltages. This feature is desirable for fabricating two-electrode photoelectrochemical cells. Overall, the photocathodes presented here have the highest performance reported to date in terms of photocurrent for peroxide production. These results offer a viable method for peroxide photosynthesis and provide a roadmap of strategies that can be used to produce photoelectrodes with even higher efficiency and productivity.

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  • 14.
    Gueskine, Viktor
    et al.
    Linköping University, Department of Science and Technology, Laboratory of Organic Electronics. Linköping University, Faculty of Science & Engineering.
    Singh, Amritpal
    Linköping University, Department of Science and Technology. Linköping University, Faculty of Science & Engineering.
    Vagin, Mikhail
    Linköping University, Department of Science and Technology, Laboratory of Organic Electronics. Linköping University, Faculty of Science & Engineering.
    Crispin, Xavier
    Linköping University, Department of Science and Technology, Laboratory of Organic Electronics. Linköping University, Faculty of Science & Engineering.
    Zozoulenko, Igor
    Linköping University, Department of Science and Technology, Laboratory of Organic Electronics. Linköping University, Faculty of Science & Engineering.
    Molecular Oxygen Activation at a Conducting Polymer: Electrochemical Oxygen Reduction Reaction at PEDOT Revisited, a Theoretical Study2020In: The Journal of Physical Chemistry C, ISSN 1932-7447, E-ISSN 1932-7455, Vol. 124, no 24, p. 13263-13272Article in journal (Refereed)
    Abstract [en]

    Molecular oxygen requires activation in order to be reduced, which prompts extensive searching for efficient and sustainable electrode materials to drive electrochemical oxygen reduction reaction (ORR), of primary importance for energy production and storage. A conjugated polymer PEDOT is a metal-free material for which promising ORR experimental results have been obtained. However, sound theoretical understanding of this reaction at an organic electrode is insufficient, as the concepts inherited from electrocatalysis at transition metals are not necessarily relevant for a molecular organic material. In this work, we critically analyze the basics of electrochemical ORR and build a model for our DFT calculations of the reaction thermodynamics based on this analysis. Altogether, this work leads to a conclusion that outer sphere electron transfer that currently attracts increasing attention in the context of ORR is a viable mechanism at a conducting polymer electrode.

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  • 15.
    Gueskine, Viktor
    et al.
    Linköping University, Department of Science and Technology, Laboratory of Organic Electronics. Linköping University, Faculty of Science & Engineering.
    Vagin, Mikhail
    Linköping University, Department of Science and Technology, Laboratory of Organic Electronics. Linköping University, Faculty of Science & Engineering.
    Berggren, Magnus
    Linköping University, Department of Science and Technology, Laboratory of Organic Electronics. Linköping University, Faculty of Science & Engineering.
    Crispin, Xavier
    Linköping University, Department of Science and Technology, Laboratory of Organic Electronics. Linköping University, Faculty of Science & Engineering.
    Zozoulenko, Igor
    Linköping University, Department of Science and Technology, Laboratory of Organic Electronics. Linköping University, Faculty of Science & Engineering.
    Oxygen reduction reaction at conducting polymer electrodes in a wider context: Insights from modelling concerning outer and inner sphere mechanisms2023In: ELECTROCHEMICAL SCIENCE ADVANCES, ISSN 2698-5977, Vol. 3, no 2, article id e2100191Article, review/survey (Refereed)
    Abstract [en]

    Practical interest in oxygen reduction reaction (ORR) has traditionally been due to its application at fuel cells' cathode following its complete 4e route to the water. In search of new electrode materials, it was discovered that conducting polymers (CPs) also are capable of driving ORR, though predominantly halting the process at 2e reduction leading to hydrogen peroxide generation. As alternative ways to produce this "green oxidant" are attracting increasing attention, a detailed study of the ORR mechanism at CP electrodes gains importance. Here, we summarize our recent theoretical work on the topic, which underscores the fundamental difference between CP and electrocatalytic metal ORR electrodes. Our insights also bring to us the attention of outer-sphere electron transfer, not unknown but somewhat ignored in the field. We also put the action of CP electrodes in a more general context of chemical ORR and redox mediation responsible for the electrocatalytic ORR mechanism.

  • 16.
    Ibupoto, Zafar Hussain
    et al.
    Division of Material Science, Department of Engineering Sciences and Mathematics, Luleå University of Technology, Luleå, Sweden; Dr. M.A Kazi Institute of Chemistry University of Sindh Jamshoro, Sindh, Pakistan.
    Tahira, Aneela
    Division of Material Science, Department of Engineering Sciences and Mathematics, Luleå University of Technology, Luleå, Sweden.
    Tang, PengYi
    Catalan Institute of Nanoscience and Nanotechnology (ICN2), CSIC and BIST, Campus UAB, Bellaterra, Barcelona, Catalonia, Spain; Catalonia Institute for Energy Research (IREC), Jardins de les Dones de Negre 1, Sant Adrià del Besòs, Barcelona, Catalonia, Spain.
    Liu, Xianjie
    Linköping University, Department of Physics, Chemistry and Biology, Surface Physics and Chemistry. Linköping University, Faculty of Science & Engineering.
    Morante, Joan Ramon
    Catalonia Institute for Energy Research (IREC), Jardins de les Dones de Negre 1, Sant Adrià del Besòs, Barcelona, Catalonia, Spain.
    Fahlman, Mats
    Linköping University, Department of Physics, Chemistry and Biology, Surface Physics and Chemistry. Linköping University, Faculty of Science & Engineering.
    Arbiol, Jordi
    Catalan Institute of Nanoscience and Nanotechnology (ICN2), CSIC and BIST, Campus UAB, Bellaterra, Barcelona, Catalonia, Spain; ICREA, Pg. Lluís Companys 23, Barcelona, Catalonia, Spain.
    Vagin, Mikhail
    Linköping University, Department of Science and Technology, Laboratory of Organic Electronics. Linköping University, Faculty of Science & Engineering.
    Vomiero, Alberto
    Division of Material Science, Department of Engineering Sciences and Mathematics, Luleå University of Technology, Luleå, Sweden.
    MoSx@NiO Composite Nanostructures: An Advanced Nonprecious Catalyst for Hydrogen Evolution Reaction in Alkaline Media2019In: Advanced Functional Materials, ISSN 1616-301X, E-ISSN 1616-3028, Vol. 29, no 7, article id 1807562Article in journal (Refereed)
    Abstract [en]

    The design of the earth-abundant, nonprecious, efficient, and stable electrocatalysts for efficient hydrogen evolution reaction (HER) in alkaline media is a hot research topic in the field of renewable energies. A heterostructured system composed of MoSx deposited on NiO nanostructures (MoSx@NiO) as a robust catalyst for water splitting is proposed here. NiO nanosponges are applied as cocatalyst for MoS2 in alkaline media. Both NiO and MoS2@NiO composites are prepared by a hydrothermal method. The NiO nanostructures exhibit sponge-like morphology and are completely covered by the sheet-like MoS2. The NiO and MoS2 exhibit cubic and hexagonal phases, respectively. In the MoSx@NiO composite, the HER experiment in 1 m KOH electrolyte results in a low overpotential (406 mV) to produce 10 mA cm(-2) current density. The Tafel slope for that case is 43 mV per decade, which is the lowest ever achieved for MoS2-based electrocatalyst in alkaline media. The catalyst is highly stable for at least 13 h, with no decrease in the current density. This simple, cost-effective, and environmentally friendly methodology can pave the way for exploitation of MoSx@NiO composite catalysts not only for water splitting, but also for other applications such as lithium ion batteries, and fuel cells.

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  • 17.
    Imar, Shahzad
    et al.
    Dundalk Institute Technology, Ireland.
    Maccato, Chiara
    University of Padua, Italy.
    Dickinson, Calum
    University of Limerick, Ireland.
    Laffir, Fathima
    University of Limerick, Ireland.
    Vagin, Mikhail
    Linköping University, Department of Physics, Chemistry and Biology, Chemical and Optical Sensor Systems. Linköping University, The Institute of Technology.
    McCormac, Timothy
    Dundalk Institute Technology, Ireland.
    Enhancement of Nitrite and Nitrate Electrocatalytic Reduction through the Employment of Self-Assembled Layers of Nickel- and Copper-Substituted Crown-Type Heteropolyanions2015In: Langmuir, ISSN 0743-7463, E-ISSN 1520-5827, Vol. 31, no 8, p. 2584-2592Article in journal (Refereed)
    Abstract [en]

    Multilayer assemblies of two crown-type type heteropolyanions (HPA), [Cu20Cl(OH)(24)(H2O)(12)(P8W48O184)](25-) and Ni-4(P8W48O148)(WO2)](28-), have been immobilized onto glassy carbon electrode surfaces via the layer-by-layer (LBL) technique employing polycathion-stabilized silver nanoparticles (AgNP) as the cationic layer within the resulting thin films characterized by electrochemical and physical methods. The redox behaviors of both HPA monitored during LBL assembly with cyclic voltammetry and impedance spectroscopy revealed significant changes by immobilization. The presence of AgNPs led to the retention of film porosity and electronic conductivity, which has been shown with impedance and voltammeric studies of film permeabilities toward reversible redox probes. The resulting films have been characterized by physical methods. Finally, the electrocatalytic performance of obtained films with respect to nitrite and nitrate electrocatalytic reduction has been comparatively studied for both catalysts. Nickel atoms trapped inside HPA exhibited a higher specific activity for reduction.

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  • 18.
    Imar, Shahzad
    et al.
    Dundalk Institute Technology, Ireland.
    Yaqub, Mustansara
    Dundalk Institute Technology, Ireland.
    Maccato, Chiara
    University of Padua, Italy.
    Dickinson, Calum
    University of Limerick, Ireland.
    Laffir, Fathima
    University of Limerick, Ireland.
    Vagin, Mikhail
    Linköping University, Department of Science and Technology, Physics and Electronics. Linköping University, Faculty of Science & Engineering.
    McCormac, Timothy
    Dundalk Institute Technology, Ireland.
    Nitrate and Nitrite Electrocatalytic Reduction at Layer-by-Layer Films Composed of Dawson-type Heteropolyanions Mono-substituted with Transitional Metal Ions and Silver Nanoparticles2015In: Electrochimica Acta, ISSN 0013-4686, E-ISSN 1873-3859, Vol. 184, p. 323-330Article in journal (Refereed)
    Abstract [en]

    A series of Dawson-type heteropolyanions (HPAs) mono-substituted with transitional metal ions ((alpha 2)- [P2W17O61FeIII](8-), (alpha 2)-[P2W17O61CuII](8-) and (alpha 2)-[P2W17O61NiII](8-)) have exhibited electrocatalytic properties towards nitrate and nitrite reduction in slightly acidic media (pH 4.5). The immobilization of these HPAs into water-processable films developed via layer-by layer assembly with polymer-stabilized silver nanoparticles led to the fabrication of the electrocatalytic interfaces for both nitrate and nitrite reduction. The LBL assembly as well as the changes in the HPA properties by immobilization has been characterized by electrochemical methods. The effects of the substituent ions, outer layers and the cationic moieties utilized for the films assembly of the developed film on the performances of nitrate electrocatalysis has been elucidated. (C) 2015 Elsevier Ltd. All rights reserved.

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  • 19.
    Kangkamano, Tawatchai
    et al.
    Linköping University, Department of Physics, Chemistry and Biology, Sensor and Actuator Systems. Linköping University, Faculty of Science & Engineering. Prince Songkla Univ, Thailand; Thaksin Univ, Thailand.
    Vagin, Mikhail
    Linköping University, Department of Science and Technology, Laboratory of Organic Electronics. Linköping University, Faculty of Science & Engineering.
    Meng, Lingyin
    Linköping University, Department of Physics, Chemistry and Biology, Sensor and Actuator Systems. Linköping University, Faculty of Science & Engineering.
    Thavarungkul, Panote
    Prince Songkla Univ, Thailand.
    Kanatharana, Proespichaya
    Prince Songkla Univ, Thailand.
    Crispin, Xavier
    Linköping University, Department of Science and Technology, Laboratory of Organic Electronics. Linköping University, Faculty of Science & Engineering.
    Mak, Wing Cheung
    Linköping University, Department of Physics, Chemistry and Biology, Sensor and Actuator Systems. Linköping University, Faculty of Science & Engineering.
    Product-to-intermediate relay achieving complete oxygen reduction reaction (cORR) with Prussian blue integrated nanoporous polymer cathode in fuel cells2020In: Nano Energy, ISSN 2211-2855, E-ISSN 2211-3282, Vol. 78, article id 105125Article in journal (Refereed)
    Abstract [en]

    The oxygen reduction reaction (ORR) is an essential process in electrocatalysis limiting the commercialization of sustainable energy conversion technologies, such as fuel cells. The use of conducting polymers as molecular porous and conducting catalysts obtained from the high abundance elements enables the route towards low cost and high-throughput fabrication of disposable plastic electrodes of fuel cells. Poly(3,4-ethylenedioxythiophene) (PEDOT) is a 2-electron ORR electrocatalyst yielding specifically hydrogen peroxide that limits the full utilization of chemical energy of oxygen. Here, we demonstrated an innovative product-to-intermediate relay approach achieving complete oxygen reduction reaction (cORR) with Prussian blue (PB) integrated microporous PEDOT cathode in fuel cells. The microporous structured PEDOT electrode prepared via a simple cryosynthesis allows the bulk integration and stabilization of the poor conducting PB co-catalyst into the PEDOT ion-electron conductor, while the microporous PEDOT allows effective oxygen diffusion into the matrix. We evaluated systematically the effect of sequential PEDOT 2-electron ORR followed by PB co-catalysis launching hydrogen peroxide reduction reaction (HPRR) into H2O. This resulted in the establishment of electronic and ionic transport between PEDOT and PB catalyst enabling the combination of enhanced ORR electrocatalysis by means of the ORR course extension from 2to 4-electron reduction to achieve cORR. The cORR performance delivered by the product-to-intermediate relay between microporous PEDOT and PB co-catalysis led to a four times increase in power density of model proton-exchange membrane fuel cell (PEMFC) assembled from the polymer-based air breathing cathode.

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  • 20.
    Karimian, Najmeh
    et al.
    Linköping University, Department of Physics, Chemistry and Biology, Biosensors and Bioelectronics. Linköping University, The Institute of Technology. Ferdowsi University of Mashhad, Iran.
    Vagin, Mikhail
    Linköping University, Department of Physics, Chemistry and Biology, Applied Physics. Linköping University, The Institute of Technology.
    Hossein Arbab Zavar, Mohammad
    Ferdowsi University of Mashhad, Iran .
    Chamsaz, Mahmoud
    Ferdowsi University of Mashhad, Iran .
    Turner, Anthony
    Linköping University, Department of Physics, Chemistry and Biology, Biosensors and Bioelectronics. Linköping University, The Institute of Technology.
    Tiwari, Ashutosh
    Linköping University, Department of Physics, Chemistry and Biology, Biosensors and Bioelectronics. Linköping University, The Institute of Technology.
    An ultrasensitive molecularly-imprinted human cardiac troponin sensor2013In: Biosensors & bioelectronics, ISSN 0956-5663, E-ISSN 1873-4235, Vol. 50, p. 492-498Article in journal (Refereed)
    Abstract [en]

    Cardiac troponin T (TnT) is a highly sensitive cardiac biomarker for myocardial infarction. In this study, the fabrication and characterisation of a novel sensor for human TnT based on a molecularly-imprinted electrosynthesised polymer is reported. A TnT sensitive layer was prepared by electropolymerisation of o-phenylenediamine (o-PD) on a gold electrode in the presence of TnT as a template. To develop the molecularly imprinted polymer (MIP), the template molecules were removed from the modified electrode surface by washing with alkaline ethanol. Electrochemical methods were used to monitor the processes of electropolymerisation, template removal and binding. The imprinted layer was characterised by cyclic voltammetry (CV), electrochemical impedance spectroscopy (EIS) and atomic force microscopy (AFM). The incubation of the MIP-modified electrode with respect to TnT concentration resulted in a suppression of the ferro/ferricyanide redox process. Experimental conditions were optimised and a linear relationship was observed between the peak current of [Fe(CN)(6)](3-)/[Fe (CN)(6)](4-) and the concentration of TnT in buffer over the range 0.009-0.8 ng/mL, with a detection limit of 9 pg/mL. The TnT MIP sensor was shown to have a high affinity to TnT in comparison with nonimprinted polymer (NIP) electrodes in both buffer and blood serum.

  • 21.
    Khan, Ziyauddin
    et al.
    Linköping University, Department of Science and Technology, Laboratory of Organic Electronics. Linköping University, Faculty of Science & Engineering.
    Vagin, Mikhail
    Linköping University, Department of Science and Technology, Laboratory of Organic Electronics. Linköping University, Faculty of Science & Engineering.
    Crispin, Xavier
    Linköping University, Department of Science and Technology, Laboratory of Organic Electronics. Linköping University, Faculty of Science & Engineering.
    Can Hybrid Na-Air Batteries Outperform Nonaqueous Na-O-2 Batteries?2020In: Advanced Science, E-ISSN 2198-3844, Vol. 7, no 5, article id 1902866Article in journal (Refereed)
    Abstract [en]

    In recent years, there has been an upsurge in the study of novel and alternative energy storage devices beyond lithium-based systems due to the exponential increase in price of lithium. Sodium (Na) metal-based batteries can be a possible alternative to lithium-based batteries due to the similar electrochemical voltage of Na and Li together with the thousand times higher natural abundance of Na compared to Li. Though two different kinds of Na-O-2 batteries have been studied specifically based on electrolytes until now, very recently, a hybrid Na-air cell has shown distinctive advantage over nonaqueous cell systems. Hybrid Na-air batteries provide a fundamental advantage due to the formation of highly soluble discharge product (sodium hydroxide) which leads to low overpotentials for charge and discharge processes, high electrical energy efficiency, and good cyclic stability. Herein, the current status and challenges associated with hybrid Na-air batteries are reported. Also, a brief description of nonaqueous Na-O-2 batteries and its close competition with hybrid Na-air batteries are provided.

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  • 22.
    Kim, Nara
    et al.
    Linköping University, Department of Science and Technology, Laboratory of Organic Electronics. Linköping University, Faculty of Science & Engineering.
    Lienemann, Samuel
    Linköping University, Department of Science and Technology, Laboratory of Organic Electronics. Linköping University, Faculty of Science & Engineering.
    Khan, Ziyauddin
    Linköping University, Department of Science and Technology, Laboratory of Organic Electronics. Linköping University, Faculty of Medicine and Health Sciences.
    Greczynski, Grzegorz
    Linköping University, Department of Physics, Chemistry and Biology, Thin Film Physics. Linköping University, Faculty of Science & Engineering.
    Rahmanudin, Aiman
    Linköping University, Department of Science and Technology, Laboratory of Organic Electronics. Linköping University, Faculty of Science & Engineering.
    Vagin, Mikhail
    Linköping University, Department of Science and Technology, Laboratory of Organic Electronics. Linköping University, Faculty of Science & Engineering.
    Ahmed, Fareed
    Linköping University, Department of Science and Technology, Laboratory of Organic Electronics. Linköping University, Faculty of Science & Engineering.
    Petsagkourakis, Ioannis
    Linköping University, Department of Science and Technology, Laboratory of Organic Electronics. Linköping University, Faculty of Science & Engineering.
    Edberg, Jesper
    Linköping University, Department of Science and Technology, Laboratory of Organic Electronics. Linköping University, Faculty of Medicine and Health Sciences.
    Crispin, Xavier
    Linköping University, Department of Science and Technology, Laboratory of Organic Electronics. Linköping University, Faculty of Science & Engineering.
    Tybrandt, Klas
    Linköping University, Department of Science and Technology, Laboratory of Organic Electronics. Linköping University, Faculty of Science & Engineering.
    An intrinsically stretchable symmetric organic battery based on plant-derived redox molecules2023In: Journal of Materials Chemistry A, ISSN 2050-7488, E-ISSN 2050-7496, Vol. 11, no 46, p. 25703-25714Article in journal (Refereed)
    Abstract [en]

    Intrinsically stretchable energy storage devices are essential for the powering of imperceptible wearable electronics. Organic batteries based on plant-derived redox-active molecules can offer critical advantages from a safety, sustainability, and economic perspective, but such batteries are not yet available in soft and stretchable form factors. Here we report an intrinsically stretchable organic battery made of elastomeric composite electrodes formulated with alizarin, a natural dye derived from the plant Rubia tinctorum, whose two quinone motifs enable its uses in both positive and negative electrodes. The quaternary biocomposite electrodes possess excellent electron-ion conduction/coupling and superior stretchability (>300%) owing to self-organized hierarchical morphology. In a full-cell configuration, its energy density of 3.8 mW h cm(-3) was preserved at 100% strain, and assembled modules on stretchy textiles and rubber gloves can power integrated LEDs during various deformations. This work paves the way for low-cost, eco-friendly, and deformable batteries for next generation wearable electronics.

  • 23.
    Lander, Sanna
    et al.
    Linköping University, Department of Science and Technology, Laboratory of Organic Electronics. Linköping University, Faculty of Science & Engineering. BillerudKorsnas Gruvon, Sweden.
    Erlandsson, Johan
    KTH Royal Inst Technol, Sweden.
    Vagin, Mikhail
    Linköping University, Department of Science and Technology, Laboratory of Organic Electronics. Linköping University, Faculty of Science & Engineering.
    Gueskine, Viktor
    Linköping University, Department of Science and Technology, Laboratory of Organic Electronics. Linköping University, Faculty of Science & Engineering.
    Korhonen, Leena
    BillerudKorsnas Frovi, Sweden.
    Berggren, Magnus
    Linköping University, Department of Science and Technology, Laboratory of Organic Electronics. Linköping University, Faculty of Science & Engineering. KTH Royal Inst Technol, Sweden.
    Wågberg, Lars
    KTH Royal Inst Technol, Sweden; KTH Royal Inst Technol, Sweden.
    Crispin, Xavier
    Linköping University, Department of Science and Technology, Laboratory of Organic Electronics. Linköping University, Faculty of Science & Engineering. KTH Royal Inst Technol, Sweden.
    Sulfonated Cellulose Membranes: Physicochemical Properties and Ionic Transport versus Degree of Sulfonation2022In: Advanced Sustainable Systems, ISSN 2366-7486, Vol. 6, no 11, article id 2200275Article in journal (Refereed)
    Abstract [en]

    The next generation of green ion selective membranes is foreseen to be based on cellulosic nanomaterials with controllable properties. The introduction of ionic groups into the cellulose structure via chemical modification is one strategy to obtain desired functionalities. In this work, bleached softwood fibers are oxidatively sulfonated and thereafter homogenized to liberate the cellulose nanofibrils (CNFs) from the fiber walls. The liberated CNFs are subsequently used to prepare and characterize novel cellulose membranes. It is found that the degree of sulfonation collectively affects several important properties of the membranes via the density of fixed charged groups on the surfaces of the CNFs, in particular the membrane morphology, water uptake and swelling, and correspondingly the ionic transport. Both ionic conductivity and cation transport increase with the increased level of sulfonation of the starting material. Thus, it is shown that the chemical modification of the CNFs can be used as a tool for precise and rational design of green ion selective membranes that can replace expensive conventional fluorinated ionomer membranes.

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  • 24.
    Lander, Sanna
    et al.
    Linköping University, Department of Science and Technology, Laboratory of Organic Electronics. Linköping University, Faculty of Science & Engineering. BillerudKorsnas Gruvon, Sweden.
    Vagin, Mikhail
    Linköping University, Department of Science and Technology, Laboratory of Organic Electronics. Linköping University, Faculty of Science & Engineering.
    Gueskine, Viktor
    Linköping University, Department of Science and Technology, Laboratory of Organic Electronics. Linköping University, Faculty of Science & Engineering.
    Erlandsson, Johan
    KTH Royal Inst Technol, Sweden.
    Boissard, Yselaure
    BillerudKorsnas Frovi, Sweden.
    Korhonen, Leena
    BillerudKorsnas Frovi, Sweden.
    Berggren, Magnus
    Linköping University, Department of Science and Technology, Laboratory of Organic Electronics. Linköping University, Faculty of Science & Engineering. KTH Royal Inst Technol, Sweden.
    Wagberg, Lars
    KTH Royal Inst Technol, Sweden; KTH Royal Inst Technol, Sweden.
    Crispin, Xavier
    Linköping University, Department of Science and Technology, Laboratory of Organic Electronics. Linköping University, Faculty of Science & Engineering. KTH Royal Inst Technol, Sweden.
    Sulfonated Cellulose Membranes Improve the Stability of Aqueous Organic Redox Flow Batteries2022In: Advanced Energy and Sustainability Research, ISSN 2699-9412, Vol. 3, no 9, article id 2200016Article in journal (Refereed)
    Abstract [en]

    The drawbacks of current state-of-the-art selective membranes, such as poor barrier properties, high cost, and poor recyclability, limit the large-scale deployment of electrochemical energy devices such as redox flow batteries (RFBs) and fuel cells. In recent years, cellulosic nanomaterials have been proposed as a low-cost and green raw material for such membranes, but their performance in RFBs and fuel cells is typically poorer than that of the sulfonated fluoropolymer ionomer membranes such as Nafion. Herein, sulfonated cellulose nanofibrils densely cross-linked to form a compact sulfonated cellulose membrane with limited swelling and good stability in water are used. The membranes possess low porosity and excellent ionic transport properties. A model aqueous organic redox flow battery (AORFB) with alizarin red S as negolyte and tiron as posolyte is assembled with the sulfonated cellulose membrane. The performance of the nanocellulose-based battery is superior in terms of cyclability in comparison to that displayed by the battery assembled with commercially available Nafion 115 due to the mitigation of crossover of the redox-active components. This finding paves the way to new green organic materials for fully sustainable AORFB solutions.

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  • 25.
    Mitraka, Evangelia
    et al.
    Linköping University, Department of Science and Technology, Laboratory of Organic Electronics. Linköping University, Faculty of Science & Engineering.
    Gryszel, Maciej
    Linköping University, Department of Science and Technology, Laboratory of Organic Electronics. Linköping University, Faculty of Science & Engineering.
    Vagin, Mikhail
    Linköping University, Department of Science and Technology, Laboratory of Organic Electronics. Linköping University, Faculty of Science & Engineering.
    Jafari, Mohammad Javad
    Linköping University, Department of Physics, Chemistry and Biology, Molecular Physics. Linköping University, Faculty of Science & Engineering.
    Singh, Amritpal
    Linköping University, Department of Science and Technology, Laboratory of Organic Electronics. Linköping University, Faculty of Science & Engineering.
    Warczak, Magdalena
    Linköping University, Department of Science and Technology, Laboratory of Organic Electronics. Linköping University, Faculty of Science & Engineering.
    Mitrakas, Manassis
    Aristotle University of Thessaloniki, Thessaloniki, Greece.
    Berggren, Magnus
    Linköping University, Department of Science and Technology, Laboratory of Organic Electronics. Linköping University, Faculty of Science & Engineering.
    Ederth, Thomas
    Linköping University, Department of Physics, Chemistry and Biology, Molecular Physics. Linköping University, Faculty of Science & Engineering.
    Zozoulenko, Igor
    Linköping University, Department of Science and Technology, Laboratory of Organic Electronics. Linköping University, Faculty of Science & Engineering.
    Crispin, Xavier
    Linköping University, Department of Science and Technology, Laboratory of Organic Electronics. Linköping University, Faculty of Science & Engineering.
    Glowacki, Eric
    Linköping University, Department of Science and Technology, Laboratory of Organic Electronics. Linköping University, Faculty of Science & Engineering.
    Electrocatalytic Production of Hydrogen Peroxide with Poly(3,4-ethylenedioxythiophene) Electrodes2019In: Advanced Sustainable Systems, ISSN 2366-7486, Vol. 3, no 2, p. 1-6, article id 1800110Article in journal (Refereed)
    Abstract [en]

    Electrocatalysis for energy‐efficient chemical transformations is a central concept behind sustainable technologies. Numerous efforts focus on synthesizing hydrogen peroxide, a major industrial chemical and potential fuel, using simple and green methods. Electrochemical synthesis of peroxide is a promising route. Herein it is demonstrated that the conducting polymer poly(3,4‐ethylenedioxythiophene), PEDOT, is an efficient and selective heterogeneous catalyst for the direct reduction of oxygen to hydrogen peroxide. While many metallic catalysts are known to generate peroxide, they subsequently catalyze decomposition of peroxide to water. PEDOT electrodes can support continuous generation of high concentrations of peroxide with Faraday efficiency remaining close to 100%. The mechanisms of PEDOT‐catalyzed reduction of O2 to H2O2 using in situ spectroscopic techniques and theoretical calculations, which both corroborate the existence of a chemisorbed reactive intermediate on the polymer chains that kinetically favors the selective reduction reaction to H2O2, are explored. These results offer a viable method for peroxide electrosynthesis and open new possibilities for intrinsic catalytic properties of conducting polymers.

  • 26.
    Mitraka, Evangelia
    et al.
    Linköping University, Department of Science and Technology, Physics and Electronics. Linköping University, Faculty of Science & Engineering.
    Jafari, Mohammad Javad
    Linköping University, Department of Physics, Chemistry and Biology, Molecular Physics. Linköping University, Faculty of Science & Engineering.
    Vagin, Mikhail
    Linköping University, Department of Science and Technology, Physics and Electronics. Linköping University, Faculty of Science & Engineering.
    Liu, Xianjie
    Linköping University, Department of Physics, Chemistry and Biology, Surface Physics and Chemistry. Linköping University, Faculty of Science & Engineering.
    Fahlman, Mats
    Linköping University, Department of Physics, Chemistry and Biology, Surface Physics and Chemistry. Linköping University, Faculty of Science & Engineering.
    Ederth, Thomas
    Linköping University, Department of Physics, Chemistry and Biology, Molecular Physics. Linköping University, Faculty of Science & Engineering.
    Berggren, Magnus
    Linköping University, Department of Science and Technology, Physics and Electronics. Linköping University, Faculty of Science & Engineering.
    Jonsson, Magnus
    Linköping University, Department of Science and Technology, Physics and Electronics. Linköping University, Faculty of Science & Engineering.
    Crispin, Xavier
    Linköping University, Department of Science and Technology, Physics and Electronics. Linköping University, Faculty of Science & Engineering.
    Oxygen-induced doping on reduced PEDOT2017In: Journal of Materials Chemistry A, ISSN 2050-7488, Vol. 5, no 9, p. 4404-4412Article in journal (Refereed)
    Abstract [en]

    The conducting polymer poly(3,4-ethylenedioxythiophene) (PEDOT) has shown promise as air electrode in renewable energy technologies like metal-air batteries and fuel cells. PEDOT is based on atomic elements of high abundance and is synthesized at low temperature from solution. The mechanism of oxygen reduction reaction (ORR) over chemically polymerized PEDOT: Cl still remains controversial with eventual role of transition metal impurities. However, regardless of the mechanistic route, we here demonstrate yet another key active role of PEDOT in the ORR mechanism. Our study demonstrates the decoupling of conductivity (intrinsic property) from electrocatalysis (as an extrinsic phenomenon) yielding the evidence of doping of the polymer by oxygen during ORR. Hence, the PEDOT electrode is electrochemically reduced (undoped) in the voltage range of ORR regime, but O-2 keeps it conducting; ensuring PEDOT to act as an electrode for the ORR. The interaction of oxygen with the polymer electrode is investigated with a battery of spectroscopic techniques.

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  • 27.
    Mitraka, Evangelia
    et al.
    Linköping University, Department of Science and Technology, Laboratory of Organic Electronics. Linköping University, Faculty of Science & Engineering.
    Vagin, Mikhail
    Linköping University, Department of Science and Technology, Laboratory of Organic Electronics. Linköping University, Faculty of Science & Engineering.
    Sjoestedt, Anna
    RISE Bioecon, Sweden.
    Berggren, Magnus
    Linköping University, Department of Science and Technology, Laboratory of Organic Electronics. Linköping University, Faculty of Science & Engineering.
    Hakansson, Karl M. O.
    RISE Bioecon, Sweden.
    Jonsson, Magnus
    Linköping University, Department of Science and Technology, Laboratory of Organic Electronics. Linköping University, Faculty of Science & Engineering.
    Crispin, Xavier
    Linköping University, Department of Science and Technology, Laboratory of Organic Electronics. Linköping University, Faculty of Science & Engineering.
    PEDOT-Cellulose Gas Diffusion Electrodes for Disposable Fuel CellsIn: ADVANCED SUSTAINABLE SYSTEMS, ISSN 2366-7486, article id 1900097Article in journal (Refereed)
    Abstract [en]

    The mass implementation of renewable energy sources is limited by the lack of energy storage solutions operating on various timescales. Electrochemical technologies such as supercapacitors and batteries cannot handle long storage time because of self-discharge issues. The combination of fuel storage technology and fuel cells is an attractive solution for long storage times. In that context, large-scale fuel cell solutions are required for massive energy storage in cities, which leads to possible concepts such as low-cost disposable fully organic membrane assemblies in fuel cells to avoid regeneration of expensive poisoned electrodes. Here, the formation of an organic gas diffusion electrode (GDE) fabricated by paper-making production, combined with in situ polymerization is demonstrated for the first time. Cellulose is used as a 3D scaffold functionalized with poly(3,4-ethylenedioxythiophene) (PEDOT) serving as both an electrical conductor and an electrocatalyst of high efficiency for the oxygen reduction reaction. The PEDOT-cellulose porous GDE is implemented in a membrane assembly and demonstrated in a H-2-O-2 fuel cell. The demonstration of low-cost material/manufacturing that is environmentally friendly is a paradigm shift in the development of fuel cells for a sustainable society.

  • 28.
    Musumeci, Chiara
    et al.
    Linköping University, Department of Science and Technology, Physics and Electronics. Linköping University, Faculty of Science & Engineering.
    Vagin, Mikhail
    Linköping University, Department of Science and Technology, Physics and Electronics. Linköping University, Faculty of Science & Engineering.
    Zeglio, Erica
    Linköping University, Department of Physics, Chemistry and Biology, Biomolecular and Organic Electronics. Linköping University, Faculty of Science & Engineering.
    Ouyang, Liangqi
    Linköping University, Department of Physics, Chemistry and Biology, Biomolecular and Organic Electronics. Linköping University, Faculty of Science & Engineering.
    Gabrielsson, Roger
    Linköping University, Department of Science and Technology, Physics and Electronics. Linköping University, Faculty of Science & Engineering.
    Inganäs, Olle
    Linköping University, Department of Physics, Chemistry and Biology, Biomolecular and Organic Electronics. Linköping University, Faculty of Science & Engineering.
    Organic electrochemical transistors from supramolecular complexes of conjugated polyelectrolyte PEDOTS2019In: Journal of Materials Chemistry C, ISSN 2050-7526, E-ISSN 2050-7534, Vol. 7, no 10, p. 2987-2993Article in journal (Refereed)
    Abstract [en]

    Counterion exchange strategies are used to modify the hydrophilic character of the self-doped conjugated polyelectrolyte PEDOTS. The supramolecular complexes, soluble in organic solvents, are suitable to fabricate finely performing thin active layers in organic electrochemical transistors (OECTs). We demonstrate that ionic transport in these PEDOTS based complexes, thus their performance in OECT devices, is governed by a delicate balance among degree of doping, wettability and porosity, which can be controlled by a precise tuning of the polyelectrolyte/hydrophobic counterion ratio. We also show that the device operation can be modulated by varying the composition of the aqueous electrolyte in a range compatible with biological processes, making these materials suitable candidates to be interfaced with living cells.

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  • 29.
    Méhes, Gábor
    et al.
    Linköping University, Department of Science and Technology, Laboratory of Organic Electronics. Linköping University, Faculty of Science & Engineering.
    Vagin, Mikhail
    Linköping University, Department of Science and Technology, Laboratory of Organic Electronics. Linköping University, Faculty of Science & Engineering.
    Mulla, Yusuf
    Linköping University, Department of Science and Technology, Laboratory of Organic Electronics. Linköping University, Faculty of Science & Engineering.
    Granberg, Hjalmar
    Res Inst Sweden, Sweden.
    Che, Canyan
    Linköping University, Department of Science and Technology, Laboratory of Organic Electronics. Linköping University, Faculty of Science & Engineering.
    Beni, Valerio
    Res Inst Sweden, Sweden.
    Crispin, Xavier
    Linköping University, Department of Science and Technology, Laboratory of Organic Electronics. Linköping University, Faculty of Science & Engineering.
    Berggren, Magnus
    Linköping University, Department of Science and Technology, Laboratory of Organic Electronics. Linköping University, Faculty of Science & Engineering.
    Stavrinidou, Eleni
    Linköping University, Department of Science and Technology, Laboratory of Organic Electronics. Linköping University, Faculty of Science & Engineering.
    Simon, Daniel
    Linköping University, Department of Science and Technology, Laboratory of Organic Electronics. Linköping University, Faculty of Science & Engineering.
    Solar Heat-Enhanced Energy Conversion in Devices Based on Photosynthetic Membranes and PEDOT:PSS-Nanocellulose Electrodes2020In: ADVANCED SUSTAINABLE SYSTEMS, ISSN 2366-7486, Vol. 4, no 1, article id 1900100Article in journal (Refereed)
    Abstract [en]

    Energy harvesting from photosynthetic membranes, proteins, or bacteria through bio-photovoltaic or bio-electrochemical approaches has been proposed as a new route to clean energy. A major shortcoming of these and solar cell technologies is the underutilization of solar irradiation wavelengths in the IR region, especially those in the far IR region. Here, a biohybrid energy-harvesting device is demonstrated that exploits IR radiation, via convection and thermoelectric effects, to improve the resulting energy conversion performance. A composite of nanocellulose and the conducting polymer system poly(3,4-ethylenedioxythiophene):polystyrene sulfonate (PEDOT:PSS) is used as the anode in biohybrid cells that includes thylakoid membranes (TMs) and redox mediators (RMs) in solution. By irradiating the conducting polymer electrode by an IR light-emitting diode, a sixfold enhancement in the harvested bio-photovoltaic power is achieved, without compromising stability of operation. Investigation of the output currents reveals that IR irradiation generates convective heat transfer in the electrolyte bulk, which enhances the redox reactions of RMs at the anode by suppressing diffusion limitations. In addition, a fast-transient thermoelectric component, originating from the PEDOT:PSS-nanocellulose-electrolyte interphase, further increases the bio-photocurrent. These results pave the way for the development of energy-harvesting biohybrids that make use of heat, via IR absorption, to enhance energy conversion efficiency.

  • 30.
    Naseer, Rashda
    et al.
    Dundalk Institute Technology, Ireland .
    Sankar Mal, Sib
    Jacobs University, Bremen, Germany .
    Ibrahim, Masooma
    Jacobs University, Bremen, Germany .
    Kortz, Ulrich
    Jacobs University, Bremen, Germany .
    Armstrong, Gordon
    University of Limerick, Ireland .
    Laffir, Fathima
    University of Limerick, Ireland .
    Dickinson, Calum
    University of Limerick, Ireland .
    Vagin, Mikhail
    Linköping University, Department of Physics, Chemistry and Biology, Chemical and Optical Sensor Systems. Linköping University, The Institute of Technology.
    McCormac, Timothy
    Dundalk Institute Technology, Ireland .
    Redox, surface and electrocatalytic properties of layer-by-layer films based upon Fe(III)-substituted crown polyoxometalate [P8W48O184Fe16(OH)(28)(H2O)(4)](20-)2014In: Electrochimica Acta, ISSN 0013-4686, E-ISSN 1873-3859, Vol. 134, p. 450-458Article in journal (Refereed)
    Abstract [en]

    The electrocatalytic ability of the iron-substituted crown-type polyoxometalate (POM) Li4K16[P8W48O184Fe16(OH)(28)(H2O)(4)]center dot 66H(2)O center dot 2KCl (P8W48Fe16) towards the reduction of both nitrite and hydrogen peroxide reduction has been studied in both the solution and immobilized states for the POM. P8W48Fe16 was surface immobilised onto carbon electrode surfaces through employment of the layer-by-layer technique (LBL) using pentaerythritol-based Ru(II)-metallodendrimer [RuD](PF6)(8) as the cationic layer within the resulting films. The constructed multilayer films have been extensively studied by various electrochemical techniques and surface based techniques. Cyclic voltammetry and impedance spectroscopy have been utilized to monitor the construction of the LBL film after the deposition of each monolayer. The electrochemical behaviour of both a cationic and anionic redox probes at the LBL films has been undertaken to give indications as to the films porosity. The elemental composition and the surface morphology of the LBL films was conifmrde through the employment of AFM, XPS and SEM.

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  • 31.
    Naseer, Rashda
    et al.
    Dundalk Institute Technology, Ireland.
    Sankar Mal, Sib
    Jacobs University of Bremen, Germany.
    Kortz, Ulrich
    Jacobs University of Bremen, Germany.
    Armstrong, Gordon
    University of Limerick, Ireland.
    Laffir, Fathima
    University of Limerick, Ireland.
    Dickinson, Calum
    University of Limerick, Ireland.
    Vagin, Mikhail
    Linköping University, Department of Science and Technology, Physics and Electronics. Linköping University, Faculty of Science & Engineering.
    McCormac, Timothy
    Dundalk Institute Technology, Ireland.
    Electrocatalysis by crown-type polyoxometalates multi-substituted by transition metal ions: Comparative study2015In: Electrochimica Acta, ISSN 0013-4686, E-ISSN 1873-3859, Vol. 176, p. 1248-1255Article in journal (Refereed)
    Abstract [en]

    The difference in electrochemical properties of three crown-type polyoxometalates multi-substituted by Fe3+, Ni2+ or Co2+ ions and their precursor has been rationalized with respect to their electrocatalytic performances studied in solution and in the immobilized state within the layer-by-layer film formed with a positively charged pentaerythritol-based Ru(II)-metallodendrimer. The film assembly was monitored with electrochemical methods and characterized by surface analysis techniques. An influence of the terminal layer on the electrode reaction and on film porosity has been observed. The electrocatalytic performance of the compounds on nitrite reduction was assessed in solution and in the immobilized state. (C) 2015 Elsevier Ltd. All rights reserved.

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  • 32.
    Pozhitkov, Alex E.
    et al.
    University of Washington, WA 98195 USA.
    Daubert, Diane
    University of Washington, WA 98195 USA.
    Brochwicz Donimirski, Ashley
    University of Washington, WA 98195 USA.
    Goodgion, Douglas
    University of Washington, WA 98195 USA.
    Vagin, Mikhail
    Linköping University, Department of Science and Technology, Physics and Electronics. Linköping University, Faculty of Science & Engineering.
    Leroux, Brian G.
    University of Washington, WA 98195 USA.
    Hunter, Colby M.
    Alabama State University, AL 36101 USA.
    Flemmig, Thomas F.
    University of Hong Kong, Peoples R China.
    Noble, Peter A.
    Alabama State University, AL 36101 USA.
    Bryers, James D.
    University of Washington, WA 98195 USA.
    Interruption of Electrical Conductivity of Titanium Dental Implants Suggests a Path Towards Elimination Of Corrosion2015In: PLOS ONE, E-ISSN 1932-6203, Vol. 10, no 10, p. e0140393-Article in journal (Refereed)
    Abstract [en]

    Peri-implantitis is an inflammatory disease that results in the destruction of soft tissue and bone around the implant. Titanium implant corrosion has been attributed to the implant failure and cytotoxic effects to the alveolar bone. We have documented the extent of titanium release into surrounding plaque in patients with and without peri-implantitis. An in vitro model was designed to represent the actual environment of an implant in a patients mouth. The model uses actual oral microbiota from a volunteer, allows monitoring electrochemical processes generated by biofilms growing on implants and permits control of biocorrosion electrical current. As determined by next generation DNA sequencing, microbial compositions in experiments with the in vitro model were comparable with the compositions found in patients with implants. It was determined that the electrical conductivity of titanium implants was the key factor responsible for the biocorrosion process. The interruption of the biocorrosion current resulted in a 4-5 fold reduction of corrosion. We propose a new design of dental implant that combines titanium in zero oxidation state for osseointegration and strength, interlaid with a nonconductive ceramic. In addition, we propose electrotherapy for manipulation of microbial biofilms and to induce bone healing in peri-implantitis patients.

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  • 33.
    Priyadarshini, Diana
    et al.
    Linköping University, Department of Science and Technology, Laboratory of Organic Electronics. Linköping University, Faculty of Science & Engineering.
    Musumeci, Chiara
    Linköping University, Department of Science and Technology, Laboratory of Organic Electronics. Linköping University, Faculty of Science & Engineering.
    Bliman, David
    Department of Chemistry and Molecular Biology, University of Gothenburg, Gothenburg, Sweden.
    Abrahamsson, Tobias
    Linköping University, Department of Science and Technology, Laboratory of Organic Electronics. Linköping University, Faculty of Science & Engineering.
    Lindholm, Caroline
    Linköping University, Department of Science and Technology, Laboratory of Organic Electronics. Linköping University, Faculty of Science & Engineering.
    Vagin, Mikhail
    Linköping University, Department of Science and Technology, Laboratory of Organic Electronics. Linköping University, Faculty of Science & Engineering.
    Strakosas, Xenofon
    Linköping University, Department of Science and Technology, Laboratory of Organic Electronics. Linköping University, Faculty of Science & Engineering.
    Olsson, Roger
    Department of Chemistry and Molecular Biology, University of Gothenburg, 412 96 Gothenburg, Sweden;Chemical Biology and Therapeutics, Department of Experimental Medical Science, Lund University, Lund, Sweden.
    Berggren, Magnus
    Linköping University, Department of Science and Technology, Laboratory of Organic Electronics. Linköping University, Faculty of Science & Engineering.
    Gerasimov, Jennifer Y.
    Linköping University, Department of Science and Technology, Laboratory of Organic Electronics. Linköping University, Faculty of Science & Engineering.
    Simon, Daniel T.
    Linköping University, Department of Science and Technology, Laboratory of Organic Electronics. Linköping University, Faculty of Science & Engineering.
    Enzymatically Polymerized Organic Conductors on Model Lipid Membranes2023In: Langmuir, ISSN 0743-7463, E-ISSN 1520-5827, Vol. 39, no 23, p. 8196-8204Article in journal (Refereed)
    Abstract [en]

    Seamless integration between biological systems and electrical components is essential for enabling a twinned biochemical–electrical recording and therapy approach to understand and combat neurological disorders. Employing bioelectronic systems made up of conjugated polymers, which have an innate ability to transport both electronic and ionic charges, provides the possibility of such integration. In particular, translating enzymatically polymerized conductive wires, recently demonstrated in plants and simple organism systems, into mammalian models, is of particular interest for the development of next-generation devices that can monitor and modulate neural signals. As a first step toward achieving this goal, enzyme-mediated polymerization of two thiophene-based monomers is demonstrated on a synthetic lipid bilayer supported on a Au surface. Microgravimetric studies of conducting films polymerized in situ provide insights into their interactions with a lipid bilayer model that mimics the cell membrane. Moreover, the resulting electrical and viscoelastic properties of these self-organizing conducting polymers suggest their potential as materials to form the basis for novel approaches to in vivo neural therapeutics.

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  • 34.
    Qian, Deping
    et al.
    Linköping University, Faculty of Science & Engineering. Linköping University, Department of Physics, Chemistry and Biology, Biomolecular and Organic Electronics.
    Liu, Bo
    Linköping University, Department of Physics, Chemistry and Biology, Biomolecular and Organic Electronics. Linköping University, The Institute of Technology.
    Wang, Suhao
    Linköping University, Department of Science and Technology, Physics and Electronics. Linköping University, Faculty of Science & Engineering.
    Himmelberger, Scott
    Stanford University, CA 94305 USA.
    Linares, Mathieu
    Linköping University, Department of Physics, Chemistry and Biology, Theoretical Chemistry. Linköping University, Faculty of Science & Engineering.
    Vagin, Mikhail
    Linköping University, Department of Science and Technology, Physics and Electronics. Linköping University, Faculty of Science & Engineering.
    Muller, Christian
    Chalmers, Sweden.
    Zaifei, Zaifei
    Linköping University, Department of Physics, Chemistry and Biology, Biomolecular and Organic Electronics. Linköping University, Faculty of Science & Engineering.
    Fabiano, Simone
    Linköping University, Department of Science and Technology, Physics and Electronics. Linköping University, Faculty of Science & Engineering.
    Berggren, Magnus
    Linköping University, Department of Science and Technology, Physics and Electronics. Linköping University, Faculty of Science & Engineering.
    Salleo, Alberto
    Stanford University, CA 94305 USA.
    Inganäs, Olle
    Linköping University, Department of Physics, Chemistry and Biology, Biomolecular and Organic Electronics. Linköping University, Faculty of Science & Engineering.
    Zou, Yingping
    Central S University, Peoples R China.
    Zhang, Fengling
    Linköping University, Department of Physics, Chemistry and Biology, Biomolecular and Organic Electronics. Linköping University, Faculty of Science & Engineering.
    Modulating molecular aggregation by facile heteroatom substitution of diketopyrrolopyrrole based small molecules for efficient organic solar cells2015In: Journal of Materials Chemistry A, ISSN 2050-7488, Vol. 3, no 48, p. 24349-24357Article in journal (Refereed)
    Abstract [en]

    In conjugated polymers and small molecules of organic solar cells, aggregation induced by intermolecular interactions governs the performance of photovoltaics. However, little attention has been paid to the connection between molecular structure and aggregation within solar cells based on soluble small molecules. Here we demonstrate modulation of intermolecular aggregation of two synthesized molecules through heteroatom substitution to develop an understanding of the role of aggregation in conjugated molecules. Molecule 1 (M1) based on 2-ethylhexyloxy-benzene substituted benzo[1,2-b:4,5-b]dithiophene (BDTP) and diketopyrrolopyrrole (DPP) displays strong aggregation in commonly used organic solvents, which is reduced in molecule 2 (M2) by facile oxygen atom substitution on the BDTP unit confirmed by absorption spectroscopy and optical microscopy, while it successfully maintains molecular planarity and favorable charge transport characteristics. Solar cells based on M2 exhibit more than double the photocurrent of devices based on M1 and yield a power conversion efficiency of 5.5%. A systematic investigation of molecular conformation, optoelectronic properties, molecular packing and crystallinity as well as film morphology reveals structure dependent aggregation responsible for the performance difference between the two conjugated molecules.

  • 35.
    Sankoh, Supannee
    et al.
    Linköping University, Department of Physics, Chemistry and Biology, Biosensors and Bioelectronics. Linköping University, Faculty of Science & Engineering. Prince Songkla University, Thailand.
    Vagin, Mikhail
    Linköping University, Department of Science and Technology, Physics and Electronics. Linköping University, Faculty of Science & Engineering.
    Sekretareva, Alina
    Linköping University, Faculty of Science & Engineering. Linköping University, Department of Physics, Chemistry and Biology, Biosensors and Bioelectronics. Stanford University, CA 94305 USA.
    Thavarungkul, Panote
    Prince Songkla University, Thailand.
    Kanatharana, Proespichaya
    Prince Songkla University, Thailand.
    Mak, Wing Cheung
    Linköping University, Department of Physics, Chemistry and Biology, Biosensors and Bioelectronics. Linköping University, Faculty of Science & Engineering.
    Colloid electrochemistry of conducting polymer: towards potential-induced in-situ drug release2017In: Electrochimica Acta, ISSN 0013-4686, E-ISSN 1873-3859, Vol. 228, p. 407-412Article in journal (Refereed)
    Abstract [en]

    Over the past decades, controlled drug delivery system remains as one of the most important area in medicine for various diseases. We have developed a new electrochemically controlled drug release system by combining colloid electrochemistry and electro-responsive microcapsules. The pulsed electrode potential modulation led to the appearance of two processes available for the time-resolved registration in colloid microenvironment: change of the electronic charge of microparticles (from 0.5 ms to 0.1 s) followed by the drug release associated with ionic equilibration (1-10 s). The dynamic electrochemical measurements allow the distinction of drug release associated With ionic relaxation and the change of electronic charge of conducting polymer colloid microparticles. The amount of released drug (methylene blue) could be controlled by modulating the applied potential. Our study demonstrated a surface-potential driven controlled drug release of dispersion of conducting polymer carrier at the electrode interfaces, while the bulk colloids dispersion away from the electrode remains as a reservoir to improve the efficiency of localized drug release. The developed new methodology creates a model platform for the investigations of surface potential-induced in-situ electrochemical drug release mechanism. (C) 2017 Elsevier Ltd. All rights reserved.

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  • 36.
    Santangelo, Francesca
    et al.
    Linköping University, Department of Physics, Chemistry and Biology, Sensor and Actuator Systems. Linköping University, Faculty of Science & Engineering.
    Shtepliuk, Ivan
    Linköping University, Department of Physics, Chemistry and Biology, Semiconductor Materials. Linköping University, Faculty of Science & Engineering.
    Filippini, Daniel
    Linköping University, Department of Physics, Chemistry and Biology, Sensor and Actuator Systems. Linköping University, Faculty of Science & Engineering.
    Puglisi, Donatella
    Linköping University, Department of Physics, Chemistry and Biology, Sensor and Actuator Systems. Linköping University, Faculty of Science & Engineering.
    Vagin, Mikhail
    Linköping University, Department of Science and Technology, Physics and Electronics. Linköping University, Faculty of Science & Engineering.
    Yakimova, Rositsa
    Linköping University, Department of Physics, Chemistry and Biology, Semiconductor Materials. Linköping University, Faculty of Science & Engineering.
    Eriksson, Jens
    Linköping University, Department of Physics, Chemistry and Biology, Sensor and Actuator Systems. Linköping University, Faculty of Science & Engineering.
    Epitaxial Graphene Sensors Combined with 3D-Printed Microfluidic Chip for Heavy Metals Detection2019In: Sensors, E-ISSN 1424-8220, Vol. 19, no 10, article id 2393Article in journal (Refereed)
    Abstract [en]

    In this work, we investigated the sensing performance of epitaxial graphene on Si-face 4H-SiC (EG/SiC) for liquid-phase detection of heavy metals (e.g., Pb and Cd), showing fast and stable response and low detection limit. The sensing platform proposed includes 3D-printed microfluidic devices, which incorporate all features required to connect and execute lab-on-chip (LOC) functions. The obtained results indicate that EG exhibits excellent sensing activity towards Pb and Cd ions. Several concentrations of Pb2+ solutions, ranging from 125 nM to 500 mu M, were analyzed showing Langmuir correlation between signal and Pb2+ concentrations, good stability, and reproducibility over time. Upon the simultaneous presence of both metals, sensor response is dominated by Pb2+ rather than Cd2+ ions. To explain the sensing mechanisms and difference in adsorption behavior of Pb2+ and Cd2+ ions on EG in water-based solutions, we performed van-der-Waals (vdW)-corrected density functional theory (DFT) calculations and non-covalent interaction (NCI) analysis, extended charge decomposition analysis (ECDA), and topological analysis. We demonstrated that Pb2+ and Cd2+ ions act as electron-acceptors, enhancing hole conductivity of EG, due to charge transfer from graphene to metal ions, and Pb2+ ions have preferential ability to binding with graphene over cadmium. Electrochemical measurements confirmed the conductometric results, which additionally indicate that EG is more sensitive to lead than to cadmium.

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  • 37.
    Sekretareva, Alina
    et al.
    Linköping University, Department of Physics, Chemistry and Biology. Linköping University, Faculty of Science & Engineering. Stanford University, CA 94305 USA.
    Vagin, Mikhail
    Linköping University, Department of Science and Technology, Physics and Electronics. Linköping University, Faculty of Science & Engineering.
    Turner, Anthony
    Linköping University, Department of Physics, Chemistry and Biology, Biosensors and Bioelectronics. Linköping University, Faculty of Science & Engineering.
    Eriksson, Mats
    Linköping University, Department of Physics, Chemistry and Biology, Chemical and Optical Sensor Systems. Linköping University, Faculty of Science & Engineering.
    Correspondence on "Can Nanoimpacts Detect Single-Enzyme Activity? Theoretical Considerations and an Experimental Study of Catalase Impacts"2017In: ACS Catalysis, ISSN 2155-5435, E-ISSN 2155-5435, Vol. 7, no 5, p. 3591-3593Article in journal (Other academic)
    Abstract [en]

    n/a

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  • 38.
    Sekretareva, Alina
    et al.
    Linköping University, Department of Physics, Chemistry and Biology, Chemical and Optical Sensor Systems. Linköping University, Faculty of Science & Engineering.
    Vagin, Mikhail
    Linköping University, Department of Science and Technology, Physics and Electronics. Linköping University, Faculty of Science & Engineering.
    Volkov, Anton V.
    Linköping University, Department of Science and Technology, Physics and Electronics. Linköping University, Faculty of Science & Engineering.
    Zozoulenko, Igor V.
    Linköping University, Department of Science and Technology, Physics and Electronics. Linköping University, Faculty of Science & Engineering.
    Turner, Anthony
    Linköping University, Department of Physics, Chemistry and Biology, Biosensors and Bioelectronics. Linköping University, Faculty of Science & Engineering.
    Eriksson, Mats
    Linköping University, Department of Physics, Chemistry and Biology, Chemical and Optical Sensor Systems. Linköping University, Faculty of Science & Engineering.
    Screen printed microband array based biosensor for water monitoring2015In: The Frumkin Symposium, 2015Conference paper (Refereed)
  • 39.
    Sekretareva, Alina
    et al.
    Linköping University, Department of Physics, Chemistry and Biology. Linköping University, Faculty of Science & Engineering. Uppsala Univ, Sweden.
    Vagin, Mikhail
    Linköping University, Department of Science and Technology, Physics and Electronics. Linköping University, Faculty of Science & Engineering.
    Volkov, Anton
    Linköping University, Department of Science and Technology, Laboratory of Organic Electronics. Linköping University, Faculty of Science & Engineering.
    Zozoulenko, Igor
    Linköping University, Department of Science and Technology, Laboratory of Organic Electronics. Linköping University, Faculty of Science & Engineering.
    Eriksson, Mats
    Linköping University, Department of Physics, Chemistry and Biology, Sensor and Actuator Systems. Linköping University, Faculty of Science & Engineering.
    Evaluation of the Electrochemically Active Surface Area of Microelectrodes by Capacitive and Faradaic Currents2019In: ChemElectroChem, E-ISSN 2196-0216, Vol. 6, no 17, p. 4411-4417Article in journal (Refereed)
    Abstract [en]

    Two experimental methods to estimate the electrochemically active surface area (EASA) of microelectrodes are investigated. One method is based on electrocapacitive measurements and depends significantly on the surface roughness as well as on other parameters. The other method is based on faradaic current measurements and depends on the geometric surface area. The experimental results are supplemented with numerical modeling of electrodes with different surface roughness. A systematic study reveals a strong influence of the scale and arrangement of the surface roughness, the measurement potential and the electrolyte concentration on the EASA of microelectrodes estimated from the electrocapacitive measurements. The results show that electrocapacitive measurements should not be used to estimate the faradaic EASA of microelectrodes with a non-negligible surface roughness.

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  • 40.
    Sekretareva, Alina
    et al.
    Linköping University, Department of Physics, Chemistry and Biology, Chemical and Optical Sensor Systems. Linköping University, Faculty of Science & Engineering.
    Vagin, Mikhail Yu
    Linköping University, Department of Science and Technology, Physics and Electronics. Linköping University, Faculty of Science & Engineering.
    Volkov, Anton V.
    Linköping University, Department of Science and Technology, Physics and Electronics. Linköping University, Faculty of Science & Engineering.
    Zozoulenko, Igor V.
    Linköping University, Department of Science and Technology, Physics and Electronics. Linköping University, Faculty of Science & Engineering.
    Turner, Anthony P.F.
    Linköping University, Department of Physics, Chemistry and Biology, Biosensors and Bioelectronics. Linköping University, Faculty of Science & Engineering.
    Eriksson, Mats.
    Linköping University, Department of Physics, Chemistry and Biology, Chemical and Optical Sensor Systems. Linköping University, Faculty of Science & Engineering.
    Total phenol analysis of water using a laccase-based microsensor array2015In: Program of the XXIII International Symposium on Bioelectrochemistry and Bioenergetics of the Bioelectrochemical Society. 14-18 June, 2015. Malmö, Sweden, Lausanne: Bioelectrochemical Society , 2015, p. 155-155Conference paper (Other academic)
    Abstract [en]

    The monitoring of phenolic compounds in raw waters and wastewaters is of great importance for environmental control. Use of biosensors for rapid, specific and simple detection of phenolic compounds is a promising approach. A number of biosensors have been developed for phenol detection. A general drawback of previously reported biosensors is their insufficient detection limits for phenols in water samples. One way to improve the detection limit is by the use of microelectrodes.

    Microband design of the microelectrodes combines convergent mass transport due to the microscale width and high output currents due to the macroscopic length. Among the various techniques available for microband electrode fabrication, we have chosen screen-printing which is a cost-effective production method.

    In this study, we report on the development of a laccase-based microscale biosensor operating under a convergent diffusion regime. Screen-printing followed by simple cutting was utilized for the fabrication of graphite microbands as a platform for further covalent immobilization of laccase. Numerical simulations, utilizing the finite element method with periodic boundary conditions, were used for modeling the voltammetric response of the developed microband electrodes. Anodization followed by covalent immobilization was used for the electrode modification with laccase. Direct and mediated laccase bioelectrocatalytic oxidation of phenols was studied on macro- and microscale graphite electrodes. Significant enhancement of the analytical performance was achieved by the establishment of convergent diffusion in the microscale sensor. Finally, the developed microsensor was utilized to monitor phenolic compounds in real waste water.

  • 41.
    Sekretaryova, Alina
    et al.
    Linköping University, Department of Physics, Chemistry and Biology, Chemical and Optical Sensor Systems. Linköping University, The Institute of Technology.
    Beni, Valerio
    Linköping University, Department of Physics, Chemistry and Biology, Biosensors and Bioelectronics. Linköping University, The Institute of Technology.
    Eriksson, Mats
    Linköping University, Department of Physics, Chemistry and Biology, Chemical and Optical Sensor Systems. Linköping University, The Institute of Technology.
    Karyakin, Arkady A.
    Moscow MV Lomonosov State University, Russia.
    Turner, Anthony
    Linköping University, Department of Physics, Chemistry and Biology, Biosensors and Bioelectronics. Linköping University, The Institute of Technology.
    Vagin, Mikhail
    Linköping University, Department of Physics, Chemistry and Biology, Chemical and Optical Sensor Systems. Linköping University, The Institute of Technology.
    Cholesterol Self-Powered Biosensor2014In: Analytical Chemistry, ISSN 0003-2700, E-ISSN 1520-6882, Vol. 86, no 19, p. 9540-9547Article in journal (Refereed)
    Abstract [en]

    Monitoring the cholesterol level is of great importance, especially for people with high risk of developing heart disease. Here we report on reagentless cholesterol detection in human plasma with a novel single-enzyme, membrane-free, self-powered biosensor, in which both cathodic and anodic bioelectrocatalytic reactions are powered by the same substrate. Cholesterol oxidase was immobilized in a sol-gel matrix on both the cathode and the anode. Hydrogen peroxide, a product of the enzymatic conversion of cholesterol, was electrocatalytically reduced, by the use of Prussian blue, at the cathode. In parallel, cholesterol oxidation catalyzed by mediated cholesterol oxidase occurred at the anode. The analytical performance was assessed for both electrode systems separately. The combination of the two electrodes, formed on high surface-area carbon cloth electrodes, resulted in a self-powered biosensor with enhanced sensitivity (26.0 mA M-1 cm(-2)), compared to either of the two individual electrodes, and a dynamic range up to 4.1 mM cholesterol. Reagentless cholesterol detection with both electrochemical systems and with the self-powered biosensor was performed and the results were compared with the standard method of colorimetric cholesterol quantification.

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  • 42.
    Sekretaryova, Alina
    et al.
    Linköping University, Department of Physics, Chemistry and Biology, Biosensors and Bioelectronics. Linköping University, The Institute of Technology.
    Beni, Valerio
    Linköping University, Department of Physics, Chemistry and Biology, Biosensors and Bioelectronics. Linköping University, The Institute of Technology.
    Eriksson, Mats
    Linköping University, Department of Physics, Chemistry and Biology, Chemical and Optical Sensor Systems. Linköping University, The Institute of Technology.
    Turner, Anthony
    Linköping University, Department of Physics, Chemistry and Biology, Biosensors and Bioelectronics. Linköping University, The Institute of Technology.
    Vagin, Mikhail Y
    Linköping University, Department of Physics, Chemistry and Biology, Chemical and Optical Sensor Systems. Linköping University, The Institute of Technology.
    A highly sensitive and self-powered cholesterol biosensor2014In: 24th Anniversary World Congress on Biosensors – Biosensors 2014, Elsevier, 2014Conference paper (Other academic)
    Abstract [en]

    Blood cholesterol is a very important parameter for the assessment of atherosclerosis and other lipid disorders. The total cholesterol concentration in human blood should be less than 5.17 mM. Concentrations in the range 5.17 – 6.18 mM are considered borderline high risk and levels above 6.21 mM, high risk. Cholesterol determination with high accuracy is therefore necessary in order to differentiate these levels for medical screening or diagnosis. Several attempts to develop highly sensitive cholesterol biosensors have been described, but, to the best of our knowledge, this is the first report of a self-powered cholesterol biosensor, i.e. a device delivering the analytical information from the current output of the energy of the biocatalytic conversion of cholesterol, without any external power source. This is particularly relevant to the development of inexpensive screening devices based on printed electronics.

     

    We present two complementary bioelectrocatalytic platforms suitable for the fabrication of a self-powered biosensor. Both are based on cholesterol oxidase (ChOx) immobilisation in a sol-gel matrix, as illustrated in Fig. 1 [1]. Mediated biocatalytic cholesterol oxidation [2] was used as the anodic reaction and electrocatalytic reduction of hydrogen peroxide on Prussian Blue (PB) as the cathodic reaction. Due to a synergistic effect in the self-powered cholesterol biosensor, the analytical parameters of the overall device exceeded those of the individual component half-cells, yielding a sensitivity of 0.19 A M-1 cm-2 and a dynamic range that embraces the free cholesterol concentrations found in human blood.

     

    Thus, we have demonstrated the novel concept of highly sensitive cholesterol determination using the first self-powered cholesterol biosensor. This configuration is particularly promising for incorporation in emerging plastic- and paper-based analytical instruments for decentralised diagnostics and mobile health.

     

  • 43.
    Sekretaryova, Alina N
    et al.
    Linköping University, Department of Physics, Chemistry and Biology, Biosensors and Bioelectronics. Linköping University, The Institute of Technology.
    Beni, Valerio
    Linköping University, Department of Physics, Chemistry and Biology, Biosensors and Bioelectronics. Linköping University, The Institute of Technology.
    Eriksson, Mats
    Linköping University, Department of Physics, Chemistry and Biology, Chemical and Optical Sensor Systems. Linköping University, The Institute of Technology.
    Karyakin, Arkady A
    Moscow State University, Russia.
    Turner, Anthony
    Linköping University, Department of Physics, Chemistry and Biology, Biosensors and Bioelectronics. Linköping University, The Institute of Technology.
    Vagin, Mikhail Y
    Linköping University, Department of Physics, Chemistry and Biology, Chemical and Optical Sensor Systems. Linköping University, The Institute of Technology.
    Novel single-enzyme based self-powered biosensor2014In: 15th International Conference on Electroanalysis (ESEAC), 2014Conference paper (Other academic)
  • 44.
    Sekretaryova, Alina N
    et al.
    Linköping University, Department of Physics, Chemistry and Biology, Biosensors and Bioelectronics. Linköping University, The Institute of Technology.
    Vagin, Mikhail Y
    Linköping University, Department of Physics, Chemistry and Biology, Chemical and Optical Sensor Systems. Linköping University, The Institute of Technology.
    Turner, Anthony
    Linköping University, Department of Physics, Chemistry and Biology, Biosensors and Bioelectronics. Linköping University, The Institute of Technology.
    Eriksson, Mats
    Linköping University, Department of Physics, Chemistry and Biology, Chemical and Optical Sensor Systems. Linköping University, The Institute of Technology.
    A screen-printed microband array biosensor for water monitoring2014In: 15th International Conference on Electroanalysis (ESEAC), 2014Conference paper (Other academic)
  • 45.
    Sekretaryova, Alina N.
    et al.
    Linköping University, Department of Physics, Chemistry and Biology, Chemical and Optical Sensor Systems. Linköping University, Faculty of Science & Engineering.
    Vagin, Mikhail Yu.
    Linköping University, Department of Science and Technology, Physics and Electronics. Linköping University, Faculty of Science & Engineering.
    Eriksson, Mats
    Linköping University, Department of Physics, Chemistry and Biology, Chemical and Optical Sensor Systems. Linköping University, Faculty of Science & Engineering.
    Evaluation of the electrochemically active surface area of microelectrodes by capacitive and faradaic currentsManuscript (preprint) (Other academic)
    Abstract [en]

    Two methods to estimate the electrochemically active surface area (EASA) of microelectrodes were compared. One is based on electrocapacitive measurements and the other on faradaic measuements. A systematic study revealed a strong influence of the surface roughness and the electrolyte concentration on the EASA of microelectrodes estimated from the electrocapacitive measurements, yielding a lack of reliability compared to the faradaic method.

  • 46.
    Sekretaryova, Alina N.
    et al.
    Linköping University, Department of Physics, Chemistry and Biology, Chemical and Optical Sensor Systems. Linköping University, Faculty of Science & Engineering.
    Vagin, Mikhail Yu.
    Linköping University, Department of Science and Technology, Physics and Electronics. Linköping University, Faculty of Science & Engineering.
    Turner, Anthony P.F.
    Linköping University, Department of Physics, Chemistry and Biology, Biosensors and Bioelectronics. Linköping University, Faculty of Science & Engineering.
    Eriksson, Mats
    Linköping University, Department of Physics, Chemistry and Biology, Chemical and Optical Sensor Systems. Linköping University, Faculty of Science & Engineering.
    Electrocatalytic Currents from Single Enzyme Molecules2016In: Journal of the American Chemical Society, ISSN 0002-7863, E-ISSN 1520-5126, Vol. 138, no 8, p. 2504-2507Article in journal (Refereed)
    Abstract [en]

    Single molecule enzymology provides an opportunity to examine details of enzyme mechanisms that are not distinguishable in biomolecule ensemble studies. Here we report, for the first time, detection of the current produced in an electrocatalytic reaction by a single redox enzyme molecule when it collides with an ultramicroelectrode. The catalytic process provides amplification of the current from electron-transfer events at the catalyst leading to a measurable current. This new methodology monitors turnover of a single enzyme molecule. The methodology might complement existing single molecule techniques, giving further insights into enzymatic mechanisms and filling the gap between fundamental understanding of biocatalytic processes and their potential for bioenergy production.

  • 47.
    Sekretaryova, Alina
    et al.
    Linköping University, Department of Physics, Chemistry and Biology, Biosensors and Bioelectronics. Linköping University, The Institute of Technology.
    Vagin, Mikhail
    Linköping University, Department of Physics, Chemistry and Biology, Applied Physics. Linköping University, The Institute of Technology.
    Beni, Valerio
    Linköping University, Department of Physics, Chemistry and Biology, Biosensors and Bioelectronics. Linköping University, The Institute of Technology.
    Eriksson, Mats
    Linköping University, Department of Physics, Chemistry and Biology, Applied Physics. Linköping University, The Institute of Technology.
    Turner, Anthony
    Linköping University, Department of Physics, Chemistry and Biology, Biosensors and Bioelectronics. Linköping University, The Institute of Technology.
    Unsubstitutedand insoluble phenothiazine as an electron-transfer mediator in enzymaticelectrochemical biosensors2013In: Nano-scaled arrangements of proteins, aptamers, andother nucleic acid structures – and their potential applications , COST Thematic Workshop, 8-9 October 2013, Helmholtz Zentrum fürUmweltforschung, Leipzig, Germany, Leipzig: Helmholtz Zentrum für Umweltforschung , 2013, p. O1-Conference paper (Refereed)
  • 48.
    Sekretaryova, Alina
    et al.
    Linköping University, Department of Physics, Chemistry and Biology. Linköping University, The Institute of Technology. Lomonosov Moscow State University, Russia.
    Vagin, Mikhail
    Linköping University, Department of Physics, Chemistry and Biology, Applied Physics. Linköping University, The Institute of Technology.
    Beni, Valerio
    Linköping University, Department of Physics, Chemistry and Biology, Biosensors and Bioelectronics. Linköping University, The Institute of Technology.
    Turner, Anthony P.F.
    Linköping University, Department of Physics, Chemistry and Biology, Biosensors and Bioelectronics. Linköping University, The Institute of Technology.
    Karyakin, Arkady A.
    Lomonosov Moscow State University, Russia.
    Unsubstituted phenothiazine as a superior water-insoluble mediator for oxidases2014In: Biosensors & bioelectronics, ISSN 0956-5663, E-ISSN 1873-4235, Vol. 53, p. 275-282Article in journal (Refereed)
    Abstract [en]

    The mediation of oxidases glucose oxidase (GOx), lactate oxidase (LOx) and cholesterol oxidase (ChOx) by a new electron shuttling mediator, unsubstituted phenothiazine (PTZ), was studied. Cyclic voltammetry and rotating-disk electrode measurements in nonaqueous media were used to determine the diffusion characteristics of the mediator and the kinetics of its reaction with GOx, giving a second-order rate constant of 7.6×103–2.1×104 M−1 s−1 for water–acetonitrile solutions containing 5–15% water. These values are in the range reported for commonly used azine-type mediators, indicating that PTZ is able to function as an efficient mediator. PTZ and GOx, LOx and ChOx were successfully co-immobilised in sol–gel membrane on a screen-printed electrode to construct glucose, lactate and cholesterol biosensors, respectively, which were then optimised in terms of stability and sensitivity. The electrocatalytic oxidation responses showed a dependence on substrate concentration ranging from 0.6 to 32 mM for glucose, from 19 to 565 mM for lactate and from 0.015 to 1.0 mM for cholesterol detection. Oxidation of substrates on the surface of electrodes modified with PTZ and enzyme membrane was investigated with double-step chronoamperometry and the results showed that the PTZ displays excellent electrochemical catalytic activities even when immobilised on the surface of the electrode.

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  • 49.
    Sekretaryova, Alina
    et al.
    Linköping University, Department of Physics, Chemistry and Biology. Linköping University, Faculty of Science & Engineering.
    Vagin, Mikhail
    Linköping University, Department of Science and Technology, Physics and Electronics. Linköping University, Faculty of Science & Engineering.
    Turner, Anthony
    Linköping University, Department of Physics, Chemistry and Biology, Biosensors and Bioelectronics. Linköping University, Faculty of Science & Engineering.
    Eriksson, Mats
    Linköping University, Department of Physics, Chemistry and Biology, Chemical and Optical Sensor Systems. Linköping University, Faculty of Science & Engineering.
    Collision-based Electrochemistry for Investigation of Direct Electron Transfer of a Single Enzyme Molecule2017In: 26th Anniversary World Congress on Biosensors (Biosensors), Elsevier, 2017, p. 238-239Conference paper (Refereed)
    Abstract [en]

    Eldectron transfer between a biorecognition element and an electrode is an essential element of bioelectrocatalytic systems, such as biosensors and biofuel cells. The number of working systems based on direct electron communication is limited and detailed investigations of the mechanism of the process are still required. Here, we present the use of a novel approach of collision-based bioelectrocatalysis to monitor electrocatalytic currents from individual redox enzyme molecules. This approach allowed us to calculate the individual turnover rates of these molecules and investigate the influence of the applied potential, pH and additions of inhibitor on the observed rates of direct electron transfer.

  • 50.
    Sekretaryova, Alina
    et al.
    Linköping University, Department of Physics, Chemistry and Biology, Chemical and Optical Sensor Systems. Linköping University, Faculty of Science & Engineering.
    Volkov, Anton V.
    Linköping University, Department of Science and Technology, Physics and Electronics. Linköping University, Faculty of Science & Engineering.
    Zozoulenko, Igor V.
    Linköping University, Department of Science and Technology, Physics and Electronics. Linköping University, Faculty of Science & Engineering.
    Turner, Anthony
    Linköping University, Department of Physics, Chemistry and Biology, Biosensors and Bioelectronics. Linköping University, Faculty of Science & Engineering.
    Vagin, Mikhail Yu
    Linköping University, Department of Science and Technology, Physics and Electronics. Linköping University, Faculty of Science & Engineering.
    Eriksson, Mats
    Linköping University, Department of Physics, Chemistry and Biology, Chemical and Optical Sensor Systems. Linköping University, Faculty of Science & Engineering.
    Total phenol analysis of weakly supported water using a laccase-based microband biosensor.2016In: Analytica Chimica Acta, ISSN 0003-2670, E-ISSN 1873-4324, Vol. 907, p. 45-53Article in journal (Refereed)
    Abstract [en]

    The monitoring of phenolic compounds in wastewaters in a simple manner is of great importance for environmental control. Here, a novel screen printed laccase-based microband array for in situ, total phenol estimation in wastewaters and for water quality monitoring without additional sample pre-treatment is presented. Numerical simulations using the finite element method were utilized for the characterization of micro-scale graphite electrodes. Anodization followed by covalent modification was used for the electrode functionalization with laccase. The functionalization efficiency and the electrochemical performance in direct and catechol-mediated oxygen reduction were studied at the microband laccase electrodes and compared with macro-scale electrode structures. The reduction of the dimensions of the enzyme biosensor, when used under optimized conditions, led to a significant improvement in its analytical characteristics. The elaborated microsensor showed fast responses towards catechol additions to tap water – a weakly supported medium – characterized by a linear range from 0.2 to 10 μM, a sensitivity of 1.35 ± 0.4 A M−1 cm−2 and a dynamic range up to 43 μM. This enhanced laccase-based microsensor was used for water quality monitoring and its performance for total phenol analysis of wastewater samples from different stages of the cleaning process was compared to a standard method.

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