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  • 1.
    Ail, Ujwala
    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.
    Wang, Hui
    Linköping University, Department of Science and Technology. 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.
    Crispin, Xavier
    Linköping University, Department of Science and Technology, Physics and Electronics. Linköping University, Faculty of Science & Engineering.
    Thermoelectric Properties of Polymeric Mixed Conductors2016In: Advanced Functional Materials, ISSN 1616-301X, E-ISSN 1616-3028, Vol. 26, no 34, p. 6288-6296Article in journal (Refereed)
    Abstract [en]

    The thermoelectric (TE) phenomena are intensively explored by the scientific community due to the rather inefficient way energy resources are used with a large fraction of energy wasted in the form of heat. Among various materials, mixed ion-electron conductors (MIEC) are recently being explored as potential thermoelectrics, primarily due to their low thermal conductivity. The combination of electronic and ionic charge carriers in those inorganic or organic materials leads to complex evolution of the thermovoltage (Voc) with time, temperature, and/or humidity. One of the most promising organic thermoelectric materials, poly(3,4-ethyelenedioxythiophene)-polystyrene sulfonate (PEDOT-PSS), is an MIEC. A previous study reveals that at high humidity, PEDOT-PSS undergoes an ionic Seebeck effect due to mobile protons. Yet, this phenomenon is not well understood. In this work, the time dependence of the Voc is studied and its behavior from the contribution of both charge carriers (holes and protons) is explained. The presence of a complex reorganization of the charge carriers promoting an internal electrochemical reaction within the polymer film is identified. Interestingly, it is demonstrated that the time dependence behavior of Voc is a way to distinguish between three classes of polymeric materials: electronic conductor, ionic conductor, and mixed ionic–electronic conductor

  • 2.
    Ail, Ujwala
    et al.
    Linköping University, Department of Science and Technology, Physics and Electronics. Linköping University, Faculty of Science & Engineering.
    Ullah Khan, Zia
    Linköping University, Department of Science and Technology, Physics and Electronics. Linköping University, Faculty of Science & Engineering.
    Granberg, Hjalmar
    Innventia AB, Sweden.
    Berthold, Fredrik
    Innventia AB, Sweden.
    Parasuraman, Rajasekar
    Mat Research Centre, India.
    Urnarji, Arun M.
    Mat Research Centre, India.
    Slettengren, Kerstin
    Innventia AB, Sweden.
    Pettersson, Henrik
    Innventia AB, Sweden.
    Crispin, Xavier
    Linköping University, Department of Science and Technology, Physics and Electronics. Linköping University, Faculty of Science & Engineering.
    Room temperature synthesis of transition metal silicide-conducting polymer micro-composites for thermoelectric applications2017In: Synthetic metals, ISSN 0379-6779, E-ISSN 1879-3290, Vol. 225, p. 55-63Article in journal (Refereed)
    Abstract [en]

    Organic polymer thermoelectrics (TE) as well as transition metal (TM) silicides are two thermoelectric class of materials of interest because they are composed of atomic elements of high abundatice; which is a prerequisite for mass implementation of thermoelectric (TE) solutions for solar and waste heat recovery. But both materials have drawbacks when it comes to finding low-cost manufacturing. The metal silicide needs high temperature (amp;gt;1000 degrees C) for creating TE legs in a device from solid powder, but it is easy to achieve long TE legs in this case. On the contrary, organic TEs are synthesized at low temperature from solution. However, it is difficult to form long legs or thick films because of their low solubility. In this work, we propose a novel method for the room temperature synthesis of TE composite containing the microparticles of chromium disilicide; CrSi2 (inorganic filler) in an organic matrix of nanofibrillated cellulose-poly(3,4-ethyelenedioxythiophene)-polystyrene sulfonate (NFC-PEDOT:PSS). With this method, it is easy to create long TE legs in a room temperature process. The originality of the approach is the use of conducting polymer aerogel microparticles mixed with CrSi2 microparticles to obtain a composite solid at room temperature under pressure. We foresee that the method can be scaled up to fabricate and pattern TE modules. The composite has an electrical conductivity (sigma) of 5.4 +/- 0.5 S/cm and the Seebeck coefficient (a) of 88 +/- 9 mu V/K, power factor (alpha(2)sigma) of 4 +/- 1 mu Wm(-1) K-2 at room temperature. At a temperature difference of 32 degrees C, the output power/unit area drawn across the load, with the resistance same as the internal resistance of the device is 0.6 +/- 0.1 mu W/cm(2). (C) 2017 Elsevier B.V. All rights reserved.

  • 3.
    Jiao, Fei
    et al.
    Linköping University, Department of Science and Technology, Physics and Electronics. Linköping University, Faculty of Science & Engineering.
    Naderi, Ali
    Innventia AB, Sweden.
    Zhao, Dan
    Linköping University, Department of Science and Technology, Physics and Electronics. Linköping University, Faculty of Science & Engineering.
    Schlueter, Joshua
    University of Kentucky, KY 40506 USA.
    Shahi, Maryam
    University of Kentucky, KY 40506 USA.
    Sundstrom, Jonas
    Innventia AB, Sweden.
    Granberg, Hjalmar
    Innventia AB, Sweden.
    Edberg, Jesper
    Linköping University, Department of Science and Technology, Physics and Electronics. Linköping University, Faculty of Science & Engineering.
    Ail, Ujwala
    Linköping University, Department of Science and Technology, Physics and Electronics. Linköping University, Faculty of Science & Engineering.
    Brill, Joseph
    University of Kentucky, KY 40506 USA.
    Lindstrom, Tom
    Innventia AB, Sweden.
    Berggren, 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.
    Correction: Ionic thermoelectric paper (vol 5, pg 16883, 2017)2017In: Journal of Materials Chemistry A, ISSN 2050-7488, Vol. 5, no 37, p. 20053-20053Article in journal (Other academic)
    Abstract [en]

    n/a

  • 4.
    Jiao, Fei
    et al.
    Linköping University, Department of Science and Technology, Physics and Electronics. Linköping University, Faculty of Science & Engineering.
    Naderi, Ali
    Billerudkorsnäs AB, SE-71830 Frövi, Sweden.
    Zhao, Dan
    Linköping University, Department of Science and Technology, Physics and Electronics. Linköping University, Faculty of Science & Engineering.
    Schlueter, Joshua
    Department of Physics and Astronomy, University of Kentucky, Lexington, KY40506-0055, USA.
    Shahi, Maryam
    Department of Physics and Astronomy, University of Kentucky, Lexington, KY40506-0055, USA.
    Sundström, Jonas
    Innventia AB Box 5604, SE-11486 Stockholm, Sweden.
    Granberg, Hjalmar
    Innventia AB Box 5604, SE-11486 Stockholm, Sweden.
    Edberg, Jesper
    Linköping University, Department of Science and Technology, Physics and Electronics. Linköping University, Faculty of Science & Engineering.
    Ail, Ujwala
    Linköping University, Department of Science and Technology, Physics and Electronics. Linköping University, Faculty of Science & Engineering.
    Brill, Joseph W.
    Department of Physics and Astronomy, University of Kentucky, Lexington, KY40506-0055, USA.
    Lindström, Tom
    Innventia AB Box 5604, SE-11486 Stockholm, Sweden.
    Berggren, 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.
    Ionic Thermoelectric Paper2017In: Journal of Materials Chemistry A, ISSN 2050-7488, Vol. 5, no 32, p. 16883-16888Article in journal (Refereed)
    Abstract [en]

    Ionic thermoelectric materials, such as polyelectrolyte like polystyrene sulfonate sodium (PSSNa), constitute a new class ofmaterial attracting interest due to their large Seebeck coefficient and the possibility to be used in ionic thermoelectricsupercapacitors (ITESCs) and field effect transistors. However pure polyelectrolyte membranes are not robust neitherflexible. In this article, we demonstrate the preparation of ionic thermoelectric paper by a simple, scalable and cost-effectivemethod. After composite with nanofibrillated cellulose (NFC), the resulting NFC-PSSNa paper is flexible and mechanicallyrobust; which is desirable of using roll-to-roll processes. The robust thermoelectric paper NFC-PSSNa combines high ionicconductivity (9 mS/cm), high ionic Seebeck coefficient (8.4 mV/K) and low thermal conductivity (0.75 Wm-1K-1) at 100 RH%,resulting in overall figure-of-merit of 0.025 at room temperature slightly better than the PSSNa. Enabling flexibility androbustness by compositing with cellulose constitutes an advance for scaling up the manufacturing of ionic thermoelectricsupercapacitors; but also enables new applications for conformable thermoelectric devices and flexible electronics

  • 5.
    Volkov, Anton
    et al.
    Linköping University, Department of Science and Technology, Physics and Electronics. Linköping University, Faculty of Science & Engineering.
    Wijeratne, Kosala
    Linköping University, Department of Science and Technology, Physics and Electronics. Linköping University, Faculty of Science & Engineering.
    Mitraka, Evangelia
    Linköping University, Department of Science and Technology, Physics and Electronics. Linköping University, Faculty of Science & Engineering.
    Ail, Ujwala
    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.
    Tybrandt, Klas
    Linköping University, Department of Science and Technology, Physics and Electronics. Linköping University, Faculty of Science & Engineering.
    Wenzel Andreasen, Jens
    Technical University of Denmark, Denmark.
    Berggren, Magnus
    Linköping University, Department of Science and Technology, Physics and Electronics. Linköping University, Faculty of Science & Engineering. Stellenbosch University, South Africa.
    Crispin, Xavier
    Linköping University, Department of Science and Technology, Physics and Electronics. Linköping University, Faculty of Science & Engineering.
    Zozoulenko, Igor
    Linköping University, Department of Science and Technology, Physics and Electronics. Linköping University, Faculty of Science & Engineering.
    Understanding the Capacitance of PEDOT:PSS2017In: Advanced Functional Materials, ISSN 1616-301X, E-ISSN 1616-3028, Vol. 27, no 28, article id 1700329Article in journal (Refereed)
    Abstract [en]

    Poly(3,4-ethylenedioxythiophene): polystyrene sulfonate (PEDOT:PSS) is the most studied and explored mixed ion-electron conducting polymer system. PEDOT: PSS is commonly included as an electroactive conductor in various organic devices, e.g., supercapacitors, displays, transistors, and energy-converters. In spite of its long-term use as a material for storage and transport of charges, the fundamentals of its bulk capacitance remain poorly understood. Generally, charge storage in supercapacitors is due to formation of electrical double layers or redox reactions, and it is widely accepted that PEDOT: PSS belongs to the latter category. Herein, experimental evidence and theoretical modeling results are reported that significantly depart from this commonly accepted picture. By applying a two-phase, 2D modeling approach it is demonstrated that the major contribution to the capacitance of the two-phase PEDOT: PSS originates from electrical double layers formed along the interfaces between nanoscaled PEDOT-rich and PSS-rich interconnected grains that comprises two phases of the bulk of PEDOT: PSS. This new insight paves a way for designing materials and devices, based on mixed ion-electron conductors, with improved performance.

  • 6.
    Wang, Hui
    et al.
    Linköping University, Department of Science and Technology.
    Ail, Ujwala
    Linköping University, Department of Science and Technology, Physics and 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.
    Berggren, 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.
    Ionic Seebeck Effect in Conducting Polymers2015In: ADVANCED ENERGY MATERIALS, ISSN 1614-6832, Vol. 5, no 11, article id 1500044Article in journal (Refereed)
    Abstract [en]

    Conducting polymers display an ionic thermoelectric effect in addition to the known electronic thermoelectric effect. Their Seebeck coefficient is as large as ≈200 μV K−1. This finding discloses a new possible approach to improve the thermoelectric properties of conducting polymers by combining various types of charge carriers of the same sign.

  • 7.
    Wang, Suhao
    et al.
    Linköping University, Department of Science and Technology, Physics and Electronics. Linköping University, Faculty of Science & Engineering.
    Sun, Hengda
    Linköping University, Department of Science and Technology. Linköping University, Faculty of Science & Engineering.
    Ail, Ujwala
    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.
    Persson, Per O. Å.
    Linköping University, Department of Physics, Chemistry and Biology, Thin Film Physics. Linköping University, Faculty of Science & Engineering.
    Andreasen, Jens W.
    Technical University of Denmark Department of Energy Conversion and Storage Roskilde Denmark.
    Thiel, Walter
    Max‐Planck‐Institut für Kohlenforschung Mülheim an der Ruhr Germany.
    Berggren, 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.
    Fazzi, Daniele
    Max‐Planck‐Institut für Kohlenforschung Mülheim an der Ruhr Germany.
    Fabiano, Simone
    Linköping University, Department of Science and Technology, Physics and Electronics. Linköping University, Faculty of Science & Engineering.
    Thermoelectric Properties of Solution-Processed n-Doped Ladder-Type Conducting Polymers2016In: Advanced Materials, ISSN 0935-9648, E-ISSN 1521-4095, Vol. 28, no 48, p. 10764-Article in journal (Refereed)
    Abstract [en]

    Ladder-type “torsion-free” conducting polymers (e.g., polybenzimidazobenzophenanthroline (BBL)) can outperform “structurally distorted” donor–acceptor polymers (e.g., P(NDI2OD-T2)), in terms of conductivity and thermoelectric power factor. The polaron delocalization length is larger in BBL than in P(NDI2OD-T2), resulting in a higher measured polaron mobility. Structure–function relationships are drawn, setting material-design guidelines for the next generation of conducting thermoelectric polymers.

  • 8.
    Wijeratne, Kosala
    et al.
    Linköping University, Department of Science and Technology, Physics and Electronics. Linköping University, Faculty of Science & Engineering.
    Ail, Ujwala
    Linköping University, Department of Science and Technology, Physics and Electronics. Linköping University, Faculty of Science & Engineering.
    Brooke, Robert
    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.
    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.
    Crispin, Xavier
    Linköping University, Department of Science and Technology, Physics and Electronics. Linköping University, Faculty of Science & Engineering.
    Bulk electronic transport impacts on electron transfer at conducting polymer electrode-electrolyte interfaces.2018In: Proceedings of the National Academy of Sciences of the United States of America, ISSN 0027-8424, E-ISSN 1091-6490, no 7, p. 11899-11904Article in journal (Refereed)
    Abstract [en]

    Electrochemistry is an old but still flourishing field of research due to the importance of the efficiency and kinetics of electrochemical reactions in industrial processes and (bio-)electrochemical devices. The heterogeneous electron transfer from an electrode to a reactant in the solution has been well studied for metal, semiconductor, metal oxide, and carbon electrodes. For those electrode materials, there is little correlation between the electronic transport within the electrode material and the electron transfer occurring at the interface between the electrode and the solution. Here, we investigate the heterogeneous electron transfer between a conducting polymer electrode and a redox couple in an electrolyte. As a benchmark system, we use poly(3,4-ethylenedioxythiophene) (PEDOT) and the Ferro/ferricyanide redox couple in an aqueous electrolyte. We discovered a strong correlation between the electronic transport within the PEDOT electrode and the rate of electron transfer to the organometallic molecules in solution. We attribute this to a percolation-based charge transport within the polymer electrode directly involved in the electron transfer. We show the impact of this finding by optimizing an electrochemical thermogalvanic cell that transforms a heat flux into electrical power. The power generated by the cell increased by four orders of magnitude on changing the morphology and conductivity of the polymer electrode. As all conducting polymers are recognized to have percolation transport, we believe that this is a general phenomenon for this family of conductors.

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