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Seamless integration of bioelectronic interface in an animal model via in vivo polymerization of conjugated oligomers
Istituto di Scienze Applicate e Sistemi Intelligenti “E. Caianiello”, Consiglio Nazionale delle Ricerche, Via Campi Flegrei, Pozzuoli, Italy.
Linköping University, Department of Science and Technology, Laboratory of Organic Electronics. Linköping University, Faculty of Science & Engineering.
Istituto di Scienze Applicate e Sistemi Intelligenti “E. Caianiello”, Consiglio Nazionale delle Ricerche, Via Campi Flegrei, Pozzuoli, Italy.
Linköping University, Department of Science and Technology, Laboratory of Organic Electronics. Linköping University, Faculty of Science & Engineering.ORCID iD: 0000-0001-5757-8565
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2022 (English)In: Bioactive Materials, ISSN 2452-199X, Vol. 10, p. 107-116Article in journal (Refereed) Published
Abstract [en]

Leveraging the biocatalytic machinery of living organisms for fabricating functional bioelectronic interfaces, in vivo, defines a new class of micro-biohybrids enabling the seamless integration of technology with living biological systems. Previously, we have demonstrated the in vivo polymerization of conjugated oligomers forming conductors within the structures of plants. Here, we expand this concept by reporting that Hydra, an invertebrate animal, polymerizes the conjugated oligomer ETE-S both within cells that expresses peroxidase activity and within the adhesive material that is secreted to promote underwater surface adhesion. The resulting conjugated polymer forms electronically conducting and electrochemically active μm-sized domains, which are inter-connected resulting in percolative conduction pathways extending beyond 100 μm, that are fully integrated within the Hydra tissue and the secreted mucus. Furthermore, the introduction and in vivo polymerization of ETE-S can be used as a biochemical marker to follow the dynamics of Hydra budding (reproduction) and regeneration. This work paves the way for well-defined self-organized electronics in animal tissue to modulate biological functions and in vivo biofabrication of hybrid functional materials and devices.

Place, publisher, year, edition, pages
Elsevier, 2022. Vol. 10, p. 107-116
Keywords [en]
polymerization, Bioelectronics interfaces, Conjugated oligomers, Model organism
National Category
Neurosciences
Identifiers
URN: urn:nbn:se:liu:diva-181716DOI: 10.1016/j.bioactmat.2021.08.025ISI: 000743377900002PubMedID: 34901533OAI: oai:DiVA.org:liu-181716DiVA, id: diva2:1617501
Note

Funding agencies: European Unions Horizon 2020 research and innovation programme [800926]; Swedish Research CouncilSwedish Research CouncilEuropean Commission [VR-2017-04910]; Knut and Alice Wallenberg FoundationKnut & Alice Wallenberg Foundation; Swedish Foundation for Strategic Research (SSF)Swedish Foundation for Strategic Research; European Research Council (ERC)European Research Council (ERC)European Commission [834677]; Swedish Government Strategic Research Area in Materials Science on Advanced Functional Materials at Linkoping University (Faculty Grant SFO-Mat-LiU) [2009-00971]; MultiPark - A Strategic Research Area at Lund University; MIURMinistry of Education, Universities and Research (MIUR) [SHARID - ARS01-01270]

Available from: 2021-12-07 Created: 2021-12-07 Last updated: 2022-10-12Bibliographically approved
In thesis
1. Synthetic Functionalities for Ion and Electron Conductive Polymers: Applications in Organic Electronics and Biological Interfaces
Open this publication in new window or tab >>Synthetic Functionalities for Ion and Electron Conductive Polymers: Applications in Organic Electronics and Biological Interfaces
2021 (English)Doctoral thesis, comprehensive summary (Other academic)
Abstract [en]

In the search for understanding and communicating with all biological systems, in humans, animals, plants, and even microorganisms, we find a common language of all communicating via electrons, ions and molecules. Since the discovery of organic electronics, the ability to bridge the gap and communicate be-tween modern technology and biology has emerged. Organic chemistry pro-vides us with tools for understanding and a material platform of polymer electronics for communication. Such insights give us not only the ability to observe fundamental phenomenon but to actively design and construct materials with chemical functionalities towards better interfaces and applications. Organic electronic materials and devices have found their way to be implemented in the field of medicine for diagnostic and therapeutic purposes, but also in water purification and to help tackle the monumental task in creating the next generation of sustainable energy production and storage. Ultimately it’s safe to say that organic electronics are not going to replace our traditional technology based on inorganic materials but rather the two fields can find a way to complement each other for various purposes and applications. Compared to conventional silicon based technology, production of carbon-based organic electronic polymer materials are extremely cheap and devices can even be made flexible and soft with great compatibility towards biology.  

The main focus of this thesis has been developing and synthesizing new types of organic electronic and ionic conductive polymeric materials. Rational chemical design and modifications of the materials have been utilized to introduce specific functionalities to the materials. The functionalities serving the purpose to facilitate ion and electron conductive charge transport for organic electronics and with biological interface implementation of the polymer materials. 

Multi-functional ionic conductive hyperbranched polyglycerol polyelectrolytes (dendrolytes) were developed comprising both ionically charged groups and cross-linkable groups. The hyperbranched polyglycerol core structure of the material possesses a hydrophilic solvating platform for both ions and maintenance of solvent molecules, while being a biocompatible structure. Coupled with the peripheral charged ionic functionalities of the polymer, the dendrolyte materials are highly ionic conductive and selective towards cationic and anionic charged atoms and large molecules when implemented as ion-exchange membranes. Homogenous ion-exchange membrane casting has been achieved by the implementation of cross-linkable functionalities in the dendrolytes, utilizing robust click-chemistry for efficient micro and macro fabrication processing of the ion-ex-change membranes for organic electronic devices. The ion-exchange membrane material was implemented in electrophoretic drug delivery devices (organic electronic ion pumps), which are used for delivery of ions and neurotransmitters with spatiotemporal resolution and are able to communicate and be used for therapeutic drug delivery purposes in biological interfaces. The dendrolyte materials were also able to form free-standing membranes, making it possible for implementation in fuel cell and desalination purposes. 

Trimeric conjugated thiophene pre-polymer structures were also developed in the thesis and synthesized for the purpose of implementation of the material in vivo to form electrically conductive polymer structures, and in such manner to be able to create electrodes and ultimately to connect with the central nervous system. The conjugated pre-polymers being both water soluble and enzymatically polymerizable serve as a platform to realize such a concept. Also, modifying the trimeric structure with cross-linkable functionality created the capability to form better interfaces and stability towards biological environments.   

Place, publisher, year, edition, pages
Linköping: Linköping University Electronic Press, 2021. p. 97
Series
Linköping Studies in Science and Technology. Dissertations, ISSN 0345-7524 ; 2193
National Category
Polymer Chemistry
Identifiers
urn:nbn:se:liu:diva-181717 (URN)10.3384/9789179291341 (DOI)9789179291334 (ISBN)9789179291341 (ISBN)
Public defence
2022-01-14, K1, Kåkenhus, Campus Norrköping, Norrköping, 10:15 (English)
Opponent
Supervisors
Available from: 2021-12-07 Created: 2021-12-07 Last updated: 2021-12-07Bibliographically approved
2. Living biohybrid systems via in vivo polymerization of thiophene oligomers
Open this publication in new window or tab >>Living biohybrid systems via in vivo polymerization of thiophene oligomers
2022 (English)Doctoral thesis, comprehensive summary (Other academic)
Abstract [en]

Life is the result of a multitude of electrical signals which drives our nervous system but also accomplishes a cascade of electrochemical reactions. In the 18th century, Lucia Galeazzi and Luigi Galvani got the idea to stimulate frog legs with electrodes. This first step into the world of bioelectronics showed that electronic systems were able to communicate with living organisms through electrical stimulation, as well as by recording electrical signals from organisms. Until the end of the 20th century, the field of bioelectronics kept progressing using metal electrodes. This class of material inherently exhibits a high conductivity from their dispersed cloud of shared electrons. However, an obvious physical mismatch occurs when inserting metal electrodes inside a living organism. Since these materials are not as soft as living tissues, internal damage followed by an immune response impacts the impedance of such probes.

In the late 80s', the large-scale commercialization of water processable conducting polymers brought a new paradigm in the choice of electronic material for bioelectronics devices. Compared to metals, conducting polymers are composed of semi-crystalline blocks that interact through electrostatic forces. These soft structures make these materials permeable to aqueous solutions, which allow the introduction of ionic species in the vicinity of the polymer backbone. Ions close to the polymer backbone can tune the conductivity of the material creating a unique ion/electron dialogue that increases the electronic signal resolution. Additionally, these soft structures considerably reduce scaring effects and therefore enable the devices to trigger lower immune responses. Conducting polymers could also be directly inserted within living tissues to create electronic platforms inside a host. Living organisms with new material properties could unravel new functions such as collecting electrophysiological data without surgery.

Plants are living organisms that made their way out of the ocean and conquered most of the available land on earth. Saying that plants are good climate controllers is a euphemism since plants are legitimately the organisms that have settled the climate conditions for the development of more advanced life forms. Plant biohybrid is a new technological concept where plants are not only seen for their nutritious or environmental aspect but also as devices that can record and transfer information about their local environmental conditions. Such data could be used in a positive feedback loop to improve the production yield of crops or understand the underlying communication mechanism that occurs between plants or with plant micro-biomes. Most of the approaches toward plant biohybrids nowadays focus on nanomaterials that act as fluorescent probes in leaves and detect analytes from plants' local environment.

In this thesis, we push forward a plant biohybrid strategy that instead uses conducting polymers as vectors to build conductors inside plants with the aim to build electrochemical platforms that could be used for applications such as energy storage, sensing, and energy production. Works developed in this thesis are going in an array of directions that aims for the better integration of electronic platforms in living systems with more focus on plants.

We first identified a plant enzymatic mechanism that triggers the polymerization of a thiophene oligomer, namely ETE-S in vivo and in vitro. Such plant enzymatic pathways can then be reused to develop electronic systems in plantae without additional reagents. In the next work, we presented the synthesis of three new oligomers called ETE-N, EEE-S, and EEE-N that have a similar architecture compared to ETE-S but with different chemical moieties such as a different ionic side chain or an EDOT instead of thiophene in the middle position of the oligomer. We then demonstrated the effective enzymatic polymerization of these oligomers both in vivo and in vitro and how the resulting polymers' optoelectronic and tissue integrations properties differ. Towards even more versatility, we demonstrated that this electronic integration in vivo was also observed in the case of an animal: the freshwater hydra polyp. The polymerization was observed mostly in differentiated cells from the gastric column of the animal that normally secretes an adhesive used to fix the animal underwater. P(ETE-S) was incorporated in this glue that we managed to characterize using electrochemical methods. Lastly, we performed demonstrations of electrochemical applications with a plant root system. By dipping several roots in an ETE-S solution, we created a network of conducting roots that can effectively store charge as a capacitor with performance comparable to what is classically obtained with conducting polymers. In addition, we modified roots with two different surface modification concepts to make them specific to glucose oxidation: the first method uses a traditional redox hydrogel with a crosslinker and glucose oxidase. The second one uses the embedment of a glucosespecific enzyme inside the p(ETE-S) layer during its formation. These devices are presented as possible new solutions for environmental glucose sensors that could collect current from the environment and store it in neighbouring capacitive roots.

Overall, this thesis shows that the enzymatic activity of living systems can be used from an engineering point of view as part of a deposition methods for the development of biohybrid applications. 

Place, publisher, year, edition, pages
Linköping: Linköping University Electronic Press, 2022. p. 136
Series
Linköping Studies in Science and Technology. Dissertations, ISSN 0345-7524 ; 2255
Keywords
Conducting polymers, Living tissue engineering, In vivo polymerization, Plant Biohybrids, Hydra polyps, Energy storage, Glucose sensor
National Category
Polymer Chemistry
Identifiers
urn:nbn:se:liu:diva-189185 (URN)10.3384/9789179294861 (DOI)9789179294854 (ISBN)9789179294861 (ISBN)
Public defence
2022-11-11, K1, Kåkenhus, Campus Norrköping, Norrköping, 10:00 (English)
Opponent
Supervisors
Available from: 2022-10-12 Created: 2022-10-12 Last updated: 2022-10-13Bibliographically approved

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Dufil, GwennaelStrakosas, XenofonAbrahamsson, TobiasBerggren, MagnusStavrinidou, Eleni

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