Energetic Control of Redox-Active Polymers toward Safe Organic Bioelectronic Materials

Alexander Giovannitti; Reem B. Rashid; Quentin Thiburce; Bryan D. Paulsen; Camila Cendra; Karl Thorley; Davide Moia; J. Tyler Mefford; David Hanifi; Du Weiyuan; Maximilian Moser; Alberto Salleo; Jenny Nelson; Iain McCulloch; Jonathan Rivnay

doi:10.1002/adma.201908047

Energetic Control of Redox-Active Polymers toward Safe Organic Bioelectronic Materials

Alexander Giovannitti^*, Reem B. Rashid, Quentin Thiburce, Bryan D. Paulsen, Camila Cendra, Karl Thorley, Davide Moia, J. Tyler Mefford, David Hanifi, Du Weiyuan, Maximilian Moser, Alberto Salleo, Jenny Nelson, Iain McCulloch, Jonathan Rivnay

^*Corresponding author for this work

Biomedical Engineering

Research output: Contribution to journal › Article › peer-review

158 Scopus citations

Abstract

Avoiding faradaic side reactions during the operation of electrochemical devices is important to enhance the device stability, to achieve low power consumption, and to prevent the formation of reactive side-products. This is particularly important for bioelectronic devices, which are designed to operate in biological systems. While redox-active materials based on conducting and semiconducting polymers represent an exciting class of materials for bioelectronic devices, they are susceptible to electrochemical side-reactions with molecular oxygen during device operation. Here, electrochemical side reactions with molecular oxygen are shown to occur during organic electrochemical transistor (OECT) operation using high-performance, state-of-the-art OECT materials. Depending on the choice of the active material, such reactions yield hydrogen peroxide (H₂O₂), a reactive side-product, which may be harmful to the local biological environment and may also accelerate device degradation. A design strategy is reported for the development of redox-active organic semiconductors based on donor–acceptor copolymers that prevents the formation of H₂O₂ during device operation. This study elucidates the previously overlooked side-reactions between redox-active conjugated polymers and molecular oxygen in electrochemical devices for bioelectronics, which is critical for the operation of electrolyte-gated devices in application-relevant environments.

Original language	English (US)
Article number	1908047
Journal	Advanced Materials
Volume	32
Issue number	16
DOIs	https://doi.org/10.1002/adma.201908047
State	Published - Apr 1 2020

Funding

The authors thank Eric Daniel Głowacki for fruitful discussions about oxygen reduction reactions. A.G, J.N., and I.M. acknowledge funding from Engineering and Physical Sciences Research Council (EPSRC) project EP/G037515/1, EP/N509486/1; D.M. and J.N. are grateful for receiving funding from EPSRC project Supersolar Hub EP/P02484X/1; and J.N. acknowledges funding from the European Research Council (ERC) (grant agreement No 742708). A.G. and A.S. acknowledge funding from the TomKat Center for Sustainable Energy at Stanford University. Part of this work was performed at the Stanford Nanofabrication Facilities (SNF) and Stanford Nano Shared Facilities (SNSF), supported by the National Science Foundation as part of the National Nanotechnology Coordinated Infrastructure under award ECCS‐1542152. J.R. and B.P. acknowledge funding from the National Science Foundation (grant no. NSF DMR‐1751308). This work utilized Northwestern University Micro/Nano Fabrication Facility (NUFAB) and the Keck‐II facility of NUANCE Center, which is partially supported by Soft and Hybrid Nanotechnology Experimental (SHyNE) Resource (NSF ECCS‐1542205), the Materials Research Science and Engineering Center (DMR‐1720139) at the Materials Research Center, the State of Illinois, and Northwestern University. NUANCE was further supported by the International Institute for Nanotechnology (IIN); and the Keck Foundation. Measurements at Stanford Synchrotron Radiation Lightsource, SLAC National Accelerator Laboratory, were supported by the U.S. Department of Energy, Office of Science, Office of Basic Energy Sciences under Contract No. DE‐AC02‐76SF00515. The authors thank Eric Daniel Głowacki for fruitful discussions about oxygen reduction reactions. A.G, J.N., and I.M. acknowledge funding from Engineering and Physical Sciences Research Council (EPSRC) project EP/G037515/1, EP/N509486/1; D.M. and J.N. are grateful for receiving funding from EPSRC project Supersolar Hub EP/P02484X/1; and J.N. acknowledges funding from the European Research Council (ERC) (grant agreement No 742708). A.G. and A.S. acknowledge funding from the TomKat Center for Sustainable Energy at Stanford University. Part of this work was performed at the Stanford Nanofabrication Facilities (SNF) and Stanford Nano Shared Facilities (SNSF), supported by the National Science Foundation as part of the National Nanotechnology Coordinated Infrastructure under award ECCS-1542152. J.R. and B.P. acknowledge funding from the National Science Foundation (grant no. NSF DMR-1751308). This work utilized Northwestern University Micro/Nano Fabrication Facility (NUFAB) and the Keck-II facility of NUANCE Center, which is partially supported by Soft and Hybrid Nanotechnology Experimental (SHyNE) Resource (NSF ECCS-1542205), the Materials Research Science and Engineering Center (DMR-1720139) at the Materials Research Center, the State of Illinois, and Northwestern University. NUANCE was further supported by the International Institute for Nanotechnology (IIN); and the Keck Foundation. Measurements at Stanford Synchrotron Radiation Lightsource, SLAC National Accelerator Laboratory, were supported by the U.S. Department of Energy, Office of Science, Office of Basic Energy Sciences under Contract No. DE-AC02-76SF00515.

Keywords

bioelectronics
donor–acceptor copolymers
electrochemical transistors
organic mixed ionic/electronic conductors
oxygen reduction reaction

ASJC Scopus subject areas

General Materials Science
Mechanics of Materials
Mechanical Engineering

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Cite this

Giovannitti, A., Rashid, R. B., Thiburce, Q., Paulsen, B. D., Cendra, C., Thorley, K., Moia, D., Mefford, J. T., Hanifi, D., Weiyuan, D., Moser, M., Salleo, A., Nelson, J., McCulloch, I., & Rivnay, J. (2020). Energetic Control of Redox-Active Polymers toward Safe Organic Bioelectronic Materials. Advanced Materials, 32(16), Article 1908047. https://doi.org/10.1002/adma.201908047

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Energetic Control of Redox-Active Polymers toward Safe Organic Bioelectronic Materials

Abstract

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Keywords

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