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

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. In this work, 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.

Authors:
ORCiD logo [1];  [2];  [3];  [2];  [3];  [4];  [4];  [3];  [3];  [5];  [4];  [3];  [4];  [6];  [2]
  1. Imperial College, London (United Kingdom); Stanford Univ., CA (United States)
  2. Northwestern Univ., Evanston, IL (United States)
  3. Stanford Univ., CA (United States)
  4. Imperial College, London (United Kingdom)
  5. King Abdullah Univ. of Science and Technology (KAUST), Thuwal (Saudi Arabia)
  6. Imperial College, London (United Kingdom); King Abdullah Univ. of Science and Technology (KAUST), Thuwal (Saudi Arabia)
Publication Date:
Research Org.:
SLAC National Accelerator Lab., Menlo Park, CA (United States). Stanford Synchrotron Radiation Lightsource (SSRL)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES); Engineering and Physical Sciences Research Council (EPSRC); European Research Council (ERC); National Science Foundation (NSF); Soft and Hybrid Nanotechnology Experimental (SHyNE) Resource; International Institute for Nanotechnology (IIN); Keck Foundation
OSTI Identifier:
1608344
Alternate Identifier(s):
OSTI ID: 1602602
Grant/Contract Number:  
742708; ECCS‐1542152; DMR‐1751308; DMR‐1720139; AC02-76SF00515
Resource Type:
Accepted Manuscript
Journal Name:
Advanced Materials
Additional Journal Information:
Journal Volume: 32; Journal Issue: 16; Journal ID: ISSN 0935-9648
Publisher:
Wiley
Country of Publication:
United States
Language:
English
Subject:
36 MATERIALS SCIENCE; bioelectronics; donor–acceptor copolymers; electrochemical transistors; organic mixed ionic/electronic conductors; oxygen reduction reaction

Citation Formats

Giovannitti, Alexander, Rashid, Reem B., Thiburce, Quentin, Paulsen, Bryan D., Cendra, Camila, Thorley, Karl, Moia, Davide, Mefford, J. Tyler, Hanifi, David, Weiyuan, Du, Moser, Maximilian, Salleo, Alberto, Nelson, Jenny, McCulloch, Iain, and Rivnay, Jonathan. Energetic Control of Redox-Active Polymers toward Safe Organic Bioelectronic Materials. United States: N. p., 2020. Web. doi:10.1002/adma.201908047.
Giovannitti, Alexander, Rashid, Reem B., Thiburce, Quentin, Paulsen, Bryan D., Cendra, Camila, Thorley, Karl, Moia, Davide, Mefford, J. Tyler, Hanifi, David, Weiyuan, Du, Moser, Maximilian, Salleo, Alberto, Nelson, Jenny, McCulloch, Iain, & Rivnay, Jonathan. Energetic Control of Redox-Active Polymers toward Safe Organic Bioelectronic Materials. United States. doi:https://doi.org/10.1002/adma.201908047
Giovannitti, Alexander, Rashid, Reem B., Thiburce, Quentin, Paulsen, Bryan D., Cendra, Camila, Thorley, Karl, Moia, Davide, Mefford, J. Tyler, Hanifi, David, Weiyuan, Du, Moser, Maximilian, Salleo, Alberto, Nelson, Jenny, McCulloch, Iain, and Rivnay, Jonathan. Tue . "Energetic Control of Redox-Active Polymers toward Safe Organic Bioelectronic Materials". United States. doi:https://doi.org/10.1002/adma.201908047. https://www.osti.gov/servlets/purl/1608344.
@article{osti_1608344,
title = {Energetic Control of Redox-Active Polymers toward Safe Organic Bioelectronic Materials},
author = {Giovannitti, Alexander and Rashid, Reem B. and Thiburce, Quentin and Paulsen, Bryan D. and Cendra, Camila and Thorley, Karl and Moia, Davide and Mefford, J. Tyler and Hanifi, David and Weiyuan, Du and Moser, Maximilian and Salleo, Alberto and Nelson, Jenny and McCulloch, Iain and Rivnay, Jonathan},
abstractNote = {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. In this work, 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.},
doi = {10.1002/adma.201908047},
journal = {Advanced Materials},
number = 16,
volume = 32,
place = {United States},
year = {2020},
month = {3}
}

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