Understanding the Local Chemical Environment of Bioelectrocatalysis
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Authors
Edwardes Moore, Esther
Coito, Ana Margarida
Oliveira, Ana Rita
Pereira, Ines
Publication Date
2022-01-25Journal Title
Proceedings of the National Academy of Sciences of USA
ISSN
0027-8424
Publisher
National Academy of Sciences
Volume
119
Issue
4
Language
eng
Type
Article
This Version
VoR
Metadata
Show full item recordCitation
Edwardes Moore, E., Cobb, S., Coito, A. M., Oliveira, A. R., Pereira, I., & Reisner, E. (2022). Understanding the Local Chemical Environment of Bioelectrocatalysis. Proceedings of the National Academy of Sciences of USA, 119 (4) https://doi.org/10.1073/pnas.2114097119
Abstract
This work applies electrochemical and computational techniques to explore the local environment of fuel-producing oxidoreductases within porous electrode architectures. This improved understanding of the local environment enabled simple manipulation of the electrolyte solution, by adjusting the bulk pH and buffer pKa, to achieve an optimum local pH for maximal activity of the immobilised enzyme. When applied to macroporous inverse opal electrodes, the benefits of higher loading and increased mass transport were employed and, consequently, the electrolyte adjusted to reach −8.0 mA cm−2 for the H2 evolution reaction (HER) and −3.6 mA cm−2 for the CO2 reduction reaction (CO2RR), demonstrating an 18-fold improvement on previously reported enzymatic CO2RR systems.
Keywords
Enzymes, Bioelectrochemistry, Co2 Reduction, Hydrogen Evolution, Local Ph
Sponsorship
European Research Council (682833)
Leverhulme Trust (via Imperial College London) (P80336)
Identifiers
PMC8795565, 35058361
External DOI: https://doi.org/10.1073/pnas.2114097119
This record's URL: https://www.repository.cam.ac.uk/handle/1810/334309
Rights
Attribution-NonCommercial-NoDerivatives 4.0 International
Licence URL: https://creativecommons.org/licenses/by-nc-nd/4.0/
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