Liu, Yongpeng; Webb, Sophie; Moreno-García, Pavel; Kulkarni, Amogh; Maroni, Plinio; Broekmann, Peter; Milton, Ross D (2023). Facile Functionalization of Carbon Electrodes for Efficient Electroenzymatic Hydrogen Production. JACS Au, 3(1), pp. 124-130. ACS Publications 10.1021/jacsau.2c00551
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Enzymatic electrocatalysis holds promise for new biotechnological approaches to produce chemical commodities such as molecular hydrogen (H2). However, typical inhibitory limitations include low stability and/or low electrocatalytic currents (low product yields). Here we report a facile single-step electrode preparation procedure using indium-tin oxide nanoparticles on carbon electrodes. The subsequent immobilization of a model [FeFe]-hydrogenase from Clostridium pasteurianum ("CpI") on the functionalized carbon electrode permits comparatively large quantities of H2 to be produced in a stable manner. Specifically, we observe current densities of >8 mA/cm2 at -0.8 V vs the standard hydrogen electrode (SHE) by direct electron transfer (DET) from cyclic voltammetry, with an onset potential for H2 production close to its standard potential at pH 7 (approximately -0.4 V vs. SHE). Importantly, hydrogenase-modified electrodes show high stability retaining ∼92% of their electrocatalytic current after 120 h of continuous potentiostatic H2 production at -0.6 V vs. SHE; gas chromatography confirmed ∼100% Faradaic efficiency. As the bioelectrode preparation method balances simplicity, performance, and stability, it paves the way for DET on other electroenzymatic reactions as well as semiartificial photosynthesis.
Item Type: |
Journal Article (Original Article) |
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Division/Institute: |
08 Faculty of Science > Department of Chemistry, Biochemistry and Pharmaceutical Sciences (DCBP) |
UniBE Contributor: |
Moreno, Pavel, Broekmann, Peter |
Subjects: |
500 Science > 570 Life sciences; biology 500 Science > 540 Chemistry |
ISSN: |
2691-3704 |
Publisher: |
ACS Publications |
Language: |
English |
Submitter: |
Pubmed Import |
Date Deposited: |
31 Jan 2023 13:29 |
Last Modified: |
01 Feb 2023 15:24 |
Publisher DOI: |
10.1021/jacsau.2c00551 |
PubMed ID: |
36711103 |
BORIS DOI: |
10.48350/178134 |
URI: |
https://boris.unibe.ch/id/eprint/178134 |