Facile Functionalization of Carbon Electrodes for Efficient Electroenzymatic Hydrogen Production.

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

[img] Text
jacsau.2c00551.pdf - Published Version
Restricted to registered users only
Available under License Publisher holds Copyright.

Download (3MB)

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)

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

Actions (login required)

Edit item Edit item
Provide Feedback