Surface charge as activity descriptors for electrochemical CO2 reduction to multi-carbon products on organic-functionalised Cu

Page view(s)
70
Checked on Jan 15, 2025
Surface charge as activity descriptors for electrochemical CO2 reduction to multi-carbon products on organic-functionalised Cu
Title:
Surface charge as activity descriptors for electrochemical CO2 reduction to multi-carbon products on organic-functionalised Cu
Journal Title:
Nature Communications
Publication Date:
20 January 2023
Citation:
Lim, C. Y. J., Yilmaz, M., Arce-Ramos, J. M., Handoko, A. D., Teh, W. J., Zheng, Y., Khoo, Z. H. J., Lin, M., Isaacs, M., Tam, T. L. D., Bai, Y., Ng, C. K., Yeo, B. S., Sankar, G., Parkin, I. P., Hippalgaonkar, K., Sullivan, M. B., Zhang, J., & Lim, Y.-F. (2023). Surface charge as activity descriptors for electrochemical CO2 reduction to multi-carbon products on organic-functionalised Cu. Nature Communications, 14(1). https://doi.org/10.1038/s41467-023-35912-7
Abstract:
AbstractIntensive research in electrochemical CO2 reduction reaction has resulted in the discovery of numerous high-performance catalysts selective to multi-carbon products, with most of these catalysts still being purely transition metal based. Herein, we present high and stable multi-carbon products selectivity of up to 76.6% across a wide potential range of 1 V on histidine-functionalised Cu. In-situ Raman and density functional theory calculations revealed alternative reaction pathways that involve direct interactions between adsorbed histidine and CO2 reduction intermediates at more cathodic potentials. Strikingly, we found that the yield of multi-carbon products is closely correlated to the surface charge on the catalyst surface, quantified by a pulsed voltammetry-based technique which proved reliable even at very cathodic potentials. We ascribe the surface charge to the population density of adsorbed species on the catalyst surface, which may be exploited as a powerful tool to explain CO2 reduction activity and as a proxy for future catalyst discovery, including organic-inorganic hybrids.
License type:
Attribution 4.0 International (CC BY 4.0)
Funding Info:
This research / project is supported by the A*STAR - Accelerated Catalysis Development Platform
Grant Reference no. : A19E9a0103

This research / project is supported by the A*STAR - Career Development Award
Grant Reference no. : 202D800037

This research / project is supported by the National Research Foundation, Singapore, and A*STAR - LCERFI Program
Grant Reference no. : U2102d2002

This research / project is supported by the National University of Singapore - Faculty Research Committee (FRC)
Grant Reference no. : A-0004135-00-00

This research / project is supported by the A*STAR - Accelerated Materials Development for Manufacturing
Grant Reference no. : A1898b0043
Description:
ISSN:
2041-1723
Files uploaded:

File Size Format Action
s41467-023-35912-7.pdf 3.55 MB PDF Open
File Size Format Action
cu-histidine-data-upload.zip 120.79 MB ZIP Request a copy