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

Carina Yi Jing Lim, Meltem Yilmaz, Juan Manuel Arce-Ramos, Albertus D. Handoko (), Wei Jie Teh, Yuangang Zheng, Zi Hui Jonathan Khoo, Ming Lin, Mark Isaacs, Teck Lip Dexter Tam, Yang Bai, Chee Koon Ng, Boon Siang Yeo, Gopinathan Sankar, Ivan P. Parkin, Kedar Hippalgaonkar, Michael B. Sullivan, Jia Zhang () and Yee-Fun Lim ()
Additional contact information
Carina Yi Jing Lim: Agency for Science, Technology and Research (A*STAR)
Meltem Yilmaz: Agency for Science, Technology and Research (A*STAR)
Juan Manuel Arce-Ramos: Agency for Science, Technology and Research (A*STAR)
Albertus D. Handoko: Agency for Science, Technology and Research (A*STAR)
Wei Jie Teh: National University of Singapore
Yuangang Zheng: Agency for Science, Technology and Research (A*STAR)
Zi Hui Jonathan Khoo: Agency for Science, Technology and Research (A*STAR)
Ming Lin: Agency for Science, Technology and Research (A*STAR)
Mark Isaacs: Rutherford Appleton Laboratory
Teck Lip Dexter Tam: Agency of Science, Technology and Research (A*STAR)
Yang Bai: Agency for Science, Technology and Research (A*STAR)
Chee Koon Ng: Agency for Science, Technology and Research (A*STAR)
Boon Siang Yeo: National University of Singapore
Gopinathan Sankar: University College London
Ivan P. Parkin: University College London
Kedar Hippalgaonkar: Agency for Science, Technology and Research (A*STAR)
Michael B. Sullivan: Agency for Science, Technology and Research (A*STAR)
Jia Zhang: Agency for Science, Technology and Research (A*STAR)
Yee-Fun Lim: Agency for Science, Technology and Research (A*STAR)

Nature Communications, 2023, vol. 14, issue 1, 1-11

Abstract: Abstract Intensive 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.

Date: 2023
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DOI: 10.1038/s41467-023-35912-7

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