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

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 selec...

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Bibliographic Details
Main Authors: Lim, Carina Yi Jing, Yilmaz, Meltem, Arce-Ramos, Juan Manuel, Handoko, Albertus D., Teh, Wei Jie, Zheng, Yuangang, Khoo, Jonathan Zi Hui, Lin, Ming, Isaacs, Mark, Tam, Dexter Teck Lip, Bai, Yang, Ng, Chee Koon, Yeo, Boon Siang, Sankar, Gopinathan, Parkin, Ivan P., Hippalgaonkar, Kedar, Sullivan, Michael B., Zhang, Jia, Lim, Yee-Fun
Other Authors: School of Materials Science and Engineering
Format: Journal Article
Language:English
Published: 2023
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Online Access:https://hdl.handle.net/10356/169752
Description
Summary: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.