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

2023; Nature Portfolio; Volume: 14; Issue: 1 Linguagem: Inglês

10.1038/s41467-023-35912-7

2041-1723

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 A. 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, Yee‐Fun Lim,

Electrocatalysts for Energy Conversion

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.