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

Author:

Lim Carina Yi Jing,Yilmaz MeltemORCID,Arce-Ramos Juan ManuelORCID,Handoko Albertus D.ORCID,Teh Wei Jie,Zheng Yuangang,Khoo Zi Hui JonathanORCID,Lin MingORCID,Isaacs Mark,Tam Teck Lip Dexter,Bai YangORCID,Ng Chee KoonORCID,Yeo Boon SiangORCID,Sankar GopinathanORCID,Parkin Ivan P.,Hippalgaonkar Kedar,Sullivan Michael B.ORCID,Zhang JiaORCID,Lim Yee-FunORCID

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.

Funder

Agency for Science, Technology and Research

Ministry of Education - Singapore

National Research Foundation Singapore

Publisher

Springer Science and Business Media LLC

Subject

General Physics and Astronomy,General Biochemistry, Genetics and Molecular Biology,General Chemistry,Multidisciplinary

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