Issue 3, 2024

Covalency-aided electrochemical CO2 reduction to CO on sulfide-derived Cu–Sb

Abstract

p-Block dopants like sulfur have been shown to break scaling relations in the electrocatalytic CO2 reduction reaction (CO2RR) by providing alternative binding sites with altered *CO binding energy. However, most sulfide-derived catalysts reported to date tend to produce formate or hydrogen during the CO2RR by shifting the reaction pathway away from C-bound intermediates. In this work, we discovered highly selective CO production on a bimetallic Cu–Sb–S derived catalyst. The high CO selectivity is in contrast with the individual control samples of CuSx and SbSx that demonstrate a preference towards the formate product. Interestingly, different starting phases and atomic ratios of Cu–Sb–S affect the CO2RR selectivity. Post-catalysis characterization coupled with DFT calculations indicates that the key enabler towards CO formation is the substitution of Sb sites with sulfur which improves *COOH binding relative to *CO, breaking scaling relations and facilitating subsequent CO (g) formation. The highest CO production of FECO = 80.5% was observed on the tetrahedrite Cu–Sb–S-derived sample at −1.0 V RHE with 37.6 mA cm−2 geometric partial current density.

Graphical abstract: Covalency-aided electrochemical CO2 reduction to CO on sulfide-derived Cu–Sb

Supplementary files

Article information

Article type
Paper
Submitted
10 Aug 2023
Accepted
30 Nov 2023
First published
22 Dec 2023

J. Mater. Chem. A, 2024,12, 1840-1851

Covalency-aided electrochemical CO2 reduction to CO on sulfide-derived Cu–Sb

D. Y. Y. Goh, K. M. Yam, L. Rekhi, A. D. Handoko, Y. C. Tan, Y. Wang, J. M. R. Tan, T. S. Choksi, Y. Lum and L. H. Wong, J. Mater. Chem. A, 2024, 12, 1840 DOI: 10.1039/D3TA04777F

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