Issue 9, 2023

A topological chemical transition strategy of bismuth-based materials for high-efficiency electrocatalytic carbon dioxide conversion to formate

Abstract

The electrochemical reduction of carbon dioxide (ERCO2) to formate with high selectivity has been considered a promising strategy to overcome the energy and environmental crises. Bi-based materials present good application prospects, but the development of a new class of electrocatalysts with high performance remains a challenge. Herein, a novel topological chemical transition strategy is developed to rationally design highly active Bi-based materials, which are a new representative of Bi-based electrocatalysts for ERCO2. Bismuth oxysulfate (Bi2O2SO4) is prepared by a simple topological transition from the Bi2S3 precursor in air, which can further topologically transform into the metal Bi by a fast reduction treatment of NaBH4 solution. This kind of Bi2O2SO4 exhibits superior catalytic performance for ERCO2. The maximum Faraday efficiency (FE) of HCOO is up to 97% at −0.9 V vs. RHE in an H-type cell. A high FE > 90% in a wide potential range of −0.5 to −1.2 V and a large current density of 319 mA cm−2 at −0.8 V can further be realized in a flow cell. The post-characterization studies and density functional theory (DFT) calculations confirm that the Bi2O2SO4 derived Bi catalyst has an optimal (104) plane to realize the optimized free energies of OCHO* and H* reaction intermediates, leading to superior catalytic activity over the NaBH4 derived Bi sample. Our work put forward a promising strategy to exploit advanced electrocatalysts for electrolysis.

Graphical abstract: A topological chemical transition strategy of bismuth-based materials for high-efficiency electrocatalytic carbon dioxide conversion to formate

Supplementary files

Article information

Article type
Paper
Submitted
01 Nov 2022
Accepted
22 Dec 2022
First published
22 Dec 2022

J. Mater. Chem. A, 2023,11, 4691-4702

A topological chemical transition strategy of bismuth-based materials for high-efficiency electrocatalytic carbon dioxide conversion to formate

R. Ye, Y. Tong, D. Feng and P. Chen, J. Mater. Chem. A, 2023, 11, 4691 DOI: 10.1039/D2TA08521F

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