Experimental Demonstration of Topological Catalysis for CO2 Electroreduction

Xiangdong Kong; Zhao Liu; Zhigang Geng; An Zhang; Ziyang Guo; Shengtao Cui; Chuan Xia; Shijing Tan; Shiming Zhou; Zhengfei Wang; Jie Zeng

doi:10.1021/jacs.3c11088

Experimental Demonstration of Topological Catalysis for CO₂ Electroreduction

J Am Chem Soc. 2024 Mar 13;146(10):6536-6543. doi: 10.1021/jacs.3c11088. Epub 2024 Feb 27.

Authors

Xiangdong Kong¹, Zhao Liu¹, Zhigang Geng¹, An Zhang¹, Ziyang Guo¹, Shengtao Cui¹, Chuan Xia², Shijing Tan¹, Shiming Zhou¹, Zhengfei Wang¹, Jie Zeng^{1

3}

Affiliations

¹ Hefei National Research Center for Physical Sciences at the Microscale, Key Laboratory of Strongly-Coupled Quantum Matter Physics of Chinese Academy of Sciences, Key Laboratory of Surface and Interface Chemistry and Energy Catalysis of Anhui Higher Education Institutes, Department of Chemical Physics, Hefei National Laboratory, University of Science and Technology of China, Hefei, Anhui 230026, P. R. China.
² School of Materials and Energy, University of Electronic Science and Technology of China, Chengdu, Sichuan 611731, P. R. China.
³ School of Chemistry & Chemical Engineering, Anhui University of Technology, Ma'anshan, Anhui 243002, P. R. China.

PMID: 38412553
DOI: 10.1021/jacs.3c11088

Abstract

The past decade has witnessed substantial progress in understanding nontrivial band topology and discovering exotic topological materials in condensed-matter physics. Recently, topological physics has been further extended to the chemistry discipline, leading to the emergence of topological catalysis. In principle, the topological effect is detectable in catalytic reactions, but no conclusive evidence has been reported yet. Herein, by precisely manipulating the topological surface state (TSS) of Bi₂Se₃ nanosheets through thickness control and the application of a magnetic field, we provide direct experimental evidence to illustrate topological catalysis for CO₂ electroreduction. With and without the cooperation of TSS, CO₂ is mainly reduced into liquid fuels (HCOOH and H₂C₂O₄) and CO, exhibiting high (up to 90% at -1.1 V versus reversible hydrogen electrode) and low Faradaic efficiency (FE), respectively. Theoretically, the product and FE difference can be attributed to the TSS-regulated adsorption of key intermediates and the reduced barrier of the potential-determining step. Our work demonstrates the inherent correlation between band topology and electrocatalysis, paving a new avenue for designing high-performance catalysts.