中国科学技术大学曾杰团队报道了CO₂电还原拓扑催化的实验验证。相关研究成果发表在2024年2月27日出版的《美国化学会杂志》。

在过去的十年里，凝聚态物理学在理解非平凡能带拓扑和发现奇异拓扑材料方面取得了重大进展。最近，拓扑物理学进一步扩展到化学学科，导致了拓扑催化的出现。原则上，拓扑效应在催化反应中是可以检测到的，但还没有确凿的证据报道。

该文中，通过厚度控制和磁场的应用，精确控制Bi₂Se₃纳米片的拓扑表面状态（TSS），研究人员提供了直接的实验证据来说明拓扑催化对CO₂电还原的作用。在TSS的配合和不配合下，CO₂主要被还原为液体燃料（HCOOH和H₂C₂O₄）和CO，分别表现出高（在1.1V下相对于可逆氢电极高达90%）和低法拉第效率（FE）。理论上，产物和FE的差异可归因于TSS调节的关键中间体的吸附和电位决定步骤的势垒降低。

该工作证明了能带拓扑结构与电催化之间的内在相关性，为设计高性能催化剂铺平了新的途径。

附：英文原文

Title: Experimental Demonstration of Topological Catalysis for CO2 Electroreduction

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

Issue&Volume: February 27, 2024

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.

DOI: 10.1021/jacs.3c11088

Source: https://pubs.acs.org/doi/abs/10.1021/jacs.3c11088