中国科学院大连化学物理研究所章福祥团队报道了单原子Bi修饰铜合金实现电催化还原CO₂为C2+产物的C-C偶联。相关研究成果发表在2023年5月30日出版的《德国应用化学》。

单原子合金（SAA）催化剂最近已被探索用于促进各种多相催化，但其在涉及C-C偶联的二氧化碳（CO₂）选择性电催化还原为多碳（C2+）产物方面仍未被探索。

该文中，研究人员报道了一种单原子Bi修饰的Cu合金（表示为BiCu-SAA）电催化剂，它可以有效地调节CO₂还原为C2+产物的选择性，而不是以前的C1产物。与纯铜纳米颗粒或Bi纳米颗粒修饰的Cu纳米复合材料相比，BiCu-SAA催化剂表现出显著优异的C2+产物选择性，最佳法拉第效率（FE）为73.4%，并且在流动池系统下，其结构和性能可以在400mA cm^-2的电流密度下很好地保持。基于原位表征和密度泛函理论计算，发现BiCu-SAA在电催化反应过程中有利于CO₂的活化和随后的C-C偶联，这应该是其非凡的C2+选择性的原因。

附：英文原文

Title: Single Atom Bi Decorated Copper Alloy Enables C-C Coupling for Electrocatalytic Reduction of CO2 into C2+ Products

Author: Yucheng Cao, Suya Chen, Shuowen Bo, Wenjun Fan, Jiangnan Li, Chunmei Jia, Zhen Zhou, Qinghua Liu, Lirong Zheng, Fuxiang Zhang

Issue&Volume: 2023-05-30

Abstract: Single atom alloy (SAA) catalysts have been recently explored for promotion of various heterogeneous catalysis, but it remains unexplored for selective electrocatalytic reduction of carbon dioxide (CO2) into multi-carbon (C2+) products involving C-C coupling. Herein we report a single-atomic Bi decorated Cu alloy (denoted as BiCu-SAA) electrocatalyst that could effectively modulate selectivity of CO2 reduction into C2+ products instead of previous C1 ones. The BiCu-SAA catalyst exhibits remarkably superior selectivity of C2+ products with optimal Faradaic efficiency (FE) of 73.4% compared to the pure copper nanoparticle or Bi nanoparticles-decorated Cu nanocomposites, and its structure and performance can be well maintained at current density of 400 mA cm-2 under the flow cell system. Based on our in-situ characterizations and density functional theory calculations, the BiCu-SAA is found to favor the activation of CO2 and subsequent C-C coupling during the electrocatalytic reaction, as should be responsible for its extraordinary C2+ selectivity.

DOI: 10.1002/anie.202303048

Source: https://onlinelibrary.wiley.com/doi/10.1002/anie.202303048