Cao Yucheng, Chen Suya, Bo Shuowen, Fan Wenjun, Li Jiangnan, Jia Chunmei, Zhou Zhen, Liu Qinghua, Zheng Lirong, Zhang Fuxiang
State Key Laboratory of Catalysis, Dalian Institute of Chemical Physics, Chinese Academy of Sciences, Dalian National Laboratory for Clean Energy, Dalian, 116023, Liaoning, China.
Center of Materials Science and Optoelectronics Engineering, University of Chinese Academy of Sciences, Beijing, 100049, China.
Angew Chem Int Ed Engl. 2023 Jul 24;62(30):e202303048. doi: 10.1002/anie.202303048. Epub 2023 Jun 16.
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 (CO ) into multi-carbon (C ) 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 CO reduction into C products instead of previous C ones. The BiCu-SAA catalyst exhibits remarkably superior selectivity of C 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 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 CO and subsequent C-C coupling during the electrocatalytic reaction, as should be responsible for its extraordinary C selectivity.
单原子合金（SAA）催化剂最近已被用于促进各种多相催化反应，但在涉及C-C偶联的将二氧化碳（CO₂）选择性电催化还原为多碳（C₂⁺）产物方面尚未得到探索。在此，我们报道了一种单原子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，而不是之前的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催化剂对C₂⁺产物表现出显著优异的选择性，最佳法拉第效率（FE）为73.4%，并且在流动池系统下，其结构和性能在400 mA cm⁻²的电流密度下可以得到很好的保持。基于我们的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。
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