Liquid Fluxional Ga Single Atom Catalysts for Efficient Electrochemical CO2 Reduction

• Published in: Angewandte Chemie International Edition Vol. 62; no. 3; pp. e202215136 - n/a
• Main Authors: Zhang, Zedong, Zhu, Jiexin, Chen, Shenghua, Sun, Wenming, Wang, Dingsheng
• Format: Journal Article
• Language: English
• Published: Weinheim Wiley Subscription Services, Inc 16.01.2023
• Edition: International ed. in English
• Subjects: Atomic properties; Atomic structure; Carbon dioxide; Catalysis; Catalysts; Chemical synthesis; CO2RR; Dynamic stability; Electrochemistry; Fluxional Single Atom Catalysts; Gallium; Interface stability; Interfaces; Liquid Metal Ga; Reduction; Selectivity; Single atom catalysts
• ISSN: 1433-7851; 1521-3773
• DOI: 10.1002/anie.202215136

Precise design and tuning of the micro‐atomic structure of single atom catalysts (SACs) can help efficiently adapt complex catalytic systems. Herein, we inventively found that when the active center of the main group element gallium (Ga) is downsized to the atomic level, whose characteristic has significant differences from conventional bulk and rigid Ga catalysts. The Ga SACs with a P, S atomic coordination environment display specific flow properties, showing CO products with FE of ≈92 % at −0.3 V vs. RHE in electrochemical CO2 reduction (CO2RR). Theoretical simulations demonstrate that the adaptive dynamic transition of Ga optimizes the adsorption energy of the *COOH intermediate and renews the active sites in time, leading to excellent CO2RR selectivity and stability. This liquid single atom catalysts system with dynamic interfaces lays the foundation for future exploration of synthesis and catalysis. In this research, we discover the fluxional property of single atom catalysts (SACs) could effectively influence the catalytic performance. Ga SACs was firstly systematically synthesized to be used in efficient electrochemical CO2 reduction for CO. The Ga SACs with the P, S atomic coordination environment displays specific fluxional properties, showing CO products with FE of ≈92 % at −0.3 V vs. RHE in electrochemical CO2 reduction.