Liquid Fluxional Ga Single Atom Catalysts for Efficient Electrochemical CO2 Reduction

Abstract

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 (CO₂ RR). 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 CO₂ RR selectivity and stability. This liquid single atom catalysts system with dynamic interfaces lays the foundation for future exploration of synthesis and catalysis.

Keywords: CO2RR; Fluxional Single Atom Catalysts; Liquid Metal Ga.