Pd-Based Multi-Site Catalysts for Selective CO2-to-Methanol Conversion

Abstract

Developing a multi-site Pd-based electrocatalyst for CO₂-to-C1 conversion with high performance and selectivity in the hydrogenation pathway for the CO₂ electroreduction reaction is both desirable and challenging. Here, we develop triple-site metallene (Pd₈₂Bi₁₁In₇), which can achieve an unprecedented Faraday efficiency of 72.6 ± 1% for methanol production. X-ray photoelectron spectroscopy analysis indicates that some electrons transfer from In and Bi to Pd inside Pd₈₂Bi₁₁In₇, forming local electron-rich Pd-site, local primary electron-deficient center In-site, and local secondary electron-deficient center Bi-site. Meanwhile, Pd₈₂Bi₁₁In₇ has stronger adsorption for *COOH and *CO, which avoids the generation of formic acid and CO. Moreover, Pd₈₂Bi₁₁In₇ reduces the potential determining step energy barrier and controls the hydrogenation path for direct methanol production. The synergistic effect of the triple-sites enables efficient CO₂ electroreduction to methanol.