Steering the Absorption Configuration of Intermediates over Pd-Based Electrocatalysts toward Efficient and Stable CO2 Reduction

• DOI: 10.1021/jacs.4c14253
• Publication Date: 2025-01-24T19:24:18Z
• Authors: Shuting Wei; Yanchao Xu; Tao Song; Hao Dai; Fan Li; Xin Gao; Yanjie Zhai; Shanhe Gong; Rui Li; Xiao Zhang; Kangcheung Chan

Palladium (Pd) catalysts are promising for electrochemical reduction of CO2 to CO but often can be deactivated by poisoning owing the strong affinity *CO on Pd sites. Theoretical investigations reveal that different configurations endow specific adsorption energies, thereby dictating final performances. Here, a regulatory strategy toward absorption is proposed alleviate simultaneously incorporating Cu and Zn atoms into ultrathin nanosheets (NSs). As-prepared PdCuZn NSs catalyze production at wide potential window (−0.28 −0.78 V vs RHE) achieve maximum FECO 96% −0.35 V. Impressively, it exhibits stable 100 h under ∼95% with no decay. Combined results from X-ray analysis, in situ spectroscopy, theoretical simulations suggest codoping not only optimizes electronic structure also weakens binding strengths increases proportion weak-binding linear configuration catalysts' surfaces. Such targeted adoption weakly bound abates energy barrier desorption facilitates production. This work confers useful design tactic Pd-based electrocatalysts, steering highly selective CO2-to-CO conversion.