Pd–Ag Alloy Electrocatalysts for CO₂ Reduction: Composition Tuning to Break the Scaling Relationship
2019
Zeng, Jiachang | Zhang, Wenbiao | Yang, Yang | Li, Dan | Yu, Xiang | Gao, Qingsheng
Constructing solid-solution-alloy electrocatalysts with tunable surface electronic configurations is the key to optimize intermediate bindings and thereby to promote the activity and selectivity of the CO₂ reduction reaction (CO₂RR). Herein, Pd₁–ₓAgₓ alloy electrocatalysts are investigated as a platform to uncover the electronic effects on the CO₂RR. The optimal Pd₀.₇₅Ag₀.₂₅/C affords a superior CO Faradaic efficiency of 95.3% at −0.6 V (vs RHE) in 0.5 M KHCO₃, performing at a high level among recently reported electrocatalysts. Experimental and theoretical analysis further evidence that varying the composition of Pd₁–ₓAgₓ alloys can effectively alter the electronic configurations and consequently break the inherent scaling relationship of the binding energy of different intermediates (*COOH and *CO). Among Pd₁–ₓAgₓ, Pd₀.₇₅Ag₀.₂₅ gains the obviously weakened *CO and *H bindings but retained well the binding with *COOH, contributing to the facilitated kinetics toward CO product. Elucidating a feasible way to break the scaling relationship and further uncover the underlying mechanism, this work will inspire new design strategies toward active and selective electrocatalysts.
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