PdAg bimetallic electrocatalyst for highly selective reduction of CO2 with low COOH* formation energy and facile CO desorption
CO2 reduction, bimetallic, low overpotential, CO desorption
For electrocatalytic reduction of CO2 to CO, the stabilization of intermediate COOH* and the desorption of CO* are two key steps. Pd can easily stabilize COOH*, whereas the strong CO* binding to Pd surface results in severe poisoning, thus lowering catalytic activity and stability for CO2 reduction. On Ag surface, CO* desorbs readily, while COOH* requires a relatively high formation energy, leading to a high overpotential. In light of the above issues, we successfully designed the PdAg bimetallic catalyst to circumvent the drawbacks of sole Pd and Ag. The PdAg catalyst with Ag-terminated surface not only shows a much lower overpotential (−0.55 V with CO current density of 1 mA/cm2) than Ag (−0.76 V), but also delivers a CO/H2 ratio 18 times as high as that for Pd at the potential of −0.75 V vs. RHE. The issue of CO poisoning is significantly alleviated on Ag-terminated PdAg surface, with the stability well retained after 4 h electrolysis at −0.75 V vs. RHE. Density functional theory (DFT) calculations reveal that the Ag-terminated PdAg surface features a lowered formation energy for COOH* and weakened adsorption for CO*, which both contribute to the enhanced performance for CO2 reduction.
Tsinghua University Press
Rui Lin,Xuelu Ma,Weng-Chon Cheong,Chao Zhang,Wei Zhu,Jiajing Pei,Kaiyue Zhang,Bin Wang,Shiyou Liang,Yuxi Liu,Zhongbin Zhuang,Rong Yu,Hai Xiao,Jun Li,Dingsheng Wang,Qing Peng,Chen Chen,Yadong Li, PdAg bimetallic electrocatalyst for highly selective reduction of CO2 with low COOH* formation energy and facile CO desorption. NanoRes.2019, 12(11): 2866–2871