Synergism of Hydrogen-Induced Interstitial Effect and Gold-Induced Alloying Effect in PdAuH Metallene for Urea Electrosynthesis from Nitrate and Carbon Dioxide
You Xu, Junjie Wang, Youwei Sheng, Yueji Wu, Qiqi Mao, Kai Deng, Hongjie Yu, Liang Wang, Hongjing Wang
Abstract
Urea is a common agricultural fertilizer and industrial raw material, but at present, the traditional industrial production of urea is energy-and pollution-intensive. Electrocatalytic coupling of CO 2 and ubiquitous nitrogen sources to synthesize urea is considered as a promising alternative method but requiring high-performance catalysts to boost the C–N coupling electrocatalysis process. Herein, hydrogen-intercalated Pd–Au bimetallene (PdAuHene) was prepared by a three-step method and used for electrosynthesis of urea from NO 3 – and CO 2, deriving an optimum urea Faradaic efficiency of 33.88% and yield rate of 6.68 mmol g –1 h –1 at an applied potential of −0.6 V vs RHE. Detailed material characterizations and electrochemical studies reveal that the metallene structure with ultrathin thickness could improve atomic utilization of precious metal atoms, and the introduction of Au and H atoms could adjust the electronic structure of Pd atoms, regulate the evolution pathway of key N-/C-intermediates, and promote the C–N coupling to form urea.