Directed Urea‐to‐Nitrite Electrooxidation via Tuning Intermediate Adsorption on Co, Ge Co‐Doped Ni Sites
作者：Pengtang Wang, Xiaowan Bai, Huanyu Jin, Xintong Gao, Kenneth Davey, Yao Zheng, Yan Jiao, Shi‐Zhang Qiao · 发表于：Advanced Functional Materials · 年份：2023 · DOI：10.1002/adfm.202300687 · 被引用次数：118 · 研究领域：Electrocatalysts for Energy Conversion、Ammonia Synthesis and Nitrogen Reduction、Advanced Photocatalysis Techniques
Abstract The electrochemical urea oxidation reaction (UOR) is an alternative to electrooxidation of water for energy–saving hydrogen (H 2 ) production. To maximize this purpose, design of catalysts for selective urea‐to‐nitrite (NO 2 – ) electrooxidation with increased electron transfer and high current is practically important. Herein, a cobalt, germanium (Co, Ge) co‐doped nickel (Ni) oxyhydroxide catalyst is reported first time that directs urea‐to‐NO 2 – conversion with a significant Faradaic efficiency of 84.9% at 1.4 V versus reversible hydrogen electrode and significantly boosts UOR activity to 448.0 mA cm −2 . Importantly, this performance is greater than for most reported Ni‐based catalysts. Based on judiciously combined synchrotron‐based measurement, in situ spectroscopy and density functional theoretical computation, significantly boosted urea‐to‐NO 2 – production results from Co, Ge co‐doping is demonstrated that optimizes electronic structure of Ni sites in which urea adsorption is altered as NO‐terminal configuration to facilitate CN cleavage for *NH formation, and thereby expedites pathway for urea to NO 2 – conversion. Findings highlight the importance of tuning intermediate adsorption behavior for design of high‐performance UOR electrocatalysts, and will be of practical benefit to a range of researchers and manufacturers in replacing conventional water electrooxidation with UOR for energy‐saving H 2 production.