Unveiling the Electrooxidation of Urea: Intramolecular Coupling of the N−N Bond
學年 109
學期 2
出版(發表)日期 2021-03-22
作品名稱 Unveiling the Electrooxidation of Urea: Intramolecular Coupling of the N−N Bond
作品名稱(其他語言)
著者 Wei Chen; Leitao Xu; Xiaorong Zhu; Yu-Cheng Huang; Wang Zhou; Dongdong Wang; Yangyang Zhou; Shiqian Du; Qiling Li; Chao Xie; Li Tao; Prof. Chung-Li Dong; Jilei Liu; Yanyong Wang; Ru Chen; Hui Su; Chen Chen; Yuqin Zou; Prof. Yafei Li; Qinghua Liu; Prof. Shuangyin Wang
單位
出版者
著錄名稱、卷期、頁數 Angewandte Chemie 60(13), p.7297-7307
摘要 The nitrogenous nucleophile electrooxidation reaction (NOR) plays a vital role in the degradation and transformation of available nitrogen. Focusing on the NOR mediated by the β-Ni(OH)2 electrode, we decipher the transformation mechanism of the nitrogenous nucleophile. For the two-step NOR, proton-coupled electron transfer (PCET) is the bridge between electrocatalytic dehydrogenation from β-Ni(OH)2 to β-Ni(OH)O, and the spontaneous nucleophile dehydrogenative oxidation reaction. This theory can give a good explanation for hydrazine and primary amine oxidation reactions, but is insufficient for the urea oxidation reaction (UOR). Through operando tracing of bond rupture and formation processes during the UOR, as well as theoretical calculations, we propose a possible UOR mechanism whereby intramolecular coupling of the N−N bond, accompanied by PCET, hydration and rearrangement processes, results in high performance and ca. 100 % N2 selectivity. These discoveries clarify the evolution of nitrogenous molecules during the NOR, and they elucidate fundamental aspects of electrocatalysis involving nitrogen-containing species.
關鍵字
語言 en
ISSN 1433-7851; 1521-3773
期刊性質 國外
收錄於 SCI
產學合作
通訊作者
審稿制度
國別 GBR
公開徵稿
出版型式 ,電子版,紙本
SDGS 優質教育,可負擔的潔淨能源,氣候行動,夥伴關係