C-Bound or O-Bound Surface: Which One Boosts Electrocatalytic Urea Synthesis?

被引：58

作者：

Liu, Yingying ^{[1
]}

Tu, Xiaojin ^{[1
]}

Wei, Xiaoxiao ^{[1
]}

Wang, Dongdong ^{[1
]}

Zhang, Xiaoran ^{[1
]}

Chen, Wei ^{[1
]}

Chen, Chen ^{[1
]}

Wang, Shuangyin ^{[1
]}

机构：

[1] Hunan Univ, Coll Chem & Chem Engn, State Key Lab Chem Biosensing & Chemometr, Changsha, Peoples R China

来源：

ANGEWANDTE CHEMIE-INTERNATIONAL EDITION | 2023年 / 62卷 / 19期

基金：

中国博士后科学基金; 中国国家自然科学基金; 国家重点研发计划;

关键词：

C-Bound; C-N Coupling; Electrocatalytic Activity; O-Bound; Urea Synthesis; CHARGE REDISTRIBUTION; CO2; REDUCTION; CARBON; 4-MERCAPTOPYRIDINE; BEHAVIOR; XPS;

D O I：

10.1002/anie.202300387

中图分类号：

O6 [化学];

学科分类号：

0703 ;

摘要：

The electrocatalytic C-N coupling from carbon dioxide and nitrate under ambient conditions is kind of sustainable and promising alternative method for urea synthesis. To date, the influence of catalyst surface properties on molecular adsorption configuration and electrocatalytic urea synthesis activity is unclear. In this work, we proposed that the urea synthesis activity is closely linked with the localized surface charge on bimetallic electrocatalysts, it is found that a negatively charged surface induces C-bound path and boosts urea synthesis. The urea yield rate can reach 13.1 mmol g(-1) h(-1) on negatively charged Cu97In3-C, which is about 13 times that of positively charged Cu30In70-C counterpart with O-bound surface. This conclusion also applies to Cu-Bi and Cu-Sn systems. The molecular modification shifts the surface of Cu97In3-C to positively charged state, which leads to a sharp decline in urea synthesis performance. We demonstrated that the C-bound surface is more favorable than O-bound one to boost electrocatalytic urea synthesis.

引用

页数：5

共 52 条

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