Positive feedback of intermediates promotes efficient electrocatalytic C-N coupling at AuPd/SnOx interfaces

被引：1

作者：

Wang, Hua ^{[1
]}

Tu, Yunchuan ^{[2
]}

Li, Sijun ^{[1
]}

Jiang, Yimin ^{[1
]}

Zhao, Niandan ^{[1
]}

Wang, Wenbin ^{[1
]}

Shen, Wei ^{[1
]}

Li A, Ming ^{[1
]}

He, Rongxing ^{[1
]}

机构：

[1] Southwest Univ, Key Lab Luminescence Anal & Mol Sensing, Coll Chem & Chem Engn, Minist Educ, Chongqing 400715, Peoples R China

[2] Chongqing Univ, Coll Chem & Chem Engn, Chongqing 400044, Peoples R China

来源：

APPLIED CATALYSIS B-ENVIRONMENT AND ENERGY | 2024年 / 358卷

基金：

中国国家自然科学基金;

关键词：

Urea synthesis; C-N coupling; Co-reduction; Interface; Feedback; CARBON-DIOXIDE; NITRITE IONS; ELECTROCHEMICAL SYNTHESIS; REDUCTION; UREA; TEMPERATURE; NITRATE;

D O I：

10.1016/j.apcatb.2024.124355

中图分类号：

O64 [物理化学（理论化学）、化学物理学];

学科分类号：

070304 ; 081704 ;

摘要：

Efficient electrocatalytic co-reduction of CO2 and NO3- to urea involves simultaneous generation and stabilization of C- and N-coupling intermediates. Herein, we report positive feedback at the interfaces of an AuPd/SnOx catalyst that enables generation and stable co-adsorption of *CO and *NH2OH at low-potential, fostering efficient C-N coupling for urea formation. A combination of in-situ spectroscopic analyses and theoretical calculations show that *CO2 captures electrons by bonding to the AuPd/SnOx interface, leading to positively charged Pd sites, which promote the NO3RR to give the key N-intermediate *NH2OH. The adsorbed *NH2OH provides electron feedback to the catalyst surface, which not only enhances the adsorption of CO2 and promotes the conversion of *CO2 to *CO to accelerate the CO2RR, but also enhances the adsorption strength of the catalyst for *CO. Owing to this positive feedback, the Faraday efficiency and yield of urea reached 21.3 % and 1280.5 mu g center dot h(-1) center dot mg(-1) at 0.2 V (versus the relative hydrogen electrode), surpassing the performance of most previously reported catalysts. This finding provides new insights into catalyst design for advancing C-N coupling systems.

引用

页数：11

共 57 条

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