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.
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页数：11
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