首页|Efficient C-N coupling in electrocatalytic urea generation on copper carbonate hydroxide electrocatalysts

Efficient C-N coupling in electrocatalytic urea generation on copper carbonate hydroxide electrocatalysts

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Urea generation through electrochemical CO2 and NO3-co-reduction reaction(CO2NO3RR)is still limited by either the low selectivity or yield rate of urea.Herein,we report copper carbonate hydroxide(Cu2(OH)2CO3)as an efficient CO2NO3RR electrocatalyst with an impressive urea Faradaic efficiency of 45.2％+2.1％and a high yield rate of 1564.5±145.2 μg h-1 mgcat-1.More importantly,H2 evolution is fully inhibited on this electrocatalyst over a wide potential range between-0.3 and-0.8 V versus reversible hydrogen electrode.Our thermodynamic simulation reveals that the first C-N coupling follows a unique pathway on Cu2(OH)2CO3 by combining the two intermediates,*COOH and*NHO.This work demon-strates that high selectivity and yield rate of urea can be simultaneously achieved on simple Cu-based electrocatalysts in CO2NO3RR,and provide guidance for rational design of more advanced catalysts.

Copper carbonate hydroxideCo-reductionUrea generationC-N couplingDFT calculation

Yinuo Wang、Yian Wang、Qinglan Zhao、Hongming Xu、Shangqian Zhu、Fei Yang、Ernest P.Delmo、Xiaoyi Qiu、Chi Song、Juhee Jang、Tiehuai Li、Ping Gao、M.Danny Gu、Minhua Shao

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Advanced Materials Thrust,The Hong Kong University of Science and Technology(Guangzhou),Guangzhou 511400,Guangdong,China

Department of Chemical and Biological Engineering The Hong Kong University of Science and Technology,Clear Water Bay,Kowloon,Hong Kong,China

Department of Chemistry,City University of Hong Kong,Tat Chee Avenue,Kowloon,Hong Kong,China

Department of Materials Science and Engineering,Southern University of Science and Technology of China,1088 Xueyuan Boulevard,Shenzhen 518055,Guangdong,China

Energy Institute,and Chinese National Engineering Research Center for Control & Treatment of Heavy Metal Pollution,The Hong Kong University of Science and Technology,Kowloon,Hong Kong,China

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Research Grants CouncilResearch Grants CouncilResearch Grants CouncilSouthern Marine Science and Engineering Guangdong Laboratory(Guangzhou)Innovation and Technology Commission of the Hong Kong Special Administrative RegionHong Kong Postdoctoral Fellowship SchemeHong Kong Postdoctoral Fellowship SchemeShenzhen fundamental research fundingShenzhen fundamental research fundingShenzhen fundamental research fundingN.Ho from HKUST for XPS measurements

262061151630482116309418SMSEGL20SC01ITC-CNERC14EG03HKUST PDFS2021-4S12HKUST PDFS2021-6S08JCYJ2021032411580902620200925154115001JCYJ20200109141216566

2024

10.1016/j.jechem.2024.02.020

能源化学
中国科学院大连化学物理研究所 中国科学院成都有机化学研究所

能源化学

CSTPCDEI
影响因子：0.654
ISSN：2095-4956
年,卷(期)：2024.93(6)
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