Electrochemical C-N coupling with perovskite hybrids toward efficient urea synthesis

doi:10.1039/d1sc01467f

	Electrochemical C-N coupling with perovskite hybrids toward efficient urea synthesis
	Yuan, Menglei 2,3; Chen, Junwu 2,3; Bai, Yiling 4,5; Liu, Zhanjun 4; Zhang, Jingxian 2,3; Zhao, Tongkun 2,3; Shi, Qiaona 6; Li, Shuwei 2; Wang, Xi 1,7; Zhang, Guangjin 1,2,3
刊名	CHEMICAL SCIENCE
	2021-04-12
页码	11
ISSN号	2041-6520
DOI	10.1039/d1sc01467f
英文摘要	Electrocatalytic C-N coupling reaction by co-activation of both N-2 and CO2 molecules under ambient conditions to synthesize valuable urea opens a new avenue for sustainable development, while the actual catalytic activity is limited by poor adsorption and coupling capability of gas molecules on the catalyst surface. Herein, theoretical calculation predicts that the well-developed built-in electric field in perovskite hetero-structured BiFeO3/BiVO4 hybrids can accelerate the local charge redistribution and thus promote the targeted adsorption and activation of inert N-2 and CO2 molecules on the generated local electrophilic and nucleophilic regions. Thus, a BiFeO3/BiVO4 heterojunction is designed and synthesized, which delivers a urea yield rate of 4.94 mmol h(-1) g(-1) with a faradaic efficiency of 17.18% at -0.4 V vs. RHE in 0.1 M KHCO3, outperforming the highest values reported as far. The comprehensive analysis further confirms that the local charge redistribution in the heterojunction effectively suppresses CO poisoning and the formation of the endothermic NNH intermediate, which thus guarantees the exothermic coupling of N=N* intermediates with the generated CO via C-N coupling reactions to form the urea precursor NCON intermediate. This work opens a new avenue for effective electrocatalytic C-N coupling under ambient conditions.
资助项目	National Key R&D Program of China[2020YFA0710200] ; Chemistry and Chemical Engineering Guangdong Laboratory[1922006] ; Key Program for International S&T Cooperation Projects - Ministry of Science and Technology of China[2018YFE0124600]
WOS研究方向	Chemistry
语种	英语
出版者	ROYAL SOC CHEMISTRY
WOS记录号	WOS:000641432600001
资助机构	National Key R&D Program of China ; Chemistry and Chemical Engineering Guangdong Laboratory ; Key Program for International S&T Cooperation Projects - Ministry of Science and Technology of China
内容类型	期刊论文
源URL	[http://ir.ipe.ac.cn/handle/122111/48411]
专题	中国科学院过程工程研究所
通讯作者	Zhang, Guangjin
作者单位	1.Chem & Chem Engn Guangdong Lab, Shantou 515031, Peoples R China 2.Chinese Acad Sci, Inst Proc Engn, State Key Lab Multiphase Complex Syst, CAS Key Lab Green Proc Engn,Beijing Key Lab Ion L, Beijing 100190, Peoples R China 3.Univ Chinese Acad Sci, Ctr Mat Sci & Optoelect Engn, Beijing 100049, Peoples R China 4.Chinese Acad Sci, Inst Coal Chem, State Key Lab Coal Convers, CAS Key Lab Carbon Mat, Taiyuan 030001, Peoples R China 5.Synfuels China Technol Co Ltd, SynCat Beijing, Beijing 101407, Peoples R China 6.Sino Shaanxi Nucl Molybdenum Ind Co Ltd, Tongguan 714300, Peoples R China 7.Beijing Jiaotong Univ, Minist Educ, Key Lab Luminescence Opt Informat, Beijing 100044, Peoples R China
推荐引用方式 GB/T 7714	Yuan, Menglei,Chen, Junwu,Bai, Yiling,et al. Electrochemical C-N coupling with perovskite hybrids toward efficient urea synthesis[J]. CHEMICAL SCIENCE,2021:11.
APA	Yuan, Menglei.,Chen, Junwu.,Bai, Yiling.,Liu, Zhanjun.,Zhang, Jingxian.,...&Zhang, Guangjin.(2021).Electrochemical C-N coupling with perovskite hybrids toward efficient urea synthesis.CHEMICAL SCIENCE,11.
MLA	Yuan, Menglei,et al."Electrochemical C-N coupling with perovskite hybrids toward efficient urea synthesis".CHEMICAL SCIENCE (2021):11.