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Host-guest molecular interaction promoted urea electrosynthesis over a precisely designed conductive metal-organic framework

文献类型：期刊论文

作者Yuan, Menglei1,2; Chen, Junwu1,2; Zhang, Honghua1,2; Li, Qiongguang1,2; Zhou, Le1,2; Yang, Chao1,2,3; Liu, Rongji1,2,4; Liu, Zhanjun2,5; Zhang, Suojiang1,2; Zhang, Guangjin1,2,3
刊名ENERGY & ENVIRONMENTAL SCIENCE
出版日期2022-03-30
页码12
ISSN号1754-5692
DOI10.1039/d1ee03918k
英文摘要The highly selective electrocatalytic activation of N-2 and CO2 to synthesize value-added urea via a C-N coupling reaction is an extremely challenging reaction that is largely inhibited by the poor chemisorption and coupling abilities of the reactant molecules. Herein, the novel conductive MOF Co-PMDA-2-mbIM (PMDA = pyromellitic dianhydride; 2-mbIM = 2-methyl benzimidazole) is designed, attaining a record-high urea yield rate of 14.47 mmol h(-1) g(-1) with a FE of 48.97% at -0.5 V vs. RHE. The host-guest interactions involved not only generate desirable local e[ectrophiEic and nudeophiEic regions but they also allow evolution from high-spin state Co3+ (HS: t(2g)(4) e(g)(2)) to intermediate-spin state Co4+ (IS: t(2g)(4)e(g)(1)) in CoO6 octahedrons. Thus, N-2 and CO2 can be adsorbed in a targeted fashion and activated to produce the desired *N=N* and *CO intermediates. Subsequently, the low e(g) orbital occupied Co4+ (t(2g)(4)e(g)(1)) easily accepts electrons from sigma orbital of *N=N* and effectively triggers the C-N coupling reaction to emerge *NCON* urea precursor.
WOS关键词ONE-POT SYNTHESIS ; NITROGEN REDUCTION ; CARBON-DIOXIDE ; SPIN-STATE ; EFFICIENT ; PEROVSKITE ; CHALLENGES ; NANOSHEETS ; MOBILITY ; CATALYST
资助项目National Key R&D Program of China[2020YFA0710200] ; National Natural Science Foundation of China[22178361] ; National Natural Science Foundation of China[21908228] ; 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 ; Energy & Fuels ; Engineering ; Environmental Sciences & Ecology
语种英语
WOS记录号WOS:000781260600001
出版者ROYAL SOC CHEMISTRY
资助机构National Key R&D Program of China ; National Natural Science Foundation of China ; Chemistry and Chemical Engineering Guangdong Laboratory ; Key Program for International S&T Cooperation Projects - Ministry of Science and Technology of China
源URL[http://ir.ipe.ac.cn/handle/122111/52647]  
专题中国科学院过程工程研究所
通讯作者Zhang, Suojiang; Zhang, Guangjin
作者单位1.Chinese Acad Sci, Inst Proc Engn, CAS Key Lab Green Proc Engn, Beijing Key Lab Ion Liquids Clean Proc,State Key, Beijing 100190, Peoples R China
2.Univ Chinese Acad Sci, Ctr Mat Sci & Optoelect Engn, Beijing 100049, Peoples R China
3.Chem & Chem Engn Guangdong Lab, Shantou 515031, Peoples R China
4.Ulm Univ, Inorgan Chem 1, D-89081 Ulm, Germany
5.Chinese Acad Sci, Inst Coal Chem, State Key Lab Coal Convers, CAS Key Lab Carbon Mat, Taiyuan 030001, Peoples R China
推荐引用方式
GB/T 7714		 Yuan, Menglei,Chen, Junwu,Zhang, Honghua,et al. Host-guest molecular interaction promoted urea electrosynthesis over a precisely designed conductive metal-organic framework[J]. ENERGY & ENVIRONMENTAL SCIENCE,2022:12.
APA Yuan, Menglei.,Chen, Junwu.,Zhang, Honghua.,Li, Qiongguang.,Zhou, Le.,...&Zhang, Guangjin.(2022).Host-guest molecular interaction promoted urea electrosynthesis over a precisely designed conductive metal-organic framework.ENERGY & ENVIRONMENTAL SCIENCE,12.
MLA Yuan, Menglei,et al."Host-guest molecular interaction promoted urea electrosynthesis over a precisely designed conductive metal-organic framework".ENERGY & ENVIRONMENTAL SCIENCE (2022):12.

入库方式： OAI收割

来源：过程工程研究所

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