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| Highly selective electroreduction of N-2 and CO2 to urea over artificial frustrated Lewis pairs | |
| Yuan, Menglei1,2; Chen, Junwu1,2; Xu, Yong3; Liu, Rongji4; Zhao, Tongkun1,2; Zhang, Jingxian1,2; Ren, Zhongyu1,2; Liu, Zhanjun5; Streb, Carsten4; He, Hongyan1,2; Yang, Chao1,2,3; Zhang, Suojiang1,2; Zhang, Guangjin1,2,3 | |
| 2021-11-10 | |
| Source Publication | ENERGY & ENVIRONMENTAL SCIENCE
 |
| ISSN | 1754-5692 |
| Pages | 11 |
| Abstract | The simultaneous electrocatalytic conversion of N-2 and CO2 into value-added urea is highly anticipated but suffers from the predicament of the poor chemisorption, activation, and coupling activity of reactant molecules. Herein, unique frustrated Lewis pairs (FLPs) were precisely designed in flower-like nickel borate [Ni-3(BO3)(2)], where the surface hydroxyl and neighboring Ni site serve as a Lewis base and acid, respectiveLy. Comprehensive investigations endorsed that the Lewis basic and acidic sites in FLPs acted synergistically in the targeted capture of inert CO2 and N-2 by orbital interaction. Subsequently, the bonding and antibonding orbitals of the inert gas interacted with the empty orbitals of the Lewis acid and nonbonding orbitals of the Lewis base, respectively, achieving molecule activation by FLPs. Afterward, the *N=N* and CO intermediates underwent electrocatalytic C-N coupling by the a orbital carbonylation strategy to produce *NCON* precursors. Thus, the prepared Ni-3(BO3)(2)-150 nanocrystal delivered the record-highest urea yield rate of 9.70 mmol h(-1) g(cat)(-1) and a Faradaic efficiency of 20.36% at -0.5 V vs. RHE. |
| DOI | 10.1039/d1ee02485j |
| Language | 英语 |
| WOS Keyword | HYDROGEN ACTIVATION ; DINITROGEN ; CHEMISTRY |
| Funding Project | National Key R&D Program of China[2020YFA0710200] ; National Natural Science Foundation of China[22178361] ; Key Program for International S&T Cooperation Projects[2018YFE0124600] ; Ministry of Science and Technology of China |
| WOS Research Area | Chemistry ; Energy & Fuels ; Engineering ; Environmental Sciences & Ecology |
| WOS Subject | Chemistry, Multidisciplinary ; Energy & Fuels ; Engineering, Chemical ; Environmental Sciences |
| Funding Organization | National Key R&D Program of China ; National Natural Science Foundation of China ; Key Program for International S&T Cooperation Projects ; Ministry of Science and Technology of China |
| WOS ID | WOS:000721520100001 |
| Publisher | ROYAL SOC CHEMISTRY |
| Citation statistics | |
| Document Type | 期刊论文 |
| Identifier | http://ir.ipe.ac.cn/handle/122111/51017 |
| Collection | 中国科学院过程工程研究所 |
| Corresponding Author | Zhang, Guangjin |
| Affiliation | 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 & Optoeletron Engn, Sch Chem Engn, Beijing 100190, Peoples R China 3.Chem & Chem Engn Guangdong Lab, Shantou 515031, Peoples R China 4.Ulm Univ, Inst Inorgan Chem, 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 |
| Recommended Citation GB/T 7714 | Yuan, Menglei,Chen, Junwu,Xu, Yong,et al. Highly selective electroreduction of N-2 and CO2 to urea over artificial frustrated Lewis pairs[J]. ENERGY & ENVIRONMENTAL SCIENCE,2021:11. |
| APA | Yuan, Menglei.,Chen, Junwu.,Xu, Yong.,Liu, Rongji.,Zhao, Tongkun.,...&Zhang, Guangjin.(2021).Highly selective electroreduction of N-2 and CO2 to urea over artificial frustrated Lewis pairs.ENERGY & ENVIRONMENTAL SCIENCE,11. |
| MLA | Yuan, Menglei,et al."Highly selective electroreduction of N-2 and CO2 to urea over artificial frustrated Lewis pairs".ENERGY & ENVIRONMENTAL SCIENCE (2021):11. |
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