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Theoretical Insights into the Effect of Cations, Anions, and Water on Fixation of CO(2)Catalyzed by Different Ionic Liquids
Xia, Yangfeng1,2; Zhang, Yanqiang1; Su, Qian1; Dong, Kun1
2020-08-21
Source PublicationCHEMSUSCHEM
ISSN1864-5631
Pages11
AbstractChemical fixation of CO(2)is an efficient means for decreasing amount of CO(2)in the atmosphere. One of promising technologies is the cycloaddition of CO(2)with epoxides to synthesize cyclic carbonates. In this reaction, ionic liquid (IL) catalysts show versatile and unique advantages. However, the reaction mechanism using ILs is not clear. In this work, a detailed theoretical investigation was performed by DFT calculations. The energetic profile shows that the reaction consists of three steps, with the ring-opening step being the rate-determining step. Based on the results, effects of cations, anions and water were calculated. Cations show strong hydrogen bonding interactions with epoxides, which decreases the energy barrier of the ring-opening step, indicating that hydrogen bonds play a positive role in promoting the reaction. The effect of anions was evaluated by nucleophilicity index (N-Nu); anions with a largerN(Nu)(stronger nucleophilicity) value show lower energy barriers. The influence of water was investigated by implicit and explicit models. Compared with the solvent-free case, water as an implicit solvent decreases the energy barriers through polarization with epoxides. In the explicit solvent model, the water molecules form new hydrogen bonds with epoxides and cations, which can efficiently reduce the energy barriers. The result indicates that there is a new synergic catalytic mechanism, in which the water acts not only as solvent but also as a catalyst in the reaction. Supporting experiments further confirm the calculation results.
KeywordCO2-epoxide cycloaddition Density functional calculations ELF (Electron Localization Function) Ionic liquids
DOI10.1002/cssc.202001447
Language英语
WOS KeywordCARBON-DIOXIDE ; CYCLIC CARBONATES ; CHEMICAL FIXATION ; CO2 ; EPOXIDES ; CATALYST ; DENSITY
Funding ProjectNational Key R&D Program of China[2016YFB0600903] ; National Natural Science Foundation of China[91534116] ; National Natural Science Foundation of China[21878296]
WOS Research AreaChemistry ; Science & Technology - Other Topics
WOS SubjectChemistry, Multidisciplinary ; Green & Sustainable Science & Technology
Funding OrganizationNational Key R&D Program of China ; National Natural Science Foundation of China
WOS IDWOS:000561082200001
PublisherWILEY-V C H VERLAG GMBH
Citation statistics
Document Type期刊论文
Identifierhttp://ir.ipe.ac.cn/handle/122111/41806
Collection中国科学院过程工程研究所
Corresponding AuthorDong, Kun
Affiliation1.Chinese Acad Sci, Inst Proc Engn, Beijing Key Lab Ion Liquids Clean Proc, Key Lab Green Proc & Engn,State Key Lab Multiphas, Beijing 100049, Peoples R China
2.Univ Chinese Acad Sci, Sch Chem Engn, Beijing 100049, Peoples R China
Recommended Citation
GB/T 7714
Xia, Yangfeng,Zhang, Yanqiang,Su, Qian,et al. Theoretical Insights into the Effect of Cations, Anions, and Water on Fixation of CO(2)Catalyzed by Different Ionic Liquids[J]. CHEMSUSCHEM,2020:11.
APA Xia, Yangfeng,Zhang, Yanqiang,Su, Qian,&Dong, Kun.(2020).Theoretical Insights into the Effect of Cations, Anions, and Water on Fixation of CO(2)Catalyzed by Different Ionic Liquids.CHEMSUSCHEM,11.
MLA Xia, Yangfeng,et al."Theoretical Insights into the Effect of Cations, Anions, and Water on Fixation of CO(2)Catalyzed by Different Ionic Liquids".CHEMSUSCHEM (2020):11.
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