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Protic vs aprotic ionic liquid for CO2 fixation: A simulation study

文献类型：期刊论文

作者Sun, Wenzhong2,3; Wang, Meichen2; Zhang, Yaqin2; Ding, Weilu2; Huo, Feng2; Wei, Li3; He, Hongyan1,2
刊名GREEN ENERGY & ENVIRONMENT
出版日期2020-04-01
卷号5期号:2页码:183-194
关键词Ionic liquid CO2 conversion Cycloaddition Synergistic catalysis DFT calculations
ISSN号2096-2797
DOI10.1016/j.gee.2020.04.004
英文摘要The cycloaddition of CO2 with epoxides catalyzed by ionic liquids (ILs) has been a widely ongoing studied hot topic over the years. Recent experimental research has shown that the protic ionic liquids (PILs) behave stronger hydrogen proton donating ability than aprotic ionic liquids (APILs), and can effectively catalyze the cycloaddition of CO2. Unfortunately, the mechanistic explanation remains primarily unraveled. Herein, a detailed simulation study on the cycloaddition reaction catalyzed by PIL ([HDBU][Mim]) in comparison with APIL ([MeDBU][Mim]) reaction catalysts was conducted, including the three-step route (ring-opening of PO (propylene oxide), insertion of CO2 and ring-closure of propylene carbonate (PC)) and two-step route (simultaneously ring-opening of PO and addition of CO2, and then ring-closure of PC). Based on the activation energy barrier of the rate-determining step, PIL preferentially activates PO as the optimal route for the reaction with the energy barrier of 23.2 kcal mol(-1), while that of APIL is 31.2 kcal mol(-1). The role of [HDBU](+) in the reaction was also explored and found that the direct formation of intermolecular hydrogen bond (H-bond) between [HDBU](+) and the reactants (PO + CO2) was unfavorable for the reaction, while the cooperation with the anion [Mim](-) to assist indirectly was more conducive. To fully consider the reaction microenvironment of ILs, ONIOM calculation was used to study the solvent effect. At last, the above conclusions were further verified by the analysis of intermediates with charge, non-covalent interaction (NCI), and atoms in molecules (AIM) methods. The computational findings show that ILs studied in this work have dual functions of catalyst and solvent, enabling a microscopic understanding of the ILs catalyst for CO2 utilization as well as providing guidance for the rational design of more efficient ILs-based catalysts. (C) 2020, Institute of Process Engineering, Chinese Academy of Sciences. Publishing services by Elsevier B.V. on behalf of KeAi Communications Co., Ltd.
WOS关键词CARBON-DIOXIDE ; CHEMICAL FIXATION ; DENSITY FUNCTIONALS ; EFFICIENT CATALYST ; HIGHLY EFFICIENT ; CYCLIC CARBONATE ; CYCLOADDITION ; TRANSFORMATION ; EPOXIDES ; DYNAMICS
资助项目National Science Fund for Excellent Young Scholars[21922813] ; Key Research Program of Frontier Sciences of CAS[QYZDB-SSW-SLH022] ; National Key Projects for Fundamental Research and Development of China[2017YFB0603301] ; DNL Cooperation Fund, CAS[DNL180202] ; Youth Innovation Promotion Association of CAS[2017066]
WOS研究方向Chemistry ; Science & Technology - Other Topics ; Energy & Fuels ; Engineering
语种英语
WOS记录号WOS:000543284000010
出版者KEAI PUBLISHING LTD
资助机构National Science Fund for Excellent Young Scholars ; Key Research Program of Frontier Sciences of CAS ; National Key Projects for Fundamental Research and Development of China ; DNL Cooperation Fund, CAS ; Youth Innovation Promotion Association of CAS
源URL[http://ir.ipe.ac.cn/handle/122111/41168]  
专题中国科学院过程工程研究所
通讯作者Wei, Li; He, Hongyan
作者单位1.Dalian Natl Lab Clean Energy, Dalian 116023, Peoples R China
2.Chinese Acad Sci, Inst Proc Engn, Beijing Key Lab Ion Liquids Clean Proc, CAS Key Lab Green Proc & Engn,State Key Lab Multi, Beijing 100190, Peoples R China
3.Dalian Polytech Univ, Sch Light Ind & Chem Engn, Dalian 116034, Peoples R China
推荐引用方式
GB/T 7714		 Sun, Wenzhong,Wang, Meichen,Zhang, Yaqin,et al. Protic vs aprotic ionic liquid for CO2 fixation: A simulation study[J]. GREEN ENERGY & ENVIRONMENT,2020,5(2):183-194.
APA Sun, Wenzhong.,Wang, Meichen.,Zhang, Yaqin.,Ding, Weilu.,Huo, Feng.,...&He, Hongyan.(2020).Protic vs aprotic ionic liquid for CO2 fixation: A simulation study.GREEN ENERGY & ENVIRONMENT,5(2),183-194.
MLA Sun, Wenzhong,et al."Protic vs aprotic ionic liquid for CO2 fixation: A simulation study".GREEN ENERGY & ENVIRONMENT 5.2(2020):183-194.

入库方式： OAI收割

来源：过程工程研究所

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