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Interfacial role of Ionic liquids in CO2 electrocatalytic Reduction: A mechanistic investigation

文献类型：期刊论文

作者Guo, Shuai1,2; Liu, Yawei2; Wang, Yanlei2; Dong, Kun2; Zhang, Xiangping1,2; Zhang, Suojiang2
刊名CHEMICAL ENGINEERING JOURNAL
出版日期2023-02-01
卷号457页码:10
关键词Ionic liquids CO(2 )electrocatalytic reduction reaction Density functional theory Transition state Hydrogen bond Molecular dynamics simulations
ISSN号1385-8947
DOI10.1016/j.cej.2022.141076
英文摘要Ionic liquids (ILs) can significantly reduce the overpotential of CO2 electrocatalytic reduction reaction (CO2RR) and thus show a huge application potential in the CO2 conversion. However, it has not been clear what role ILs play in the reaction occurring at the solid-liquid interface of the electrodes. In this work, we performed comprehensive DFT calculations to investigate the mechanism of CO2RR to CO on Ag electrode surfaces with ILs. Our results showed that the Ag(1 1 0) surface exhibits better catalytic performance than both Ag(1 0 0) and Ag(1 1 1) surfaces since the energy barrier of the transition state (Ts) is lower and the intermediate (*COOH) is more stable on the former surface. When ILs exist near the surface, the energy barrier of the Ts decreases and varies when the CO2 molecule is localized at different positions of the [Emim](+ )cation. The optimized structures showed that the CO2 molecule prefers to stay near the C-4/5 position rather than the C-2 position. It was also found that proton transferring on the Ag surface by the hydrogen bond mode has a lower energy barrier than the shuttling mode, which indicates that the IL can act as an assist-catalyst by forming hydrogen-bonding complex in the reaction. Furthermore, the role of water was explored by using the implicit-solvent model. It was found that the solvation effect of the water always decreases the energy barrier, and the decline is more pronounced when there are ILs. Molecular dynamics (MD) simulations also showed that near the electrode surface, each CO2 molecule is enclosed by 3-4 [Emim](+) cations with their C-4/5 more likely approaching the CO2. Such a distri-bution embodies the mesoscale multi-ions synergistic catalytic mechanism that will be elucidated in our future work.
WOS关键词SINGLE-CRYSTAL ELECTRODES ; ELECTROCHEMICAL REDUCTION ; CARBON-DIOXIDE ; CONVERSION ; ELECTROREDUCTION ; CATALYSTS ; INSIGHTS ; SIMULATION ; SURFACES ; AU
资助项目DNL Cooperation Fund, CAS[DNL202007] ; National Natural Science Foundation of China[21878296] ; Beijing Municipal Natural Science Foundation[2202051] ; Major Program of National Natural Science Foundation of China ; Science Fund for Creative Research Groups of the National Natural Science Foundation of China[21921005]
WOS研究方向Engineering
语种英语
WOS记录号WOS:000920235900001
出版者ELSEVIER SCIENCE SA
资助机构DNL Cooperation Fund, CAS ; National Natural Science Foundation of China ; Beijing Municipal Natural Science Foundation ; Major Program of National Natural Science Foundation of China ; Science Fund for Creative Research Groups of the National Natural Science Foundation of China
源URL[http://ir.ipe.ac.cn/handle/122111/56952]  
通讯作者Dong, Kun; Zhang, Suojiang
作者单位1.Univ Chinese Acad Sci, Sch Future Technol, Beijing 100049, Peoples R China
2.Chinese Acad Sci, CAS Key Lab Green Proc & Engn, State Key Lab Multiphase Complex Syst, Beijing Key Lab Ion Liquids Clean Proc,Inst Proc E, Beijing 100190, Peoples R China
推荐引用方式
GB/T 7714		 Guo, Shuai,Liu, Yawei,Wang, Yanlei,et al. Interfacial role of Ionic liquids in CO2 electrocatalytic Reduction: A mechanistic investigation[J]. CHEMICAL ENGINEERING JOURNAL,2023,457:10.
APA Guo, Shuai,Liu, Yawei,Wang, Yanlei,Dong, Kun,Zhang, Xiangping,&Zhang, Suojiang.(2023).Interfacial role of Ionic liquids in CO2 electrocatalytic Reduction: A mechanistic investigation.CHEMICAL ENGINEERING JOURNAL,457,10.
MLA Guo, Shuai,et al."Interfacial role of Ionic liquids in CO2 electrocatalytic Reduction: A mechanistic investigation".CHEMICAL ENGINEERING JOURNAL 457(2023):10.

入库方式： OAI收割

来源：过程工程研究所

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