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On the association of frustrated Lewis pairs in ionic liquids: a molecular dynamics simulation study
Liu, Xiaoqing1; Wang, Xiaojing1; Li, Yao2; Yu, Tianhao2; Zhao, Weizhen2; Liu, Lei2
2021-05-03
Source PublicationPHYSICAL CHEMISTRY CHEMICAL PHYSICS
ISSN1463-9076
Pages8
AbstractSterically hindered frustrated Lewis pairs (FLPs) have the ability to activate hydrogen molecules, and their reactivity is strongly determined by the geometric parameters of the Lewis acids and bases. A recent experimental study showed that ionic liquids (ILs) could largely improve the effective configuration of FLPs. However, the detailed mechanistic profile is still unclear. Herein, we performed molecular dynamics (MD) simulations to reveal the effects of ILs on the structures of FLPs, in particular, the association of Lewis acids and bases. For this purpose, mixed systems were adopted consisting of the ILs [C(n)mim][NTf2] (n = 6, 10, 14), [C(6)mim][PF6] and [C(6)mim][CTf3] and the typical FLP (tBu)(3)P/B(C6F5)(3) for MD simulations. Radial distribution functions (RDFs) results show that toluene competes with (tBu)(3)P to interact with B(C6F5)(3), resulting in a relatively low effective (tBu)(3)P/B(C6F5)(3) complex, while [C(10)mim][NTf2] shows less competition with (tBu)(3)P, which increases the amount of effective FLPs. Spatial distribution functions (SDFs) results show that toluene forms a continuum solvation-shell, which hinders the interactions between (tBu)(3)P and B(C6F5)(3), while [C(10)mim][NTf2] leaves relatively large empty spaces, which are accessible for (tBu)(3)P or B(C6F5)(3) molecules, resulting in higher probabilities of effective FLP structures. Lastly, we find that the longer alkyl chain length of [C(n)mim](+) cations, the higher the amount of effective (tBu)(3)P/B(C6F5)(3) pairs, and the anion [CTf3](-) shows negative effects, for which even less effective (tBu)(3)P/B(C6F5)(3) pairs have been found compared to those of toluene.
DOI10.1039/d1cp00479d
Language英语
WOS KeywordHYDROGEN ACTIVATION ; ORBITAL METHODS ; FORCE-FIELD ; DENSITY ; MECHANISM ; THERMOCHEMISTRY ; REACTIVITY ; CHEMISTRY ; MIXTURES ; ELEMENTS
Funding ProjectNational Natural Science Foundation of China[21978294] ; National Natural Science Foundation of China[51901209] ; National Natural Science Foundation of China[21808224]
WOS Research AreaChemistry ; Physics
WOS SubjectChemistry, Physical ; Physics, Atomic, Molecular & Chemical
Funding OrganizationNational Natural Science Foundation of China
WOS IDWOS:000651131900001
PublisherROYAL SOC CHEMISTRY
Citation statistics
Document Type期刊论文
Identifierhttp://ir.ipe.ac.cn/handle/122111/48783
Collection中国科学院过程工程研究所
Corresponding AuthorLiu, Xiaoqing; Liu, Lei
Affiliation1.North Univ China, Sch Environm & Safety Engn, Taiyuan 030051, Peoples R China
2.Chinese Acad Sci, Beijing Key Lab Ion Liquids Clean Proc, Inst Proc Engn, Key Lab Green Proc & Engn, Beijing 100190, Peoples R China
Recommended Citation
GB/T 7714
Liu, Xiaoqing,Wang, Xiaojing,Li, Yao,et al. On the association of frustrated Lewis pairs in ionic liquids: a molecular dynamics simulation study[J]. PHYSICAL CHEMISTRY CHEMICAL PHYSICS,2021:8.
APA Liu, Xiaoqing,Wang, Xiaojing,Li, Yao,Yu, Tianhao,Zhao, Weizhen,&Liu, Lei.(2021).On the association of frustrated Lewis pairs in ionic liquids: a molecular dynamics simulation study.PHYSICAL CHEMISTRY CHEMICAL PHYSICS,8.
MLA Liu, Xiaoqing,et al."On the association of frustrated Lewis pairs in ionic liquids: a molecular dynamics simulation study".PHYSICAL CHEMISTRY CHEMICAL PHYSICS (2021):8.
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