首页|Do certain imidazolium-based ionic liquid ion pairs/mordenite capture H2S by conformational traps? An ONIOM-DFT study

Do certain imidazolium-based ionic liquid ion pairs/mordenite capture H2S by conformational traps? An ONIOM-DFT study

扫码查看
原文链接
  • NSTL
We present detailed ONIOM(ωB97X-D:PM6)calculations for the formation mechanism of novel composites combining protonic mordenites(H-MOR)with various ionic liquids:1,3-dimethyl-imidazolium chloride[MMIm] CI,1-ethyl-3-methyl-imidazolium chloride[EMIm] CI; l-methyl-3-propyl-imidazolium chloride[PMIm]Cl; 1-butyl-3-methyl-imidazolium chloride[BMImJCl,1-(2-hydroxyethyl)-3-methyl-imidazolium chloride[HEMIm] CI,1,3-dimethyl-1,3,2-diazasilolium chloride[MMSiN]Cl,and l,3-dimethyl-1,3-diphospholium chloride[MMPP] Cl.The most feasible[MJ-MOR formation mechanism([M]~+ =[MMIm]~+,[EMIm]~+,[PMIm]~+,[BMIm]~+,[HEMIm][MMSiN]~+[MMPP]~+)involves an ion exchange at the T4010 position favoring the isolation of a minimal number of[M]~+ isomers(i.e.,conformational traps).The interaction of these[M]-MOR composites with pollutant gases has afterward been evaluated.Among the studied sytems,[EMIm]-MOR and[HEMIm]-MOR present electronic and steric conditions for potential applications in gas separation,capture,and storage(H2 and H2S).The H-MOR framework exhibits two structural conformers with the[HEMIm]~+ cation in the confined space.Both,the MOR-T4O10-[HEMIm] and MOR-T4O10-[HEMIm]~(HB)conformers,interconvert by a dynamic equilibrium with a transition state MOR-T4010-TS1 acting as a conformational switch(ON~OFF)that selectively recognizes and captures H2S through a plier-like conformation.

ONIOM calculationsZeolitesH-MORIonic liquidH2S capture And storage

Rodolfo Izquierdo、Gustavo Chacon、Nestor Cubillan

展开 >

Grupo de Quimica Teorica,Instituto de Quimica,UFRGS,Av.Bento Gongalves,9500,Porto Alegre,RS,91540 180,Brazil

Laboratory of Molecular Catalysis,Instituto de Quimica,UFRGS,Av.Bento Gongalves,9500,Porto Alegre,RS,91501 970,Brazil

Programa de Quimica,Facultad de Ciencias Basicas,Universidad del Atlantico,Barranquilla,Colombia

2022

10.1016/j.micromeso.2022.112053

Microporous and mesoporous materials

Microporous and mesoporous materials

EISCI
ISSN：1387-1811
年,卷(期)：2022.341
  • 88