ie8b01148_si_001.pdf (658.27 kB)
Protic Quaternary Ammonium Ionic Liquids for Catalytic Conversion of CO2 into Cyclic Carbonates: A Combined Ab Initio and MD Study
journal contribution
posted on 2018-04-30, 00:00 authored by Huiqing Yang, Danning Zheng, Jingshun Zhang, Ke Chen, Junfeng Li, Li Wang, Jinglai Zhang, Hongyan He, Suojiang ZhangThe mechanism of CO2 fixation
catalyzed by protic hydroxyl-functionalized
quaternary ammonium ionic liquids (ILs) is investigated by two different
models, the Single-IL model and the Double-IL model. The relative
sequence of catalytic activity calculated by the Single-IL model is
contradictory with the experimental result. The situation is totally
varied when the Double-IL model is utilized. In this system, ILs are
not limited to the catalyst but solvent. The ILs are incorporated
into the catalytic system to consider the solvent effect rather than
by the existing solvent model. When the solvent effect is included,
it is better to distinguish the catalytic activity of three ILs. According
to the noncovalent interaction and the atoms in molecules analysis,
the highest catalytic activity of tris(2-hydroxyethyl)ammonium bromide
([HTEA]Br) is attributed to its strongest nucleophilic attack and
moderate hydrogen bond interaction between IL and reactant. It is
necessary to consider the interaction between ILs to get a reliable
result. Moreover, the solvent effect aroused by ILs should be carefully
considered.