文献类型：期刊文献

英文题名：Hydroxyl-Functionalization Promoted Activity and Recovery of Ionic Liquids in Direct Dimethyl Carbonate Synthesis from Co2

作者：Ruan, Jiawei[1]; Chen, Lifang[2]; Wu, Xinzi[1]; Qian, Shaokang[1]; Xie, Kunchi[1]; Zhang, Xiaoyi[1]; Cheng, Hongye[1]; Song, Zhen[2]; Qi, Zhiwen[2]

机构：[1] State Key Laboratory of Chemical Engineering, School of Chemical Engineering, East China University of Science and Technology, 130 Meilong Road, Shanghai, 200237, China; [2] Max Planck Partner Group, Germany

年份：2024

外文期刊名：SSRN

收录：EI(收录号：20240233664)

语种：英文

外文关键词：Carbonation - Catalyst activity - Chemical activation - Density functional theory - Diffusion in liquids - Fourier transform infrared spectroscopy - Ionic liquids - Molecular dynamics - Phase separation - Reaction kinetics

摘要：Direct synthesis of dimethyl carbonate (DMC) from CO2 is promising for CO2 utilization, however its efficiency remains far from industrial-scale implementation for lack of customized catalysts. Herein, a hydroxyl-functionalized ionic liquid (HFIL) was developed to enhance catalytic activity, and importantly, to facilitate IL recovery through spontaneous phase separation. A significantly higher DMC yield (6.5 gDMC·kgcat-1·h-1) over HFIL was achieved under mild conditions. Self-diffusion coefficient characterization revealed intensified diffusion of CH3OH and HFIL, alongside diminished ion pairing owing to hydroxyl functionalization. Density functional theory calculations elucidated cation polarization induced by the hydroxyl group, facilitating the synergistic activation of substrates and monomethyl carbonate intermediate. The reaction mechanism was further verified through diffuse reflectance infrared Fourier transform spectroscopy with theoretical calculations. The self-separation behavior was demonstrated by molecular dynamics simulations. The deep insights into hydroxyl effects towards direct DMC synthesis provide a pioneering perspective for CO2 capture and utilization using functionalized ILs. ? 2024, The Authors. All rights reserved.