Yuan Fang, Yang Zhifang, Zhang Xiaoying, Tong Cuiyan, Gahungu Godefroid, Li Wenliang, Zhang Jingping
Faculty of Chemistry, Northeast Normal University, Changchun, China.
Faculté des Sciences, Centre de Recherche en Sciences Naturelles et Environnementales (CRSNE), Université du Burundi, Bujumbura, Burundi.
J Comput Chem. 2021 May 15;42(13):888-896. doi: 10.1002/jcc.26510. Epub 2021 Mar 13.
The effects of functional groups (including OH, OCH , NH , CH NH , COOH, SO H, OCO(CH ) COOH(E-COOH), and (CH ) COOH(c-COOH)) in 3D covalent organic frameworks (3D-COFs) on CO adsorption and separation are investigated by grand canonical Monte Carlo (GCMC) simulations and density functional theory calculations. The results indicate that interaction between CO and the framework is the main factor for determining CO uptakes at low pressure, while pore size becomes the decisive factor at high pressure. The binding energy of CO with functionalized linker is correlated to CO uptake at 0.3 bar and 298 K on 3D-COF-1, suggesting functional groups play a key role in CO capture in microporous 3D-COFs. Moreover, CO selectivity over CH , N , and H can be significantly enhanced by functionalization, where CH NH , COOH, SO H, and E-COOH enhance CO adsorption more effectively at 1 bar. Among them, SO H is the most promising functional group in 3D-COFs for CO separation.
通过巨正则蒙特卡罗（GCMC）模拟和密度泛函理论计算，研究了三维共价有机框架（3D - COF）中的官能团（包括OH、OCH₃、NH₂、CH₂NH₂、COOH、SO₃H、OCO(CH₂)₂COOH(E - COOH)和(CH₂)₃COOH(c - COOH)）对CO吸附和分离的影响。结果表明，CO与框架之间的相互作用是决定低压下CO吸收量的主要因素，而孔径在高压下成为决定性因素。CO与功能化连接体的结合能与3D - COF - 1在0.3 bar和298 K时的CO吸收量相关，表明官能团在微孔3D - COF中CO捕获中起关键作用。此外，通过功能化可以显著提高CO对CH₄、N₂和H₂的选择性，其中CH₂NH₂、COOH、SO₃H和E - COOH在1 bar时更有效地增强CO吸附。其中，SO₃H是3D - COF中用于CO分离最有前景的官能团。
