Improved selectivity of CH_(4)/CO_(2)within 1D channel of COFs realized by pore wall functionalization strategyOA
CO_(2)removal is a critical step in natural gas purification to upgrade the gas stream for practical use.Although covalent organic frameworks(COFs)show promise for gas separation,research in this area remains in its early stages,and their separation performance requires further improvement.Here,a combined quantum chemical calculations and molecular dynamics simulations were performed to elucidate the fundamental mechanisms governing CH_(4)/CO_(2)separation in COF materials.Calculated results demonstrated that the adsorption of CO_(2)within the onedimensional(1D)channels of COF10 is more favorable than that of CH_(4),and the adsorption selectivity(Sads)exhibits a significant enhancement by Cl-functionalization.Moving rate of CH_(4)is much larger than that of CO_(2)in the 1D channel of COF10,and Cl-functionalization creates stronger diffusion barriers for CO_(2)than for CH_(4).Cl-functionalized COFs exhibit substantially stronger CH_(4)/CO_(2)selectivity than COF10.It is verified that the interaction energies of more polarized CO_(2)on the pore wall of COF10 are larger than those of CH_(4),and the increased polarity induced by the highly electronegative Cl groups strengthens the framework’s affinity for gas molecules.As a result,improved CO_(2)/CH_(4)selectivity of COF10 by Cl-functionalization can be explained.
Zhou Fang;Chengjun Wang;Chunyang Li;Xinxia Li;Xin Feng;Lisheng Zhang;Huifang Li
College of Electromechanical Engineering,Shandong Engineering Laboratory for Preparation and Application of High-performance Carbon-Materials,Qingdao University of Science and Technology,Qingdao 266061,ChinaCollege of Electromechanical Engineering,Shandong Engineering Laboratory for Preparation and Application of High-performance Carbon-Materials,Qingdao University of Science and Technology,Qingdao 266061,ChinaCollege of Electromechanical Engineering,Shandong Engineering Laboratory for Preparation and Application of High-performance Carbon-Materials,Qingdao University of Science and Technology,Qingdao 266061,ChinaCollege of Electromechanical Engineering,Shandong Engineering Laboratory for Preparation and Application of High-performance Carbon-Materials,Qingdao University of Science and Technology,Qingdao 266061,ChinaCollege of Electromechanical Engineering,Shandong Engineering Laboratory for Preparation and Application of High-performance Carbon-Materials,Qingdao University of Science and Technology,Qingdao 266061,ChinaCollege of Electromechanical Engineering,Shandong Engineering Laboratory for Preparation and Application of High-performance Carbon-Materials,Qingdao University of Science and Technology,Qingdao 266061,ChinaCollege of Electromechanical Engineering,Shandong Engineering Laboratory for Preparation and Application of High-performance Carbon-Materials,Qingdao University of Science and Technology,Qingdao 266061,China
能源科技
covalent organic frameworks(COFs)functionalization strategydiffusion behaviorseparation propertiestheoretical exploration
《Nano Research》 2026 (3)
P.1058-1071,14
supported by the National Natural Science Foundation of China(No.22373054)the Natural Science Foundation of Shandong Province(No.ZR2024MB013)the Key R&D Program of Shandong Province(Major Science and Technology Innovation Project,No.2023CXGC010315).
评论