▎ 摘　　要

Fast response and adjustable selectivity have always been the main goals pursued by the manufacture of smart membranes. Herein, we demonstrate smart membrane materials composed of ionic liquid (IL), PVDF, and graphene. The infusion of IL aims to increase the beta crystal phase of PVDF, which is also assisted by the presence of graphene in the system. beta-PVDF increased from 48.9% to 79.8% when the ionic liquid content [BMIM][BF4] increases from 2 to 10 wt.%, which makes the membrane more electro responsive. The optimum membrane of PG-BF4 10 wt.%, upon supply of 3 V DC electricity, exhibited CO2/N-2 selectivity value of about 129.03 and CO2 permeability of 193.55 Barrer, exceeding the 2008 Robeson upper bound. Positron Annihilation Lifetime Spectroscopy (PALS) data and Density Function Theory (DFT) simulations helped to realize the mechanism of selective transportation of CO2 gas through the membrane both theoretically and experimentally. PALS results indicated that the free volume of PVDF increased; indicating that CO2 molecules can easily pass through the system. DFT simulation revealed that the CO2 molecules show more attraction and lower adsorption energy under electric stimuli, confirming that CO2 molecules adsorb and diffuse quickly through the system than O-2 or N-2 . Overall, tuning the free volume and molecular interactions within the membrane channels provide a rational molecular sieving approach to improve membrane selectivity. (C) 2022 Elsevier Ltd. All rights reserved.