▎ 摘　　要

The development of science and technology is accompanied by a complex composition of multiple pollutants. Conventional passive separation processes are not sufficient for current industrial applications. The advent of active or responsive separation methods has become highly essential for future applications. In this work, we demonstrate the preparation of a smart electrically responsive membrane, a poly(vinylidene difluoride) (PVDF)-graphene composite membrane. The high graphene content induces the self-assembly of PVDF with a high beta-phase content, which displays a unique self-piezoelectric property. Additionally, the membrane exhibits excellent electrical conductivity and unique capacitive properties, and the resultant nanochannels in the membrane can be reversibly adjusted by external voltage applications, resulting in the tailored gas selectivity of a single membrane. After the application of voltage to the membrane, the permeability and selectivity toward carbon dioxide increase simultaneously. Moreover, atomic-level positron annihilation spectroscopic studies reveal the piezoelectric effect on the free volume of the membrane, which helps us to formulate a gas permeation mechanism for the electrically responsive membrane. Overall, the novel active membrane separation process proposed in this work opens new avenues for the development of a new generation of responsive membranes.