▎ 摘　　要

Defective graphene holds great potential to enable the permeation of gas molecules at high rates with high selectivity due to its one-atom thickness and resultant atomically small pores at the defect sites. However, precise control and tuning of the size and density of the defects remain challenging. In this work, we introduce atomic-scale defects into bilayer graphene via a decoupled strategy of defect nucleation using helium ion irradiation followed by defect expansion using hydrogen plasma treatment. The cotreated membranes exhibit high permeability and simultaneously high selectivity compared to those singly treated by ion irradiation or hydrogen plasma only. High permeation selectivity values for H-2/N-2 and H-2/CH4 of 495 and 877, respectively, are achieved for optimally cotreated membranes. The method presented can also be scaled up to prepare large-area membranes for gas separation, e.g., for hydrogen purification and recovery from H-2/CH4 and H-2/N-2 mixtures.