ABSTRACT
Membranes with ultrapermeability for CO2 are desired for future large-scale carbon capture projects, because of their excellent separative productivity and economic efficiency. Herein, we demonstrate that a membrane with ultrapermeability for CO2 can be constructed by combining N/O para-doped noble carbons, C2NxO1-x, with high-permeability polymer PIM-1. The optimal PIM-1/C2NxO1-x membranes exhibit superior CO2 permeability (22110 Barrer) with a CO2/N2 selectivity of 15.5, and an unprecedented CO2 permeability of 37272 Barrer can be obtained after a PEG activation treatment, far surpassing the 2008 upper bound. Both broad experiments and molecular dynamics simulations reveal that the numerous ordered polar channels of C2NxO1-x and their excellent compatibility with PIM-1 are responsible for the superior CO2 separation performance of the membrane. Although this is the first study on C2N-type gas separation membranes, the outstanding results indicate that noble carbon building blocks may pave a new avenue to advance high-performance CO2 separation membranes.