Tunable sieving of small gas molecules using horizontal graphene oxide membrane

Graphene oxide membrane (GOM) has attracted extensive attraction as a molecular sieve for the separation of water, ions, and gases. However, Å-level control of the GOM interlayer spacing for separating the specific size of gas molecule is difficult and the vertical transport mechanism of molecules through the GOM is highly complex because of the existence of several possible pathways. Here we fabricated GOMs with different Å-scale interlayer spacing through heat treatment and made them allow horizontal entrance and transport of gas molecules. The GOMs with angstrom channels exhibited superior performance in permeance in horizontal mode and moderate selectivity for H₂/CO₂ and He/CO₂ by tuning the sieving size of the channels. Molecular dynamics (MD) simulations reveal that the precisely controlled interlayer spacing plays a primary role as a molecular sieve indeed, but increased graphitic area, a result of heat treatment, also affects observed selectivity. Our results provide insight into the transport mechanism of gas molecules through GO nanochannel, which has not been accurately identified due to its complex behavior and suggest the possibility of studying nanochannels as effective vehicle for separating molecules precisely.