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Significance The energy efficiency of gas separation is expected to benefit from the development of membranes yielding selective but large permeance. The ultimate limit of this is two-dimensional films hosting a high density of molecular-selective apertures (e.g., nanoporous single-layer graphene). Currently, pores are incorporated in single-layer graphene by postsynthetic etching route, and the direct bottom-up synthesis of nanoporous graphene, especially targeting a high pore density, remains a grand challenge attributing to a number of crystallization bottlenecks. We address this by increasing the density of molecular-sized intrinsic vacancy defects in graphene by developing crystallization conditions which promote the growth of misoriented grains, limiting the grains to a few nanometers in size and preventing a complete grain intergrowth while yielding mechanically robust films.

Bottom-up synthesis of graphene films hosting atom-thick molecular-sieving apertures