Single-layer graphene membrane is proven to be highly efficient in separating hydrogen isotopes. But the defects of large-scale graphene during preparation and transfer and the high swelling rate(15%) of Nafion(support of graphene) in a liquid-phase environment limit the applications of single-layer graphene. In this work, interfacial polymerization was employed to seal the defect and cracks on graphene, while replacing graphene support from Nafion to Polyimide track-etched membrane (PITEM), whose extremely low swelling rate (0.329%) guarantees that graphene will not be destroyed in a liquid-phase environment. The H/D separation ratio is elevated from 6.0 to 7.9 after interfacial polymerization. We also proposed a new theory based on the kinetic isotope effect (KIE) to explain the high H/D separation ratio (~10) of monolayer graphene. This theory shows that the role of graphene is to completely break the O-H/O-D bond in the process of H/D separation, which can maximize the H/D separation ratio based on KIE (4.0 to 7.9). This work not only makes the industrial application of single-layer graphene possible but also makes people a clearer understanding of proton transport in graphene

Sieving hydrogen isotopes in liquid phase through large scale monolayer graphene repaired by interfacial polymerization

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