▎ 摘　　要

Graphene membranes with subnanopores are considered to be the next-generation materials for water desalination and ion separation,; while their Performance is mainly determined by the relative ion selectivity of the pores. However, the origin of this phenomenon has been controversial in the past few Years) which strongly limits the development of related applications. Here, using direct Au ion bombardment, we fabricated the desired subnanopores with average diameters of 0.8 +/- 0.16 nm monolayer graphene. The Pores showed the ability to sieve K+, Na+, Li+, Cs+, Mg2+, and Ca2+ cations, and the observed K+/Mg2+ selectivity ratio was over 4. With further molecular dynamics simulations, we demonstrated that the ion selectivity is primarily attributed to the dehydration process of ions that can be quantitatively described by the ion-dependent free-energy barriers. Hopefully, this work is helpful in further enhancing the ion selectivity of graphene nanopores and also Presenting a new Paradigm for improving the performance of other nanoporous atomically thin membranes, such as MXenes and MoS2.