Construction of Hydration Layer for Proton Transport by Implanting the Hydrophilic Center Ag0 in Nickel Metal‐Organic Frameworks

Abstract The directional arrangement of H 2 O molecules can effectively regulate the ordered protons transfer to improve transport efficiency, which can be controlled by the interaction between materials and H 2 O. Herein, a strategy to build a stable hydration layer in metal‐organic framework (MOF) platforms, in which hydrophilic centers that can manipulate H 2 O molecules are implanted into MOF cavities is presented. The rigid grid‐Ni‐MOF is selected as the supporting material due to the uniformly distributed cavities and rigid structures. The Ag 0 possesses potential combination ability with the hydrophilic substances, so it is introduced into the MOF as hydration layer centers. Relying on the strong interaction between Ag 0 and H 2 O, the H 2 O molecules can rearrange around Ag 0 in the cavity, which is intuitively verified by DFT calculation and molecular dynamics simulation. The establishment of a hydration layer in Ag@Ni‐MOF regulates the chemical properties of the material and gives the material excellent proton conduction performance, with a proton conductivity of 4.86 × 10 −2 S cm −1 .