Chemically Robust, Cu-based Porous Coordination Polymer Nanosheets for Efficient Hydrogen Evolution: Experimental and Theoretical Studies

Due to the extremely high number of accessible active sites and short diffusion path, porous coordination polymer (PCP) nanosheets have demonstrated a variety of promising applications, especially for energy conversion and mass transfer. However, the development of chemically stable PCP nanosheets with dense active sites and large lateral size is a great challenge in terms of feasible considerations. Herein, we first designed and prepared a kind of chemically stable PCP nanosheets via a bottom-up and a top-down integral strategy. Featuring densely exposed and periodic Cu²⁺ active sites (2.1 × 10⁶ per μm²), as well as ultrathin nature (5 nm) and significant pores (18 Å), this nanosheet demonstrated remarkable performance of electrocatalytic hydrogen evolution. Furthermore, one plausible process and the effect of Cu²⁺ active sites were proposed and validated by density functional theory calculations.