Water‐Stable High‐Entropy Metal‐Organic Framework Nanosheets for Photocatalytic Hydrogen Production

Abstract Metal‐organic frameworks (MOFs) have emerged as promising platforms for photocatalytic hydrogen evolution reaction (HER) due to their fascinating physiochemical properties. Rationally engineering the compositions and structures of MOFs can provide abundant opportunities for their optimization. In recent years, high‐entropy materials (HEMs) have demonstrated great potential in the energy and environment fields. However, there is still no report on the development of high‐entropy MOFs (HE‐MOFs) for photocatalytic HER in aqueous solution. Herein, the authors report the synthesis of a novel p‐type HE‐MOFs single crystal (HE‐MOF‐SC) and the corresponding HE‐MOFs nanosheets (HE‐MOF‐NS) capable of realizing visible‐light‐driven photocatalytic HER. Both HE‐MOF‐SC and HE‐MOF‐NS exhibit higher photocatalytic HER activity than all the single‐metal MOFs, which are supposed to be ascribed to the interplay between the different metal nodes in the HE‐MOFs that enables more efficient charge transfer. Moreover, impressively, the HE‐MOF‐NS demonstrates much higher photocatalytic activity than the HE‐MOF‐SC due to its thin thickness and enhanced surface area. At optimum conditions, the rate of H₂ evolution on the HE‐MOF‐NS is ≈13.24 mmol h⁻¹ g⁻¹, which is among the highest values reported for water‐stable MOF photocatalysts. This work highlights the importance of developing advanced high‐entropy materials toward enhanced photocatalysis.