Organizing Photosensitive and Photothermal Single‐Sites Uniformly in a Trimetallic Metal‐Organic Framework for Efficient Photocatalytic Hydrogen Evolution

Effective combination of the photosensitivity and photothermal property in photocatalyst is vital to achieve the maximum light utilization for superior photocatalytic efficiency. Herein, this work successfully organizes photosensitive Cd-NS single-sites and photothermal Ni-NS single-sites uniformly at a molecular level within a tailored trimetallic metal-organic framework. The optimized Ho6-Cd0.76Ni0.24-NS exhibits a superior photocatalytic hydrogen evolution rate of 40.06 mmol g-1 h-1 under visible-light irradiation and an apparent quantum efficiency of 29.37% at 420 nm without using cocatalysts or photosensitizers. A systematical mechanism study reveals that the uniformly organized photosensitive and photothermal single-sites have synergistic effect, which form ultrashort pathways for efficient transport of photoinduced electrons, suppress the recombination of photogenerated charge carriers, hence promote the hydrogen evolution activity. This work provides a promising approach for organizing dual-functional single-sites uniformly in photocatalyst for high-performance photocatalytic activity.