Zhang Shiqi, Lu Lele, Jiang Jialong, Liu Ning, Zhao Bin, Xu Mingming, Cheng Peng, Shi Wei
Key Laboratory of Advanced Energy Materials Chemistry (MOE) and State Key Laboratory of Advanced Chemical Power Sources, Nankai University, Tianjin, 300071, China.
Adv Mater. 2024 Jun;36(26):e2403464. doi: 10.1002/adma.202403464. Epub 2024 Apr 15.
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 Ho-CdNi-NS exhibits a superior photocatalytic hydrogen evolution rate of 40.06 mmol g h 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.
光催化剂中光敏性和光热性能的有效结合对于实现最大程度的光利用以获得卓越的光催化效率至关重要。在此，本工作成功地在定制的三金属金属有机框架内将光敏性Cd-NS单位点和光热Ni-NS单位点在分子水平上均匀地组织起来。优化后的Ho-CdNi-NS在可见光照射下表现出40.06 mmol g⁻¹ h⁻¹的优异光催化析氢速率，在420 nm处的表观量子效率为29.37%，且无需使用助催化剂或光敏剂。系统的机理研究表明，均匀组织的光敏和光热单位点具有协同效应，形成了光生电子高效传输的超短路径，抑制了光生载流子的复合，从而促进了析氢活性。这项工作为在光催化剂中均匀组织双功能单位点以实现高性能光催化活性提供了一种有前景的方法。
