Wu Shuangzhi, Zhang Shengyu, Zhang Qingsheng, Liu Guowei, Yang Jianjun, Guan Zhongjie, Zou Zhigang
National & Local Joint Engineering Research Center for Applied Technology of Hybrid Nanomaterials, Henan University, Kaifeng, Henan, 475004, China.
Eco-materials and Renewable Energy Research Center (ERERC), Jiangsu Key Laboratory for Nano Technology, National Laboratory of Solid State Microstructures and Department of Physics, Nanjing University, Nanjing, Jiangsu, 210093, China.
Small. 2024 Nov;20(45):e2405153. doi: 10.1002/smll.202405153. Epub 2024 Jul 23.
Developing efficient photocatalysts for two-electron water splitting with simultaneous HO and H generation shows great promise for practical application. Currently, the efficiency of two-electron water splitting is still restricted by the low utilization of photogenerated charges, especially holes, of which the transfer rate is much slower than that of electrons. Herein, Ru single atoms and RuO clusters are co-decorated on ZnInS (RuO/Ru-ZIS) to employ as multifunctional sites for efficient photocatalytic pure water splitting. Doping of Ru single atoms in the ZIS basal plane enhances holes abstraction from bulk ZIS by regulating the electronic structure, and RuO clusters offer a strong interfacial electric field to remarkably promote the out-of-plane migration of holes from ZIS. Moreover, Ru single atoms and RuO clusters also serve as active sites for boosting surface water oxidation. As a result, an excellent H and HO evolution rates of 581.9 µmol g h and 464.4 µmol g h is achieved over RuO/Ru-ZIS under visible light irradiation, respectively, with an apparent quantum efficiency (AQE) of 4.36% at 400 nm. This work paves a new way to increase charge utilization by manipulating photocatalyst using single atom and clusters.
开发用于双电子水分解同时产生氢气和过氧化氢的高效光催化剂在实际应用中显示出巨大的潜力。目前，双电子水分解的效率仍然受到光生电荷（特别是空穴）利用率低的限制，其中空穴的转移速率比电子慢得多。在此，钌单原子和氧化钌团簇共修饰在硫化锌铟（RuO/Ru-ZIS）上，用作高效光催化纯水分解的多功能位点。钌单原子掺杂在ZIS基面中通过调节电子结构增强了从体相ZIS中提取空穴的能力，并且氧化钌团簇提供了强界面电场以显著促进空穴从ZIS的面外迁移。此外，钌单原子和氧化钌团簇还作为促进表面水氧化的活性位点。结果，在可见光照射下，RuO/Ru-ZIS上分别实现了581.9 μmol g⁻¹ h⁻¹和464.4 μmol g⁻¹ h⁻¹的优异氢气和过氧化氢析出速率，在400 nm处的表观量子效率（AQE）为4.36%。这项工作为通过使用单原子和团簇操纵光催化剂来提高电荷利用率开辟了一条新途径。
