Yu Jinxing, Huang Jie, Li Ronghua, Li Yanbo, Liu Gang, Xu Xiaoxiang
Shanghai Key Lab of Chemical Assessment and Sustainability, School of Chemical Science and Engineering, Tongji University, Shanghai, China.
Shenyang National laboratory for Materials Science, Institute of Metal Research, Chinese Academy of Sciences, 72 Wenhua Road, Shenyang, China.
Nat Commun. 2025 Jan 3;16(1):361. doi: 10.1038/s41467-024-55748-z.
Photocatalytic overall water splitting is a promising approach for a sustainable hydrogen provision using solar energy. For sufficient solar energy utilization, this reaction ought to be operated based on visible-light-active semiconductors, which is very challenging. In this work, an F-expedited nitridation strategy is applied to modify the wide-bandgap semiconductor SrTiO for visible-light-driven photocatalytic overall water splitting. Compared to the conventional nitridation approach, F-expedited nitridation introduces the desirable integration of a high concentration of N dopant for strong visible light absorption and a low concentration of defects (i.e. Ti and oxygen vacancies) for effective separation of photocarriers. After being coated with Ti-oxyhydroxide protection layer and deposited with RhCrO cocatalyst, the product from F-expedited nitridation can stably run photocatalytic overall water splitting with apparent quantum efficiency of 0.39% at 420 ± 20 nm and solar-to-hydrogen efficiency of 0.028%. These findings justify the effectiveness of F-expedited nitridation strategy and serve as a guidance to upgrade the photocatalytic activity of many other wide-bandgap semiconductors.
光催化全分解水是一种利用太阳能可持续制氢的很有前景的方法。为了充分利用太阳能，该反应应该基于可见光活性半导体来进行，而这极具挑战性。在这项工作中，采用氟促进氮化策略对宽带隙半导体SrTiO进行改性，以实现可见光驱动的光催化全分解水。与传统的氮化方法相比，氟促进氮化引入了理想的整合，即高浓度的氮掺杂剂用于强烈的可见光吸收，以及低浓度的缺陷（即钛和氧空位）用于光生载流子的有效分离。在用氢氧化钛保护层包覆并沉积RhCrO助催化剂后，氟促进氮化产物能够稳定地进行光催化全分解水，在420±20nm处的表观量子效率为0.39%，太阳能到氢能的效率为0.028%。这些发现证明了氟促进氮化策略的有效性，并为提升许多其他宽带隙半导体的光催化活性提供了指导。
