Pd single atoms cooperate with S vacancies in ZnIn2S4 nanosheets for photocatalytic pure-water splitting

• Published in: Science China. Chemistry 2024-03, Vol.67 (3), p.855-861
• Main Authors: Sun, Lin, Peng, Huiping, Xue, Fei, Liu, Shangheng, Hu, Zhiwei, Geng, Hongbo, Liu, Xiaozhi, Su, Dong, Xu, Yong, Huang, Xiaoqing
• Format: Article
• Language: English
• Subjects: Catalysis; Chemistry; Chemistry and Materials Science; Chemistry/Food Science; Clean energy; Communications; Doping; Electron paramagnetic resonance; Fourier transforms; Holes (electron deficiencies); Hydrogen peroxide; Infrared spectroscopy; Palladium; Photocatalysis; Photocatalysts; Scanning transmission electron microscopy; Solar energy conversion; Water splitting
• ISSN: 1674-7291; 1869-1870
• DOI: 10.1007/s11426-023-1861-7

Photocatalytic water splitting has emerged as a new frontier for converting solar energy to green H 2 and value-added chemicals. Nevertheless, great challenges still remain for developing efficient photocatalysts for pure water splitting without sacrificial agents. In this work, we demonstrate that doping hexagonal ZnIn 2 S 4 (ZIS) with Pd single atoms (Pd 0.03 /ZIS) can serve as a highly efficient photocatalyst for pure water splitting to simultaneously produce H 2 and H 2 O 2 without any sacrificial agents. Results from aberration-corrected high-angle annular dark field scanning transmission electron microscopy, X-ray fine spectroscopy, in-situ electron paramagnetic resonance and diffuse Fourier transform infrared spectroscopy reveal that doping ZIS with Pd single atoms facilitates the formation of S vacancies (S v ), where the photogenerated electrons can transfer to Pd single atoms, as a result of enhanced separation of electron-hole pairs and improved photocatalytic performance. Impressively, Pd 0.03 /ZIS displays a stoichiometric ratio of H 2 and H 2 O 2 with the productivity of 1,037.9 and 1,021.4 μmol g −1 h −1 , respectively, which has largely outperformed pure ZIS and other reported catalysts for pure water splitting. This work provides an efficient photocatalyst for water splitting to produce H 2 and H 2 O 2 , which may attract rapid interest in materials science, chemistry, and heterogeneous catalysis.