Pd single atoms cooperate with S vacancies in ZnIn_(2)S_(4) nanosheets for photocatalytic pure-water splitting

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,insitu 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 1,021.4μmol 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.