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Xin, Xu; Li, Yuke; Zhang, Youzi; Wang, Yijin; Chi, Xiao; Wei, Yanping; Diao, Caozheng; Su, Jie; Wang, Ruiling; Guo, Peng; Yu, Jiakang; Zhang, Jia; Sobrido, Ana Jorge; Titirici, Maria-Magdalena; Li, Xuanhua
Nature communications, 01/2024, Volume: 15, Issue: 1Journal Article
Abstract Photocatalytic overall water splitting into hydrogen and oxygen is desirable for long-term renewable, sustainable and clean fuel production on earth. Metal sulfides are considered as ideal hydrogen-evolved photocatalysts, but their component homogeneity and typical sulfur instability cause an inert oxygen production, which remains a huge obstacle to overall water-splitting. Here, a distortion-evoked cation-site oxygen doping of ZnIn 2 S 4 (D-O-ZIS) creates significant electronegativity differences between adjacent atomic sites, with S 1 sites being electron-rich and S 2 sites being electron-deficient in the local structure of S 1 –S 2 –O sites. The strong charge redistribution character activates stable oxygen reactions at S 2 sites and avoids the common issue of sulfur instability in metal sulfide photocatalysis, while S 1 sites favor the adsorption/desorption of hydrogen. Consequently, an overall water-splitting reaction has been realized in D-O-ZIS with a remarkable solar-to-hydrogen conversion efficiency of 0.57%, accompanying a ~ 91% retention rate after 120 h photocatalytic test. In this work, we inspire an universal design from electronegativity differences perspective to activate and stabilize metal sulfide photocatalysts for efficient overall water-splitting.
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