Large electronegativity differences between adjacent atomic sites activate and stabilize ZnIn2S4 for efficient photocatalytic overall water splitting

Xu Xin, Yuke Li, Youzi Zhang, Yijin Wang, Xiao Chi, Yanping Wei, Caozheng Diao, Jie Su, Ruiling Wang, Peng Guo, Jiakang Yu, Jia Zhang, Ana Jorge Sobrido, Maria-Magdalena Titirici and Xuanhua Li ()
Additional contact information
Xu Xin: Northwestern Polytechnical University
Yuke Li: Technology and Research (A*STAR)
Youzi Zhang: Northwestern Polytechnical University
Yijin Wang: Northwestern Polytechnical University
Xiao Chi: National University of Singapore
Yanping Wei: Gansu Agricultural University
Caozheng Diao: National University of Singapore
Jie Su: Xidian University
Ruiling Wang: Northwestern Polytechnical University
Peng Guo: Northwestern Polytechnical University
Jiakang Yu: Northwestern Polytechnical University
Jia Zhang: Technology and Research (A*STAR)
Ana Jorge Sobrido: Queen Mary University of London
Maria-Magdalena Titirici: South Kensington Campus
Xuanhua Li: Northwestern Polytechnical University

Nature Communications, 2024, vol. 15, issue 1, 1-12

Abstract: 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 ZnIn2S4 (D-O-ZIS) creates significant electronegativity differences between adjacent atomic sites, with S1 sites being electron-rich and S2 sites being electron-deficient in the local structure of S1–S2–O sites. The strong charge redistribution character activates stable oxygen reactions at S2 sites and avoids the common issue of sulfur instability in metal sulfide photocatalysis, while S1 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.

Date: 2024
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DOI: 10.1038/s41467-024-44725-1

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