电负性
光催化分解水
光催化
分解水
制氢
氢
硫化氢
氧气
硫化物
吸附
化学
金属
无机化学
硫黄
材料科学
催化作用
光化学
物理化学
生物化学
有机化学
作者
Xin Xu,Yuke Li,Youzi Zhang,Yijin Wang,Xiao Chi,Yan-Ping Wei,Caozheng Diao,Jie Su,Ruiling Wang,Peng Guo,Jiakang Yu,Jia Zhang,Ana Jorge Sobrido,Maria‐Magdalena Titirici,Tongtong Li
标识
DOI:10.1038/s41467-024-44725-1
摘要
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.
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