Construction of NiS/MnCdS S-scheme heterojunction for efficient photocatalytic overall water splitting: Regulation of surface sulfur vacancy and energy band structure

空位缺陷 光催化 异质结 硫黄 分解水 制氢 材料科学 电子能带结构 X射线光电子能谱 光催化分解水 电子顺磁共振 光电子学 化学工程 化学 催化作用 物理 结晶学 冶金 工程类 量子力学 有机化学 核磁共振
作者
Wei Deng,Xuqiang Hao,Yimin Wang,Yu Fan,Zhiliang Jin
出处
期刊:Fuel [Elsevier BV]
卷期号:363: 130964-130964 被引量:34
标识
DOI:10.1016/j.fuel.2024.130964
摘要

The overall water splitting based on specific photocatalysts is one of the ultimate ways to solve the energy and environmental crisis facing humanity. Sulfide photocatalysts have greater potential in photocatalytic production of solar fuel. However, due to its easy photocorrosion phenomenon, it not effectively driving the water oxidation semi-reaction to produce oxygen, so how to use sulfide photocatalyst to decompose pure water to achieve stoichiometric reaction of H2/O2 production remains a quite challenging task. Herein, sulfur vacancies-rich MnCdS nanoparticles were modified with NiS nanosheets through the hydrothermal derivation method. Different concentration gradients of sulfur-vacancy in MnCdS nanoparticles (MnCdS-Vs-X) with tunable band structures were successful prepared by regulating the concentration of hydrazine hydrate, thus improves the efficiency of light energy utilization and charge separation and the existence of S defects was verified by transmission electron microscopy (TEM) and electron paramagnetic resonance (EPR). The density function theory (DFT) calculation bears out that the draw into of S vacancy adjusted the band structure of MnCdS. Moreover, the successful construction of an S-scheme heterojunction between NiS and MnCdS-Vs-3 has been strongly demonstrated by in-situ XPS and UPS, which promoted interfacial charge separation and further improved the photocatalytic hydrogen evolution efficiency. The as-obtained S-scheme 20 %NiS/MnCdS-Vs-3 heterojunction exhibit excellent visible-light H2 production activity of 4099.55 μmol g−1h−1, 6.75 times higher than pure MnCdS. Most importantly, the excellent and stable photocatalytic overall water splitting activity of H2-509.70 μmol g-1h−1/O2-254.90 μmol g-1h−1 were obtained over 20 % NiS/MnCdS-Vs-3, which further demonstrates the application value of NiS/MnCdS-Vs-3 photocatalysts. This work proposes new ideas for the application of S-vacancies and S-scheme heterojunction in addressing the stability issues associated with sulfide-based photocatalysts in photocatalytic water splitting.
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