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通过合理构建S型异质结来调节D带中心以优化光催化析氢性能。

Optimizing photocatalytic hydrogen evolution performance by rationally constructing S-scheme heterojunction to modulate the D-band center.

作者信息

Jin Zhiliang, Yang Cheng

机构信息

School of Chemistry and Chemical Engineering, Ningxia Key Laboratory of Solar Chemical Conversion Technology, Key Laboratory for Chemical Engineering and Technology, State Ethnic Affairs Commission, North Minzu University, Yinchuan 750021, PR China.

School of Chemistry and Chemical Engineering, Ningxia Key Laboratory of Solar Chemical Conversion Technology, Key Laboratory for Chemical Engineering and Technology, State Ethnic Affairs Commission, North Minzu University, Yinchuan 750021, PR China.

出版信息

J Colloid Interface Sci. 2025 Jan;677(Pt B):205-220. doi: 10.1016/j.jcis.2024.08.066. Epub 2024 Aug 11.

DOI:10.1016/j.jcis.2024.08.066
PMID:39142161
Abstract

The research in the field of photocatalysis has progressed, with the development of heterojunctions being recognized as an effective method to improve carrier separation efficiency in light-induced processes. In this particular study, CuCoS particles were attached to a new cubic CdS surface to create an S-scheme heterojunction, thus successfully addressing this issue. Specifically, owing to the higher conduction band and Fermi level of CuCoS compared to CdS, they serve as the foundation and driving force for the formation of an S-scheme heterojunction. Through in-situ X-ray photoelectron spectroscopy and electron paramagnetic resonance analysis, the direction of charge transfer in the composite photocatalyst under light exposure was determined, confirming the charge transfer mechanism of the S-scheme heterojunction. By effectively constructing the S-scheme heterojunction, the d-band center of the composite photocatalyst was adjusted, reducing the energy needed for electron filling in the anti-bonding energy band, promoting the transfer of photogenerated carriers, and ultimately enhancing the photocatalytic hydrogen production. performance. After optimization, the hydrogen evolution activity of the composite photocatalyst CdS-C/CuCoS-3 reached 5818.9 μmol gh, which is 2.6 times higher than that of cubic CdS (2272.3 μmol gh) and 327.4 times higher than that of CuCoS (17.8 μmol gh), showcasing exceptional photocatalytic activity. Electron paramagnetic resonance and in situ X-ray photoelectron spectroscopy have established a theoretical basis for designing and constructing S-scheme heterojunctions, offering a viable method for adjusting the D-band center to enhance the performance of photocatalytic hydrogen evolution.

摘要

随着异质结的发展被认为是提高光诱导过程中载流子分离效率的有效方法,光催化领域的研究取得了进展。在这项具体研究中,将CuCoS颗粒附着在新型立方CdS表面以形成S型异质结,从而成功解决了这一问题。具体而言,由于CuCoS的导带和费米能级高于CdS,它们成为形成S型异质结的基础和驱动力。通过原位X射线光电子能谱和电子顺磁共振分析,确定了复合光催化剂在光照下的电荷转移方向,证实了S型异质结的电荷转移机制。通过有效地构建S型异质结,调整了复合光催化剂的d带中心,降低了反键能带中电子填充所需的能量,促进了光生载流子的转移,最终提高了光催化产氢性能。优化后,复合光催化剂CdS-C/CuCoS-3的析氢活性达到5818.9 μmol g h,分别是立方CdS(2272.3 μmol g h)的2.6倍和CuCoS(17.8 μmol g h)的327.4倍,展现出优异的光催化活性。电子顺磁共振和原位X射线光电子能谱为设计和构建S型异质结奠定了理论基础,为调整d带中心以提高光催化产氢性能提供了一种可行的方法。

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