Optimizing catalytic performance of ReS2 thin films: development of Re(1−x)WxS2 alloys for enhanced hydrogen evolution via aerosol-assisted CVD

IF 1.7 4区化学 Q3 CHEMISTRY, INORGANIC & NUCLEAR

Transition Metal Chemistry Pub Date : 2025-06-07 DOI:10.1007/s11243-025-00661-7

Naktal Al-Dulaimi, Mundher Al-Shakban, Inigo Yrezabal, Andinet Ejigu

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引用次数: 0

Abstract

Transition metal dichalcogenides (M = Mo, W, Re) have gained significant attention for electrocatalytic applications in renewable energy due to their unique layered structures. However, their catalytic activity is often limited by the inert nature of basal planes, with active sites primarily located along the edges. In this study, we employed doping as a strategy to enhance the catalytic performance of Re_(1−x)W_xS₂ alloys by increasing the density of active sites. Using Re₂(µ-S)₂(S₂CNEt₂)₄ (1) and WS₃(S₂CNEt₂)₂ (2) as precursors, thin films were synthesized via aerosol-assisted chemical vapor deposition at 500 °C. Comprehensive characterization using powder X-ray diffraction, Raman spectroscopy, inductively coupled plasma optical emission spectroscopy, scanning electron microscopy, energy-dispersive X-ray spectroscopy, and transmission electron microscopy (TEM) confirmed the successful formation of Re_(1−x)W_xS₂ alloys. TEM analysis revealed a phase transition from 1T to 2H at W concentrations between 22.6 and 30.8%, indicating a structural evolution from the ReS₂ (1T) to WS₂ (2H) phase. Catalytic testing of both bulk and exfoliated materials in hydrogen evolution demonstrated that doping-induced structural modifications led to a higher density of catalytically active sites, significantly enhancing performance. These findings underscore the role of doping in tailoring the electronic and structural properties of TMDCs to optimize their catalytic efficiency, paving the way for their broader application in sustainable energy technologies.

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优化ReS2薄膜的催化性能：通过气溶胶辅助CVD制备Re(1−x)WxS2合金以促进析氢

过渡金属二硫族化合物（M = Mo， W, Re）由于其独特的层状结构在可再生能源中的电催化应用受到了极大的关注。然而，它们的催化活性往往受到基面惰性性质的限制，活性位点主要位于边缘。在这项研究中，我们采用掺杂作为策略，通过增加活性位点的密度来提高Re(1−x)WxS2合金的催化性能。以Re2（µ-S）2(S2CNEt2)4(1)和WS3(S2CNEt2)2(2)为前驱体，在500℃下采用气溶胶辅助化学气相沉积法制备薄膜。采用粉末x射线衍射、拉曼光谱、电感耦合等离子体发射光谱、扫描电镜、能量色散x射线光谱和透射电镜（TEM）进行综合表征，证实了Re(1−x)WxS2合金的成功形成。TEM分析显示，在W浓度为22.6 ~ 30.8%时，材料的相由1T向2H转变，结构由ReS2 （1T）向WS2 （2H）转变。对大块材料和脱落材料在析氢过程中的催化测试表明，掺杂诱导的结构修饰导致催化活性位点密度更高，显著提高了性能。这些发现强调了掺杂在调整TMDCs的电子和结构特性以优化其催化效率方面的作用，为其在可持续能源技术中的更广泛应用铺平了道路。

本文章由计算机程序翻译，如有差异，请以英文原文为准。

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来源期刊

Transition Metal Chemistry 化学-无机化学与核化学

CiteScore

3.60

自引率

0.00%

发文量

审稿时长

1.3 months

期刊介绍： Transition Metal Chemistry is an international journal designed to deal with all aspects of the subject embodied in the title: the preparation of transition metal-based molecular compounds of all kinds (including complexes of the Group 12 elements), their structural, physical, kinetic, catalytic and biological properties, their use in chemical synthesis as well as their application in the widest context, their role in naturally occurring systems etc. Manuscripts submitted to the journal should be of broad appeal to the readership and for this reason, papers which are confined to more specialised studies such as the measurement of solution phase equilibria or thermal decomposition studies, or papers which include extensive material on f-block elements, or papers dealing with non-molecular materials, will not normally be considered for publication. Work describing new ligands or coordination geometries must provide sufficient evidence for the confident assignment of structural formulae; this will usually take the form of one or more X-ray crystal structures.