Enhancing the catalytic activity of the alkaline hydrogen evolution reaction by tuning the S/Se ratio in the Mo(SxSe1−x)2 catalyst†,Nanoscale

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Enhancing the catalytic activity of the alkaline hydrogen evolution reaction by tuning the S/Se ratio in the Mo(SxSe1−x)2 catalyst†
Nanoscale ( IF 5.8 ) Pub Date : 2018-07-31 00:00:00 , DOI: 10.1039/c8nr05738a
Ronen Bar-Ziv _{1,

2,

3,

4,

5} , Oren E. Meiron _{1,

2,

3,

4} , Maya Bar-Sadan _{1,

2,

3,

4}

Affiliation

The alkaline hydrogen evolution reaction (HER) plays a key role in photo(electro)catalytic water splitting technologies, particularly in water–alkali electrolyzers. Unfortunately, although transition metal dichalcogenide (TMD) materials, especially MoS₂ and MoSe₂, are considered efficient, Earth-abundant catalysts for the HER in an acidic electrolyte, they are much less effective under high pH conditions due to a sluggish water dissociation process (Volmer-step) and strong adsorption of the OH⁻ intermediate on their surfaces. Herein we show a novel synergetic effect obtained by tailoring the S/Se ratio in Mo(S_xSe_1−x)₂ alloys. We were able to influence the metal oxidation state and d-band to optimize the catalytic sites for H⋯OH dissociation and OH⁻ desorption while maintaining favourable M–H energetics. The Mo(S_xSe_1−x)₂ (x = 0.58) catalyst exhibited high performance with an onset potential of −43 mV in 0.5 M KOH, i.e., ∼3 and ∼4-fold less than that for MoSe₂ and MoS₂, respectively. The results obtained in the current study have implications for the rational design of cost-effective electro-catalysts for water reduction based on TMD alloys.

中文翻译：

通过调节Mo（S _x Se _{1- x}）₂催化剂中的S / Se比来增强碱性氢释放反应的催化活性†

碱性氢放出反应（HER）在光（电）催化水分解技术中，尤其是在水-碱电解槽中，起着关键作用。不幸的是，尽管过渡金属_二硫化氢（TMD）材料（尤其是MoS ₂和MoSe ₂）被认为是酸性电解质中HER的高效，富含地球的催化剂，但由于水解离过程缓慢，它们在高pH条件下的效果要差得多（沃尔默步骤）和强吸附的OH的^-它们的表面上的中间。在这里，我们显示了通过调整Mo（S _x Se _{1- x}）_2中的S / Se比获得的新型协同效应合金。我们能够影响金属氧化态和d带，以优化用于h⋯OH解离和OH催化位点^-脱附，同时保持良好的M-H热力学。Mo（S _x Se _{1- x}）₂（x = 0.58）催化剂表现出高性能，在0.5 M KOH中的起始电位为-43 mV，即比MoSe ₂和MoS的起始电位低约3倍和约4倍。₂，分别。在当前研究中获得的结果对合理设计基于TMD合金的节水高效电催化剂具有重要意义。

更新日期：2018-07-31

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