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评估胶体法制备的PtSe和PtTe催化剂在碱性介质中的析氢反应活性。

Evaluating the Hydrogen Evolution Reaction Activity of Colloidally Prepared PtSe and PtTe Catalysts in an Alkaline Medium.

作者信息

Mxakaza Lineo F, Mashindi Victor, Linganiso Cebisa E, Moloto Nosipho, Tetana Zikhona N

机构信息

Molecular Science Institute, School of Chemistry, University of the Witwatersrand, Private Bag 3, Wits, 2050, South Africa.

DSI/NRF Centre of Excellence in Strong Materials, University of the Witwatersrand, Private Bag 3, Wits, 2050, South Africa.

出版信息

ChemistryOpen. 2024 Oct;13(10):e202400146. doi: 10.1002/open.202400146. Epub 2024 Jul 23.

Abstract

The hydrogen evolution reaction (HER) in alkaline electrolytes using transition metal dichalcogenides is a research area that is not tapped into. Alkaline HER ( ) is harder to achieve relative to acidic HER ( ), this is attributed to the additional water dissociation step that occurs in basic HER to generate H ions. In fact, for most catalysts, their HER activity decreases tremendously when the electrolyte is changed from acidic to basic conditions. Platinum dichalcogenides, PtX (X=S, Se, Te), are an interesting member of transition metal dichalcogenides (TMDs) as these show an immense hybridization of the Pt d orbitals and chalcogen p orbitals because of closely correlated orbital energies. The trend in electronic properties of these materials changes drastically as the chalcogen is changed, with PtS reported to exhibit semi-conductor properties, PtSe is semi-metallic or semi-conductive, depending on the number of layers, while PtTe is metallic. The effect of varying the chalcogen atom on the HER activity of Pt dichalcogenides will be studied. Pt dichalcogenides have previously been prepared by direct high-temperature chalcogen deposition of Pt substrate and evaluated as electrocatalysts for HER in HSO. The previously employed synthesis procedures for PtX limit these compounds' mass production and post-synthesis treatment. In this study, we demonstrated, for the first time the preparation of PtSe and PtTe by colloidal synthesis. Colloidal synthesis offers the possibility of large-scale synthesis of materials and affords the employment of the colloids at various concentrations in ink formulation. The electrochemical HER results acquired in 1 M KOH indicate that PtTe has a superior HER catalytic activity to PtSe. A potential of 108 mV for PtTe and 161 mV for PtSe is required to produce a current density of -10 mA cm from these catalysts. PtTe has a low Tafel slope of 79 mVdec, indicating faster HER kinetics on PtTe. Nonetheless, the stability of these catalysts in an alkaline medium needs to be improved to render them excellent HER electrocatalysts.

摘要

使用过渡金属二硫属化物在碱性电解质中进行析氢反应(HER)是一个尚未开发的研究领域。相对于酸性析氢反应( ),碱性析氢反应( )更难实现,这归因于在碱性析氢反应中发生的额外水离解步骤以产生H离子。事实上,对于大多数催化剂而言,当电解质从酸性条件变为碱性条件时,它们的析氢活性会大幅下降。二硫属化铂,PtX(X = S、Se、Te),是过渡金属二硫属化物(TMDs)中一个有趣的成员,因为由于轨道能量密切相关,这些材料显示出Pt d轨道和硫属元素p轨道的巨大杂化。随着硫属元素的变化,这些材料的电子性质趋势会发生巨大变化,据报道PtS表现出半导体性质,PtSe根据层数不同是半金属或半导体,而PtTe是金属。将研究改变硫属元素原子对二硫属化铂析氢活性的影响。二硫属化铂此前是通过在Pt基底上直接高温硫属化沉积制备的,并在HSO中作为析氢反应的电催化剂进行了评估。此前用于制备PtX的合成程序限制了这些化合物的大规模生产和合成后处理。在本研究中,我们首次展示了通过胶体合成制备PtSe和PtTe。胶体合成提供了大规模合成材料的可能性,并允许在油墨配方中使用各种浓度的胶体。在1 M KOH中获得的电化学析氢结果表明,PtTe具有比PtSe更高的析氢催化活性。要从这些催化剂产生-?10 mA cm的电流密度,PtTe需要108 mV的过电位,PtSe需要161 mV的过电位。PtTe的塔菲尔斜率为79 mVdec,表明在PtTe上析氢动力学更快。尽管如此,这些催化剂在碱性介质中的稳定性仍需提高,以使它们成为优异的析氢电催化剂。

https://cdn.ncbi.nlm.nih.gov/pmc/blobs/6460/11633348/91e1ce001cc5/OPEN-13-e202400146-g003.jpg

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