Basal-Plane Pores Activate Monolayer MoS2 for the Hydrogen Evolution Reaction

IF 13.1 1区 化学 Q1 CHEMISTRY, PHYSICAL ACS Catalysis Pub Date : 2025-02-18 DOI:10.1021/acscatal.4c07970
Holly M. Fruehwald, Yossarian Liebsch, Umair Javed, Henning Lebius, Clara Grygiel, Radia Rahali, Jani Kotakoski, Marika Schleberger, Rodney D. L. Smith
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Abstract

Identification of catalytically relevant sites in solid-state materials and our ability to manipulate such sites is critical to designing improved electrocatalysts. In this work, we prepare a series of monolayer MoS2 using chemical vapor deposition and install varied concentrations of defects through swift heavy ion irradiation. Electron micrographs indicate that the ion irradiation procedure generates pores within MoS2 flakes, and Raman microscopic maps show that the defects exert a strongly localized influence. The localization is strong enough that spectra acquired across individual particles can be classified in a binary fashion: regions are either affected by the irradiation-induced pore or appear as pristine MoS2. Besides providing insight into the nature of the defects within the monolayers, this feature enables spatial resolution of regions with significant densities of such pores. This capability is used to quantify the defect density across the sample series and show that the pores located within the MoS2 flakes are particularly active sites for electrocatalytic hydrogen evolution.

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基面孔隙激活二硫化钼单层析氢反应
鉴定固态材料中与催化相关的位点以及我们操纵这些位点的能力对于设计改进的电催化剂至关重要。在这项工作中,我们采用化学气相沉积方法制备了一系列单层二硫化钼,并通过快速重离子辐照安装了不同浓度的缺陷。电子显微图显示离子辐照过程在二硫化钼薄片中产生孔洞,拉曼显微图显示缺陷产生强烈的局部影响。这种定位足够强,以至于在单个粒子上获得的光谱可以以二元方式分类:区域要么受到辐射诱导孔隙的影响,要么表现为原始的二硫化钼。除了提供对单层内缺陷性质的深入了解外,该特征还可以实现具有此类孔隙显著密度的区域的空间分辨率。这种能力被用来量化整个样品系列的缺陷密度,并表明位于MoS2薄片内的孔隙是电催化析氢的特别活跃的位点。
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来源期刊
ACS Catalysis
ACS Catalysis CHEMISTRY, PHYSICAL-
CiteScore
20.80
自引率
6.20%
发文量
1253
审稿时长
1.5 months
期刊介绍: ACS Catalysis is an esteemed journal that publishes original research in the fields of heterogeneous catalysis, molecular catalysis, and biocatalysis. It offers broad coverage across diverse areas such as life sciences, organometallics and synthesis, photochemistry and electrochemistry, drug discovery and synthesis, materials science, environmental protection, polymer discovery and synthesis, and energy and fuels. The scope of the journal is to showcase innovative work in various aspects of catalysis. This includes new reactions and novel synthetic approaches utilizing known catalysts, the discovery or modification of new catalysts, elucidation of catalytic mechanisms through cutting-edge investigations, practical enhancements of existing processes, as well as conceptual advances in the field. Contributions to ACS Catalysis can encompass both experimental and theoretical research focused on catalytic molecules, macromolecules, and materials that exhibit catalytic turnover.
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