Unraveling the Effect of Rh Isolation on Shallow d States of Gallium–Rhodium Alloys,The Journal of Physical Chemistry C

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Unraveling the Effect of Rh Isolation on Shallow d States of Gallium–Rhodium Alloys
The Journal of Physical Chemistry C ( IF 3.3 ) Pub Date : 2023-10-05 , DOI: 10.1021/acs.jpcc.3c04350
Tzung-En Hsieh ₁ , Sven Maisel ₂ , Haiko Wittkämper ₂ , Johannes Frisch _{1,

3} , Julien Steffen ₂ , Regan G. Wilks _{1,

3} , Christian Papp _{2,

4} , Andreas Görling ₂ , Marcus Bär _{1,

2,

3,

5}

Affiliation

In this study, we report the electronic and chemical structure of supported GaRh alloys as model systems for the active phase in supported catalytically active liquid metal solutions (SCALMS). We prepared a series of gallium–rhodium samples with different Rh contents and tracked the evolution of the sample topography and surface electronic structure via photoemission spectroscopy in combination with ab initio calculations and electron microscopy. Our results reveal a characteristic shift of the Rh 3d core levels and narrowing and shifting of the Rh 4d derived band with decreasing Rh content. Calculations show that these spectroscopic observations can be explained by the coexistence of isolated Rh atoms in random GaRh alloys and GaRh intermetallic compounds (IMCs). These results contribute to an enhancement of the fundamental understanding of the electronic surface structure of GaRh alloys, which is crucially required for apprehending and thus further exploiting the improved catalytic activity of GaRh SCALMS.

中文翻译：

揭示 Rh 隔离对镓铑合金浅 d 态的影响

在这项研究中，我们报告了负载型 GaRh 合金的电子和化学结构，作为负载型催化活性液态金属溶液 (SCALMS) 中活性相的模型系统。我们制备了一系列不同 Rh 含量的镓铑样品，并通过光电子能谱结合从头计算和电子显微镜跟踪样品形貌和表面电子结构的演变。我们的结果揭示了随着 Rh 含量的降低，Rh 3d 核心能级的特征性变化以及 Rh 4d 衍生带的变窄和变化。计算表明，这些光谱观察结果可以通过随机 GaRh 合金和 GaRh 金属间化合物 (IMC) 中孤立的 Rh 原子的共存来解释。这些结果有助于增强对 GaRh 合金电子表面结构的基本理解，这对于理解并进一步利用 GaRh SCALMS 改进的催化活性至关重要。

更新日期：2023-10-05

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