红外反射-吸收光谱 (IRRAS) 应用于氧化物:以铈为例

IF 2.1 4区 化学 Q3 CHEMISTRY, PHYSICAL Surface Science Pub Date : 2024-07-14 DOI:10.1016/j.susc.2024.122550
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引用次数: 0

摘要

红外反射-吸收光谱(IRRAS)是研究金属表面化学的重要工具,最近在氧化物表面的研究中也获得了很大的影响,尽管其介电性能带来了固有的挑战。本综述重点介绍 IRRAS 在铈(CeO2)上的应用,铈是一种金属氧化物,已有大量相关实验数据。我们详细阐述了金属和金属氧化物在光学性质上的差异,这种差异导致吸附振动带的强度降低了约两个数量级,振动频率的偏振偏移也随之改变。我们研究了支配金属上吸附剂红外光谱的表面选择规则如何与电介质的行为形成鲜明对比,电介质的正负振带都可能出现,以及 IRRAS 如何捕捉过渡偶极矩平行于表面的振动--这种能力在金属表面上是不可行的。最后,本文探讨了这些发现的广泛意义,以加深我们对氧化物表面分子相互作用的理解,并在技术相关条件下利用红外光谱进行操作研究。
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Infrared Reflection-Absorption Spectroscopy (IRRAS) applied to oxides: Ceria as a case study

Infrared Reflection-Absorption Spectroscopy (IRRAS), a pivotal tool in the study of the surface chemistry of metals, has recently also gained substantial impact for oxide surfaces, despite the inherent challenges originating from their dielectric properties. This review focuses on the application of IRRAS to ceria (CeO2), a metal oxide for which a significant amount of experimental data exists. We elaborate on the differences in optical properties between metals and metal oxides, which result in lower intensity of adsorbate vibrational bands by approximately two orders of magnitude and polarization-dependent shifts of vibrational frequencies. We examine how the surface selection rule, governing IR spectroscopy of adsorbates on metals, contrasts sharply with the behavior of dielectrics where both positive and negative vibrational bands can occur, and how IRRAS can capture vibrations with transition dipole moments oriented parallel to the surface—a capability not feasible on metallic surfaces. Finally, this paper explores the broader implications of these findings for enhancing our understanding of molecule interactions on oxide surfaces, and for using IR spectroscopy for operando studies under technologically relevant conditions.

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来源期刊
Surface Science
Surface Science 化学-物理:凝聚态物理
CiteScore
3.30
自引率
5.30%
发文量
137
审稿时长
25 days
期刊介绍: Surface Science is devoted to elucidating the fundamental aspects of chemistry and physics occurring at a wide range of surfaces and interfaces and to disseminating this knowledge fast. The journal welcomes a broad spectrum of topics, including but not limited to: • model systems (e.g. in Ultra High Vacuum) under well-controlled reactive conditions • nanoscale science and engineering, including manipulation of matter at the atomic/molecular scale and assembly phenomena • reactivity of surfaces as related to various applied areas including heterogeneous catalysis, chemistry at electrified interfaces, and semiconductors functionalization • phenomena at interfaces relevant to energy storage and conversion, and fuels production and utilization • surface reactivity for environmental protection and pollution remediation • interactions at surfaces of soft matter, including polymers and biomaterials. Both experimental and theoretical work, including modeling, is within the scope of the journal. Work published in Surface Science reaches a wide readership, from chemistry and physics to biology and materials science and engineering, providing an excellent forum for cross-fertilization of ideas and broad dissemination of scientific discoveries.
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