Mechanistic Insights Gained by High Spatial Resolution Reactivity Mapping of Homogeneous and Heterogeneous (Electro)Catalysts,Chemical Reviews

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Mechanistic Insights Gained by High Spatial Resolution Reactivity Mapping of Homogeneous and Heterogeneous (Electro)Catalysts
Chemical Reviews ( IF 51.4 ) Pub Date : 2023-04-10 , DOI: 10.1021/acs.chemrev.2c00867
Shahar Dery ₁ , Barak Friedman ₁ , Hadar Shema ₁ , Elad Gross ₁

Affiliation

The recent development of high spatial resolution microscopy and spectroscopy tools enabled reactivity analysis of homogeneous and heterogeneous (electro)catalysts at previously unattainable resolution and sensitivity. These techniques revealed that catalytic entities are more heterogeneous than expected and local variations in reaction mechanism due to divergences in the nature of active sites, such as their atomic properties, distribution, and accessibility, occur both in homogeneous and heterogeneous (electro)catalysts. In this review, we highlight recent insights in catalysis research that were attained by conducting high spatial resolution studies. The discussed case studies range from reactivity detection of single particles or single molecular catalysts, inter- and intraparticle communication analysis, and probing the influence of catalysts distribution and accessibility on the resulting reactivity. It is demonstrated that multiparticle and multisite reactivity analyses provide unique knowledge about reaction mechanism that could not have been attained by conducting ensemble-based, averaging, spectroscopy measurements. It is highlighted that the integration of spectroscopy and microscopy measurements under realistic reaction conditions will be essential to bridge the gap between model-system studies and real-world high spatial resolution reactivity analysis.

中文翻译：

通过均相和非均相（电）催化剂的高空间分辨率反应性映射获得的机理见解

高空间分辨率显微镜和光谱工具的最新发展使得能够以以前无法达到的分辨率和灵敏度对均相和异相（电）催化剂进行反应性分析。这些技术表明，催化实体比预期的更加异质，并且由于活性位点性质的差异，例如它们的原子性质、分布和可及性，反应机制的局部变化发生在均相和异质（电）催化剂中。在这篇综述中，我们重点介绍了通过进行高空间分辨率研究获得的催化研究的最新见解。讨论的案例研究包括单粒子或单分子催化剂的反应性检测、粒子间和粒子内通讯分析、并探讨催化剂分布和可及性对所得反应性的影响。事实证明，多粒子和多位点反应性分析提供了有关反应机制的独特知识，而这些知识无法通过进行基于集合的平均光谱测量来获得。需要强调的是，在实际反应条件下整合光谱学和显微镜测量对于弥合模型系统研究与现实世界高空间分辨率反应性分析之间的差距至关重要。

更新日期：2023-04-10

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