Operando XAS/SAXS: Guiding Design of Single‐Atom and Subnanocluster Catalysts,Small Methods

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Operando XAS/SAXS: Guiding Design of Single‐Atom and Subnanocluster Catalysts
Small Methods ( IF 10.7 ) Pub Date : 2021-02-12 , DOI: 10.1002/smtd.202001194
Lingzhe Fang ₁ , Soenke Seifert ₂ , Randall E Winans ₂ , Tao Li _{1,

2}

Affiliation

Single‐atom and subnanocluster catalysts (SSCs) represent a highly promising class of low‐cost materials with high catalytic activity and high atom‐utilization efficiency. However, SSCs are susceptible to undergo restructuring during the reactions. Exploring the active sites of catalysts through in situ characterization techniques plays a critical role in studying reaction mechanism and guiding the design of optimum catalysts. In situ X‐ray absorption spectroscopy/small‐angle X‐ray scattering (XAS/SAXS) is promising and widely used for monitoring electronic structure, atomic configuration, and size changes of SSCs during real‐time working conditions. Unfortunately, there is no detailed summary of XAS/SAXS characterization results of SSCs. The recent advances in applying in situ XAS/SAXS to SSCs are thoroughly summarized in this review, including the atomic structure and oxidation state variations under open circuit and realistic reaction conditions. Furthermore, the reversible transformation of single‐atom catalysts (SACs) to subnanoclusters/nanoparticles and the application of in situ XAS/SAXS in subnanoclusters are discussed. Finally, the outlooks in modulating the SSCs and developing operando XAS/SAXS for SSCs are highlighted.

中文翻译：

Operando XAS/SAXS：单原子和亚纳米簇催化剂的指导设计

单原子和亚纳米簇催化剂（SSCs）代表了一类极具前景的低成本材料，具有高催化活性和高原子利用效率。然而，SSCs 在反应过程中容易发生重组。通过原位表征技术探索催化剂的活性位点对于研究反应机理和指导优化催化剂的设计起着至关重要的作用。原位 X 射线吸收光谱/小角 X 射线散射 (XAS/SAXS) 具有前景并广泛用于监测 SSC 在实时工作条件下的电子结构、原子构型和尺寸变化。不幸的是，没有关于 SSC 的 XAS/SAXS 表征结果的详细总结。本综述全面总结了将原位 XAS/SAXS 应用于 SSC 的最新进展，包括开路和实际反应条件下的原子结构和氧化态变化。此外，还讨论了单原子催化剂（SAC）向亚纳米团簇/纳米粒子的可逆转化以及原位 XAS/SAXS 在亚纳米团簇中的应用。最后，强调了调制 SSC 和开发 SSC 的操作 XAS/SAXS 的前景。

更新日期：2021-02-12

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