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Determining number of sites on ceria stabilizing single atoms via metal nanoparticle redispersion
Chinese Journal of Catalysis ( IF 16.5 ) Pub Date : 2020-06-01 , DOI: 10.1016/s1872-2067(19)63504-7
Aisulu Aitbekova , Cody J. Wrasman , Andrew R. Riscoe , Larissa Y. Kunz , Matteo Cargnello

Abstract Single atom catalysts have recently attracted interest due to their maximization of the utilization of expensive noble metals as well as their unique catalytic properties. Based on its surface atomic properties, CeO2 is one of the most common supports for stabilizing single metal atoms. Many single atom catalysts are limited in their metal contents by the formation of metal nanoparticles once the catalyst support capacity for single atoms has been exceeded. Currently, there are no direct measurements to determine the capacity of a support to stabilize single atoms. In this work we develop a nanoparticle-based technique that allows for quantification of that capacity by redispersing Ru nanoparticles into single atoms and taking advantage of the different catalytic properties of Ru single atoms and nanoparticles in the CO2 hydrogenation reaction. This method avoids complications in metal loading caused by counterions in incipient wetness impregnation and can eventually be applied to a variety of different metals. Results using this technique follow trends in oxygen vacancy concentration and surface oxygen content and show promise as a new method for quantifying support single atom stabilization capacity.

中文翻译:

通过金属纳米颗粒再分散确定氧化铈上稳定单原子的位点数量

摘要 单原子催化剂最近引起了人们的兴趣,因为它们最大限度地利用了昂贵的贵金属以及它们独特的催化性能。基于其表面原子特性,CeO2 是稳定单个金属原子的最常见载体之一。一旦超过单原子的催化剂承载能力,许多单原子催化剂的金属含量就会受到金属纳米颗粒的形成的限制。目前,没有直接的测量来确定载体稳定单个原子的能力。在这项工作中,我们开发了一种基于纳米颗粒的技术,该技术允许通过将 Ru 纳米颗粒重新分散成单个原子并利用 Ru 单原子和纳米颗粒在 CO2 氢化反应中的不同催化特性来量化该容量。这种方法避免了由初湿浸渍中的反离子引起的金属负载复杂化,最终可以应用于各种不同的金属。使用这种技术的结果遵循氧空位浓度和表面氧含量的趋势,并显示出作为量化支持单原子稳定能力的新方法的前景。
更新日期:2020-06-01
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