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Memory-dictated dynamics of single-atom Pt on CeO2 for CO oxidation
Nature Communications ( IF 14.7 ) Pub Date : 2023-05-09 , DOI: 10.1038/s41467-023-37776-3
Zihao Zhang 1, 2 , Jinshu Tian 1 , Yubing Lu 1 , Shize Yang 3 , Dong Jiang 2 , Weixin Huang 2 , Yixiao Li 2 , Jiyun Hong 4 , Adam S Hoffman 4 , Simon R Bare 4 , Mark H Engelhard 1 , Abhaya K Datye 5 , Yong Wang 1, 2
Affiliation  

Single atoms of platinum group metals on CeO2 represent a potential approach to lower precious metal requirements for automobile exhaust treatment catalysts. Here we show the dynamic evolution of two types of single-atom Pt (Pt1) on CeO2, i.e., adsorbed Pt1 in Pt/CeO2 and square planar Pt1 in PtATCeO2, fabricated at 500 °C and by atom-trapping method at 800 °C, respectively. Adsorbed Pt1 in Pt/CeO2 is mobile with the in situ formation of few-atom Pt clusters during CO oxidation, contributing to high reactivity with near-zero reaction order in CO. In contrast, square planar Pt1 in PtATCeO2 is strongly anchored to the support during CO oxidation leading to relatively low reactivity with a positive reaction order in CO. Reduction of both Pt/CeO2 and PtATCeO2 in CO transforms Pt1 to Pt nanoparticles. However, both catalysts retain the memory of their initial Pt1 state after reoxidative treatments, which illustrates the importance of the initial single-atom structure in practical applications.



中文翻译:

CeO2 上单原子 Pt 的记忆控制动力学用于 CO 氧化

CeO 2上的铂族金属单原子代表了一种降低汽车尾气处理催化剂对贵金属要求的潜在方法。在这里,我们展示了两种类型的单原子 Pt (Pt 1 ) 在 CeO 2上的动态演化,即Pt/CeO 2中的吸附 Pt 1和Pt AT CeO 2中的方形平面 Pt 1,在 500 °C 和通过分别为 800 °C 的原子捕获方法。Pt/CeO 2中吸附的 Pt 1在 CO 氧化过程中随着原位形成少原子 Pt 簇而移动,有助于在 CO 中具有接近零反应级数的高反应性。相比之下,方形平面 PtPt AT CeO 2中的1在 CO 氧化过程中牢固地锚定在载体上,导致在 CO 中具有正反应级的相对较低的反应性。CO 中 Pt/CeO 2和 Pt AT CeO 2的还原将 Pt 1转化为 Pt 纳米颗粒。然而,这两种催化剂在再氧化处理后都保留了其初始 Pt 1状态的记忆,这说明了初始单原子结构在实际应用中的重要性。

更新日期:2023-05-09
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