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CeO 上单原子 Pt 在 CO 氧化反应中的记忆驱动动力学。

Memory-dictated dynamics of single-atom Pt on CeO for CO oxidation.

机构信息

Institute for Integrated Catalysis, Pacific Northwest National Laboratory, Richland, WA, 99354, USA.

The Gene and Linda Voiland School of Chemical Engineering and Bioengineering, Washington State University, Pullman, WA, 99164, USA.

出版信息

Nat Commun. 2023 May 9;14(1):2664. doi: 10.1038/s41467-023-37776-3.

DOI:10.1038/s41467-023-37776-3
PMID:37160890
原文链接:https://pmc.ncbi.nlm.nih.gov/articles/PMC10169862/
Abstract

Single atoms of platinum group metals on CeO 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 (Pt) on CeO, i.e., adsorbed Pt in Pt/CeO and square planar Pt in PtCeO, fabricated at 500 °C and by atom-trapping method at 800 °C, respectively. Adsorbed Pt in Pt/CeO 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 Pt in PtCeO 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/CeO and PtCeO in CO transforms Pt to Pt nanoparticles. However, both catalysts retain the memory of their initial Pt state after reoxidative treatments, which illustrates the importance of the initial single-atom structure in practical applications.

摘要

单原子铂族金属在 CeO 上代表了降低汽车尾气处理催化剂中贵金属需求的一种潜在方法。在这里，我们展示了两种类型的单原子 Pt（Pt）在 CeO 上的动态演变，即在 500°C 下通过原子捕获法分别制备的吸附在 Pt/CeO 上的 Pt 和四方平面 PtCeO 上的 Pt。吸附在 Pt/CeO 上的 Pt 在 CO 氧化过程中具有流动性，伴随着少量原子 Pt 簇的原位形成，这导致其具有高反应活性，CO 的反应级数接近零。相比之下，CO 氧化过程中，PtCeO 上的四方平面 Pt 与载体强烈锚定，导致其反应活性相对较低，CO 的反应级数为正。CO 中的还原将 Pt/CeO 和 PtCeO 中的 Pt 转化为 Pt 纳米颗粒。然而，在再氧化处理后，两种催化剂都保留了其初始 Pt 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。

https://cdn.ncbi.nlm.nih.gov/pmc/blobs/2da2/10169862/378005f70a52/41467_2023_37776_Fig6_HTML.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/2da2/10169862/1ba274eb1cf3/41467_2023_37776_Fig1_HTML.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/2da2/10169862/ae5b6d17d338/41467_2023_37776_Fig2_HTML.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/2da2/10169862/bfaa7e2f1e8e/41467_2023_37776_Fig3_HTML.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/2da2/10169862/49a8bbbd8453/41467_2023_37776_Fig4_HTML.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/2da2/10169862/83b651687dee/41467_2023_37776_Fig5_HTML.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/2da2/10169862/378005f70a52/41467_2023_37776_Fig6_HTML.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/2da2/10169862/1ba274eb1cf3/41467_2023_37776_Fig1_HTML.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/2da2/10169862/ae5b6d17d338/41467_2023_37776_Fig2_HTML.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/2da2/10169862/bfaa7e2f1e8e/41467_2023_37776_Fig3_HTML.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/2da2/10169862/49a8bbbd8453/41467_2023_37776_Fig4_HTML.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/2da2/10169862/83b651687dee/41467_2023_37776_Fig5_HTML.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/2da2/10169862/378005f70a52/41467_2023_37776_Fig6_HTML.jpg

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