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氧等离子体功能化CeO表面上高度稳定且具反应活性的铂单原子:纳米结构与过氧效应

Highly Stable and Reactive Platinum Single Atoms on Oxygen Plasma-Functionalized CeO Surfaces: Nanostructuring and Peroxo Effects.

作者信息

Wan Weiming, Geiger Julian, Berdunov Nikolay, Lopez Luna Mauricio, Chee See Wee, Daelman Nathan, López Núria, Shaikhutdinov Shamil, Roldan Cuenya Beatriz

机构信息

Department of Interface Science, Fritz Haber Institute, Faradayweg 4-6, 14195, Berlin, Germany.

Institute of Chemical Research of Catalonia, The Barcelona Institute of Science and Technology Institution, 43007, Tarragona, Spain.

出版信息

Angew Chem Int Ed Engl. 2022 May 9;61(20):e202112640. doi: 10.1002/anie.202112640. Epub 2022 Mar 16.

Abstract

Atomically dispersed precious metals on oxide supports have recently become increasingly interesting catalytic materials. Nonetheless, their non-trivial preparation and limited thermal and environmental stability constitutes an issue for their potential applications. Here we demonstrate that an oxygen plasma pre-treatment of the ceria (CeO ) surface serves to anchor Pt single atoms, making them active and resistant towards sintering in the CO oxidation reaction. Through a combination of experimental results obtained on well-defined CeO films and theory, we show that the O plasma causes surface nanostructuring and the formation of surface peroxo (O ) species, favoring the uniform and dense distribution of isolated strongly bonded Pt atoms. The promotional effect of the plasma treatment was further demonstrated on powder Pt/CeO catalysts. We believe that plasma functionalization can be applied to other metal/oxide systems to achieve tunable and stable catalysts with a high density of active sites.

摘要

近年来,负载于氧化物载体上的原子级分散贵金属成为了愈发引人关注的催化材料。尽管如此,其复杂的制备过程以及有限的热稳定性和环境稳定性对它们的潜在应用构成了一个问题。在此,我们证明对二氧化铈(CeO₂)表面进行氧等离子体预处理有助于锚定铂单原子,使其在CO氧化反应中具有活性且抗烧结。通过结合在明确的CeO₂薄膜上获得的实验结果和理论,我们表明氧等离子体导致表面纳米结构化并形成表面过氧(O₂²⁻)物种,有利于孤立的强键合铂原子均匀且密集地分布。等离子体处理的促进作用在粉末状Pt/CeO₂催化剂上也得到了进一步证明。我们相信等离子体功能化可应用于其他金属/氧化物体系,以获得具有高密度活性位点的可调谐且稳定的催化剂。

https://cdn.ncbi.nlm.nih.gov/pmc/blobs/2e35/9315031/9a5f39006584/ANIE-61-0-g005.jpg

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