A Metastable State Facilitates Low Temperature CO Oxidation over Pt Nanoparticles

IF 16.9 1区 化学 Q1 CHEMISTRY, MULTIDISCIPLINARY Angewandte Chemie International Edition Pub Date : 2025-01-14 DOI:10.1002/anie.202423880
Samantha L. Le, Christopher R. O'Connor, Taek-Seung Kim, Christian Reece
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Abstract

The dynamic response of heterogeneous catalytic materials to their environment opens a wide variety of possible surface states which may have increased catalytic activity. In this work, we find that it is possible to generate a surface state with increased catalytic activity over metallic 2 nm Pt nanoparticles by performing a thermal treatment of the CO*-covered Pt catalyst. This state is characterised by its ability to oxidise CO to CO2 at room temperature. By combining pressure pulse experiments with in situ spectroscopy we correlate the formation of this high-activity state with the desorption of weakly bound CO* molecules from well-coordinated Pt sites. This high-activity state is metastable, degrading after elevated thermal treatments or upon readsorption of CO at room temperature. We conclude that this metastable state is highly localised to the surface of the nanoparticle, however its exact atomic structure remains open to speculation.

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亚稳态有利于铂纳米粒子上的低温CO氧化
多相催化材料对其环境的动态响应打开了各种可能的表面状态,这些表面状态可能增加了催化活性。在这项工作中,我们发现通过对CO*覆盖的Pt催化剂进行热处理,可以在金属2nm Pt纳米颗粒上产生具有更高催化活性的表面态。这种状态的特点是它能在室温下将CO氧化成CO2。通过将压力脉冲实验与原位光谱相结合,我们将这种高活性态的形成与弱结合的CO*分子从配位良好的Pt位点上的解吸联系起来。这种高活性状态是亚稳态的,在高温处理或室温下CO再吸附后降解。我们的结论是,这种亚稳态高度局限于纳米粒子的表面,但其确切的原子结构仍有待推测。
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来源期刊
CiteScore
26.60
自引率
6.60%
发文量
3549
审稿时长
1.5 months
期刊介绍: Angewandte Chemie, a journal of the German Chemical Society (GDCh), maintains a leading position among scholarly journals in general chemistry with an impressive Impact Factor of 16.6 (2022 Journal Citation Reports, Clarivate, 2023). Published weekly in a reader-friendly format, it features new articles almost every day. Established in 1887, Angewandte Chemie is a prominent chemistry journal, offering a dynamic blend of Review-type articles, Highlights, Communications, and Research Articles on a weekly basis, making it unique in the field.
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