Unravelling the Effect of Oxygen on the Sintering Mechanism of Pt/CeO2 in the CO Oxidation Reaction

IF 4.6 2区 化学 Q2 CHEMISTRY, PHYSICAL The Journal of Physical Chemistry Letters Pub Date : 2024-12-18 DOI:10.1021/acs.jpclett.4c02935
Lei Zhang, Yiming Niu, Yinghui Pu, Yongzhao Wang, Shaoming Dong, Zhong-Wen Liu, Bingsen Zhang
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Abstract

Sintering significantly contributes to the deactivation of supported metal catalysts under reaction conditions, influenced by various factors, including temperature, atmosphere, and metal–support interactions. The sintering mechanism under the reaction conditions remains complex and ambiguous. This study delves into the sintering behavior of platinum on CeO2 under CO oxidation conditions, mainly employing transmission electron microscopy to elucidate the effects of different gas components on the sintering mechanism at elevated temperatures. An atmosphere rich in oxygen promotes the sintering of Pt via the Ostwald ripening mechanism, characterized by the growth of larger nanoparticles at the expense of smaller ones. Conversely, sintering proceeds through particle migration and coalescence in the absence of oxygen, leading to the aggregation of nanoparticles. The obtained Pt/CeO2 catalysts exhibit enhanced catalytic performance after treatment with argon and stoichiometric reaction gases, contrasting with the deactivation observed under oxygen-rich conditions, which is attributed to varied Pt valence states. These findings provide insights into understanding the sintering mechanisms and inform the design of heterogeneous catalysts.

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揭示 CO 氧化反应中氧气对 Pt/CeO2 烧结机理的影响
在反应条件下,烧结对负载金属催化剂的失活有重要作用,受各种因素的影响,包括温度、气氛和金属-载体相互作用。反应条件下的烧结机理仍然复杂而不明确。本研究深入研究了CO氧化条件下铂在CeO2上的烧结行为,主要采用透射电镜技术阐明不同气体组分对高温烧结机理的影响。富氧气氛通过奥斯特瓦尔德成熟机制促进Pt的烧结,其特点是以牺牲较小的纳米颗粒为代价生长出较大的纳米颗粒。相反,在没有氧气的情况下,烧结通过颗粒迁移和聚并进行,导致纳米颗粒聚集。制备的Pt/CeO2催化剂经氩气和化学计量气体处理后,表现出较强的催化性能,而富氧条件下则表现出钝化,这是由于Pt价态的变化所致。这些发现为理解烧结机制提供了见解,并为多相催化剂的设计提供了信息。
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来源期刊
The Journal of Physical Chemistry Letters
The Journal of Physical Chemistry Letters CHEMISTRY, PHYSICAL-NANOSCIENCE & NANOTECHNOLOGY
CiteScore
9.60
自引率
7.00%
发文量
1519
审稿时长
1.6 months
期刊介绍: The Journal of Physical Chemistry (JPC) Letters is devoted to reporting new and original experimental and theoretical basic research of interest to physical chemists, biophysical chemists, chemical physicists, physicists, material scientists, and engineers. An important criterion for acceptance is that the paper reports a significant scientific advance and/or physical insight such that rapid publication is essential. Two issues of JPC Letters are published each month.
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