Pt Nanoparticle Disintegration at Oxide Interfaces Enhances CO Oxidation Catalysis.

IF 12.1 2区材料科学 Q1 CHEMISTRY, MULTIDISCIPLINARY

Small Pub Date : 2025-10-19 DOI:10.1002/smll.202506990

Eunji Kang,Jieun Yun,Hyuk Choi,Mi Yoo,Ju Hyeok Lee,Hongjin Park,Jin-Seok Choi,Kug-Seung Lee,David A Shapiro,Alex Ditter,Bob Jin Kwon,Chunjoong Kim,Young-Sang Yu,Hyun You Kim

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Abstract

Understanding how supported metal nanoparticles dynamically evolve under reaction conditions is critical for controlling their catalytic function. Here, the mechanism behind the dynamic disintegration of Pt nanoparticles (NPs) supported on CeOx-TiO2 (CT) during CO oxidation is elucidated, leading to the formation of single atoms (SAs) and/or sub-nanometer clusters. Density functional theory (DFT) calculations reveal that strong Pt-CO interactions weaken Pt─Pt cohesion, while electronic coupling between Pt and Ce ions stabilizes Pt-CO* intermediates at the oxide interface. Surface oxygen vacancies kinetically trap Pt-CO*, but the vacancies are replenished under oxygen-rich conditions, enabling Pt-CO* surface diffusion and subsequent structural reorganization. In situ spectroscopic analyses confirm the oxygen-driven transformation of Pt NPs, correlating with a threefold increase in mass-specific activity at 150 °C. These findings demonstrate that interfacial oxygen dynamics and metal-support interactions can be leveraged to induce nanoparticle disintegration and optimize catalytic performance, highlighting the catalytic potential of interface-engineered Pt nanostructures.

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铂纳米颗粒在氧化物界面上的分解增强了CO氧化催化作用。

了解负载型金属纳米颗粒在反应条件下如何动态演化是控制其催化功能的关键。本文阐明了CO氧化过程中ceoxo - tio2 （CT）负载的Pt纳米颗粒（NPs）的动态分解机制，从而导致单原子（SAs）和/或亚纳米簇的形成。密度泛函理论（DFT）计算表明，强的Pt- co相互作用削弱了Pt─Pt的内聚力，而Pt和Ce离子之间的电子耦合在氧化物界面稳定了Pt- co *中间体。表面氧空位动态捕获Pt-CO*，但空位在富氧条件下得到补充，使Pt-CO*表面扩散和随后的结构重组成为可能。原位光谱分析证实了Pt NPs的氧驱动转化，在150°C时，其质量比活性增加了三倍。这些发现表明，界面氧动力学和金属-载体相互作用可以诱导纳米颗粒分解并优化催化性能，突出了界面工程Pt纳米结构的催化潜力。

本文章由计算机程序翻译，如有差异，请以英文原文为准。

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来源期刊

Small 工程技术-材料科学：综合

CiteScore

17.70

自引率

3.80%

发文量

1830

审稿时长

2.1 months

期刊介绍： Small serves as an exceptional platform for both experimental and theoretical studies in fundamental and applied interdisciplinary research at the nano- and microscale. The journal offers a compelling mix of peer-reviewed Research Articles, Reviews, Perspectives, and Comments. With a remarkable 2022 Journal Impact Factor of 13.3 (Journal Citation Reports from Clarivate Analytics, 2023), Small remains among the top multidisciplinary journals, covering a wide range of topics at the interface of materials science, chemistry, physics, engineering, medicine, and biology. Small's readership includes biochemists, biologists, biomedical scientists, chemists, engineers, information technologists, materials scientists, physicists, and theoreticians alike.