Support defect-mediated metal-support interactions in atomic layer deposition-prepared Pt/CeO2 catalysts for enhanced acetone oxidation

IF 9.6 1区化学 Q1 CHEMISTRY, APPLIED

Journal of Rare Earths Pub Date : 2026-07-01 Epub Date: 2025-07-01 DOI:10.1016/j.jre.2025.07.001

Ben Niu, Ziyi Shui, Zhenwen Yang, Xiaoxiao Duan, Weiqi An, Ganggang Li, Jie Cheng, Zhengping Hao

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Abstract

Optimizing metal-support interactions (MSI) can significantly enhance catalytic activity, as the characteristics of the support play a decisive role in governing these interactions. Herein, this study systematically investigated the properties and catalytic performance of Pt/CeO₂ catalysts prepared by atomic layer deposition (ALD) on three distinct supports: metal–organic framework (MOF)-derived CeO₂ (CeO₂-M), ceria nanorods (CeO₂-N), and ceria cubes (CeO₂-C). Comprehensive characterization reveals that CeO₂-M possesses the highest concentration of coordinatively unsaturated cerium (Ce) sites and surface oxygen vacancies, allowing for higher platinum (Pt) loading. Furthermore, the defect-rich structure of the support creates a unique coordination microenvironment for Pt species, which leads to optimized MSI as well as redox property. Therefore, Pt/CeO₂-M catalyst achieves 99% acetone conversion at 200 °C with the lowest activation energy of 57.9 kJ/mol. In situ diffuse reflectance infrared Fourier transform spectroscopy (DRIFTS) studies demonstrate that Pt/CeO₂-M follows a distinct reaction pathway during acetone oxidation due to its unique coordination structure. These findings establish MOF-derived CeO₂ as an ideal ALD support, where defect-mediated Pt anchoring can enhance both oxygen activation capacity and catalytic stability, providing new insights for the design of high-performance oxidation catalysts.

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支持缺陷介导的金属-支持相互作用在原子层沉积制备的Pt/CeO2催化剂中用于增强丙酮氧化

优化金属-载体相互作用（MSI）可以显著提高催化活性，因为载体的特性在控制这些相互作用中起决定性作用。在此，本研究系统地研究了原子层沉积（ALD）在三种不同载体上制备的Pt/CeO2催化剂的性能和催化性能：金属有机骨架（MOF）衍生的CeO2 （CeO2- m）、铈纳米棒（CeO2- n）和铈立方（CeO2- c）。综合表征表明，CeO2-M具有最高浓度的配位不饱和铈（Ce）位点和表面氧空位，允许更高的铂（Pt）负载。此外，载体的富缺陷结构为Pt物种创造了独特的配位微环境，从而优化了MSI和氧化还原性能。因此，Pt/CeO2-M催化剂在200℃下丙酮转化率达到99%，最低活化能为57.9 kJ/mol。原位漫反射红外傅里叶变换光谱（DRIFTS）研究表明，Pt/CeO2-M由于其独特的配位结构，在丙酮氧化过程中遵循不同的反应途径。这些发现证实了mof衍生的CeO2是一种理想的ALD载体，其中缺陷介导的Pt锚定可以提高氧活化能力和催化稳定性，为高性能氧化催化剂的设计提供了新的见解。

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来源期刊

Journal of Rare Earths 化学-应用化学

CiteScore

8.70

自引率

14.30%

发文量

374

审稿时长

1.7 months

期刊介绍： The Journal of Rare Earths reports studies on the 17 rare earth elements. It is a unique English-language learned journal that publishes works on various aspects of basic theory and applied science in the field of rare earths (RE). The journal accepts original high-quality original research papers and review articles with inventive content, and complete experimental data. It represents high academic standards and new progress in the RE field. Due to the advantage of abundant RE resources of China, the research on RE develops very actively, and papers on the latest progress in this field emerge every year. It is not only an important resource in which technicians publish and obtain their latest research results on RE, but also an important way of reflecting the updated progress in RE research field. The Journal of Rare Earths covers all research and application of RE rare earths including spectroscopy, luminescence and phosphors, rare earth catalysis, magnetism and magnetic materials, advanced rare earth materials, RE chemistry & hydrometallurgy, RE metallography & pyrometallurgy, RE new materials, RE solid state physics & solid state chemistry, rare earth applications, RE analysis & test, RE geology & ore dressing, etc.