揭示用于 CO 氧化反应的 LaFeO3 支持金催化剂的预处理诱导结构演变

IF 13.2 1区 材料科学 Q1 CHEMISTRY, MULTIDISCIPLINARY Nano Today Pub Date : 2024-06-14 DOI:10.1016/j.nantod.2024.102341
Yongjun Jiang , Lian Zou , Haiyan Zhang , Xuan Tang , Lihui Zhou , Chengcheng Tian , Sheng Dai
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引用次数: 0

摘要

异相催化剂在化学工业中起着举足轻重的作用。人们广泛利用还原或氧化气氛中的预处理来改变异相催化剂的结构,从而提高其催化性能。然而,预处理气氛有时会引发催化剂发生意想不到的结构变化,甚至导致催化降解。因此,为异质催化剂选择合适的预处理气氛至关重要,需要清楚地了解其相应的动态演化,特别是依靠原位观测,有针对性地提高其性能。本研究选择了一种很有前景的一氧化碳氧化催化剂--LaFeO3支撑的金纳米颗粒(Au/LFO),并利用原位透射电子显微镜(TEM)和密度泛函理论(DFT)计算探讨了不同气氛下的预处理对 Au/LFO 的影响。我们的研究结果表明,贵金属催化剂常用的还原预处理会在 Au/LFO 中引发强烈的金属-支撑相互作用,从而抑制其 CO 吸附性能。相比之下,氧化预处理保留了金属金和金属/支撑界面作为有效的活性位点,从而同时提高了 CO 氧化活性和稳定性。这项研究揭示了贵金属与包晶氧化物支撑物界面在不同气相处理下的结构演变,并阐明了它们之间的结构-性能关系。
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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Revealing pretreatment-induced structure evolution of LaFeO3 supported Au catalyst for CO oxidation reaction

Heterogeneous catalysts play a pivotal role in the chemical industry. Pretreatments in reducing or oxidizing atmospheres have been widely utilized to alter the structure of heterogeneous catalysts, with the aim of enhancing their catalytic performance. However, the pretreatment atmosphere can, at times, trigger unexpected structural changes in catalysts and even lead to catalytic degradation. Hence, the selection of an appropriate pretreatment atmosphere for heterogeneous catalysts is critical and requires a clear understanding of their corresponding dynamic evolution to improve their performance in a targeted manner, particularly relying on in situ observation. In this study, a promising CO oxidation catalyst, LaFeO3 supported Au nanoparticles (Au/LFO) is selected, and the influence of the pretreatments in different atmospheres on Au/LFO is explored by using in situ transmission electron microscopy (TEM) and density functional theory (DFT) calculation. Our findings reveal that the commonly used reducing pretreatment for noble-metal catalysts triggered strong metal-support interactions in Au/LFO, suppressing its CO adsorption performance. In contrast, the oxidizing pretreatment preserves the metallic Au and the metal/support interface as efficient active sites to promote CO oxidation activity and stability simultaneously. This work discloses the structure evolution at the interface between noble metals and perovskite oxide supports in response to different gas phase treatments and clarifies their structure-property relationships.

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来源期刊
Nano Today
Nano Today 工程技术-材料科学:综合
CiteScore
21.50
自引率
3.40%
发文量
305
审稿时长
40 days
期刊介绍: Nano Today is a journal dedicated to publishing influential and innovative work in the field of nanoscience and technology. It covers a wide range of subject areas including biomaterials, materials chemistry, materials science, chemistry, bioengineering, biochemistry, genetics and molecular biology, engineering, and nanotechnology. The journal considers articles that inform readers about the latest research, breakthroughs, and topical issues in these fields. It provides comprehensive coverage through a mixture of peer-reviewed articles, research news, and information on key developments. Nano Today is abstracted and indexed in Science Citation Index, Ei Compendex, Embase, Scopus, and INSPEC.
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