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气氛环境下Au/CeO2催化剂烧结行为的原位电镜研究

In-situ TEM study of gas-dependent sintering behavior of Au/CeO2

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【作者】 陈炳伟吴哲敏韩仲康袁文涛姜颖杨杭生王勇张泽

【Author】 CHEN Bingwei;WU Zhemin;HAN Zhongkang;YUAN Wentao;JIANG Ying;YANG Hangsheng;WANG Yong;ZHANG Ze;Center of Electron Microscopy, State Key Laboratory of Silicon Materials, and Department of Materials Science and Engineering;

【通讯作者】 吴哲敏;姜颖;

【机构】 浙江大学电子显微镜中心,硅材料国家重点实验室,材料科学与工程学院

【摘要】 气氛环境下原位研究催化剂的烧结行为,能够为理解催化剂在预处理以及反应条件下的烧结机理和高稳定催化剂的设计提供重要的实验依据。本文以Au/CeO2模型纳米催化剂为研究对象,利用环境透射电子显微镜原位观察其在O2与CO气氛下的高温动态烧结过程。实验发现,负载在CeO2上的Au纳米颗粒在O2与CO气氛环境中表现出不同的烧结行为,其在O2气氛下具有较高的烧结速度,同时存在颗粒迁移与聚集长大(particle migration and coalescence, PMC)和奥斯特瓦尔德熟化(Ostwald ripening, OR)两种烧结过程;在CO气氛下烧结速度较慢,烧结过程以OR为主。对比不同气氛环境下烧结后催化剂的表面结构可知,CO增加了CeO2表面台阶的数量以及表面氧空位浓度,增强了载体对Au颗粒的锚定作用,从而提升Au/CeO2催化剂的稳定性。

【Abstract】 In-situ investigation of catalyst sintering behavior under atmospheric conditions provides the crucial experimental evidence for understanding the sintering mechanism of catalysts during pretreatments and reactions, and for designing highly stable catalysts. In this study, a model nanocatalyst system composed of Au/CeO2 was employed to examine the high-temperature dynamic sintering process using an environmental transmission electron microscopy(ETEM). It was observed that the Au nanoparticles supported on CeO2 exhibited distinct sintering behaviors in O2 and CO atmospheres. In the O2 atmosphere, the sintering rate was significantly accelerated by the presence of both particle migration and coalescence(PMC) and Ostwald ripening(OR) processes. In contrast, in the CO atmosphere, the sintering rate was slow and predominantly governed by the OR process. The comparative analysis of the surface structures of sintered catalysts under different atmospheres revealed that the CO gas increased the number of surface steps and the concentration of surface oxygen vacancies in CeO2, thereby enhancing the anchoring effect of the support on Au particles, and improving the stability of the Au/CeO2 catalyst.

【基金】 国家自然科学基金资助项目(No.51971202,No.52025011,No.92045301,No.52171019);国家重点研发计划青年科学家项目(No.2022YFA1505500);浙江省重点研发计划(No.2021C01003);浙江省自然科学基金(No.LR23B030004,No.LD19B030001);山西-浙大先进材料与化学工程研究所;中央高校基本科研业务费基金
  • 【文献出处】 电子显微学报 ,Journal of Chinese Electron Microscopy Society , 编辑部邮箱 ,2024年01期
  • 【分类号】TQ426
  • 【下载频次】36
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