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Capping experiments reveal multiple surface active sites in CeO2 and their cooperative catalysis

机译：封盖实验显示CEO2中的多个表面活性位点及其合作催化

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摘要

Understanding of surface active sites (SAS) of CeO2 is crucial to its catalytic applications. In the present study, we have employed capping experiments, DFT calculations, and spectroscopic characterization to study pristine CeO2 catalyst. We find that multiple SAS coexist on the CeO2 surface: oxygen vacancies as redox sites and the coordinately unsaturated Ce cations near the oxygen vacancies and the neighboring oxygen ions as Lewis acid-base sites. Dimethylsulfoxide (DMSO), pyridine, and benzoic acid are utilized to cap the redox sites, Lewis acid sites, and base sites, respectively. Selective capping on the redox site does not have much effect on the acid-base catalysis, and vice versa, indicating the distinct surface proximity and independent catalysis of these SAS. We draw attention to a relationship between the well-known redox sites and the surface Lewis acid and Lewis base pairs on CeO2 surface, which are responsible for driving various heterogeneous catalytic reactions.
机译：理解CEO2的表面活性位点（SAS）对其催化应用至关重要。 在本研究中，我们使用封盖实验，DFT计算和光谱性表征，以研究原始CeO2催化剂。 我们发现CEO2表面上的多个SAS共存：氧气空位作为氧化还原位点以及氧空位附近的坐标不饱和CE阳离子，以及作为路易斯酸碱基位的邻近氧离子。 利用二甲基磺砜（DMSO），吡啶和苯甲酸分别覆盖氧化还原位点，路易斯酸位点和基本位点。 在氧化还原遗址上的选择性封盖对酸碱催化没有太大影响，反之亦然，表明这些SAS的不同表面接近和独立催化。 我们注意在CeO 2表面上众所周知的氧化还原位点和表面路易斯酸和Lewis碱对之间的关系，这负责驱动各种异质催化反应。

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  • 来源
    《RSC Advances》 |2019年第27期|共9页
  • 作者

    Ren Xiaoning; Zhang Zhixin; Wang Yehong; Lu Jianmin; An Jinghua; Zhang Jian; Wang Min; Wang Xinkui; Luo Yi;

  • 作者单位

    Dalian Univ Technol Sch Chem State Key Lab Fine Chem Dalian 116024 Liaoning Peoples R China;

    Chinese Acad Sci Dalian Inst Chem Phys State Key Lab Catalysis Dalian Natl Lab Clean Energy Dalian 116023 Liaoning Peoples R China;

    Chinese Acad Sci Dalian Inst Chem Phys State Key Lab Catalysis Dalian Natl Lab Clean Energy Dalian 116023 Liaoning Peoples R China;

    Chinese Acad Sci Dalian Inst Chem Phys State Key Lab Catalysis Dalian Natl Lab Clean Energy Dalian 116023 Liaoning Peoples R China;

    Chinese Acad Sci Dalian Inst Chem Phys State Key Lab Catalysis Dalian Natl Lab Clean Energy Dalian 116023 Liaoning Peoples R China;

    Chinese Acad Sci Dalian Inst Chem Phys State Key Lab Catalysis Dalian Natl Lab Clean Energy Dalian 116023 Liaoning Peoples R China;

    Dalian Univ Technol Sch Chem State Key Lab Fine Chem Dalian 116024 Liaoning Peoples R China;

    Dalian Univ Technol Sch Chem State Key Lab Fine Chem Dalian 116024 Liaoning Peoples R China;

    Dalian Univ Technol Sch Chem State Key Lab Fine Chem Dalian 116024 Liaoning Peoples R China;

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  • 正文语种 eng
  • 中图分类 化学;
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