物理化学学报 >> 2017, Vol. 33 >> Issue (12): 2424-2437.doi: 10.3866/PKU.WHXB201707171

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催化剂活性位本质和构效关系的模型催化研究

陈明树*()   

  • 收稿日期:2017-06-17 发布日期:2017-09-05
  • 通讯作者: 陈明树 E-mail:chenms@xmu.edu.cn
  • 作者简介:陈明树,厦门大学化学化工学院教授。1969年5月出生于福建省。1991年成都科技大学(现四川大学)本科毕业,1994年厦门大学化学系硕士毕业,1997年厦门大学化学系催化专业博士毕业,毕业后留校工作。1999–2002年到日本九州大学进修表面科学专业获工学博士学位。2002–2007年美国德州农工大学化学系博士后/Research Scientist。2007年厦门大学特聘教授。主要开展多相催化、表面化学以及模型催化研究,发展高灵敏度的原位动态催化表征技术,以期明确有关重要催化反应的催化剂作用机理和催化反应机理
  • 基金资助:
    973重大研究计划(2013CB933102);国家自然科学基金(21273178);国家自然科学基金(21573180);国家自然科学基金(91545204)

Toward Understanding the Nature of the Active Sites and Structure-Activity Relationships of Heterogeneous Catalysts by Model Catalysis Studies

Mingshu CHEN*()   

  • Received:2017-06-17 Published:2017-09-05
  • Contact: Mingshu CHEN E-mail:chenms@xmu.edu.cn
  • Supported by:
    the National Basic Research Program of China(2013CB933102);National Natural Science Foundation of China(21273178);National Natural Science Foundation of China(21573180);National Natural Science Foundation of China(91545204)

摘要:

明确催化剂的活性位本质和构建多相催化的结构和反应性能之间的准确关系是催化基础研究的重点,表面科学研究基于丰富的表征测试手段能够较好地在分子原子水平测定表面结构以明确催化剂活性位本质,并通过高压原位反应池测定相关催化反应性能,获得较可靠的催化剂构效关系。本文简要总结了近年来本人参与的几个模型催化研究例子,包括贵金属表面上CO和烷烃催化氧化的活性表面、纳米Au膜的制备和CO氧化的催化活性位、VOx/Pt(111)上丙烷氧化的协同作用、AuPd合金上醋酸乙烯酯合成Au的助催化作用、模型氧化物上纳米Pt的庚烷脱氢环化制甲苯的粒径关系等,以及相关模型催化研究技术的进展。

关键词: 模型催化, 构效关系, CO氧化, 烷烃临氧转化, 原位谱学

Abstract:

Understanding the nature of the active sites and the relationship between the catalyst structure and its performance are fundamental aspects of heterogeneous catalysis. With the development of modern surface science techniques, atomically resolved surface structures of heterogeneous catalysts and their properties can be studied with ease. Combined with an in situ high pressure cell, model catalysis studies can provide convincing information about the relationship between the catalyst structure and its performance. In this mini-review, several case studies of model catalysts have been summarized, including those of the active surfaces for CO and alkane oxidation using the Pt group metals as catalysts, the active site of gold nanoparticles for CO oxidation, synergistic effects between VOx and Pt for propane oxidation, promotional effects of Au in Pd-Au catalysts for vinyl acetate synthesis, structure-sensitivity of n-heptane dehydrocyclization on model oxide-supported Pt, as well as several significant improvements of the model catalysis techniques.

Key words: Model catalysis study, Structure-activity, CO oxidation, Alkanes oxidation, In situ spectroscopy