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化学进展 2012, Vol. 24 Issue (06): 873-878 前一篇   后一篇

• 量子化学专辑 •

Pd/ZnO催化甲醇水蒸气重整理论研究

陈兆旭*1, 黄玉成1,2, 何翔1   

  1. 1. 南京大学理论与计算化学研究所 南京 210093;
    2. 安徽师范大学化学与材料学院 芜湖 241000
  • 收稿日期:2011-12-01 修回日期:2012-04-01 出版日期:2012-06-24 发布日期:2012-05-11
  • 通讯作者: 陈兆旭 E-mail:zxchen@nju.edu.cn
  • 基金资助:

    国家自然科学基金项目(No.20973090)资助

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Theoretical Study of the Mechanism of Methanol Steam Reforming over Pd/ZnO

Chen Zhaoxu1, Huang Yucheng1,2, He Xiang1   

  1. 1. Institute of Theoretical and Computational Chemistry, Nanjing University, Nanjing 210093, China;
    2. College of Chemistry and Materials, Anhui Normal University, 241000, China
  • Received:2011-12-01 Revised:2012-04-01 Online:2012-06-24 Published:2012-05-11
随着化石能源的日渐枯竭和人们对环境保护的日益重视,发展清洁高效的新能源成为世界各国高度关注的战略课题。甲醇水蒸气重整是生产氢能的有效方法之一,Pd/ZnO催化剂热稳定性好、选择性高,是可能替代Cu/ZnO的催化剂。本文综述了近十年来采用理论方法对Pd/ZnO催化甲醇水蒸气重整制氢机理的研究工作。文章首先论述了催化剂的研究进展,然后对水在单体和聚集状态下在单层及多层平整的和阶梯状的合金表面的吸附和解离进行了总结;接着对甲醇、甲氧基和甲醛在合金表面的吸附和化学反应的热力学和动力学作了介绍;随后基于计算结果,对甲醇反应机理给予了详细的描述。最后对全文进行了总结并对未来的研究作了展望。
关键词： 甲醇水蒸气重整, Pd-Zn合金, 反应机理, 理论模拟
With the ever-increasing attention to clean energy and environmental protection, developing new energy sources becomes a heated issue all over the world. Hydrogen energy is a clean and efficient energy source, and methanol steam reforming (MSR) is an important means to produce hydrogen. In this paper we review the theoretical studies of the MSR on Pd/ZnO during the past decade. We first review the investigations on the structures and compositions of Pd/ZnO catalysts modeled by Pd-Zn alloy. Then we summarize the work of adsorption and dissociation of water on the flat and stepped surfaces of Pd-Zn alloy. Surface chemistry of methanol, methoxy and formaldehyde on Pd-Zn alloy and other pertinent surfaces is described, followed by the discussion of the MSR reaction mechanism. Finally the conclusions and outlook are presented. Contents
1 Introduction
2 Investigations on Pd/ZnO catalysts
3 Water adsorption and dissociation on alloy surfaces
3.1 Water on mono-and multi-layer Pd-Zn(111) surfaces
3.2 Water on mono-and multi-layer Pd-Zn(221) surfaces
4 The chemistry of methanol and related species
4.1 Adsorption and dissociation of methanol
4.2 Adsorption and dissociation of methoxy
4.3 Adsorption and dissociation of formaldehyde
5 Reaction mechanism of methanol steam reforming
6 Conclusions and Outlook
Key words: methanol steam reforming, Pd-Zn alloy, reaction mechanism, theoretical simulation

中图分类号: 

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