Pd/ZnO催化甲醇水蒸气重整理论研究

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

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。

With the ever-increasing attention to clean energy and environmental protection,developing new energy sources becomes a strategic 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.