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个人信息Personal Information
教授
博士生导师
硕士生导师
任职 : 大连理工大学成都研究院院长
性别：男
毕业院校：中科院大连化学物理研究所
学位：博士
所在单位：化工学院
学科：化学工艺. 物理化学. 功能材料化学与化工
办公地点：大连理工大学西部校区化工综合楼A401室
联系方式：辽宁省大连市高新区凌工路2号，邮编116024
电子邮箱：changhai@dlut.edu.cn
The oxidation of methanol on hydroxylated m-ZrO2(-111): a first-principles study
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论文类型：期刊论文
发表时间：2018-02-28
发表刊物：THEORETICAL CHEMISTRY ACCOUNTS
收录刊物：SCIE
卷号：137
期号：3
ISSN号：1432-881X
关键字：Methanol; Oxidation; Zirconia; First-principles study
摘要：The oxidation of methanol (CH3OH) on hydroxylated monoclinic zirconia (H-m-ZrO2 (-111)) surface has been studied using slab periodic model and density functional theory. Both terminal-and bridging-type mechanisms were examined on the basis of two possible adsorption modes between CH3OH and hydroxyl groups (terminal and bridging) on H-m-ZrO2 (-111) surface. The calculation results show that the whole catalytic cycle can be marked by three reaction stages: the formation of CH3O via the decomposition of CH3OH (Stage I), the formation of HCOO via the oxidation of CH3O (Stage II), and the CO formation and regeneration of hydroxyl groups (Stage III). Taking potential energy surface (PES) into account, the bridging-type mechanism appeared to be the preferred one (CH3OH -> CH3O -> CH2O -> H2COO -> HCOO -> CO). The rate-determining step is identified to be the transformation of H2COO to HCOO and H2O with a barrier of 1.42 eV. The calculated results of this work should be useful in the search and design of new catalysts.