La-O小团簇上超氧物种与过氧物种间的连接途径

doi:10.1016/S1872-2067(12)60694-9

催化学报 ›› 2013, Vol. 34 ›› Issue (11): 2130-2137.DOI: 10.1016/S1872-2067(12)60694-9

La-O小团簇上超氧物种与过氧物种间的连接途径

夏文生, 张达, 翁维正, 万惠霖

厦门大学化学化工学院, 福建省理论与计算化学重点实验室, 醇醚酯清洁化工生产国家工程实验室, 固体表面物理化学国家重点实验室, 福建厦门361005

收稿日期:2013-07-04 修回日期:2013-08-26 出版日期:2013-10-18 发布日期:2013-10-18
通讯作者: Wensheng Xia,Huilin Wan
基金资助:
国家重点基础研究发展计划(973计划,2010CB732303);国家自然科学基金(21033006,21373169,20373054);长江学者和创新团队发展计划(IRT1036).

Pathways between superoxide and peroxide species on small La-O clusters

Wensheng Xia, Da Zhang, Weizheng Weng, Huilin Wan

State Key Laboratory of Physical Chemistry of Solid State Surfaces, National Engineering Laboratory for Green Chemical Productions of Alcohols-Ethers-Esters, Fujian Province Key Laboratory of Theoretical and Computational Chemistry, College of Chemistry and Chemical Engineering, Xiamen University, Xiamen 361005, Fujian, China

Received:2013-07-04 Revised:2013-08-26 Online:2013-10-18 Published:2013-10-18
Contact: Wensheng Xia,Huilin Wan
Supported by:
This work was supported by the National Basic Research Program of China (973 Program, 2010CB732303), the National Natural Science Foundation of China (21033006, 21373169, 20373054), and the Program for Changjiang Scholars and Innovative Research Team in the University (IRT1036).

摘要/Abstract

摘要：

采用密度泛函理论方法考察了La-O团簇上超氧物种与过氧物种间转化的连接途径. 单重态下, 团簇上单个超氧物种可通过一系列臭氧物种转化为过氧物种, 且转化能垒较高;三重态下, 单个超氧物种则并无与过氧物种间连接的途径. 然而, La-O团簇上两超氧物种间的相互作用及其转化也具单重态和三重态两条途径. 三重态下, 超氧物种可很容易地转化为过氧物种(O₂^- + O₂^-↔O₂²^- + O₂), 超氧物种与过氧物种处于快速的交换状态之中;单重态下, 超氧物种转化为过氧物种则需较高的活化能垒, 表明在单重态下这些氧物种具有较高的稳定性.

关键词: 氧, 超氧, 过氧, 氧化镧, 密度泛函理论

Abstract:

Density functional theory calculations were used to investigate the connection between superoxide and peroxide species on La-O clusters. In the singlet state, a superoxide species can transition into a peroxide species by moving through a substantial energy barrier via a series of ozonides. In the triplet state, there is no connection between the two species, although there are two paths (singlet and triplet) that allow the interaction and subsequent transformation of two superoxide molecules on a La-O cluster. The superoxide species readily transitions to a peroxide species through a triplet pathway (O₂^-+ O₂^-↔O₂^{2 -} + O₂), in which the superoxide species undergoes rapid exchange with the peroxide. In the singlet path, however, the superoxide species must move through a pronounced energy barrier to change into a peroxide species, demonstrating that these oxygen species are highly stable in the singlet state.

Key words: Oxygen, Superoxide, Peroxide, Lanthanide oxide, Density functional theory

夏文生, 张达, 翁维正, 万惠霖. La-O小团簇上超氧物种与过氧物种间的连接途径[J]. 催化学报, 2013, 34(11): 2130-2137.

Wensheng Xia, Da Zhang, Weizheng Weng, Huilin Wan. Pathways between superoxide and peroxide species on small La-O clusters[J]. Chinese Journal of Catalysis, 2013, 34(11): 2130-2137.

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La-O小团簇上超氧物种与过氧物种间的连接途径

Pathways between superoxide and peroxide species on small La-O clusters

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