Gas-Phase Reaction of CeV2O7+ with C2H4 : Activation of C-C and C-H Bonds

被引:8
|
作者
Ma, Jia-Bi [1 ]
Yuan, Zhen [2 ]
Meng, Jing-Heng [2 ]
Liu, Qing-Yu [2 ]
He, Sheng-Gui [2 ]
机构
[1] Beijing Inst Technol, Sch Chem, Inst Chem Phys, Key Lab Cluster Sci, Beijing 100081, Peoples R China
[2] Chinese Acad Sci, Inst Chem, State Key Lab Struct Chem Unstable & Stable Speci, Beijing 100190, Peoples R China
基金
中国国家自然科学基金; 北京市自然科学基金;
关键词
cluster compounds; density functional calculations; gas-phase reactions; mass spectrometry; reaction mechanisms; OXIDE CLUSTER CATIONS; DENSITY-FUNCTIONAL THEORY; HYDROGEN-ATOM ABSTRACTION; OXYGEN-CENTERED RADICALS; METHANE ACTIVATION; PARTIAL OXIDATION; REACTION COORDINATE; VANADIA CATALYSTS; PROPENE OXIDATION; THERMAL-REACTIONS;
D O I
10.1002/cphc.201402347
中图分类号
O64 [物理化学(理论化学)、化学物理学];
学科分类号
070304 ; 081704 ;
摘要
The reactivity of metal oxide clusters toward hydrocarbon molecules can be changed, tuned, or controlled by doping. Cerium-doped vanadium cluster cations CeV2O7+ are generated by laser ablation, mass-selected by a quadrupole mass filter, and then reacted with C2H4 in a linear ion trap reactor. The reaction is characterized by a reflectron time-of-flight mass spectrometer. Three types of reaction channels are observed: 1) single oxygen-atom transfer, 2) double oxygen-atom transfer, and 3) C=C bond cleavage. This study provides the first bimetallic oxide cluster ion, CeV2O7+, which gives rise to C=C bond cleavage of ethene. Neither CexOy +/- nor VxOy +/- alone possess the necessary topological and electronic properties to bring about such a reaction.
引用
收藏
页码:4117 / 4125
页数:9
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