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CeV2O7+与C2H4的气相反应:C-C键和C-H键的活化

Gas-phase reaction of CeV2O7+ with C2H4: activation of C-C and C-H bonds.

作者信息

Ma Jia-Bi, Yuan Zhen, Meng Jing-Heng, Liu Qing-Yu, He Sheng-Gui

机构信息

The Institute for Chemical Physics, Key Laboratory of Cluster Science, School of Chemistry, Beijing Institute of Technology, 100081, Beijing (P.R. China).

出版信息

Chemphyschem. 2014 Dec 15;15(18):4117-25. doi: 10.1002/cphc.201402347. Epub 2014 Sep 11.

Abstract

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 Ce(x)O(y)(±) nor V(x)O(y)(±) alone possess the necessary topological and electronic properties to bring about such a reaction.

摘要

金属氧化物团簇对烃类分子的反应活性可以通过掺杂来改变、调节或控制。通过激光烧蚀产生铈掺杂的钒团簇阳离子CeV2O7(+),用四极质量过滤器进行质量选择,然后在线性离子阱反应器中与C2H4反应。该反应由反射式飞行时间质谱仪进行表征。观察到三种类型的反应通道:1)单氧原子转移,2)双氧原子转移,3)C=C键断裂。本研究提供了第一个导致乙烯C=C键断裂的双金属氧化物团簇离子CeV2O7(+)。单独的Ce(x)O(y)(±)或V(x)O(y)(±)都不具备引发这种反应所需的拓扑和电子性质。

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