Reactivity of oxygen radical anions bound to scandia nanoparticles in the gas phase: C-H bond activation

Chemistry : a European Journal
Li-Hua TianTong-Mei Ma

Abstract

The activation of C-H bonds in alkanes is currently a hot research topic in chemistry. The atomic oxygen radical anion (O(-·)) is an important species in C-H activation. The mechanistic details of C-H activation by O(-·) radicals can be well understood by studying the reactions between O(-·) containing transition metal oxide clusters and alkanes. Here the reactivity of scandium oxide cluster anions toward n-butane was studied by using a high-resolution time-of-flight mass spectrometer coupled with a fast flow reactor. Hydrogen atom abstraction (HAA) from n-butane by (Sc2O3)(N)O(-) (N=1-18) clusters was observed. The reactivity of (Sc2O3)(N)O(-) (N=1-18) clusters is significantly sizedependent and the highest reactivity was observed for N=4 (Sc8O13(-)) and 12 (Sc24O37(-)). Larger (Sc2O3)(N)O(-) clusters generally have higher reactivity than the smaller ones. Density functional theory calculations were performed to interpret the reactivity of (Sc2O3)(N)O(-) (N=1-5) clusters, which were found to contain the O(-·) radicals as the active sites. The local charge environment around the O(-·) radicals was demonstrated to control the experimentally observed size-dependent reactivity. This work is among the first to report HAA reactivity...Continue Reading

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Citations

Dec 13, 2016·Journal of the American Chemical Society·Mei-Qi ZhangSheng-Gui He
Sep 20, 2017·Chemistry : a European Journal·Jiao-Jiao ChenSheng-Gui He
Jun 28, 2016·Dalton Transactions : an International Journal of Inorganic Chemistry·Yan-Xia ZhaoSheng-Gui He
Apr 20, 2019·Angewandte Chemie·Yan-Xia ZhaoSheng-Gui He
Dec 31, 2015·Chemphyschem : a European Journal of Chemical Physics and Physical Chemistry·Jia-Bi MaSheng-Gui He
Jun 24, 2014·Chemphyschem : a European Journal of Chemical Physics and Physical Chemistry·Anna TroianiGiulia de Petris

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