Characterization of mononuclear oxygen-centered radical (O~-~(-?)) in Zr_2O_8~- cluster

Ma J.-B.; Wu X.-N.; Zhao Y.-X.; Ding X.-L.; He S.-G.

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Characterization of mononuclear oxygen-centered radical (O~-~(-?)) in Zr_2O_8~- cluster

机译：Zr_2O_8〜-团簇中单核氧中心自由基（O〜-〜（-？））的表征

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Zirconium oxide cluster anions Zr_xO_y~- are prepared by laser ablation and are reacted with n-butane in a fast flow reactor under near room temperature conditions. A time-of-flight mass spectrometer is used to detect the cluster distribution before and after the reactions. Observation of a hydrogen atom pickup product Zr_2O_8H ~- indicates a C-H activation reaction: Zr_2O _8~- + n-C_4H_(10) → Zr _2O_8H~- + C_4H_9. Density functional theory calculations predict that the oxygen-very-rich cluster Zr _2O_8~- contains one mononuclear oxygen-centered radical (O~(--?)), which leads to a high C-H activation reactivity, in agreement with the experiments. This study provides one example for how the highly oxidative O~(--?) radical may be generated by adsorption of O_2 onto unreactive metal oxide clusters.

机译：氧化锆团簇阴离子Zr_xO_y-是通过激光烧蚀制备的，并在快流动反应器中在接近室温的条件下与正丁烷反应。飞行时间质谱仪用于检测反应前后的簇分布。观察到氢原子拾取产物Zr_2O_8H〜-表示C-H活化反应：Zr_2O_8〜-+ n-C_4H_（10）→Zr_2O_8H〜-+ C_4H_9。密度泛函理论计算预测，氧非常富集团簇Zr _2O_8〜-包含一个单核氧中心自由基（O〜（-？）），与实验一致，导致高C-H活化反应性。这项研究提供了一个示例，说明如何通过将O_2吸附到未反应的金属氧化物簇上来生成高氧化性的O〜（-？）自由基。

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《The journal of physical chemistry, A. Molecules, spectroscopy, kinetics, environment, & general theory》 |2010年第37期|共4页
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Ma J.-B.; Wu X.-N.; Zhao Y.-X.; Ding X.-L.; He S.-G.;
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1. Characterization of mononuclear oxygen-centered radical (O~-~(-?)) in Zr_2O_8~- cluster [J] . Ma J.-B., Wu X.-N., Zhao Y.-X., The journal of physical chemistry, A. Molecules, spectroscopy, kinetics, environment, & general theory . 2010,第37期

机译：Zr_2O_8〜-团簇中单核氧中心自由基（O〜-〜（-？））的表征
2. Thermal methane activation by a binary V-Nb transition-metal oxide cluster cation: A further example for the crucial role of oxygen-centered radicals [J] . Wang Z.-C., Liu J.-W., Schlangen M., Chemistry: A European journal . 2013,第35期

机译：二元V-Nb过渡金属氧化物簇阳离子对甲烷的热活化：氧中心自由基至关重要的另一个例子
3. C–H Bond Activation by Oxygen-Centered Radicals over Atomic Clusters [J] . Xun-Lei Ding† Xiao-Nan Wu†‡ Yan-Xia Zhao† and Sheng-Gui He† Accounts of Chemical Research . 2012,第3期

机译：原子团簇上以氧为中心的自由基活化C–H键
4. Detection of Oxygen-Centered Radicals Using EPR Spin-Trap DEPMPO: The Effect of Oxygen [C] . MILO? MOJOVI?, MIRJANA VULETI?, GORAN G. BA?I? International Biophysics Symposium . 2005

机译：使用EPR Spin-Trap DEPMPO检测富含氧的自由基：氧气的效果
5. Cerium dioxide-supported gold catalysts for carbon monoxide oxidation: Synthesis, reactivity, activation, and characterization for site-isolated mononuclear species and clusters. [D] . Aguilar-Guerrero, Veronica Illeana. 2008

机译：二氧化铈负载的用于一氧化碳氧化的金催化剂：现场分离的单核物种和簇的合成，反应性，活化和表征。
6. Characterization by electron paramagnetic resonance of the role of the Escherichia coli nitrate reductase (NarGHI) iron-sulfur clusters in electron transfer to nitrate and identification of a semiquinone radical intermediate. [O] . A Magalon, R A Rothery, G Giordano, 1997

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Characterization of mononuclear oxygen-centered radical (O~-~(-?)) in Zr_2O_8~- cluster

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