Reactions of Neutral Vanadium Oxide Clusters with Methanol

Feng Dong; Scott Heinbuch; Yan XieJorge J. RoccaElliot R. Bernstein

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Reactions of Neutral Vanadium Oxide Clusters with Methanol

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Reactions of neutral vanadium oxide clusters with methanol and ethanol in a fast-flow reactor are investigated by time-of-flight mass spectrometry. Single-photon ionization through soft X-ray (46.9 nm, 26.5 eV) and vacuum ultraviolet (VUV, 118 nm, 10.5 eV) lasers is employed to detect both neutral cluster distributions and reaction products. In order to distinguish isomeric products generated in the reactions V_mO_n,+ CH_3OH, partially deuterated methanol (CD_3OH) is also used as a reactant in the experiments. Association products are observed for most vanadium oxide clusters in reaction with methanol. Products VOD, V_20_3D, V_30_6D, and V_40_9D are observed for oxygen-deficient vanadium oxide clusters reacting with methanol, while oxygen-rich and the most stable clusters can extract more than one hydrogen atom (H/D) from CD_3OH to form products VO_2DH_(0,1), V_20_4DH_(0,1), V_20_5DH_(0,1), V_30_7DH_(0,1), and V_40_(10)DH_(0,1). Species V0_2(CH_3)_2, V0_3(CH_3)_2, V_20_5(CH_3)_2, V_30_7(CH_3)_2, and V_30_8(CH_3)_2 are identified as some of the main products generated from a dehydration reaction for V_mO_n + CH_3OH. A minor reaction channel that generates VOCH_2O (VOCD_2O) and VO_2CH_2O (VO_2CD_20) can also be identified. An obviously different behavior appears in the reaction V_mO_n + C_2H_5OH. The main observed products for this reaction are association products of the form V_mO_n C_2H_5OH. In order to explore the mechanism of V_mO_n + CH_3OH reactions, DFT calculations are performed to study the reaction pathways of VO_2 + CH_3OH and VO + CH_3OH reaction systems. The calculation results are in good agreement with the experimental observations.

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《The journal of physical chemistry, A. Molecules, spectroscopy, kinetics, environment, & general theory》 |2009年第13期|3029-3040|共12页
作者
Feng Dong; Scott Heinbuch; Yan XieJorge J. RoccaElliot R. Bernstein;
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作者单位

Department of Electrical and Computer Engineering, and NSF ERC for Extreme Ultraviolet Science and Technology, Colorado State University, Fort Collins, Colorado 80523;

Department of Chemistry, and NSF ERC for Extreme Ultraviolet Science and Technology, Colorado State University, Fort Collins, Colorado 80523;

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正文语种英语
中图分类 542B0006-1A;
关键词
Vanadium Oxide; Methanol; ethanol;

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Reactions of Neutral Vanadium Oxide Clusters with Methanol

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