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首页> 外文期刊>The journal of physical chemistry, A. Molecules, spectroscopy, kinetics, environment, & general theory >Reactions of Vanadium Oxide Cluster Ions with 1,3-Butadiene and Isomers of Butene
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Reactions of Vanadium Oxide Cluster Ions with 1,3-Butadiene and Isomers of Butene

机译：钒氧化物簇离子与1,3-丁二烯和丁烯异构体的反应

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摘要

The gas-phase reactions of vanadium oxide cluster ions with 1,3-butadiene and the isomers of butene are examined. The correlation between the reaction products and the cluster stoichiometry, oxidation and charge-state are explored by studying the reactivity of 1,3-butadiene (C_4H_6) and the deuterated 1,3-butadienes C_4D_6 and 1,1,4,4-C_4D_4H_2 with the clusters cations V_3O_6~+, V_3O_7~, and V_3O_8~+ and the anions VO_(2,3)~-, V_2O_(4-6)~-, V_3O_(6-9)~- and V_4O_(10,11)~-. These studies further our understanding of the reactions of V_xO_y~+ clusters with hydrocarbons, as reported previously [Bell, R. C.; Zemski, K. A.; Kerns, K. P.; Deng, H.T.; Castleman, Jr., A. W. J. Phys. Chem. A 1998M 102M 1733], by examining the reaction of the anions (V_xO_y~-), deuterated butadiene species and the 2-butenes. The reactions of C_4D_6 and 1,1,4,4-C_4D_4H_2 with the cluster V_3O_7~+ demonstrate pathways for the loss of a single oxygen, oxidative dehydrogenation, and molecular association, as well as other minor products, analogous to the products previously reported for the reactions of these clusters with C_4H_6. The reactions of V_3O_7~+ with the isomers of butene (1-butene, cis-2-butene and trans-2-butene) display many of the same reaction pathways that the observed for 1,3-butadiene, namely, oxidation of the hydrocarbion, oxidative dehydrogenation, and molecular association. In addition, a major channel representing the dehydrogenation of the alkene and a minor channel for C2-C3 cracking of the alkene, along with other minor products is also observed. The anionic clusters VO_(2,3)~-, V_2O_(4,5)~-, V_3O_(6-8)~-, and V_4O_(10)~- do not react with either 1,3-butadiene or 1-butene, whereas clusters of higher oxygen content, V_2O_6~-, V_3O_9~-, and V_4O_(11)~- display a minor reaction channel for the loss of a single oxygen atom, presumably through oxidation of the hydrocarbon and resulting in the cluster V_xO_(y-1)~-.
机译：研究了钒氧化物簇离子与1,3-丁二烯和丁烯异构体的气相反应。通过研究1,3-丁二烯（C_4H_6）与氘代1,3-丁二烯C_4D_6和1,1,4,4-C_4D_4H_2的反应性，探索了反应产物与簇化学计量，氧化和电荷态之间的关系。具有簇阳离子V_3O_6〜+，V_3O_7〜和V_3O_8〜+以及阴离子VO_（2,3）〜-，V_2O_（4-6）〜-，V_3O_（6-9）〜-和V_4O_（10,11 ）〜-。这些研究进一步加深了我们对V_xO_y +簇与烃的反应的理解，如先前报道的[Bell，R.C。 Zemski，K. A .; Kerns，K.P .;邓洪涛; J.Castleman，A.W.J. Phys。化学1998M 102M 1733]，通过检查阴离子（V_xO_y〜-），氘化丁二烯种类和2-丁烯的反应。 C_4D_6和1,1,4,4-C_4D_4H_2与簇V_3O_7〜+的反应证明了单个氧的损失，氧化脱氢和分子缔合的途径以及其他次要产物，类似于先前报道的产物这些簇与C_4H_6的反应。 V_3O_7〜+与丁烯的异构体（1-丁烯，顺式-2-丁烯和反式-2-丁烯）的反应显示出与1,3-丁二烯所观察到的许多相同的反应路径，即碳氢化合物，氧化脱氢和分子缔合。另外，还观察到代表烯烃脱氢的主通道和用于烯烃的C 2 -C 3裂解的次要通道，以及其他次要产物。阴离子簇VO_（2,3）〜-，V_2O_（4,5）〜-，V_3O_（6-8）〜-和V_4O_（10）〜-不会与1,3-丁二烯或1-丁烯，而较高氧含量的簇V_2O_6〜-，V_3O_9〜-和V_4O_（11）〜-显示出一个较小的反应通道，可以损失单个氧原子，大概是通过碳氢化合物的氧化，从而导致了簇V_xO_ （y-1）〜-。

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