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首页> 外文期刊>The journal of physical chemistry, A. Molecules, spectroscopy, kinetics, environment, & general theory >Reactivity of hydrated monovalent first row transition metal ions M~+(H_2O)_n, M = V, Cr, Mn, Fe, Co, Ni, Cu, Zn, toward molecular oxygen, nitrous oxide, and carbon dioxide
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Reactivity of hydrated monovalent first row transition metal ions M~+(H_2O)_n, M = V, Cr, Mn, Fe, Co, Ni, Cu, Zn, toward molecular oxygen, nitrous oxide, and carbon dioxide

机译：水合一价第一行过渡金属离子M〜+（H_2O）_n，M = V，Cr，Mn，Fe，Co，Ni，Cu，Zn对分子氧，一氧化二氮和二氧化碳的反应性

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摘要

The reactions of hydrated monovalent transition metal ions M~+(H_2O)_n, M = V, Cr, Mn, Fe, Co, Ni, Cu, Zn, toward molecular oxygen, nitrous oxide, and carbon dioxide were studied by Fourier transform ion cyclotron resonance (FT-ICR) mass spectrometry. Clusters containing monovalent chromium, cobalt, nickel, or zinc were reactive toward O_2, while only hydrated cobalt was reactive toward N_2O. A strongly size dependent reactivity was observed. Chromium and cobalt react very slowly with carbon dioxide. Nanocalorimetric analysis, ~(18)O_2 exchange, and collision induced dissociation (CID) experiments were done to learn more about the structure of the O_2 products. The thermochemistry for cobalt, nickel, and zinc is comparable to the formation of O_2 ~- from hydrated electrons. These results suggest that cobalt, nickel, and zinc are forming M~(2+)/O_2 ~- ion pairs in the cluster, while chromium rather forms a covalently bound dioxygen complex in large clusters, followed by an exothermic dioxide formation in clusters with n ≤ 5. The results show that hydrated singly charged transition metal ions exhibit highly specific reactivities toward O_2, N_2O, and CO_2.
机译：利用傅立叶变换离子研究了水合一价过渡金属离子M〜+（H_2O）_n，M = V，Cr，Mn，Fe，Co，Ni，Cu，Zn对分子氧，一氧化二氮和二氧化碳的反应回旋共振（FT-ICR）质谱。含有一价铬，钴，镍或锌的簇对O_2具有反应性，而只有水合钴对N_2O具有反应性。观察到强烈的尺寸依赖性反应性。铬和钴与二氧化碳的反应非常缓慢。进行了纳米量热分析，〜（18）O_2交换和碰撞诱导解离（CID）实验，以了解有关O_2产物结构的更多信息。钴，镍和锌的热化学性质可与由水合电子形成O_2〜-相媲美。这些结果表明，钴，镍和锌在簇中形成M〜（2 +）/ O_2〜-离子对，而铬在大簇中形成共价键结合的双氧配合物，随后在簇中形成放热的二氧化物n≤5。结果表明，水合单电荷过渡金属离子对O_2，N_2O和CO_2表现出高比活度。

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