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首页> 外文期刊>The journal of physical chemistry, A. Molecules, spectroscopy, kinetics, environment, & general theory >Coordination and Chemistry of Stable Cu(II) Complexes in the Gas Phase
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Coordination and Chemistry of Stable Cu(II) Complexes in the Gas Phase

机译：气相中稳定的Cu（II）配合物的配位与化学

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摘要

A technique has been developed that provides a solution to the very considerable technical problem of preparing gas-phase complexes from transition metals in their higher oxidation states, i.e., Cu(ll), Cr(m), Fe(ll), etc. Charge transfer prevents complexes, such as [Cuo(H_2O)n]~(2+), from being prepared via nucleation about an ion core, and yet these ions are pivotal to an understanding of transition metal chemistry .Discussed here are new results from a technique that appears capable of producing complexes from a wide variety of metals and ligands. Data are presented for copper(ll) in association with 20 different ligands. including water, ammonia, pyridine, tetrahydrofuran, and benzene. For each [Cu*oLn]~(2+) system, two important quantities are identified: (i) the minimum number of ligands required to form astable unit and (ii) the value of n for which the intensity distribution reaches a maximum. The data show considerable variation as a function of the composition and size of solvent molecule, with evidence of stable coordination shells containing between 2 and 8 molecules. In most instances, coordination shells containing more than four molecules can be attributed to the formation of an extended network of hydrogen bonds. Collisional activation of size-selected clusters reveals the presence of extensive ligand-to-metal electron transfer in the smaller complexes, and in several cases, charge transfer is also accompanied by chemical reactivity. The extent of charge transfer is frequently observed to be determined by the stability of the singly charged metal-containing product.
机译：已经开发出一种技术，该技术可以解决非常重要的技术问题，该技术问题是由处于较高氧化态的过渡金属（例如Cu（II），Cr（m），Fe（II）等）制备气相配合物。转移阻止了诸如[Cuo（H_2O）n]〜（2+）之类的络合物通过围绕离子核的成核而制备，但是这些离子对于理解过渡金属化学至关重要。似乎能够从多种金属和配体生产复合物的技术。给出了与20种不同配体相关的铜（II）数据。包括水，氨，吡啶，四氢呋喃和苯。对于每个[Cu * oLn]〜（2+）系统，确定了两个重要的数量：（i）形成稳定单元所需的最小配体数量;（ii）强度分布达到最大值的n值。数据显示，随溶剂分子的组成和大小而变化很大，有稳定的配位壳包含2至8个分子的证据。在大多数情况下，包含多于四个分子的配位壳可归因于氢键扩展网络的形成。大小选择的簇的碰撞活化揭示了在较小的络合物中存在大量的配体-金属电子转移，并且在某些情况下，电荷转移还伴随着化学反应性。经常观察到电荷转移的程度取决于单电荷含金属产物的稳定性。

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