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首页> 外文期刊>The journal of physical chemistry, A. Molecules, spectroscopy, kinetics, environment, & general theory >Fragmentation pathways of [Mg(NH3)(n)](2+) complexes: Electron capture versus charge separation
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Fragmentation pathways of [Mg(NH3)(n)](2+) complexes: Electron capture versus charge separation

机译：[Mg（NH3）（n）]（2+）配合物的碎裂途径：电子捕获与电荷分离

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New experimental results are presented from a detailed study of gas-phase [Mg(NH3)(n)](2+) complexes and their fragmentation pathways. The reactions examined range from those observed as metastable (unimolecular) decompositions through to collision-induced processes, which have been accessed using a variety of collision gases. Measurements of ion intensity distributions coupled with unimolecular decay studies show that [Mg(NH3)(4)](2+) not only is the most intense species detected but also sits at a critical boundary between complexes that are unstable with respect to charge separation and those that are sufficiently solvated to be deemed stable on the time scale of the experiment. Metastable fragmentation patterns have been used to provide information on the evolution of solvent structure around the central dication. In addition to highlighting the particular significance of [Mg(NH3)(4)](2+), these measurements show some evidence to suggest the buildup of structures via a hydrogen-bonded network to give conformers of the form (4+1) and (4+2), respectively. Collision-induced dissociation studies show the ions to exhibit several fragmentation pathways, including the loss of NH3 and NH3 + H, which are promoted primarily through electron capture dissociation (ECD). This picture contrasts with the conclusion from a number of earlier studies that collisional activation mainly promotes charge separation. From the results presented it is suggested that electron capture may play a more dominant role in the charge reduction of multiply charged metal-ligand species than had previously been appreciated.
机译：气相[Mg（NH3）（n）]（2+）配合物及其裂解途径的详细研究提出了新的实验结果。所检查的反应范围从观察到的亚稳态（单分子）分解一直到碰撞引发的过程，已使用多种碰撞气体进行了反应。离子强度分布的测量以及单分子衰减研究表明，[Mg（NH3）（4）]（2+）不仅是检测到的最强物种，而且位于电荷分离不稳定的复合物之间的临界边界以及已充分溶剂化以在实验时间范围内被认为稳定的那些。亚稳碎片模式已用于提供有关中心指示剂周围溶剂结构演变的信息。这些测量结果除了突出了[Mg（NH3）（4）]（2+）的特殊意义外，还显示了一些证据，表明通过氢键网络形成结构以形成（4 + 1）形式的构象异构体和（4 + 2）。碰撞诱导的离解研究表明，离子具有几种断裂途径，包括NH3和NH3 + H的损失，这主要是通过电子俘获解离（ECD）促进的。这张图片与许多早期研究得出的结论相反，碰撞激活主要促进电荷分离。根据给出的结果，表明电子俘获在多电荷金属配体物种的电荷减少中可能比以前认识到的起更大的作用。

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