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首页> 外文期刊>The journal of physical chemistry, A. Molecules, spectroscopy, kinetics, environment, & general theory >In-plume thermodynamics of the MALDI generation of fluorofullerene anions
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In-plume thermodynamics of the MALDI generation of fluorofullerene anions

机译：氟富勒烯阴离子的MALDI生成的管内热力学

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摘要

The mechanism of formation of fluorofullerene (FF) negative ions derived from the compounds C60F18, C60F36, and (CF48)-F-60 was studied by matrix-assisted laser desorption/ionization (MALDI) time-of-flight (ToF) mass spectrometry (MS). A combined experimental/theoretical approach provides compelling evidence of nondissociative, thermodynamically controlled electron transfer from matrix-derived negative ions to the FF analyte as the main secondary-ionization process. Consistent with this thermochemical model, analyte parent molecular ion yield and degree of fragmentation for a particular MALDI experiment was found to depend on the nature of the matrix material (the five matrices investigated were sulfur, trans-2-[3-{4-tert-butylphenyl}-2-methyl-2-propenylidene]malononitrile, 9-nitroanthracene, 2,6-bis((furan-2-yl)methylene)cyclohexanone, and 2,6-bis((thiophen-2-yl)methylene)cyclohexanone). For mixtures of C60Fn compounds with different it values and therefore different electron affinitites, unwanted electron-transfer reactions, which can lead to the suppression of C60Fn- ions with low it values, were successfully blocked for the first time by judicious choice of the matrix. Therefore, reliable qualitative MS analysis of FF mixtures with wide ranges of composition is now possible.
机译：通过基质辅助激光解吸/电离（MALDI）飞行时间（ToF）质谱研究了衍生自化合物C60F18，C60F36和（CF48）-F-60的氟富勒烯（FF）负离子的形成机理（多发性硬化症）。实验/理论相结合的方法提供了令人信服的证据，证明非分解，热力学控制的电子从基质衍生的负离子转移至FF分析物是主要的二次电离过程。与该热化学模型一致，发现特定MALDI实验的分析物母体分子离子产率和碎片化程度取决于基质材料的性质（所研究的五个基质是硫，反式-2- [3- {4-叔丁基-丁基苯基} -2-甲基-2-丙烯基]丙二腈，9-硝基蒽，2,6-双（（呋喃-2-基）亚甲基）环己酮和2,6-双（（噻吩-2-基）亚甲基）环己酮）。对于具有不同it值并因此具有不同电子亲和力的C60Fn化合物的混合物，通过明智地选择基质，首次成功地阻止了有害的电子转移反应，该反应可导致抑制低it值的C60Fn离子。因此，现在可以对组成范围很广的FF混合物进行可靠的定性MS分析。

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