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首页> 外文期刊>Journal of mass spectrometry: JMS >Correlation between the shape of the ion mobility signals and the stepwise folding process of polylactide ions
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Correlation between the shape of the ion mobility signals and the stepwise folding process of polylactide ions

机译：离子迁移率信号的形状与聚酰胺离子的逐步折叠过程之间的相关性

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摘要

In the field of polymer characterization, the use of ion mobility mass spectrometry (IMMS) remains mainly devoted to the temporal separation of cationized oligomers according to their charge states, molecular masses and macromolecular architectures in order to probe the presence of different structures. When analyzing multiply charged polymer ions by IMMS, the most striking feature is the observation of breaking points in the evolution of the average collision cross sections with the number of monomer units. Those breaking points are associated to the folding of the polymer chain around the cationizing agents. Here, we scrutinize the shape of the arrival time distribution (ATD) of polylactide ions and associate the broadening as well as the loss of symmetry of the ATD signals to the coexistence of different populations of ions attributed to the transition from opened to folded stable structures. The observation of distinct distributions reveals the absence of folded/extended structure interconversion on the ion mobility time scale (1-10 ms) and then on the lifetime of ions within the mass spectrometer at room temperature. In order to obtain information on the possible interconversion between the different observed populations upon ion activation, we performed IM-IM-MS experiments (tandem ion mobility measurements). To do so, mobility-selected ions were activated by collisions before a second mobility measurement. Interestingly, the conversion by collisional activation from a globular structure into a (partially) extended structure, i. e. the gas phase unfolding of the ions, was not observed in the energetic regime available with the used experimental setup. The absence of folded/extended interconversion, even upon collisional activation, points to the fact that the polylactide ions are ` frozen' in their specific 3D structure during the desolvation/ionization electrospray processes. Copyright (C) 2017 John Wiley & Sons, Ltd.
机译：在聚合物表征领域，离子迁移率质谱（IMMS）主要用于根据阳离子化低聚物的电荷状态、分子质量和大分子结构对其进行时间分离，以探测不同结构的存在。在用IMMS分析多电荷聚合物离子时，最显著的特点是观察到平均碰撞截面随单体单元数的变化过程中的破裂点。这些断裂点与阳离子化剂周围聚合物链的折叠有关。在这里，我们研究了聚乳酸离子到达时间分布（ATD）的形状，并将ATD信号的展宽和对称性的丧失与不同离子群的共存联系起来，这归因于从开放结构到折叠稳定结构的过渡。对不同分布的观察表明，在离子迁移率时间尺度（1-10 ms）上，以及在室温下质谱仪内离子的寿命上，没有折叠/扩展结构相互转换。为了获得离子活化后不同观察群体之间可能相互转换的信息，我们进行了IM-IM-MS实验（串联离子迁移率测量）。为此，在第二次迁移率测量之前，通过碰撞激活迁移率选择离子。有趣的是，在所用实验装置可用的高能区中，没有观察到通过碰撞活化从球状结构转化为（部分）扩展结构，即离子的气相展开。即使在碰撞活化时，也没有折叠/延伸的相互转化，这表明聚乳酸离子在去溶剂/电离电喷雾过程中在其特定的3D结构中“冻结”。版权所有（C）2017约翰威利父子有限公司。

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  • 来源
    《Journal of mass spectrometry: JMS》 |2017年第3期|共6页
  • 作者

    Duez Q.; Josse T.; Lemaur V.; Chirot F.; Choi C. M.; Dubois P.; Dugourd P.; Cornil J.; Gerbaux P.; De Winter J.;

  • 作者单位

    Univ Mons Organ Synth &

    Mass Spectrometry Lab Interdisciplinary Ctr Mass Spectrometry CISMa 23 Pl Parc B-7000 Mons Belgium;

    Univ Mons Organ Synth &

    Mass Spectrometry Lab Interdisciplinary Ctr Mass Spectrometry CISMa 23 Pl Parc B-7000 Mons Belgium;

    Univ Mons CIRMAP Lab Chem Novel Mat 23 Pl Parc B-7000 Mons Belgium;

    Univ Claude Bernard Lyon 1 Ens Lyon CNRS Inst Sci Analyt UMR 5280 5 Rue Doua F-69100 Villeurbanne France;

    Univ Claude Bernard Lyon 1 CNRS Inst Lumiere Matiere F-69622 Lyon France;

    Univ Mons CIRMAP Lab Polymer &

    Composite Mat 23 Pl Parc B-7000 Mons Belgium;

    Univ Claude Bernard Lyon 1 CNRS Inst Lumiere Matiere F-69622 Lyon France;

    Univ Mons CIRMAP Lab Chem Novel Mat 23 Pl Parc B-7000 Mons Belgium;

    Univ Mons Organ Synth &

    Mass Spectrometry Lab Interdisciplinary Ctr Mass Spectrometry CISMa 23 Pl Parc B-7000 Mons Belgium;

    Univ Mons Organ Synth &

    Mass Spectrometry Lab Interdisciplinary Ctr Mass Spectrometry CISMa 23 Pl Parc B-7000 Mons Belgium;

  • 收录信息
  • 原文格式 PDF
  • 正文语种 eng
  • 中图分类 分析化学;
  • 关键词

    ion mobility; mass spectrometry; polymers; arrival time distribution; ATD; tandem ion mobility; IM-IM-MS;

    机译：None;

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