New mass spectrometry concepts for characterization of synthetic polymers and additives
New mass spectrometry concepts for characterization of synthetic polymers and additives
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用于表征合成聚合物和添加剂的新质谱概念
DOI：
10.1002/rcm.8768
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发表时间：
2020
影响因子：
2
通讯作者：
Trimpin, Sarah
中科院分区：
文献类型：
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作者：
Inutan, Ellen D.;Meher, Anil K.;Karki, Santosh;Fischer, Joshua L.;Imperial, Lorelie F.;Foley, Casey D.;Jarois, Dean R.;El‐Baba, Tarick J.;Lutomski, Corinne A.;Trimpin, Sarah
生物质谱（MS）已经开发了新的电离过程，其中基质将非挥发性分析物作为离子提升到气相中，而无需任何额外的能量输入。我们合理化，需要额外的基础知识，以评估合成聚合物和additives.MethodsDifferent质谱仪（Thermo Orbitrap（Q‐）Exactive（Focus）;沃茨SYNAPT G2（S））的分析效用领域。在将基质/分析物（/盐）样品直接从固态和表面暴露于低于大气压时形成多电荷聚合物离子促进了使用先进的质谱仪来检测聚合物材料，包括消费品（例如，结果令人惊讶的是，仅仅使用小分子基质化合物（例如，2-甲基-2-硝基丙烷-1，3-二醇或3-硝基苄腈）和盐（例如，一价或二价阳离子），这些样品在暴露于低于大气压时将非挥发性聚合物和非挥发性盐作为多电荷离子转移到气相中。这些成功与MS中离子化的传统理解相矛盾，因为非挥发性聚合物在气相中作为离子不仅可以通过与挥发性基质一样少的物质，而且还可以通过通过非共价金属阳离子加合物电离分析物所需的盐而被提升。原型真空基质辅助电离（vMAI）和使用非接触式方法的自动源被证明可用于合成聚合物和增塑剂的直接分析，通过将样品直接引入质谱仪真空中，最大限度地降低污染风险。或甚至施加的热量被证明用于使用（超）通过多电荷离子扩展高性能质谱仪的质量范围和使用一种分体式探针进样装置，我们的愿景是，随着基本面和专用源的进一步发展，如果解决了减少样本量测量的灵敏度问题，空间和时间分辨率测量都是可以实现的。
RationaleNew ionization processes have been developed for biological mass spectrometry (MS) in which the matrix lifts the nonvolatile analyte into the gas phase as ions without any additional energy input. We rationalized that additional fundamental knowledge is needed to assess analytical utility for the field of synthetic polymers and additives.MethodsDifferent mass spectrometers (Thermo Orbitrap (Q‐)Exactive (Focus); Waters SYNAPT G2(S)) were employed. The formation of multiply charged polymer ions upon exposure of the matrix/analyte(/salt) sample to sub‐atmospheric pressure directly from the solid state and surfaces facilitates the use of advanced mass spectrometers for detection of polymeric materials including consumer products (e.g., gum).ResultsAstonishingly, using nothing more than a small molecule matrix compound (e.g., 2‐methyl‐2‐nitropropane‐1,3‐diol or 3‐nitrobenzonitrile) and a salt (e.g., mono‐ or divalent cation(s)), such samples upon exposure to sub‐atmospheric pressure transfer nonvolatile polymersandnonvolatile salts into the gas phase as multiply charged ions. These successes contradict the conventional understanding of ionization in MS, because can nonvolatile polymers be lifted in the gas phase as ions not only by as little as a volatile matrix but also by the salt required for ionizing the analyte through noncovalent metal cation adduction(s). Prototypevacuummatrix‐assisted ionization (vMAI) and automated sources using a contactless approach are demonstrated for direct analyses of synthetic polymers and plasticizers, minimizing the risk of contamination using direct sample introduction into the mass spectrometer vacuum.ConclusionsDirect ionization methods from surfaces without the need of high voltage, a laser, or even applied heat are demonstrated for characterization of detailed materials using (ultra)high‐resolution and accurate mass measurements enabled by the multiply charged ions extending the mass range of high‐performance mass spectrometers and use of a split probe sample introduction device. Our vision is that, with further development of fundamentals and dedicated sources, both spatial‐ and temporal‐resolution measurements are within reach if sensitivity is addressed for decreasing sample‐size measurements.