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首页> 外文期刊>Journal of mass spectrometry: JMS >Detection and assignment of inorganic aqueous polymers relevant to environmental nanogeoscience by direct infusion electrospray ionization mass spectrometry
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Detection and assignment of inorganic aqueous polymers relevant to environmental nanogeoscience by direct infusion electrospray ionization mass spectrometry

机译：直接输注电喷雾电离质谱法检测和分配与环境纳米科学相关的无机含水聚合物

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摘要

Inorganic polymers in aqueous solutions are being proposed as essential components in new theories concerning nonclassical nucleation and growth of nanominerals relevant to environmental nanogeosciences. The study of those complex natural processes requires multi-technique analytical approaches able to characterize the solutions and their constituents (solutes, oligomers, polymers, clusters and nanominerals) from atomic to micrometric scales. A novel analytical approach involving an electrospray ionization source (ESI) coupled to time-of-flight mass spectrometry (TOF/MS) was developed to identify inorganic polymers in aqueous solution. To this end, the presence of initial Al oligomers and their polymerization processes was studied during a nanomineral aqueous synthesis (hydrobasaluminte, Al4SO4(OH)(10)center dot 12-36H(2)O). Ensuring the feasibility and robustness of the methodology as well as the stability of the polymers under study (avoiding undesirable fragmentation), a meticulous study of the ESI-TOF MS working conditions was performed. Precision of the methodology was evaluated obtaining relative standard deviations below 3.3%. For the first time in the study of inorganic polymers in the earth sciences, the mass accuracy error (ppm) has been reported and the use of significant decimal figures of the m/z signal has been taken into account. Complementary to this, a four-step polymer assignment methodology and a database with the Al- and Al-SO42- polymers assigned were created. Several polymers have been assigned for the first time, including Al (SO4)(+)center dot H2O, Al2O(SO4)(2+)center dot H2O, Al5O4(OH)(5)(2+)center dot 2H(2)O, and Al3O5(OH)(2-)center dot 4H(2)O, among others. The results obtained in the present study help create a foundation to include mass spectrometry as a routine analytical technique to study mineral formation in aqueous solution.
机译：水溶液中的无机聚合物在新的理论中提出了关于与环境纳米疗程相关的非生物核肉和生长的新理论中的基本组分。对这些复杂的自然过程的研究需要多技术的分析方法，该方法能够将溶液及其成分（溶质，低聚物，聚合物，簇和纳米植物和纳米植物）从原子分析到微米尺度。开发了一种涉及电喷雾电离源（ESI）的新型分析方法，其耦合到飞行时间质谱（TOF / MS）以鉴定水溶液中的无机聚合物。为此，在纳米内水合合成期间研究了初始Al低聚物及其聚合方法的存在（氢萘铝，Al4SO4（OH）（10）中心点12-36H（2）O）。确保方法的可行性和稳健性以及研究的聚合物的稳定性（避免不希望的碎片），进行了对ESI-TOF MS工作条件的细致研究。评估方法的精度获得的相对标准差低于3.3％。首次在地球科学中的无机聚合物研究中，已经报道了质量准确误差（PPM）并考虑了使用M / Z信号的显着小数图。互补地，创建了四步聚合物分配方法和具有分配的AL-和AL-SO42-聚合物的数据库。已经首次分配了几种聚合物，包括Al（SO 4）（+）中心点H2O，Al2O（SO 4）（2+）中心点H2O，Al5O4（OH）（5）（2+）中心点2H（2 ）o，Al3O5（OH）（2-）中心点4h（2）o等。在本研究中获得的结果有助于创造基础，包括质谱法作为常规分析技术，以研究水溶液中矿物质的矿物质形成。

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