Poly(ethylene glycol) Hydrogel Crosslinking Chemistries Identified via Atmospheric Solids Analysis Probe Mass Spectrometry,Macromolecules

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Poly(ethylene glycol) Hydrogel Crosslinking Chemistries Identified via Atmospheric Solids Analysis Probe Mass Spectrometry
Macromolecules ( IF 5.1 ) Pub Date : 2021-08-28 , DOI: 10.1021/acs.macromol.1c00765
Kevin J. Endres ₁ , Rodger A. Dilla ₂ , Matthew L. Becker ₂ , Chrys Wesdemiotis _{1,

3}

Affiliation

Hydrogels are hydrophilic, crosslinked polymer networks that can absorb several times their own mass in water; they are frequently used in biomedical applications as a native tissue mimic. The characterization of hydrogels and other covalently crosslinked networks is often limited by their insolubility and infinite molecular weight conferred by crosslinking. In this study, chemically crosslinked hydrogel materials based on poly(ethylene glycol) (PEG) have been characterized directly, without any sample preparation, by mild thermal degradation using atmospheric solids analysis probe mass spectrometry (ASAP-MS) coupled with ion mobility (IM) separation and tandem mass spectrometry (MS/MS) characterization of the degradants. The structural insight gained from these experiments is illustrated with the analysis of oxime-crosslinked PEG hydrogels formed by the click reaction between 4-arm PEG star polymers with either ketone or aminooxy end group functionalities and PEG dimethacrylate (PEGDMA) copolymeric hydrogel networks formed by photopolymerization of PEGDMA. The ASAP-MS, IM, and MS/MS methods were combined to identify the crosslinking chemistry and obtain precursor chemistry information retained in the end-group substituents of the thermal degradation products.

中文翻译：

通过大气固体分析探针质谱法鉴定的聚（乙二醇）水凝胶交联化学物质

水凝胶是亲水的、交联的聚合物网络，可以吸收数倍于自身质量的水；它们经常作为天然组织模拟物用于生物医学应用。水凝胶和其他共价交联网络的表征通常受到它们的不溶性和交联赋予的无限分子量的限制。在这项研究中，基于聚乙二醇 (PEG) 的化学交联水凝胶材料已直接表征，无需任何样品制备，通过使用大气固体分析探针质谱 (ASAP-MS) 与离子迁移率 (IM) 的温和热降解) 降解物的分离和串联质谱 (MS/MS) 表征。通过对具有酮或氨基氧基端基官能团的 4 臂 PEG 星形聚合物与通过光聚合形成的 PEG 二甲基丙烯酸酯 (PEGDMA) 共聚水凝胶网络之间的点击反应形成的肟交联 PEG 水凝胶的分析，说明了从这些实验中获得的结构见解PEGDMA。结合 ASAP-MS、IM 和 MS/MS 方法来鉴定交联化学并获得保留在热降解产物的端基取代基中的前体化学信息。

更新日期：2021-09-14

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