Mass Spectrometry Methods for the Comprehensive Analysis of Emerging Functional Materials

新兴功能材料综合分析的质谱方法

• 批准号: 1808115
• 负责人: Chrys Wesdemiotis
• 金额: $ 21.9万
• 依托单位: University of Akron
• 依托单位国家: 美国
• 项目类别: Continuing Grant
• 财政年份: 2018
• 资助国家: 美国
• 起止时间: 2018-09-01 至 2022-02-28
• 项目状态: 已结题
• 来源: https://www.nsf.gov/awardsearch/showAward?AWD_ID=1808115&HistoricalAwards=false
• 关键词: Mass; Spectrometry; Methods; Comprehensive; Analysis

In this project, funded by the Chemical Measurement and Imaging Program of the Chemistry Division, Professor Chrys Wesdemiotis and his group at the University of Akron are developing new methods for the characterization of advanced materials used in mechanical, electrical, biomedical, optical, or environmental applications (such as implants, coatings, adhesives, membranes, and "smart surfaces"). The methods are based on mass spectrometry, a powerful tool for characterizing the compositions and structures. They allow accurate and sensitive analysis of the molecular structures of the synthetic macromolecular compounds comprising these materials, enabling meaningful understanding of the relationships between molecular structure and useful properties, thus facilitating the design of better, commercially viable products with desired macroscopic features. The research provides opportunities for undergraduate and graduate students (including students from underrepresented groups) to engage in modern chemical analysis and materials research, two areas with growing employment opportunities that are vital for our nation's technological advancement.A major objective of this research is to integrate mild thermal desorption/degradation with online mass spectrometry for the microstructural characterization of crosslinked polymers and materials with very high molecular weight, such as hydrogels and rubber copolymers. Relatively low temperatures are employed in order to preferentially break weak bonds or to probe sterically crowded sites, yielding oligomeric species that provide molecular connectivity detail as well as insight into crosslinkers and polymer precursors. A further objective concerns the development of surface-layer matrix assisted laser desorption ionization mass spectrometric imaging for the detection of intact molecules within the top 2 nm of synthetic material surfaces. Understanding of the surface composition and detection and characterization of unwanted defects or deliberate surface modifications is imperative for deciding a material?s suitability for a given application, since the surface is the first point of contact with the environment. The Wesdemiotis group uses multidimensional approaches (combining mass analysis, tandem mass spectrometry, and orthogonal separation by polarity and/or shape) to enable sensitive and precise analysis of the composition, structure, and architecture of synthetic macromolecular compounds that are widely employed in industrial, biomedical, and technological applications. They specifically target materials that are challenging to characterize by other methods because of their complexity, size, or topology.This award reflects NSF's statutory mission and has been deemed worthy of support through evaluation using the Foundation's intellectual merit and broader impacts review criteria.

在这个由化学系化学测量和成像计划资助的项目中，阿克伦大学的Chris Wesdemiotis教授和他的团队正在开发用于机械、电气、生物医学、光学或环境应用(如植入物、涂层、粘合剂、薄膜和“智能表面”)的先进材料的新方法。这些方法是基于质谱学的，这是表征成分和结构的强大工具。它们可以对包含这些材料的合成大分子化合物的分子结构进行准确和灵敏的分析，从而能够有意义地了解分子结构和有用特性之间的关系，从而有助于设计出具有所需宏观特征的更好的、商业上可行的产品。这项研究为本科生和研究生(包括来自代表性不足群体的学生)提供了从事现代化学分析和材料研究的机会，这两个领域的就业机会越来越多，对我国的技术进步至关重要。这项研究的一个主要目标是将温和的热解吸/降解与在线质谱学相结合，用于表征交联聚合物和具有非常高分子质量的材料(如水凝胶和橡胶共聚物)的微观结构。使用相对较低的温度是为了优先打破弱键或探测空间密集的位置，产生低聚物种，提供分子连接性细节以及对交联剂和聚合物前体的洞察。另一个目标是发展表面层基质辅助激光解吸电离质谱学成像，用于检测合成材料表面顶端2 nm内的完整分子。由于表面是与环境接触的第一点，因此了解表面组成以及检测和表征不需要的缺陷或有意的表面改性对于确定材料是否适合特定应用至关重要。Wesdemiotis小组使用多维方法(结合质量分析、串联质谱仪和按极性和/或形状的正交分离)，能够对工业、生物医学和技术应用中广泛使用的合成高分子化合物的组成、结构和结构进行灵敏和精确的分析。他们专门针对那些因其复杂性、大小或拓扑结构而难以通过其他方法进行表征的材料。该奖项反映了NSF的法定使命，并通过使用基金会的智力优势和更广泛的影响审查标准进行评估，被认为值得支持。

项目成果

Synthesis and Characterization of Well-Defined, Tadpole-Shaped Polystyrene with a Single Atom Junction Point

• DOI: 10.1021/acs.macromol.8b01384
• 发表时间: 2018-11
• 期刊: Macromolecules
• 影响因子: 5.5
• 作者: Fan Zhang;R. Quirk;Selim Gerişlioğlu;C. Wesdemiotis;Selemon Bekele;M. Tsige;Yung P. Koh;S. Simon;M. Foster

Separation, identification, and confirmation of cyclic and tadpole macromolecules via UPLC-MS/MS

通过 UPLC-MS/MS 分离、鉴定和确认环状和蝌蚪大分子

• DOI: 10.1039/d2an00208f
• 发表时间: 2022
• 期刊: The Analyst
• 作者: O'Neill, Jason M.;Mao, Jialin;Haque, Farihah M.;Barroso-Bujans, Fabienne;Grayson, Scott M.;Wesdemiotis, Chrys
• 通讯作者: Wesdemiotis, Chrys

Sequence isomeric giant surfactants with distinct self-assembly behaviors in solution

测序在溶液中具有独特自组装行为的异构巨型表面活性剂

• DOI: 10.1039/c8cc09207a
• 发表时间: 2019
• 期刊: Chemical Communications
• 影响因子: 4.9
• 作者: Zhang Wei;Shan Wenpeng;Zhang Shuailin;Liu Yuchu;Su Hao;Luo Jiancheng;Xia Yanfeng;Li Tao;Wesdemiotis Chrys;Liu Tianbo;Cui Honggang;Li Yiwen;Cheng Stephen Z D
• 通讯作者: Cheng Stephen Z D

Analysis of Thermoplastic Copolymers by Mild Thermal Degradation Coupled to Ion Mobility Mass Spectrometry

通过轻度热降解与离子淌度质谱联用分析热塑性共聚物

• DOI: 10.1002/marc.202200306
• 发表时间: 2022
• 期刊: Macromolecular Rapid Communications
• 影响因子: 4.6
• 作者: Alawani, Nadrah;Barrère‐Mangote, Caroline;Wesdemiotis, Chrys
• 通讯作者: Wesdemiotis, Chrys

Analysis of monodisperse, sequence-defined, and POSS-functionalized polyester copolymers by MALDI tandem mass spectrometry

• DOI: 10.1177/1469066719828875
• 发表时间: 2019-02-01
• 期刊: EUROPEAN JOURNAL OF MASS SPECTROMETRY
• 影响因子: 1.3
• 作者: Mao, Jialin;Zhang, Wei;Wesdemiotis, Chrys
• 通讯作者: Wesdemiotis, Chrys