Interfacing Mass Spectrometry with New Materials Developed for Fast Targeted Analysis

广泛而多样的环境污染源导致公众担心清洁水、空气和食物的可获得性受到威胁。这种压力增加了对广泛和频繁检测的需求，以确保健康、安全和资源质量。在这种背景下，我正在进行的研究计划是开发对水样进行高通量筛选所必需的灵敏、快速、简单的分析方法，这些方法也适用于废水评估和处理计划。这里提出的工作有两个相互关联的研究主题：A)开发选择性材料，主要是分子印迹聚合物(MIP)膜，用于从水溶液中吸收目标分析物；B)开发解吸电喷雾电离-质谱仪(DESI-MS)方法，用于直接询问选择性吸附剂中的分析物。 MIPS因其在制造和使用方面的选择性和简单性而具有吸引力。在为有问题的水污染物创建新的MIP时，将研究组成的影响，以确定和优化分析性能。其基本目标将是：i)了解制造更好的MIP所需的化学成分；ii)确定影响质谱学界面效率的MIP的特征；以及iii)探索MIP在薄膜格式中的内在局限性。这将导致改进的薄膜制备方法、新的功能材料以及更高效和更可重复性的分析。MIP结合的分析物的DISI-MS可以在几秒钟内完成；而质谱学增加了分析的选择性和灵敏度。将研究MIP的组成和结构对i)DESI的分析物解吸和电离机理的影响，以及ii)质谱学质量(如噪声和干扰)，以及iii)应用MIP进行现场环境采样的方法。MIP与DESI-MS的结合将创造出简单而灵敏的分析方法。 随着对分子印迹聚合物和二异氰酸酯的化学驱动性能认识的提高，这一研究将提供新的功能材料和新的分析方法。此外，这些技术将推动消耗更少、产生更少废物的绿色分析方法，同时保持敏感和可靠的分析标准。由此产生的分析方法将适应监测工业流程和确保水资源质量所需的高通量分析。我们的方法将提高精度，允许更高的测量频率，并为实时或接近实时的检测提供先进的技术。这项工作将支持本科生和研究生研究人员的培训，并为与行业和学术研究人员的合作创造机会。

Widespread and varied sources of environmental contamination has led to public concern about threats to the availability of clean water, air and food. Such pressures increase demands to test broadly and frequently to assure health, safety and resource quality. This context motivates my ongoing research program to develop sensitive, fast, simple analytical approaches necessary for high throughput screening of aqueous samples, which are also suitable for use in wastewater assessment and treatment programs. The work proposed here has two interrelated research themes: A) development of selective materials, principally molecularly imprinted polymer (MIP) films, for uptake of target analytes from aqueous solutions, and B) development of desorption electrospray ionization-mass spectrometry (DESI-MS) methods for direct interrogation of analytes in the selective sorbents. MIPs are attractive because of their selectivity and simplicity in terms of fabrication and use. In creating new MIPs for problematic water contaminants, the effect of composition will be studied to determine and optimize analytical performance. The underlying goals will be to i) understand the chemistry needed to make better MIPs, ii) identify the features of the MIP that influence the efficiency of mass spectrometric interface, and iii) probe the intrinsic limitations of MIPs in a film format. This will lead to improved film fabrication methods, new functional materials, and more efficient and reproducible analyses. DESI-MS of the MIP-bound analyte can be completed in seconds; and mass spectrometry adds selectivity and sensitivity to analysis. The influence of MIP composition and structure on i) analyte desorption and ionization mechanisms for DESI and ii) mass spectral quality (e.g. noise and interferences) will be studied, and iii) methods to apply MIPs for in situ environmental sampling will be examined. The combination of MIPs with DESI-MS will create simple and sensitive analytical methods. Along with improvements in the understanding of the chemistry driving performance of MIPs and DESI, this research will provide novel functional materials and new analytical methods. Furthermore, the techniques will advance green analytical methods that consume less and generate less waste, while maintaining standards for sensitive and robust analyses. The resulting analytical methods will accommodate high throughput analyses needed for monitoring of industrial process streams and assuring water resource quality. Our methods will improve accuracy, allow for higher frequency of measurements, and offer advances for real-time or near real-time sensing. This work will support the training of undergraduate and graduate researchers and build opportunities for collaboration with industry and academic researchers.