Interfacing Mass Spectrometry with New Materials Developed for Fast Targeted Analysis

环境污染的来源广泛而多样，导致公众对清洁水、空气和食物的供应受到威胁表示关切。这种压力增加了广泛和频繁测试的需求，以确保健康，安全和资源质量。这种情况下，激励我正在进行的研究计划，以开发敏感，快速，简单的分析方法所需的高通量筛选的水样品，这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）薄膜，用于从水溶液中吸收目标分析物，以及B）开发解吸电喷雾电离质谱（ES-MS）方法，用于直接询问选择性吸附剂中的分析物。MIP由于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。 基本目标将是i）理解制造更好的MIP所需的化学，ii）识别影响质谱接口效率的MIP的特征，以及iii）探测膜形式的MIP的固有限制。这将导致改进的薄膜制造方法，新的功能材料，以及更有效和可重复的分析。MIP结合的分析物的质谱可以在几秒钟内完成;质谱增加了分析的选择性和灵敏度。将研究MIP组成和结构对i）DESI分析物解吸和电离机制的影响，以及ii）质谱质量（例如噪声和干扰）的影响，iii）将检查将MIP应用于现场环境采样的方法。MIPs与EST-MS的结合将创建简单而灵敏的分析方法。沿着人们对分子印迹聚合物和分子印迹聚合物的化学驱动性能认识的不断深入，本研究将为分子印迹聚合物和分子印迹聚合物提供新的功能材料和新的分析方法。此外，这些技术还将推动绿色分析方法，减少消耗和产生废物，同时保持敏感和稳健分析的标准。由此产生的分析方法将适应高通量分析需要监测工业过程流和确保水资源质量。我们的方法将提高精度，允许更高的测量频率，并为实时或近实时传感提供进步。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.**