Interfacing Mass Spectrometry with New Materials Developed for Fast Targeted Analysis

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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.