Advancing Design and Application of Porous Polymeric Sorptive Phases for Direct Introduction Mass Spectrometry

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This program aims to create a fresh approach to small-volume sample analysis using devices that rely on thin coatings of porous polymer to effectively grab molecules from complex sample solutions. These coatings will be tailor-made to target environmental contaminants, pharmaceuticals, and illicit drugs in water and biological samples. The novel materials will be incorporated into innovative devices that can be coupled directly to ultra-sensitive analytical instruments for fast automatable sample preparation and online analysis. We will create a new approach to rational design using predictive mathematical and chemical models based on fundamental science involved in how these materials are formed and the processes by which they recognize molecules. This research stands on the principles of green analytical chemistry, with attention given to economical use of reagents (i.e., most of the atoms used end up in the material with little waste), reduced use of harmful chemicals, and awareness of the life cycle of analytical devices to reduce environmental footprint while allowing for expanded screening capacity (i.e., increased temporal or spatial measurements). To achieve these goals my research will focus on four goals. 1) Develop new tools for fast characterization of polymer properties (e.g., porosity and adsorption behavior) in thin porous polymer films. In this work, we will advance novel ways to characterize porous polymer coatings using solid state nuclear magnetic resonance, differential scanning calorimetry, and direct introduction mass spectrometry (i.e., desorption electrospray ionization, blade spray, etc.). 2) Develop a new predictive model of how these polymers form porous coatings on solid devices surfaces. Here we will build on existing models of how polymers form to incorporate factors to account for more complex processes that occur when the polymer components are first mixed (equilibria), and then how these factors change as the polymerization proceeds. 3) Build on the porosity and adsorption models to understand how introduction of functionalities to exclude or trap matrix components influence polymer morphology and performance, particularly to understand the selectivity in sampling. 4) Use these discoveries to build devices for direct sampling and introduction to mass spectrometry for clinical and environmental applications. The new model of phase separation, porosity, and surface chemistry will equip scientists with dramatically better tools to predict and control the physical and chemical properties of porous sorbent coatings. This has the potential to revolutionize the development of new analytical devices while reducing the time and resources consumed by trial-and-error refinement. By developing a comprehensive model for porous polymer coatings fabrication and function, performance can be assured with as little waste as possible, making these environmentally-friendly analytical methods even greener.