This work involves the creation and optimization of polymer thin films as enabling technology for robust point-of-care diagnostic platforms and drug delivery carriers. Recognitive polymeric networks can be rationally designed and produced through tailoring non-covalent complexation interactions between “guest” template molecules and functional monomers to produce polymer films with ‘macromolecular memory.' The resulting networks can be highly selective to the template molecule or control release due to the particular chemistry and orientation of the polymer chains. In this work, structural characteristics of polymer films were altered and template binding/transport properties were analyzed. Specifically, crosslinking monomer length and concentration as well as free-radical initiation scheme were changed resulting in different polymer structures with various mesh sizes, polymer volume fractions, and template binding characteristics such as affinity, capacity, selectivity, and diffusion. Methacrylic acid-co-poly ethylene glycol dimethacrylate (poly(MAA-co-PEGDMA)) copolymer recognitive networks were prepared via UV-photopolymerization with template molecules such as ethyl adenine-9-acetate and testosterone. Results demonstrate that a living/controlled initiation scheme significantly increases the affinity and capacity of recognitive polymers. This is hypothesized to be due to a more uniform and homogeneous structural architecture. Additionally, a 77% increase in crosslinking monomer length resulted in polymers with a 6 fold decrease in affinity, a 2 fold decrease in capacity, and decreased selectivity with increased template diffusional transport. Similarly, increasing the crosslinking monomer concentration from 50 to 90% yielded polymers with a 4 fold increase in binding affinity, a 1.5 fold increase in capacity, as well as increased selectivity with decreased template transport. Engineering of templated polymer structural properties is vital to the further development of novel platform technologies that will utilize recognitive mechanisms and structures. Increasing the tailorability of recognitive biomaterials yields promising materials for robust, inexpensive, future point-of- care diagnostic and therapeutic devices.

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