Molecular and Biofunctional Modification of Conformal POEGMA Bottlebrush Coatings and Applications Toward In Vitro Diagnostics

Abstract

In vitro diagnostic assays (IVDs) play a crucial role in modern biomedical research and clinical decision-making. The overall performance and cost of IVDs depends considerably on the quality of the assay surface being used and the steps/reagents required to complete the assay. Synthetic “bottlebrush” polymers have garnered considerable attention as molecularly defined and tunable biointerfacial coatings for a diverse set of biomedical applications; in particular, their bio-inertness, ability to eliminate nonspecific binding events and stabilize biorecognition elements make them attractive candidates as biosensing surfaces. This dissertation describes the use of “nonfouling” (protein- and cell-resistant) nanoscale polymer bottlebrush films derived from poly(oligo(ethylene glycol) methyl ether methacrylate) (POEGMA) for IVD applications. POEGMA coatings are grown from planar surfaces by surface-initiated atom transfer radical polymerization (SI-ATRP), and then undergo biofunctional modification with biorecognition elements to target specific analytes of interest. This strategy is used to assemble low-cost, “point of care” diagnostic tests which exhibit performance comparable to those used in central laboratories. Further, molecular modification of bottlebrush architecture is used as a controllable design parameter for fine-tuning the physiochemical properties and biological behavior of these surfaces. Taken together, these studies highlight the potential for using POEGMA bottlebrush films as biointerfacial coatings for next-generation IVDs and medical devices.