Biodegradable, pH-responsive hydrogel networks composed of poly(methacrylic acid) crosslinked with varying mol percentages of polycaprolactone diacrylate were synthesized. These materials were characterized using NMR and FTIR. The equilibrium and dynamic swelling properties of these pH-responsive materials were studied. Also, the materials’ degradation was characterized using swelling studies and gel permeation chromatography.
Methods were developed to incorporate these novel hydrogels as sensing components in silicon-based microsensors. Extremely thin layers of hydrogels were prepared by photopolymerizion atop silicon microcantilever arrays that served to transduce the pH-responsive volume change of the material into an optical signal. Organosilane chemistry allowed covalent adhesion of the hydrogel to the silicon beam. As the hydrogel swelled, the stress generated at the surface between the hydrogel and the silicon caused a beam deflection downward. The resulting sensor demonstrated a maximum sensitivity of 1nm/4.5E-5 pH unit. Sensors were tested in protein-rich solutions to mimic biological conditions and found to retain their high sensitivity. The existing theory was evaluated and developed to predict deflection of these composite cantilever beams.
Another type of hydrogel-based microsensor was fabricated utilizing porous silicon rugate filters as transducers. Porous silicon rugate filters are garnering increased attention as components of in vivo biosensors due to their ability for remote readout through tissue. Here, the biodegradable, pH-responsive hydrogel was polymerized within the pores of a porous silicon rugate filter to generate a novel, completely degradable sensor. Silicon was electrochemically etched in hydrofluoric acid to generate the porous silicon rugate filter with its reflectance peak in the near infrared region. Poly(methacrylic acid) crosslinked with polycaprolactone diacrylate was polymerized within the pores using UV free radical photopolymerization. The reflectance peak of this sensor varied linearly with pH in the region pH 2.2 to 8.8. This work shows promise towards utilizing porous silicon rugate filters as transducers for environmentally responsive hydrogels for biosensing applications. / text
| Identifer | oai:union.ndltd.org:UTEXAS/oai:repositories.lib.utexas.edu:2152/ETD-UT-2010-05-741 |
| Date | 01 September 2010 |
| Creators | Snelling, Diana Kathryn |
| Source Sets | University of Texas |
| Language | English |
| Detected Language | English |
| Type | thesis |
| Format | application/pdf |
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