Functionalized hydrogel systems for molecular sensing and transport
type: CreativeWork
description: Hydrogels are a unique class of materials. The combination of many outstanding properties, including responsiveness, elasticity, transparency, porosity, high water content, biocompatibility, and the ability to immobilize functional species makes hydrogels attractive multifunctional materials for a broad range of applications. This dissertation focuses on modulating hydrogel properties for applications in molecular sensing and transport. There are two focus areas under the hydrogel theme within this dissertation. The first area is focused on the design, synthesis, and characterization of hydrogel glucose sensor materials with a liner fast response, small hysteresis and good stability under simulated physiological conditions. The first step was to study the interactions of glucose with phenylboronic acid (PBA) which is the glucose sensing functionality inside hydrogels. We find that (i) linear and slow responses are observed on hydrogels containing PBAs of low reactivity to glucose, (ii) linear and slow responses are coupled, (iii) the intramolecular ring formed in such PBAs is responsible for the low reactivity, (iv) PBAs of low pKa generally lead to low sensitivity, (v) hydrogels containing PBAs without intramolecular ring show fast and nonlinear response, (vi) nonlinear and fast responses are coupled, (vii) 1:1 and 2:1 PBA-glucose complexes exist universally in PBA-modified hydrogels and their coexistence leads to the nonlinear response. Based on these observations, a linear and fast sensor design is developed by tailoring the binding of nonlinear PBAs with glucose. A volume resetting agent is incorporated into the PBA-modified hydrogels to crosslink the PBA moieties and shrink the hydrogel volume in the absence of glucose. When glucose is present, the crosslinks are displaced into 1:1 PBA-glucose complexes, leading to a linear volume expansion. The coexistence of 1:1 and 2:1 PBA-glucose complexes during glucose sensing is largely eliminated. The sensor performance…
abstract: Hydrogels are a unique class of materials. The combination of many outstanding properties, including responsiveness, elasticity, transparency, porosity, high water content, biocompatibility, and the ability to immobilize functional species makes hydrogels attractive multifunctional materials for a broad range of applications. This dissertation focuses on modulating hydrogel properties for applications in molecular sensing and transport. There are two focus areas under the hydrogel theme within this dissertation. The first area is focused on the design, synthesis, and characterization of hydrogel glucose sensor materials with a liner fast response, small hysteresis and good stability under simulated physiological conditions. The first step was to study the interactions of glucose with phenylboronic acid (PBA) which is the glucose sensing functionality inside hydrogels. We find that (i) linear and slow responses are observed on hydrogels containing PBAs of low reactivity to glucose, (ii) linear and slow responses are coupled, (iii) the intramolecular ring formed in such PBAs is responsible for the low reactivity, (iv) PBAs of low pKa generally lead to low sensitivity, (v) hydrogels containing PBAs without intramolecular ring show fast and nonlinear response, (vi) nonlinear and fast responses are coupled, (vii) 1:1 and 2:1 PBA-glucose complexes exist universally in PBA-modified hydrogels and their coexistence leads to the nonlinear response. Based on these observations, a linear and fast sensor design is developed by tailoring the binding of nonlinear PBAs with glucose. A volume resetting agent is incorporated into the PBA-modified hydrogels to crosslink the PBA moieties and shrink the hydrogel volume in the absence of glucose. When glucose is present, the crosslinks are displaced into 1:1 PBA-glucose complexes, leading to a linear volume expansion. The coexistence of 1:1 and 2:1 PBA-glucose complexes during glucose sensing is largely eliminated. The sensor performance…
author: Zhang, Chunjie
language: en
keywords: hydrogel, boronic acid, sensor, glucose, photonic crystal, gradient, diffusion, transport
date published: 2015-01-21T19:59:03Z
date modified: 2026-07-22T22:26:07Z
provider: University of Illinois - Urbana-Champaign
publisher: Networked Digital Library of Theses and Dissertations
type: WebPage
source organization: University of Illinois at Urbana-Champaign

PropertyValue
property ID: Handle
value: http://hdl.handle.net/2142/73065