The development of an antifouling interpenetrating polymer network hydrogel film for salivary glucose monitoring.

Abstract

Owing to its rapid response and broad detection range, a phenylboronic acid (PBA)-functionalized hydrogel film-coated quartz crystal microbalance (QCM) sensor is used to non-invasively monitor salivary glucose in diabetic patients. However, nonspecific protein adsorption on the PBA-functionalized hydrogel film can cause dramatic loss of sensitivity and accuracy of the sensor. A traditional zwitterionic polymer surface with ultra-low protein fouling can hinder the interaction of PBA in the hydrogel matrix with glucose molecules owing to its steric hindrance, resulting in poor glucose sensitivity of the sensor. Herein, we developed a novel hydrogel film that enhanced the antifouling properties and sensitivity of the QCM sensor by infiltrating a glucose-sensitive monomer (i.e., PBA) into a zwitterionic polymer brush matrix to form an interpenetrating polymer network (IPN). The IPN hydrogel film could minimize the glucose sensitivity loss since the antifouling polymer distributed in its matrix. Moreover, a stable hydration layer was formed in this film that could prevent water from transporting out of the matrix, thus further improving its antifouling properties and glucose sensitivity. The experimental results confirmed that the IPN hydrogel film possessed excellent resistance to protein fouling by mucin from whole saliva with reductions in adsorption of nearly 88% and could also enhance the glucose sensitivity by nearly 2 fold, compared to the PBA-functionalized hydrogel film. Therefore, the IPN hydrogel film provides improved antifouling properties and sensitivity of the QCM sensor, which paves the way for non-invasive monitoring of low concentrations of glucose in saliva.