Designing Tough Hydrogel Shells for Glucose Sensing

Abstract Conventional hydrogel microcapsules often suffer from inadequate mechanical stability, hindering their use. Here, water‐cored double‐network (DN) hydrogel shells are designed, formed by polyacrylamide and calcium alginate networks using triple‐emulsion templates. These DN hydrogel shells offer robust mechanical stability, optical transparency, and a precisely‐defined cut‐off threshold. The feasibility of this platform is demonstrated through the development of a fluorometric glucose sensor. Glucose oxidase is enclosed within the water core, while a pH‐responsive fluorescent dye is incorporated into the DN shells. Glucose diffuses into the core through the DN shells, where the glucose oxidase converts glucose into gluconic acid, leading to pH reduction and a subsequent decrease in fluorescence intensity of DN shells. Additionally, the pH‐sensitive colorant dissolved in the medium enables visual pH assessment. Thus, glucose levels can be determined using both fluorometric and colorimetric methods. Notably, the DN shells exhibit exceptional stability, enduring intense mechanical stress and cycles of drying and rehydration without leakage. Moreover, the DN shells act as effective barriers, safeguarding glucose oxidase against proteolysis by large disruptive proteins, like pancreatin. This versatile DN shell platform extends beyond glucose oxidase encapsulation, serving as a foundation for various capsule sensors utilizing enzymes and heterogeneous catalysts.