Colloidal Hydrogel with Staged Sequestration and Release of Molecules Undergoing Competitive Binding.

Competitive binding of distinct molecules in the hydrogel interior can facilitate dynamic exchange between the hydrogel and the surrounding environment. The ability to control the rates of sequestration and release of these molecules would enhance the hydrogel's functionality and enable targeting of a specific task. Here, we report the design of a colloidal hydrogel with two distinct pore dimensions to achieve staged, diffusion-controlled scavenging and release dynamics of molecules undergoing competitive binding. The staged scavenging and release strategy was shown for CpG oligodeoxynucleotide (ODN) and human epidermal growth factor (hEGF), two molecules exhibiting different affinities to the quaternary ammonium groups of the hydrogel. Fast ODN scavenging from the ambient environment occurred via diffusion through submicrometer-size hydrogel pores, while delayed hEGF release from the hydrogel was governed by its diffusion through nanometer-size pores. The results of the experiments were in agreement with simulation results. The significance of staged ODN-hEGF exchange was highlighted by the dual anti-inflammation and tissue proliferation hydrogel performance.