Adhesion to biological interfaces is dominated by carbohydrate interactions, where multivalency has a crucial role in determining binding specificity. Carbohydrate ligand-protein complexes control many physiological processes in healthy or diseased states. New models and data are needed to understand how ligand presentation and material properties drive these processes. We study the underlying interaction principles with respect to elastic modulus, ligand type and density using well-defined hydrogel materials as probes. A key finding states that for carbohydrate interactions the binding cooperativity and multivalency of ligands are controlled by the stiffness of the hydrogel and ligand density (statistical effects). Having established the basic material requirements for carbohydrate mediated adhesion on hydrogels, we designed switchable microgels that bind and release clinically relevant carbohydrate binding pathogens and cancer cells by a temperature stimulus. Upon temperature transition the density and spacing of carbohydrate ligands as well as the microgels elastic modulus and steric repulsion changes dramatically, which allows controlling cell or pathogen binding. By using sequence controlled glycopolymers we can further address multivalent receptor binding and clustering, which leads to strong adhesion and, potentially, cell instructive properties. Taken together, these responsive carbohydrate presenting hydrogels synthetic could provide new avenues toward scaffolds for tissue engineering, arrays for detecting disease, and an in-depth picture of how interfacial carbohydrate recognition is dependent on material properties.

Capture and release of cells via glycocalyx mimetic hydrogels

ACS Spring Meeting 2021

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