This study presents the preparation and phase behavior of glycan-functionalized polyelectrolytes for capturing carbohydrate-binding proteins and bacteria in liquid condensate droplets. The droplets are formed by complex coacervation of poly(active… Click to show full abstract
This study presents the preparation and phase behavior of glycan-functionalized polyelectrolytes for capturing carbohydrate-binding proteins and bacteria in liquid condensate droplets. The droplets are formed by complex coacervation of poly(active ester)-derived polyanions and polycations. This approach allows for a straightforward modular introduction of charged motifs and specifically interacting units; mannose and galactose oligomers are used here as first examples. The introduction of carbohydrates has a notable effect on the phase separation and the critical salt concentration, potentially by reducing the charge density. Two mannose binding species, concanavalin A (ConA) and Escherichia coli, are shown to not only specifically bind to mannose-functionalized coacervates but also to some degree to unfunctionalized, carbohydrate-free coacervates. This suggests non-carbohydrate-specific charge-charge interactions between the protein/bacteria and the droplets. However, when mannose interactions are inhibited or when non-binding galactose-functionalized polymers are used, interactions are significantly weakened. This confirms specific mannose-mediated binding functionalization and suggests that introducing carbohydrates reduces non-specific charge-charge interactions by a so far unidentified mechanism. Overall, the presented route toward glycan-presenting polyelectrolytes enables new functional liquid condensate droplets with specific biomolecular interactions.
               
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