Glycan-Presenting Coacervates Derived from Charged Poly(active esters): Preparation, Phase Behavior, and Lectin Capture

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.

Sweet Janus Particles: Multifunctional Inhibitors of Carbohydrate-Based Bacterial Adhesion

“…coliemploys the mannose (Man)-specific adhesion receptor FimH at the tip of their fimbriae . It has been shown for a variety of Man-based natural and synthetic carbohydrates, glycoconjugates and glycofunctionalized materials that they can be used as inhibitors of the FimH receptor, reducing pathogen adhesion and thus infection. − Furthermore, glycofunctionalized materials such as glycoparticles can capture bacteria, e.g., in water purification or to detect biological contaminants. ,, The ability to actively release the bacteria from the glycoparticles, for example, using responsive polymers, further enables material recovery and reuse. − Glycoparticle–bacteria interactions typically lead to the formation of large aggregates composed of multiple bacteria and particles, which in a filtration setup facilitate easier separation. However, in antiadhesion therapy, large bacterial clusters are more likely to withstand clearance by the immune system from the infected site.…”

Nanodroplets Engineered with Folate Carbon Dots for Enhanced Cancer Cell Uptake toward Theranostic Application

“…Coacervation is an eco-friendly, single-step process that occurs in water without requiring special instrumentation . Given these advantages, droplets have several applications in diverse fields such as tissue engineering, drug delivery, food, gene delivery, and catalysis …”

Interface Binding Mechanism of Nanoclay Hybridized Coacervate Microdroplets for the Controllable Construction of Protocells

“…Functional compartments, including membrane-free phase separation compartments, lipid vesicles, or rock pores, have played a pivotal role in facilitating the emergence and evolution of encapsulated complex primitive chemical systems. − In the 1930s, Oparin − postulated that the origin of life involved the formation of coacervate microdroplets, referred to as protocells, through phase separation. These coacervate microdroplets result from inducing liquid–liquid phase separation (LLPS) through various weak associations, including charge–charge and cation−π interactions. − Because of their liquid-like fluidity and high isolation capacity, coacervate microdroplets offer a viable means to create chemically enriched environments. − Much like the crowded conditions within a cell, these enriched environments facilitate material exchange with the surrounding environment, − making coacervate microdroplets the classical protocell model for studying the origin of life. , In 1951, Bernal proposed that minerals mediated the origin of life on the early Earth . As a result of water or hydrothermal alteration of iron-rich magnesium-silicate on the sea floor, clay mineral reserves on the primitive early Earth are abundant.…”