Homopolymer self-assembly of poly(propylene sulfone) hydrogels via dynamic noncovalent sulfone–sulfone bonding

Abstract

Natural biomolecules such as peptides and DNA can dynamically self-organize into diverse hierarchical structures. Mimicry of this homopolymer self-assembly using synthetic systems has remained limited but would be advantageous for the design of adaptive bio/nanomaterials. Here, we report both experiments and simulations on the dynamic network self-assembly and subsequent collapse of the synthetic homopolymer poly(propylene sulfone). The assembly is directed by dynamic noncovalent sulfone–sulfone bonds that are susceptible to solvent polarity. The hydration history, specified by the stepwise increase in water ratio within lower polarity water-miscible solvents like dimethylsulfoxide, controls the homopolymer assembly into crystalline frameworks or uniform nanostructured hydrogels of spherical, vesicular, or cylindrical morphologies. These electrostatic hydrogels have a high affinity for a wide range of organic solutes, achieving >95% encapsulation efficiency for hydrophilic small molecules and biologics. This system validates sulfone–sulfone bonding for dynamic self-assembly, presenting a robust platform for controllable gelation, nanofabrication, and molecular encapsulation.

Surface chemistry-mediated modulation of adsorbed albumin folding state specifies nanocarrier clearance by distinct macrophage subsets

“…To examine the cellular uptake of nanocarriers, we incubated MΦ with nanocarriers for 2 h, washed cells with PBS, and measured the emission of nanocarrier-loaded fluorescent dye using flow cytometry. Our past work demonstrates that this general procedure quantifies fluorescence resulting from the cellular internalization of dye-loaded PEG-b-PPS nanocarriers, and the extensive washing procedure minimizes signal that would otherwise arise from nanocarriers associated with the plasma membrane (on the extracellular side) after the preceding media aspiration step [60][61][62] . Here this is further supported by lysosomal colocalization studies (Supplementary Fig.…”

Current hydrogel advances in physicochemical and biological response-driven biomedical application diversity

“…To make the stiffness of hydrogel scaffolds meet the demands of practical biomedical application, many methods have been developed to modulate the stiffness of hydrogels. 3,37,45 Lots of experiences indicate that nanoparticles doping [193][194][195] or chemical cross-linking 7,196,197 are two dominant methods for enhancing mechanical properties. Nevertheless, stiffness is not the sole cause capable of determining cell behaviors in the 3D context, and some other parameters, such as matrix pore size, viscoelasticity, etc., could also exert roust influences on cell biology simultaneously.…”

Facile Preparation of Drug-Releasing Supramolecular Hydrogel for Preventing Postoperative Peritoneal Adhesion

“…Because hydrogels usually maintain a delicate balance between their amphiphilic skeleton and hydrophilic circumstances, loading hydrophobic drugs in the hydrogel to form a homogeneous, stable, and clear combination is challenging, − and most likely, insoluble precipitates are formed. Many effective natural small molecules, such as luteolin, quercetin, and other anticancer or anti-inflammatory drugs, are highly hydrophobic: designing hydrogels suitable for hydrophobic drugs is of great importance to expand the field of biomedicine .…”