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

Du, Fanfan; Qiao, Baofu; Nguyen, Trung Dac; Vincent, Michael P.; Bobbala, Sharan; Yi, Sijia; Lescott, Chamille; Dravid, Vinayak P.; de la Cruz, Monica Olvera; Scott, Evan Alexander

doi:10.1038/s41467-020-18657-5

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

Journal Article · Tue Sep 29 00:00:00 EDT 2020 · Nature Communications

DOI:https://doi.org/10.1038/s41467-020-18657-5· OSTI ID:1671119

Du, Fanfan ^[1]; Qiao, Baofu ^[1]; Nguyen, Trung Dac ^[1]; Vincent, Michael P. ^[1]; Bobbala, Sharan ^[1]; Yi, Sijia ^[1]; Lescott, Chamille ^[1]; Dravid, Vinayak P. ^[1]; de la Cruz, Monica Olvera ^[1]; Scott, Evan Alexander ^[1]

Northwestern Univ., Evanston, IL (United States)

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.

View Accepted Manuscript (DOE)

Research Organization:: Argonne National Laboratory (ANL), Argonne, IL (United States)

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES)

Contributing Organization:: Advanced Photon Source (APS), Argonne National Laboratory (ANL), Argonne, IL (US)

Grant/Contract Number:: AC02-06CH11357

OSTI ID:: 1671119

Journal Information:: Nature Communications, Journal Name: Nature Communications Journal Issue: 1 Vol. 11; ISSN 2041-1723

Publisher:: Nature Publishing GroupCopyright Statement

Country of Publication:: United States

Language:: ENGLISH

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