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

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

Nature Communications, 2020, vol. 11, issue 1, 1-9

Abstract: 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.

Date: 2020
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DOI: 10.1038/s41467-020-18657-5

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