Journal
NATURE COMMUNICATIONS
Volume 11, Issue 1, Pages -Publisher
NATURE RESEARCH
DOI: 10.1038/s41467-020-18657-5
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Funding
- Center for Computation & Theory of Soft Materials
- BioCryo facility of Northwestern University's NUANCE Center
- Integrated Molecular Structure Education and Research Center
- Structural Biology Facility
- NU Atomic
- Nanoscale Characterization Experimental Center
- Robert H. Lurie Comprehensive Cancer Center Flow Cytometry Core
- Biological Imaging Facility at Northwestern University
- Northwestern University
- E.I. DuPont de Nemours Co.
- The Dow Chemical Company
- DOE Office of Science [DE-AC02-06CH11357]
- National Institutes of Health Director's New Innovator Award [1DP2HL132390-01]
- National Institute of Allergy and Infectious Diseases [5R21AI137932-02]
- National Science Foundation CAREER Award [1453576]
- Louis A. Simpson & Kimberly K. Querrey Center for Regenerative Nanomedicine Regenerative Nanomedicine Catalyst Award
- Department of Energy Award [DE-FG02-08ER46539]
- Sherman Fairchild Foundation
- U.S. Department of Energy (DOE) [DE-FG02-08ER46539] Funding Source: U.S. Department of Energy (DOE)
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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.
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