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Title: Reversible self-assembly of superstructured networks

Abstract

Soft structures in nature, such as protein assemblies, can organize reversibly into functional and often hierarchical architectures through noncovalent interactions. Molecularly encoding this dynamic capability in synthetic materials has remained an elusive goal. We report on hydrogels of peptide-DNA conjugates and peptides that organize into superstructures of intertwined filaments that disassemble upon the addition of molecules or changes in charge density. Experiments and simulations demonstrate that this response requires large-scale spatial redistribution of molecules directed by strong noncovalent interactions among them. Simulations also suggest that the chemically reversible structures can only occur within a limited range of supramolecular cohesive energies. Storage moduli of the hydrogels change reversibly as superstructures form and disappear, as does the phenotype of neural cells in contact with these materials.

Authors:
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Publication Date:
Research Org.:
Energy Frontier Research Centers (EFRC) (United States). Center for Bio-Inspired Energy Science (CBES); Northwestern Univ., Evanston, IL (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22)
OSTI Identifier:
1566718
DOE Contract Number:  
FG02-00ER45810; SC0000989
Resource Type:
Journal Article
Journal Name:
Science
Additional Journal Information:
Journal Volume: 362; Journal Issue: 6416; Journal ID: ISSN 0036-8075
Publisher:
AAAS
Country of Publication:
United States
Language:
English
Subject:
catalysis (homogeneous), solar (photovoltaic), bio-inspired, charge transport, mesostructured materials, materials and chemistry by design, synthesis (novel materials), synthesis (self-assembly)

Citation Formats

Freeman, Ronit, Han, Ming, Álvarez, Zaida, Lewis, Jacob A., Wester, James R., Stephanopoulos, Nicholas, McClendon, Mark T., Lynsky, Cheyenne, Godbe, Jacqueline M., Sangji, Hussain, Luijten, Erik, and Stupp, Samuel I. Reversible self-assembly of superstructured networks. United States: N. p., 2018. Web. doi:10.1126/science.aat6141.
Freeman, Ronit, Han, Ming, Álvarez, Zaida, Lewis, Jacob A., Wester, James R., Stephanopoulos, Nicholas, McClendon, Mark T., Lynsky, Cheyenne, Godbe, Jacqueline M., Sangji, Hussain, Luijten, Erik, & Stupp, Samuel I. Reversible self-assembly of superstructured networks. United States. doi:10.1126/science.aat6141.
Freeman, Ronit, Han, Ming, Álvarez, Zaida, Lewis, Jacob A., Wester, James R., Stephanopoulos, Nicholas, McClendon, Mark T., Lynsky, Cheyenne, Godbe, Jacqueline M., Sangji, Hussain, Luijten, Erik, and Stupp, Samuel I. Thu . "Reversible self-assembly of superstructured networks". United States. doi:10.1126/science.aat6141.
@article{osti_1566718,
title = {Reversible self-assembly of superstructured networks},
author = {Freeman, Ronit and Han, Ming and Álvarez, Zaida and Lewis, Jacob A. and Wester, James R. and Stephanopoulos, Nicholas and McClendon, Mark T. and Lynsky, Cheyenne and Godbe, Jacqueline M. and Sangji, Hussain and Luijten, Erik and Stupp, Samuel I.},
abstractNote = {Soft structures in nature, such as protein assemblies, can organize reversibly into functional and often hierarchical architectures through noncovalent interactions. Molecularly encoding this dynamic capability in synthetic materials has remained an elusive goal. We report on hydrogels of peptide-DNA conjugates and peptides that organize into superstructures of intertwined filaments that disassemble upon the addition of molecules or changes in charge density. Experiments and simulations demonstrate that this response requires large-scale spatial redistribution of molecules directed by strong noncovalent interactions among them. Simulations also suggest that the chemically reversible structures can only occur within a limited range of supramolecular cohesive energies. Storage moduli of the hydrogels change reversibly as superstructures form and disappear, as does the phenotype of neural cells in contact with these materials.},
doi = {10.1126/science.aat6141},
journal = {Science},
issn = {0036-8075},
number = 6416,
volume = 362,
place = {United States},
year = {2018},
month = {10}
}

Works referenced in this record:

Self-Assembly at All Scales
journal, March 2002

  • Whitesides, George M.; Grzybowski, Bartosz
  • Science, Vol. 295, Issue 5564, p. 2418-2421
  • DOI: 10.1126/science.1070821

Self-Assembly of Large and Small Molecules into Hierarchically Ordered Sacs and Membranes
journal, March 2008

  • Capito, R. M.; Azevedo, H. S.; Velichko, Y. S.
  • Science, Vol. 319, Issue 5871, p. 1812-1816
  • DOI: 10.1126/science.1154586