Controlling the structure and length of self-synthesizing supramolecular polymers through nucleated growth and disassembly

A. Pal, M. Malakoutikhah, G. Leonetti, M. Tezcan, M. Colomb-Delsuc, V.D. Nguyen, J. van der Gucht, S. Otto

Research output: Contribution to journalArticleAcademicpeer-review

75 Citations (Scopus)

Abstract

Directing self-assembly processes out-of-equilibrium to yield kinetically trapped materials with well-defined dimensions remains a considerable challenge. Kinetically controlled assembly of self-synthesizing peptide-functionalized macrocycles through a nucleation–growth mechanism is reported. Spontaneous fiber formation in this system is effectively shut down as most of the material is diverted into metastable non-assembling trimeric and tetrameric macrocycles. However, upon adding seeds to this mixture, well-defined fibers with controllable lengths and narrow polydispersities are obtained. This seeded growth strategy also allows access to supramolecular triblock copolymers. The resulting noncovalent assemblies can be further stabilized through covalent capture. Taken together, these results show that self-synthesizing materials, through their interplay between dynamic covalent bonds and noncovalent interactions, are uniquely suited for out-of-equilibrium self-assembly.
Original languageEnglish
Pages (from-to)7852-7856
JournalAngewandte Chemie-International Edition
Volume54
Issue number27
DOIs
Publication statusPublished - 2015

Fingerprint

Polymers
Self assembly
Covalent bonds
Fibers
Polydispersity
Peptides
Block copolymers
Seed

Keywords

  • dynamic combinatorial libraries
  • systems chemistry
  • co-micelles
  • polymerization
  • replication
  • driven
  • complexity
  • mechanism
  • selection

Cite this

Pal, A. ; Malakoutikhah, M. ; Leonetti, G. ; Tezcan, M. ; Colomb-Delsuc, M. ; Nguyen, V.D. ; van der Gucht, J. ; Otto, S. / Controlling the structure and length of self-synthesizing supramolecular polymers through nucleated growth and disassembly. In: Angewandte Chemie-International Edition. 2015 ; Vol. 54, No. 27. pp. 7852-7856.
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abstract = "Directing self-assembly processes out-of-equilibrium to yield kinetically trapped materials with well-defined dimensions remains a considerable challenge. Kinetically controlled assembly of self-synthesizing peptide-functionalized macrocycles through a nucleation–growth mechanism is reported. Spontaneous fiber formation in this system is effectively shut down as most of the material is diverted into metastable non-assembling trimeric and tetrameric macrocycles. However, upon adding seeds to this mixture, well-defined fibers with controllable lengths and narrow polydispersities are obtained. This seeded growth strategy also allows access to supramolecular triblock copolymers. The resulting noncovalent assemblies can be further stabilized through covalent capture. Taken together, these results show that self-synthesizing materials, through their interplay between dynamic covalent bonds and noncovalent interactions, are uniquely suited for out-of-equilibrium self-assembly.",
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Controlling the structure and length of self-synthesizing supramolecular polymers through nucleated growth and disassembly. / Pal, A.; Malakoutikhah, M.; Leonetti, G.; Tezcan, M.; Colomb-Delsuc, M.; Nguyen, V.D.; van der Gucht, J.; Otto, S.

In: Angewandte Chemie-International Edition, Vol. 54, No. 27, 2015, p. 7852-7856.

Research output: Contribution to journalArticleAcademicpeer-review

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AU - Pal, A.

AU - Malakoutikhah, M.

AU - Leonetti, G.

AU - Tezcan, M.

AU - Colomb-Delsuc, M.

AU - Nguyen, V.D.

AU - van der Gucht, J.

AU - Otto, S.

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AB - Directing self-assembly processes out-of-equilibrium to yield kinetically trapped materials with well-defined dimensions remains a considerable challenge. Kinetically controlled assembly of self-synthesizing peptide-functionalized macrocycles through a nucleation–growth mechanism is reported. Spontaneous fiber formation in this system is effectively shut down as most of the material is diverted into metastable non-assembling trimeric and tetrameric macrocycles. However, upon adding seeds to this mixture, well-defined fibers with controllable lengths and narrow polydispersities are obtained. This seeded growth strategy also allows access to supramolecular triblock copolymers. The resulting noncovalent assemblies can be further stabilized through covalent capture. Taken together, these results show that self-synthesizing materials, through their interplay between dynamic covalent bonds and noncovalent interactions, are uniquely suited for out-of-equilibrium self-assembly.

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KW - co-micelles

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KW - replication

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