Responsive biomimetic networks from polyisocyanopeptide hydrogels
Thermal transitions of polyisocyanide single molecules to polymer bundles and finally networks lead to hydrogels mimicking the properties of biopolymer intermediate-filament networks; their analysis shows that bundling and chain stiffness are crucial design parameters for hydrogels. Biomimetic polym...
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| Published in: | Nature (London) Vol. 493; no. 7434; pp. 651 - 655 |
|---|---|
| Main Authors: | , , , , , , , , , , , , , |
| Format: | Journal Article |
| Language: | English |
| Published: |
London
Nature Publishing Group UK
31.01.2013
Nature Publishing Group |
| Subjects: | |
| ISSN: | 0028-0836, 1476-4687, 1476-4687 |
| Online Access: | Get full text |
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| Abstract | Thermal transitions of polyisocyanide single molecules to polymer bundles and finally networks lead to hydrogels mimicking the properties of biopolymer intermediate-filament networks; their analysis shows that bundling and chain stiffness are crucial design parameters for hydrogels.
Biomimetic polymer networks
This paper describes a new class of water-soluble, relatively stiff polymers that bundle in a controlled manner on heating to produce very stiff fibres. These fibres, in turn, form hydrogels that very closely mimic components of the cell cytoskeleton, intermediate filaments. Synthesis involves the thermal transition of polyisocyanide polymers from single molecules to bundles of polymer chains. Networks made with this material demonstrate a stress-stiffening behaviour that is usually absent in synthetic polymer gels, and their mechanical properties can be modified by altering the chemical structure of the polymer, offering greater versatility than biopolymer networks.
Mechanical responsiveness is essential to all biological systems down to the level of tissues and cells
1
,
2
. The intra- and extracellular mechanics of such systems are governed by a series of proteins, such as microtubules, actin, intermediate filaments and collagen
3
,
4
. As a general design motif, these proteins self-assemble into helical structures and superstructures that differ in diameter and persistence length to cover the full mechanical spectrum
1
. Gels of cytoskeletal proteins display particular mechanical responses (stress stiffening) that until now have been absent in synthetic polymeric and low-molar-mass gels. Here we present synthetic gels that mimic in nearly all aspects gels prepared from intermediate filaments. They are prepared from polyisocyanopeptides
5
,
6
,
7
grafted with oligo(ethylene glycol) side chains. These responsive polymers possess a stiff and helical architecture, and show a tunable thermal transition where the chains bundle together to generate transparent gels at extremely low concentrations. Using characterization techniques operating at different length scales (for example, macroscopic rheology, atomic force microscopy and molecular force spectroscopy) combined with an appropriate theoretical network model
8
,
9
,
10
, we establish the hierarchical relationship between the bulk mechanical properties and the single-molecule parameters. Our results show that to develop artificial cytoskeletal or extracellular matrix mimics, the essential design parameters are not only the molecular stiffness, but also the extent of bundling. In contrast to the peptidic materials, our polyisocyanide polymers are readily modified, giving a starting point for functional biomimetic hydrogels with potentially a wide variety of applications
11
,
12
,
13
,
14
, in particular in the biomedical field. |
|---|---|
| AbstractList | Mechanical responsiveness is essential to all biological systems down to the level of tissues and cells1,2. The intra- and extracellular mechanics of such systems are governed by a series of proteins, such as microtubules, actin, intermediate filaments and collagen3,4. As a general design motif, these proteins self-assemble into helical structures and superstructures that differ in diameter and persistence length to cover the full mechanical spectrum1. Gels of cytoskeletal proteins display particular mechanical responses (stress stiffening) that until now have been absent in synthetic polymeric and low-molar-mass gels. Here we present synthetic gels that mimic in nearly all aspects gels prepared from intermediate filaments. They are prepared from polyisocyanopeptides5-7 grafted with oligo(ethylene glycol) side chains. These responsive polymers possess a stiffand helical architecture, and show a tunable thermal transition where the chains bundle together to generate transparent gels at extremely low concentrations. Using characterization techniques operating at different length scales (for example, macroscopic rheology, atomic force microscopy and molecular force spectroscopy) combined with an appropriate theoretical network model8-10, we establish the hierarchical relationship between the bulk mechanical properties and the single-molecule parameters. Our results show that to develop artificial cytoskeletal or extracellular matrix mimics, the essential design parameters are not only the molecular stiffness, but also the extent of bundling. In contrast to the peptidic materials, our polyisocyanide polymers are readily modified, giving a starting point for functional biomimetic hydrogels with potentially a wide variety of applications11-14, in particular in the biomedical field. [PUBLICATION ABSTRACT] Thermal transitions of polyisocyanide single molecules to polymer bundles and finally networks lead to hydrogels mimicking the properties of biopolymer intermediate-filament networks; their analysis shows that bundling and chain stiffness are crucial design parameters for hydrogels. Mechanical responsiveness is essential to all biological systems down to the level of tissues and cells. The intra- and extracellular mechanics of such systems are governed by a series of proteins, such as microtubules, actin, intermediate filaments and collagen. As a general design motif, these proteins self-assemble into helical structures and superstructures that differ in diameter and persistence length to cover the full mechanical spectrum. Gels of cytoskeletal proteins display particular mechanical responses (stress stiffening) that until now have been absent in synthetic polymeric and low-molar-mass gels. Here we present synthetic gels that mimic in nearly all aspects gels prepared from intermediate filaments. They are prepared from polyisocyanopeptides grafted with oligo(ethylene glycol) side chains. These responsive polymers possess a stiff and helical architecture, and show a tunable thermal transition where the chains bundle together to generate transparent gels at extremely low concentrations. Using characterization techniques operating at different length scales (for example, macroscopic rheology, atomic force microscopy and molecular force spectroscopy) combined with an appropriate theoretical network model, we establish the hierarchical relationship between the bulk mechanical properties and the single-molecule parameters. Our results show that to develop artificial cytoskeletal or extracellular matrix mimics, the essential design parameters are not only the molecular stiffness, but also the extent of bundling. In contrast to the peptidic materials, our polyisocyanide polymers are readily modified, giving a starting point for functional biomimetic hydrogels with potentially a wide variety of applications, in particular in the biomedical field. Mechanical responsiveness is essential to all biological systems down to the level of tissues and cells. The intra- and extracellular mechanics of such systems are governed by a series of proteins, such as microtubules, actin, intermediate filaments and collagen. As a general design motif, these proteins self-assemble into helical structures and superstructures that differ in diameter and persistence length to cover the full mechanical spectrum. Gels of cytoskeletal proteins display particular mechanical responses (stress stiffening) that until now have been absent in synthetic polymeric and low-molar-mass gels. Here we present synthetic gels that mimic in nearly all aspects gels prepared from intermediate filaments. They are prepared from polyisocyanopeptides grafted with oligo(ethylene glycol) side chains. These responsive polymers possess a stiff and helical architecture, and show a tunable thermal transition where the chains bundle together to generate transparent gels at extremely low concentrations. Using characterization techniques operating at different length scales (for example, macroscopic rheology, atomic force microscopy and molecular force spectroscopy) combined with an appropriate theoretical network model, we establish the hierarchical relationship between the bulk mechanical properties and the single-molecule parameters. Our results show that to develop artificial cytoskeletal or extracellular matrix mimics, the essential design parameters are not only the molecular stiffness, but also the extent of bundling. In contrast to the peptidic materials, our polyisocyanide polymers are readily modified, giving a starting point for functional biomimetic hydrogels with potentially a wide variety of applications, in particular in the biomedical field.Mechanical responsiveness is essential to all biological systems down to the level of tissues and cells. The intra- and extracellular mechanics of such systems are governed by a series of proteins, such as microtubules, actin, intermediate filaments and collagen. As a general design motif, these proteins self-assemble into helical structures and superstructures that differ in diameter and persistence length to cover the full mechanical spectrum. Gels of cytoskeletal proteins display particular mechanical responses (stress stiffening) that until now have been absent in synthetic polymeric and low-molar-mass gels. Here we present synthetic gels that mimic in nearly all aspects gels prepared from intermediate filaments. They are prepared from polyisocyanopeptides grafted with oligo(ethylene glycol) side chains. These responsive polymers possess a stiff and helical architecture, and show a tunable thermal transition where the chains bundle together to generate transparent gels at extremely low concentrations. Using characterization techniques operating at different length scales (for example, macroscopic rheology, atomic force microscopy and molecular force spectroscopy) combined with an appropriate theoretical network model, we establish the hierarchical relationship between the bulk mechanical properties and the single-molecule parameters. Our results show that to develop artificial cytoskeletal or extracellular matrix mimics, the essential design parameters are not only the molecular stiffness, but also the extent of bundling. In contrast to the peptidic materials, our polyisocyanide polymers are readily modified, giving a starting point for functional biomimetic hydrogels with potentially a wide variety of applications, in particular in the biomedical field. Thermal transitions of polyisocyanide single molecules to polymer bundles and finally networks lead to hydrogels mimicking the properties of biopolymer intermediate-filament networks; their analysis shows that bundling and chain stiffness are crucial design parameters for hydrogels. Biomimetic polymer networks This paper describes a new class of water-soluble, relatively stiff polymers that bundle in a controlled manner on heating to produce very stiff fibres. These fibres, in turn, form hydrogels that very closely mimic components of the cell cytoskeleton, intermediate filaments. Synthesis involves the thermal transition of polyisocyanide polymers from single molecules to bundles of polymer chains. Networks made with this material demonstrate a stress-stiffening behaviour that is usually absent in synthetic polymer gels, and their mechanical properties can be modified by altering the chemical structure of the polymer, offering greater versatility than biopolymer networks. Mechanical responsiveness is essential to all biological systems down to the level of tissues and cells 1 , 2 . The intra- and extracellular mechanics of such systems are governed by a series of proteins, such as microtubules, actin, intermediate filaments and collagen 3 , 4 . As a general design motif, these proteins self-assemble into helical structures and superstructures that differ in diameter and persistence length to cover the full mechanical spectrum 1 . Gels of cytoskeletal proteins display particular mechanical responses (stress stiffening) that until now have been absent in synthetic polymeric and low-molar-mass gels. Here we present synthetic gels that mimic in nearly all aspects gels prepared from intermediate filaments. They are prepared from polyisocyanopeptides 5 , 6 , 7 grafted with oligo(ethylene glycol) side chains. These responsive polymers possess a stiff and helical architecture, and show a tunable thermal transition where the chains bundle together to generate transparent gels at extremely low concentrations. Using characterization techniques operating at different length scales (for example, macroscopic rheology, atomic force microscopy and molecular force spectroscopy) combined with an appropriate theoretical network model 8 , 9 , 10 , we establish the hierarchical relationship between the bulk mechanical properties and the single-molecule parameters. Our results show that to develop artificial cytoskeletal or extracellular matrix mimics, the essential design parameters are not only the molecular stiffness, but also the extent of bundling. In contrast to the peptidic materials, our polyisocyanide polymers are readily modified, giving a starting point for functional biomimetic hydrogels with potentially a wide variety of applications 11 , 12 , 13 , 14 , in particular in the biomedical field. |
| Audience | Academic |
| Author | Mendes, Eduardo Rowan, Alan E. Nolte, Roeland J. M. Hoogenboom, Richard Schwartz, Erik Picken, Stephen J. Kouwer, Paul H. J. Koepf, Matthieu van Buul, Arend M. Le Sage, Vincent A. A. Eksteen-Akeroyd, Zaskia H. Jaspers, Maarten Woltinge, Tim Kitto, Heather J. |
| Author_xml | – sequence: 1 givenname: Paul H. J. surname: Kouwer fullname: Kouwer, Paul H. J. email: p.kouwer@science.ru.nl organization: Department of Molecular Materials, Radboud University Nijmegen, Institute for Molecules and Materials, Heyendaalseweg 135, 6525 AJ Nijmegen, The Netherlands – sequence: 2 givenname: Matthieu surname: Koepf fullname: Koepf, Matthieu organization: Department of Molecular Materials, Radboud University Nijmegen, Institute for Molecules and Materials, Heyendaalseweg 135, 6525 AJ Nijmegen, The Netherlands – sequence: 3 givenname: Vincent A. A. surname: Le Sage fullname: Le Sage, Vincent A. A. organization: Department of Molecular Materials, Radboud University Nijmegen, Institute for Molecules and Materials, Heyendaalseweg 135, 6525 AJ Nijmegen, The Netherlands – sequence: 4 givenname: Maarten surname: Jaspers fullname: Jaspers, Maarten organization: Department of Molecular Materials, Radboud University Nijmegen, Institute for Molecules and Materials, Heyendaalseweg 135, 6525 AJ Nijmegen, The Netherlands – sequence: 5 givenname: Arend M. surname: van Buul fullname: van Buul, Arend M. organization: Department of Molecular Materials, Radboud University Nijmegen, Institute for Molecules and Materials, Heyendaalseweg 135, 6525 AJ Nijmegen, The Netherlands – sequence: 6 givenname: Zaskia H. surname: Eksteen-Akeroyd fullname: Eksteen-Akeroyd, Zaskia H. organization: Department of Molecular Materials, Radboud University Nijmegen, Institute for Molecules and Materials, Heyendaalseweg 135, 6525 AJ Nijmegen, The Netherlands – sequence: 7 givenname: Tim surname: Woltinge fullname: Woltinge, Tim organization: Department of Molecular Materials, Radboud University Nijmegen, Institute for Molecules and Materials, Heyendaalseweg 135, 6525 AJ Nijmegen, The Netherlands – sequence: 8 givenname: Erik surname: Schwartz fullname: Schwartz, Erik organization: Department of Molecular Materials, Radboud University Nijmegen, Institute for Molecules and Materials, Heyendaalseweg 135, 6525 AJ Nijmegen, The Netherlands – sequence: 9 givenname: Heather J. surname: Kitto fullname: Kitto, Heather J. organization: Department of Molecular Materials, Radboud University Nijmegen, Institute for Molecules and Materials, Heyendaalseweg 135, 6525 AJ Nijmegen, The Netherlands – sequence: 10 givenname: Richard surname: Hoogenboom fullname: Hoogenboom, Richard organization: Department of Molecular Materials, Radboud University Nijmegen, Institute for Molecules and Materials, Heyendaalseweg 135, 6525 AJ Nijmegen, The Netherlands, Present address: Supramolecular Chemistry Group, Department of Organic Chemistry, Ghent University, Krijgslaan 281-S4, 9000 Ghent, Belgium – sequence: 11 givenname: Stephen J. surname: Picken fullname: Picken, Stephen J. organization: Department of NanoStructured Materials, Delft University of Technology, Julianalaan 136, 2628 BL Delft, The Netherlands – sequence: 12 givenname: Roeland J. M. surname: Nolte fullname: Nolte, Roeland J. M. organization: Department of Molecular Materials, Radboud University Nijmegen, Institute for Molecules and Materials, Heyendaalseweg 135, 6525 AJ Nijmegen, The Netherlands – sequence: 13 givenname: Eduardo surname: Mendes fullname: Mendes, Eduardo organization: Department of NanoStructured Materials, Delft University of Technology, Julianalaan 136, 2628 BL Delft, The Netherlands – sequence: 14 givenname: Alan E. surname: Rowan fullname: Rowan, Alan E. email: a.rowan@science.ru.nl organization: Department of Molecular Materials, Radboud University Nijmegen, Institute for Molecules and Materials, Heyendaalseweg 135, 6525 AJ Nijmegen, The Netherlands |
| BackLink | http://pascal-francis.inist.fr/vibad/index.php?action=getRecordDetail&idt=26901941$$DView record in Pascal Francis https://www.ncbi.nlm.nih.gov/pubmed/23354048$$D View this record in MEDLINE/PubMed |
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| Snippet | Thermal transitions of polyisocyanide single molecules to polymer bundles and finally networks lead to hydrogels mimicking the properties of biopolymer... Mechanical responsiveness is essential to all biological systems down to the level of tissues and cells. The intra- and extracellular mechanics of such systems... Mechanical responsiveness is essential to all biological systems down to the level of tissues and cells1,2. The intra- and extracellular mechanics of such... |
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| Title | Responsive biomimetic networks from polyisocyanopeptide hydrogels |
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