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Force-induced activation of covalent bonds in mechanoresponsive polymeric materials

Force-induced activation of covalent bonds in mechanoresponsive polymeric materials
Force-induced activation of covalent bonds in mechanoresponsive polymeric materials

Mechanochemical transduction enables an extraordinary range of physiological processes such as the sense of touch, hearing, balance, muscle contraction, and the growth and remodelling of tissue and bone. Although biology is replete with materials systems that actively and functionally respond to mechanical stimuli, the default mechanochemical reaction of bulk polymers to large external stress is the unselective scission of covalent bonds, resulting in damage or failure. An alternative to this degradation process is the rational molecular design of synthetic materials such that mechanical stress favourably alters material properties. A few mechanosensitive polymers with this property have been developed; but their active response is mediated through non-covalent processes, which may limit the extent to which properties can be modified and the long-term stability in structural materials. Previously, we have shown with dissolved polymer strands incorporating mechanically sensitive chemical groupsso-called mechanophoresthat the directional nature of mechanical forces can selectively break and re-form covalent bonds. We now demonstrate that such force-induced covalent-bond activation can also be realized with mechanophore-linked elastomeric and glassy polymers, by using a mechanophore that changes colour as it undergoes a reversible electrocyclic ring-opening reaction under tensile stress and thus allows us to directly and locally visualize the mechanochemical reaction. We find that pronounced changes in colour and fluorescence emerge with the accumulation of plastic deformation, indicating that in these polymeric materials the transduction of mechanical force into the ring-opening reaction is an activated process. We anticipate that force activation of covalent bonds can serve as a general strategy for the development of new mechanophore building blocks that impart polymeric materials with desirable functionalities ranging from damage sensing to fully regenerative self-healing.

0028-0836
68-72
Davis, Douglas A.
fa13a24b-016f-4b97-9593-31ac9c8a5920
Hamilton, Andrew
9088cf01-8d7f-45f0-af56-b4784227447c
Yang, Jinglei
f3db7f2b-2bf0-453f-bb23-287e95c188ba
Cremar, Lee D.
131f7468-c410-4463-a6d3-be68e3c0317a
Van Gough, Dara
fca28bfe-a021-4e7e-867e-b554f308748c
Potisek, Stephanie L.
21f1629b-e33f-410e-bd17-140b87bafb8f
Ong, Mitchell T.
e596001d-e869-49d5-a3df-b92a6cb68f24
Braun, Paul V.
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Martínez, Todd J.
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White, Scott R.
bcdc6d47-824d-4014-a8e2-58b48cdc8c99
Moore, Jeffrey S.
94c9d588-754e-48d2-9dcb-b63e9511e32d
Sottos, Nancy R.
a329a43c-958b-46fa-9a2c-cb53cd7e4d12
Davis, Douglas A.
fa13a24b-016f-4b97-9593-31ac9c8a5920
Hamilton, Andrew
9088cf01-8d7f-45f0-af56-b4784227447c
Yang, Jinglei
f3db7f2b-2bf0-453f-bb23-287e95c188ba
Cremar, Lee D.
131f7468-c410-4463-a6d3-be68e3c0317a
Van Gough, Dara
fca28bfe-a021-4e7e-867e-b554f308748c
Potisek, Stephanie L.
21f1629b-e33f-410e-bd17-140b87bafb8f
Ong, Mitchell T.
e596001d-e869-49d5-a3df-b92a6cb68f24
Braun, Paul V.
12c73f53-cb8c-4578-933d-75fc29e10b91
Martínez, Todd J.
7e31134f-f0a8-491c-bd4a-5238b2c3cabb
White, Scott R.
bcdc6d47-824d-4014-a8e2-58b48cdc8c99
Moore, Jeffrey S.
94c9d588-754e-48d2-9dcb-b63e9511e32d
Sottos, Nancy R.
a329a43c-958b-46fa-9a2c-cb53cd7e4d12

Davis, Douglas A., Hamilton, Andrew, Yang, Jinglei, Cremar, Lee D., Van Gough, Dara, Potisek, Stephanie L., Ong, Mitchell T., Braun, Paul V., Martínez, Todd J., White, Scott R., Moore, Jeffrey S. and Sottos, Nancy R. (2009) Force-induced activation of covalent bonds in mechanoresponsive polymeric materials. Nature, 459 (7243), 68-72. (doi:10.1038/nature07970).

Record type: Letter

Abstract

Mechanochemical transduction enables an extraordinary range of physiological processes such as the sense of touch, hearing, balance, muscle contraction, and the growth and remodelling of tissue and bone. Although biology is replete with materials systems that actively and functionally respond to mechanical stimuli, the default mechanochemical reaction of bulk polymers to large external stress is the unselective scission of covalent bonds, resulting in damage or failure. An alternative to this degradation process is the rational molecular design of synthetic materials such that mechanical stress favourably alters material properties. A few mechanosensitive polymers with this property have been developed; but their active response is mediated through non-covalent processes, which may limit the extent to which properties can be modified and the long-term stability in structural materials. Previously, we have shown with dissolved polymer strands incorporating mechanically sensitive chemical groupsso-called mechanophoresthat the directional nature of mechanical forces can selectively break and re-form covalent bonds. We now demonstrate that such force-induced covalent-bond activation can also be realized with mechanophore-linked elastomeric and glassy polymers, by using a mechanophore that changes colour as it undergoes a reversible electrocyclic ring-opening reaction under tensile stress and thus allows us to directly and locally visualize the mechanochemical reaction. We find that pronounced changes in colour and fluorescence emerge with the accumulation of plastic deformation, indicating that in these polymeric materials the transduction of mechanical force into the ring-opening reaction is an activated process. We anticipate that force activation of covalent bonds can serve as a general strategy for the development of new mechanophore building blocks that impart polymeric materials with desirable functionalities ranging from damage sensing to fully regenerative self-healing.

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More information

Accepted/In Press date: 5 March 2009
Published date: 7 May 2009

Identifiers

Local EPrints ID: 413274
URI: https://eprints.soton.ac.uk/id/eprint/413274
ISSN: 0028-0836
PURE UUID: b3f05a3a-1c19-49cb-bb53-1c61e2c41256
ORCID for Andrew Hamilton: ORCID iD orcid.org/0000-0003-4627-849X

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Date deposited: 18 Aug 2017 16:31
Last modified: 20 Jul 2019 00:26

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Contributors

Author: Douglas A. Davis
Author: Andrew Hamilton ORCID iD
Author: Jinglei Yang
Author: Lee D. Cremar
Author: Dara Van Gough
Author: Stephanie L. Potisek
Author: Mitchell T. Ong
Author: Paul V. Braun
Author: Todd J. Martínez
Author: Scott R. White
Author: Jeffrey S. Moore
Author: Nancy R. Sottos

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