Mimicking active biopolymer networks with a synthetic hydrogel

Marcos Fernández-Castano Romera, Robert Göstl, Huda Shaikh, Gijs ter Huurne, Jurgen Schill, Ilja K. Voets, Cornelis Storm, Rint P. Sijbesma (Corresponding author)

Research output: Contribution to journalArticleAcademicpeer-review

1 Citation (Scopus)

Abstract

Stiffening due to internal stress generation is of paramount importance in living systems and is the foundation for many biomechanical processes. For example, cells stiffen their surrounding matrix by pulling on collagen and fibrin fibers. At the subcellular level, molecular motors prompt fluidization and actively stiffen the cytoskeleton by sliding polar actin filaments in opposite directions. Here, we demonstrate that chemical cross-linking of a fibrous matrix of synthetic semiflexible polymers with thermoresponsive poly(N-isopropylacrylamide) (PNIPAM) produces internal stress by induction of a coil-to-globule transition upon crossing the lower critical solution temperature of PNIPAM, resulting in a macroscopic stiffening response that spans more than 3 orders of magnitude in modulus. The forces generated through collapsing PNIPAM are sufficient to drive a fluid material into a stiff gel within a few seconds. Moreover, rigidified networks dramatically stiffen in response to applied shear stress featuring power law rheology with exponents that match those of reconstituted collagen and actomyosin networks prestressed by molecular motors. This concept holds potential for the rational design of synthetic materials that are fluid at room temperature and rapidly rigidify at body temperature to form hydrogels mechanically and structurally akin to cells and tissues.

LanguageEnglish
Pages1989-1997
Number of pages9
JournalJournal of the American Chemical Society
Volume141
Issue number5
DOIs
StatePublished - 6 Feb 2019

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Biopolymers
Hydrogel
Hydrogels
Collagen
Residual stresses
Actomyosin
Temperature
Fluids
Rheology
Fluidization
Fibrin
Body Temperature
Cytoskeleton
Actin Cytoskeleton
Actins
Shear stress
Polymers
Gels
Tissue
Fibers

Cite this

Fernández-Castano Romera, M., Göstl, R., Shaikh, H., ter Huurne, G., Schill, J., Voets, I. K., ... Sijbesma, R. P. (2019). Mimicking active biopolymer networks with a synthetic hydrogel. Journal of the American Chemical Society, 141(5), 1989-1997. DOI: 10.1021/jacs.8b10659
Fernández-Castano Romera, Marcos ; Göstl, Robert ; Shaikh, Huda ; ter Huurne, Gijs ; Schill, Jurgen ; Voets, Ilja K. ; Storm, Cornelis ; Sijbesma, Rint P./ Mimicking active biopolymer networks with a synthetic hydrogel. In: Journal of the American Chemical Society. 2019 ; Vol. 141, No. 5. pp. 1989-1997
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Fernández-Castano Romera, M, Göstl, R, Shaikh, H, ter Huurne, G, Schill, J, Voets, IK, Storm, C & Sijbesma, RP 2019, 'Mimicking active biopolymer networks with a synthetic hydrogel' Journal of the American Chemical Society, vol. 141, no. 5, pp. 1989-1997. DOI: 10.1021/jacs.8b10659

Mimicking active biopolymer networks with a synthetic hydrogel. / Fernández-Castano Romera, Marcos; Göstl, Robert; Shaikh, Huda; ter Huurne, Gijs; Schill, Jurgen; Voets, Ilja K.; Storm, Cornelis; Sijbesma, Rint P. (Corresponding author).

In: Journal of the American Chemical Society, Vol. 141, No. 5, 06.02.2019, p. 1989-1997.

Research output: Contribution to journalArticleAcademicpeer-review

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Fernández-Castano Romera M, Göstl R, Shaikh H, ter Huurne G, Schill J, Voets IK et al. Mimicking active biopolymer networks with a synthetic hydrogel. Journal of the American Chemical Society. 2019 Feb 6;141(5):1989-1997. Available from, DOI: 10.1021/jacs.8b10659