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Covalent poly(2‐isopropenyl‐2‐oxazoline) hydrogels with ultrahigh mechanical strength and toughness through secondary terpyridine metal‐coordination crosslinks

Xiaowen Xu (UGent) , Adriana Jerca (UGent) , Valentin-Victor Jerca (UGent) and Richard Hoogenboom (UGent)
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Abstract
The present study reports the synthesis of poly(2-isopropenyl-2-oxazoline) (PiPOx) dual-crosslinked hydrogels by both covalent and physical (i.e., metal-ligand coordination) interactions. First, chemical crosslinking of a modified PiPOx polymer containing terpyridine (TPy) unit is achieved by reacting with azelaic acid (non-anedioic acid). Transient crosslinks are subsequently introduced by complexation of the TPy units with different divalent transition metal ions. This strategy provides access to hydrogels with superior mechanical properties compared to the pure covalently crosslinked PiPOx hydrogels. The mechanical properties and water uptake of the hydrogels could be easily controlled by swelling in different aqueous metal ion solutions. PiPOx hydrogels swollen in Zn2+ solution are found to possess ultrahigh compression strength (9 MPa), remarkable toughness (99 MJ m(-3)) and outstanding self-recoverability (98% toughness recovery after swelling for 60 min without external stimuli), which are among the highest reported in literature to date. These remarkable properties are assigned to the thermodynamically stable, but kinetically labile Zn2+-TPy complexes that produce a dynamic network with fewer imperfections and better adaptive properties under mechanical stress compared to those with other metal ions.
Keywords
hydrogel, metal-ligand coordination, poly(2-isopropenyl-2-oxazoline), supramolecular chemistry, terpyridine, SUPRAMOLECULAR CHEMISTRY, POLYMER, RELAXATION, KINETICS, BRUSHES, GEL

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MLA
Xu, Xiaowen, et al. “Covalent Poly(2‐isopropenyl‐2‐oxazoline) Hydrogels with Ultrahigh Mechanical Strength and Toughness through Secondary Terpyridine Metal‐coordination Crosslinks.” ADVANCED FUNCTIONAL MATERIALS, vol. 29, no. 48, 2019.
APA
Xu, X., Jerca, A., Jerca, V.-V., & Hoogenboom, R. (2019). Covalent poly(2‐isopropenyl‐2‐oxazoline) hydrogels with ultrahigh mechanical strength and toughness through secondary terpyridine metal‐coordination crosslinks. ADVANCED FUNCTIONAL MATERIALS, 29(48).
Chicago author-date
Xu, Xiaowen, Adriana Jerca, Valentin-Victor Jerca, and Richard Hoogenboom. 2019. “Covalent Poly(2‐isopropenyl‐2‐oxazoline) Hydrogels with Ultrahigh Mechanical Strength and Toughness through Secondary Terpyridine Metal‐coordination Crosslinks.” ADVANCED FUNCTIONAL MATERIALS 29 (48).
Chicago author-date (all authors)
Xu, Xiaowen, Adriana Jerca, Valentin-Victor Jerca, and Richard Hoogenboom. 2019. “Covalent Poly(2‐isopropenyl‐2‐oxazoline) Hydrogels with Ultrahigh Mechanical Strength and Toughness through Secondary Terpyridine Metal‐coordination Crosslinks.” ADVANCED FUNCTIONAL MATERIALS 29 (48).
Vancouver
1.
Xu X, Jerca A, Jerca V-V, Hoogenboom R. Covalent poly(2‐isopropenyl‐2‐oxazoline) hydrogels with ultrahigh mechanical strength and toughness through secondary terpyridine metal‐coordination crosslinks. ADVANCED FUNCTIONAL MATERIALS. 2019;29(48).
IEEE
[1]
X. Xu, A. Jerca, V.-V. Jerca, and R. Hoogenboom, “Covalent poly(2‐isopropenyl‐2‐oxazoline) hydrogels with ultrahigh mechanical strength and toughness through secondary terpyridine metal‐coordination crosslinks,” ADVANCED FUNCTIONAL MATERIALS, vol. 29, no. 48, 2019.
@article{8634804,
  abstract     = {The present study reports the synthesis of poly(2-isopropenyl-2-oxazoline) (PiPOx) dual-crosslinked hydrogels by both covalent and physical (i.e., metal-ligand coordination) interactions. First, chemical crosslinking of a modified PiPOx polymer containing terpyridine (TPy) unit is achieved by reacting with azelaic acid (non-anedioic acid). Transient crosslinks are subsequently introduced by complexation of the TPy units with different divalent transition metal ions. This strategy provides access to hydrogels with superior mechanical properties compared to the pure covalently crosslinked PiPOx hydrogels. The mechanical properties and water uptake of the hydrogels could be easily controlled by swelling in different aqueous metal ion solutions. PiPOx hydrogels swollen in Zn2+ solution are found to possess ultrahigh compression strength (9 MPa), remarkable toughness (99 MJ m(-3)) and outstanding self-recoverability (98% toughness recovery after swelling for 60 min without external stimuli), which are among the highest reported in literature to date. These remarkable properties are assigned to the thermodynamically stable, but kinetically labile Zn2+-TPy complexes that produce a dynamic network with fewer imperfections and better adaptive properties under mechanical stress compared to those with other metal ions.},
  articleno    = {1904886},
  author       = {Xu, Xiaowen and Jerca, Adriana and Jerca, Valentin-Victor and Hoogenboom, Richard},
  issn         = {1616-301X},
  journal      = {ADVANCED FUNCTIONAL MATERIALS},
  keywords     = {hydrogel,metal-ligand coordination,poly(2-isopropenyl-2-oxazoline),supramolecular chemistry,terpyridine,SUPRAMOLECULAR CHEMISTRY,POLYMER,RELAXATION,KINETICS,BRUSHES,GEL},
  language     = {eng},
  number       = {48},
  pages        = {10},
  title        = {Covalent poly(2‐isopropenyl‐2‐oxazoline) hydrogels with ultrahigh mechanical strength and toughness through secondary terpyridine metal‐coordination crosslinks},
  url          = {http://dx.doi.org/10.1002/adfm.201904886},
  volume       = {29},
  year         = {2019},
}

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