TY - JOUR
T1 - Structure–property relations in semi-crystalline combinatorial poly(urethane-isocyanurate)-type hydrogels
AU - Driest, Piet J.
AU - Dijkstra, Dirk J.
AU - Stamatialis, Dimitrios
AU - Grijpma, Dirk W.
N1 - Funding Information:
This project has received funding from the European Union's Horizon 2020 research and innovation program under Marie Skłodowska‐Curie grant agreement no. 642890 ( http://thelink-project.eu/ ). The support of the analytical departments of Covestro Deutschland AG Leverkusen is gratefully acknowledged, as is the support of Dr. Frank Richter and his colleagues with the synthesis work.
Funding Information:
This project has received funding from the European Union's Horizon 2020 research and innovation program under Marie Skłodowska-Curie grant agreement no. 642890 (http://thelink-project.eu/). The support of the analytical departments of Covestro Deutschland AG Leverkusen is gratefully acknowledged, as is the support of Dr. Frank Richter and his colleagues with the synthesis work.
Publisher Copyright:
© 2022 Covestro Deutschland AG. Polymer International published by John Wiley & Sons Ltd on behalf of Society of Industrial Chemistry.
PY - 2022/9
Y1 - 2022/9
N2 - Within the fields of regenerative medicine and tissue engineering, the development of tough hydrogel biomaterials is a challenging topic that has received much attention over the past few years. Recently, a method was developed to synthesize tough combinatorial poly(urethane-isocyanurate) (PUI)-type hydrogels by the trimerization of mixtures of NCO-functionalized prepolymers. As this synthesis approach allows a large degree of freedom in terms of polymer network design with a high level of control over the polymer network structure, the resulting systems are ideally suited for studying structure–property relations in tough hydrogel systems. In this work, we aim to systematically investigate the influence of introducing a hydrophobic component into a PUI polymer network on the mechanical properties of the resulting PUI hydrogels. Additionally, the effect of (the degree of) crystallinity of the hydrophobic network component is investigated. For this, two series of combinatorial PUI hydrogels are synthesized, based on a hydrophilic poly(ethylene glycol) prepolymer and increasing amounts of either a crystallizable hydrophobic prepolymer (poly(ε-caprolactone)) or an amorphous hydrophobic prepolymer (poly(propylene glycol)). It is shown that the toughness of amorphous PUI hydrogels is hardly influenced by the hydrophobic content, whereas the toughness of semi-crystalline PUI hydrogels strongly increases with increasing hydrophobic content. Also, the toughness of the latter hydrogels increases further with increasing degree of crystallinity of the hydrogel. Finally, it is shown that the semi-crystalline PUI hydrogels are promising materials for biomedical adhesive and coating applications, as well as for load-bearing biomedical applications within the fields of tissue engineering and regenerative medicine.
AB - Within the fields of regenerative medicine and tissue engineering, the development of tough hydrogel biomaterials is a challenging topic that has received much attention over the past few years. Recently, a method was developed to synthesize tough combinatorial poly(urethane-isocyanurate) (PUI)-type hydrogels by the trimerization of mixtures of NCO-functionalized prepolymers. As this synthesis approach allows a large degree of freedom in terms of polymer network design with a high level of control over the polymer network structure, the resulting systems are ideally suited for studying structure–property relations in tough hydrogel systems. In this work, we aim to systematically investigate the influence of introducing a hydrophobic component into a PUI polymer network on the mechanical properties of the resulting PUI hydrogels. Additionally, the effect of (the degree of) crystallinity of the hydrophobic network component is investigated. For this, two series of combinatorial PUI hydrogels are synthesized, based on a hydrophilic poly(ethylene glycol) prepolymer and increasing amounts of either a crystallizable hydrophobic prepolymer (poly(ε-caprolactone)) or an amorphous hydrophobic prepolymer (poly(propylene glycol)). It is shown that the toughness of amorphous PUI hydrogels is hardly influenced by the hydrophobic content, whereas the toughness of semi-crystalline PUI hydrogels strongly increases with increasing hydrophobic content. Also, the toughness of the latter hydrogels increases further with increasing degree of crystallinity of the hydrogel. Finally, it is shown that the semi-crystalline PUI hydrogels are promising materials for biomedical adhesive and coating applications, as well as for load-bearing biomedical applications within the fields of tissue engineering and regenerative medicine.
KW - polyurethanes
KW - regenerative medicine
KW - semi-crystalline hydrogels
KW - structure–property relations
KW - tough hydrogels
UR - http://www.scopus.com/inward/record.url?scp=85131542449&partnerID=8YFLogxK
U2 - 10.1002/pi.6427
DO - 10.1002/pi.6427
M3 - Article
AN - SCOPUS:85131542449
SN - 0959-8103
VL - 71
SP - 1055
EP - 1061
JO - Polymer international
JF - Polymer international
IS - 9
ER -