Chemo-mechanical modelling of swelling and crosslinking reaction kinetics in alginate hydrogels: A novel theory and its numerical implementation

authored by: Aidin Hajikhani, Peter Wriggers, Michele Marino
Abstract: Hydrogels are mechanically stabilized through the action of external agents which induce the formation of crosslinks in the polymer network as a consequence of transport and reactive mechanisms. Crosslinking increases the stiffness of the construct, produces inelastic deformations in the polymer network and interacts with the swelling capacity of hydrogels. The control of this process is hence crucial for fulfilling functional criteria in several technological fields, like drug-delivery or bioprinting. Nevertheless, experimental approaches for monitoring the crosslinking kinetics with the required resolution are currently missing. The development of new computational models in the field might open the way to novel investigation tools. This paper presents a thermodynamically consistent chemo-mechanical model in large deformation for reactive-diffusive mechanisms occurring during crosslinking in alginate hydrogels. The system accounts for shrinking and swelling effects, fluid movements, as well as the reaction kinetics of calcium-induced crosslinking. Crosslinks alter mechanical and diffusive properties in the hydrogel. Moreover, on the basis of thermodynamic arguments, internal stresses directly affect the crosslinking kinetics, revealing a two-way coupling between mechanics and chemistry. The model is implemented in a finite element framework, considering a monolithic coupling between chemical transport and mechanics. The computational framework allows characterizing the (experimentally inaccessible) heterogeneous distribution of mechano-chemical quantities and properties in the hydrogel. Parametric campaigns of simulations are presented to investigate hydrogels' behaviour and compare numerical outcomes with available experimental evidence.
Organisation(s): Institute of Continuum Mechanics
External Organisation(s): Tor Vergata University of Rome
Type: Article
Journal: Journal of the Mechanics and Physics of Solids
Volume: 153
ISSN: 0022-5096
Publication date: 08.2021
Publication status: Published
Peer reviewed: Yes
ASJC Scopus subject areas: Condensed Matter Physics, Mechanics of Materials, Mechanical Engineering
Electronic version(s): https://doi.org/10.1016/j.jmps.2021.104476 (Access: Closed)
: Details in the research portal "Research@Leibniz University"

BibTeX

@article{081011d4f2ea461daf773a3320bd7245,
title = "Chemo-mechanical modelling of swelling and crosslinking reaction kinetics in alginate hydrogels: A novel theory and its numerical implementation",
abstract = "Hydrogels are mechanically stabilized through the action of external agents which induce the formation of crosslinks in the polymer network as a consequence of transport and reactive mechanisms. Crosslinking increases the stiffness of the construct, produces inelastic deformations in the polymer network and interacts with the swelling capacity of hydrogels. The control of this process is hence crucial for fulfilling functional criteria in several technological fields, like drug-delivery or bioprinting. Nevertheless, experimental approaches for monitoring the crosslinking kinetics with the required resolution are currently missing. The development of new computational models in the field might open the way to novel investigation tools. This paper presents a thermodynamically consistent chemo-mechanical model in large deformation for reactive-diffusive mechanisms occurring during crosslinking in alginate hydrogels. The system accounts for shrinking and swelling effects, fluid movements, as well as the reaction kinetics of calcium-induced crosslinking. Crosslinks alter mechanical and diffusive properties in the hydrogel. Moreover, on the basis of thermodynamic arguments, internal stresses directly affect the crosslinking kinetics, revealing a two-way coupling between mechanics and chemistry. The model is implemented in a finite element framework, considering a monolithic coupling between chemical transport and mechanics. The computational framework allows characterizing the (experimentally inaccessible) heterogeneous distribution of mechano-chemical quantities and properties in the hydrogel. Parametric campaigns of simulations are presented to investigate hydrogels' behaviour and compare numerical outcomes with available experimental evidence.",
keywords = "Chemo-mechanical modeling, Hydrogels, Poroelastic effects, Crosslinking kinetics, Finite element simulations, Chemo-mechanical modelling",
author = "Aidin Hajikhani and Peter Wriggers and Michele Marino",
note = "Funding Information: This work has been funded by the Masterplan SMART BIOTECS ( Ministry of Science and Culture of Lower Saxony, Germany ). MM acknowledges also the fundings of the 2017 Rita Levi Montalcini Program for Young Researchers ( Ministry of Education, University and Research, Italy ).",
year = "2021",
month = aug,
doi = "10.1016/j.jmps.2021.104476",
language = "English",
volume = "153",
journal = "Journal of the Mechanics and Physics of Solids",
issn = "0022-5096",
publisher = "Elsevier Ltd.",
number = "104476",
}