Thermodynamics of Water Stabilization of Carboxybetaine Hydrogels from Molecular Dynamics Simulations
Abstract
Hydrogels are highly flexible network polymers being developed as scaffolds for tissue engineering and joint replacement. Their mechanical properties depend largely on their water content. To determine the associated mechanical and thermodynamic properties, we apply the new two-phase thermodynamics method (2PT) to short, molecular dynamics (MD) trajectories of solvated carboxybetaine methacrylate (CBMA) hydrogels. The calculated optimum water content agrees well with recent experiments. We find that the thermodynamics is dominated by a competition between the enthalpy of tightly bound water molecules (which enhance the population of low-energy states of the hydrogel) and the entropy-driven formation of a quasi-liquid water phase in the void volume. These new insights into the role of water in stabilizing hydrophilic motifs is expected to guide design strategies aimed at creating hydrogels with improved performance.
Additional Information
© 2011 American Chemical Society. Published In Issue: July 21, 2011; Article ASAP: July 05, 2011. Just Accepted Manuscript: June 29, 2011; Received: June 07, 2011; Accepted: June 29, 2011. This work was supported by WCU program (31-2008-000- 10055-0) through the National Research Foundation of Korea. The MSC computational facilities were provided by ARO-DURIP and ONR-DURIP. We acknowledge the generous allocation of supercomputing time from the KISTI supercomputing center at KAIST. Partial support from Dow Chemical Company is acknowledged.Attached Files
Supplemental Material - jz200760n_si_001.pdf
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Additional details
- Eprint ID
- 24832
- Resolver ID
- CaltechAUTHORS:20110812-111657965
- National Research Foundation of Korea
- Dow Chemical Company
- Created
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2011-08-12Created from EPrint's datestamp field
- Updated
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2021-11-09Created from EPrint's last_modified field