Knowledge-based tailoring of gelatin-based materials by functionalization with tyrosine-derived groups.

Area of Science:

• Polymer Science
• Materials Science
• Computational Chemistry

Background:

• Gelatin-based materials are versatile but require tailored properties.
• Understanding polymer chain organization and cross-linking is crucial for material design.
• Computational modeling offers predictive power for material properties.

Purpose of the Study:

• To design a physically cross-linked polymer system based on gelatin.
• To investigate the effect of tyrosine-derived side groups on material properties.
• To validate computational models against experimental data for predictive applications.

Main Methods:

• Development and validation of molecular models for gelatin-based systems.
• Simulation of polymer chain organization, cross-link formation, and mechanical properties.
• Experimental characterization of material properties, including swelling and tensile strength.

Main Results:

• Computational models accurately predicted structural and mechanical properties at 25 wt.-% water content.
• Incorporation of desaminotyrosine (DAT) and desaminotyrosyl tyrosine (DATT) reduced helical conformation.
• Increased aromatic content led to enhanced physical cross-linking via pi-pi interactions and hydrogen bonds.
• Mechanical properties such as Young's modulus, elongation at break, and tensile strength increased.
• Water swelling degree decreased with higher aromatic content.

Conclusions:

• Molecular modeling is a valuable tool for the knowledge-based design of gelatin-based polymers.
• Tyrosine-derived side groups effectively enhance the mechanical performance and reduce water sensitivity.
• The developed physically cross-linked system shows promise for advanced material applications.