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Comparative Large Amplitude Oscillatory Shear (LAOS) Study of Ionically and Physically Crosslinked Hydrogels
Thomas B Goudoulas1, Anna Didonaki1, Sharadwata Pan1
1Chair of Brewing and Beverage Technology, TUM School of Life Sciences, Technical University of Munich, Weihenstephaner Steig 20, 85354 Freising, Germany.
Polymers
|March 29, 2023
Summary
This study compares alginate-calcium and gelatin-alginate hydrogels using large amplitude oscillatory shear (LAOS) rheology. Despite molecular differences, individual layer gelation yields similar microstructures for both hydrogel types.
Area of Science:
- Materials Science
- Rheology
- Biomaterials
Background:
- Hydrogels are versatile materials used across science, technology, and food industries.
- Alginate and gelatin hydrogels are common, but differ in crosslinking mechanisms (ionic vs. physical).
Purpose of the Study:
- To prepare alginate-calcium hydrogels via individual layer gelation.
- To experimentally evaluate the large amplitude oscillatory shear (LAOS) rheological behavior of these hydrogels.
- To compare the nonlinear rheological response of alginate-calcium hydrogels with gelatin-alginate hydrogels prepared ex situ.
Main Methods:
- Preparation of alginate-calcium hydrogels using individual layer gelation.
- Experimental evaluation of LAOS rheological behavior.
- Application of shear-stress decomposition using MITlaos software.
- Comparison of nonlinear responses between alginate-calcium and gelatin-alginate hydrogels.
Main Results:
- Both hydrogel types exhibited similar strain-sweep patterns with loss modulus overshoot, indicating structural breakdown under shear.
- Critical strain points differed between the two hydrogel systems.
- LAOS analysis, specifically the shear-thickening ratio T, suggested a matching bulk microstructure due to the common ex situ individual layer preparation method.
Conclusions:
- Individual layer gelation creates comparable bulk microstructures in alginate-calcium and gelatin-alginate hydrogels.
- Despite similar bulk structures, significant differences exist at the molecular-binding level.
- This highlights the importance of preparation methods in dictating hydrogel properties.

