"In-situ" formation of elastin-like recombinamer hydrogels with tunable viscoelasticity through efficient one-pot...

Area of Science:

• Biomaterials Science
• Polymer Chemistry
• Tissue Engineering

Background:

• Recombinant elastin-like (ELR) hydrogels show promise but require enhanced control over viscoelasticity.
• Current methods often involve expensive reagents, lengthy processes, and multiple purification steps.
• There is a need for efficient and scalable methods to produce ELR hydrogels with tunable properties.

Purpose of the Study:

• To investigate the reactivity of carboxylic groups in glutamic acid (E) within an amphiphilic ELR (E50I60) for one-pot amidation.
• To develop a rapid, scalable, and cost-effective method for creating irreversible ELR hydrogels.
• To explore the potential of these hydrogels for tissue regeneration applications.

Main Methods:

• A one-pot amidation reaction in aqueous solutions was employed to conjugate E50I60 with amine-containing molecules.
• High yield conjugation was confirmed using 1H NMR and MALDI-TOF spectroscopies.
• Viscoelastic irreversible hydrogels were formed via in-situ cross-linking of E50I60 with VKV24 ELR using amidation.

Main Results:

• The amidation reaction achieved immediate conjugation of E50I60 with amine groups with high yield.
• Rheology analysis revealed a dual gelation mechanism: physical cross-linking via hydrophobic interactions (I60 block) and covalent cross-linking via amidation.
• The chemical network preserved elasticity, while hydrophobic interactions provided tunable physical cross-linking.

Conclusions:

• A novel, rapid, scalable, and economical one-pot method for ELR hydrogel synthesis was successfully developed.
• The method allows for tunable viscoelastic properties by combining physical and covalent cross-linking mechanisms.
• These ELR hydrogels are promising for tissue regeneration applications due to their controlled properties and efficient production.