Lipid Network Crosslinked Hydrogels: Controlling Material Dynamics Across Multiple Length Scales Through Lipid...

Area of Science:

• Biomaterials Science
• Polymer Chemistry
• Cellular Engineering

Background:

• Replicating natural material's multi-scale network dynamics in synthetic hydrogels is challenging.
• Current hydrogel strategies link macroscale and nanoscale dynamics via crosslink kinetics.

Purpose of the Study:

• Introduce Lipid Network Crosslinked (LINC) hydrogels inspired by biological materials.
• Enable independent control over hydrogel macroscale and nanoscale dynamics.
• Investigate LINC hydrogels for applications requiring multi-scale dynamic control.

Main Methods:

• Utilized self-assembled liposomes with mobile lipids as covalent crosslinking points.
• Designed liposomes by tuning surface functionalization and tail saturation.
• Incorporated cell-adhesive ligands with varying mobility within the hydrogel network.

Main Results:

• LINC hydrogels exhibited over 20-fold increased stress relaxation rates compared to polymer-only hydrogels.
• Liposome design parameters independently controlled macroscale storage moduli and stress relaxation.
• Human neural progenitor cells showed altered phenotypes based on nanoscale ligand dynamics within LINC hydrogels.

Conclusions:

• LINC hydrogels successfully decouple macroscale and nanoscale network dynamics.
• Lipid mobility within liposomes offers a novel strategy for biomimetic material design.
• LINC hydrogels provide a platform for studying cell responses to tunable multi-scale material dynamics.