Structure–Property Relationships of 3D-Printable Chain-Extended Block Copolymers with Tunable Elasticity and Biodegradability

Elastomeric bioscaffolds with tunable elasticity and biodegradability were synthesized via ring opening polymerization of polycaprolactone (PCL) and polylactide (PLA) with a bifunctional polyethylene glycol macroinitiator, followed by chain extension with diisocyanate to form urethane linkages. Through fine tuning of the macroinitiator and PCL/PLA weight fraction and molecular weight, a data set of elastomeric bioscaffolds gives structure–property insights into their thermal, mechanical, and biodegradability properties as they relate to triblock copolymer composition and mechanical weight. These materials were targeted to be 3D-printed by commercial devices, and their unique rheological properties enable impeccable multiscale microstructure formation. Simplicity in synthesis and fabrication as well as tunable biodegradability (1 day to 2 months) and elasticity (modulus 32–94 MPa) suggest the vast wide-ranging utility and prospective application in bioscaffolds for future therapeutic treatments.