Mechanically tough poly(L-lactide) (PLLA)/N,N-dimethylacetamide (DMAc) gels by rapid quenching using liquid nitrogen (LN) were synthesized. PLLA/DMAc solution at 110 °C was cooled at room temperature (PLLA-RT), or quenched by LN before keeping at RT (PLLA-LN). PLLA-RT with the PLLA concentrations of 5, 8, and 11 wt% did not form gel, while PLLA-RT with 14 and 17 wt% could form brittle gel exhibiting coarse structures. In contrast, PLLA-LN could form stable gel regardless of the PLLA concentration. The storage modulus of the gel with the PLLA concentration of 17 wt% increased from 78.7 kPa (PLLA-RT) to 563.7 kPa (PLLA-LN) at the strain of 0.1%. From the structural analysis, PLLA-RT formed spherulites (100–200 μm in diameter), whereas PLLA-LN formed relatively uniform network structures with continuous microporous skeletons without spherulites. The structural changes significantly contributed to the formation of stable, re-moldable, biodegradable, and biocompatible physical gels with ecofriendly and enhanced mechanical properties.
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