Biodegradable poly(ε-caprolactone)/poly(silyl fumarate) shape memory scaffolds.

Authors

Jenlyan Negrón Hernández, Kaley Beach, Paola Chavarria, Melissa A Grunlan

Published in

Polymer. Volume 348. Mar 19, 2026. Epub Feb 10, 2026.

Abstract

Biodegradable shape memory scaffolds have the unique potential to heal irregularly shaped craniomaxillofacial (CMF) defects through conformal 'self-fitting'. These have been previously prepared from poly(ε-caprolactone) diacrylate (PCL-DA), but the slow biodegradation rate of PCL is expected to limit neotissue formation. Subsequently, telechelic siloxane macromers polydimethylsiloxane-dimethacrylate (PDMS-DMA) and polymethylhydrosiloxane-DMA (PMHS-DMA) were combined with PCL-DA at varying weight (wt)% ratios, resulting in PCL/PDMS and PCL/PMHS co-network scaffolds with accelerated degradation rates owing to phase separation that increased water uptake. Still, these siloxane macromers lack a hydrolytically unstable backbone thus limiting degradation. Herein, poly(silyl fumarate) (PSF) was synthesized as a hybrid siloxane macromer with a hydrolytically unstable backbone as well as interchain crosslinkability. PCL/PSF scaffolds were prepared at 90:10, 75:25, 60:40, and 50:50 wt% of PCL-DA to PSF via solvent-casting particulate leaching (SCPL) with a fused salt template. Despite a reduction in PCL crystallinity (i.e., switching segments) with 40 and 50 wt% PSF, all scaffolds maintained excellent shape memory behavior. PCL/PSF scaffolds with 10 and 25 wt% PSF also maintained the modulus of the PCL-only scaffold as well as the corresponding PCL/PDMS and PCL/PMHS scaffolds. In vitro degradation under basic conditions revealed that PCL/PSF scaffolds with just 10 wt% PSF degraded faster than the PCL-only scaffold and further increased with 25 wt% PSF to surpass that of the corresponding PCL/PDMS scaffold. A lack of phases separation was observed, and thus indicated that faster degradation was achieved by the hydrolytic instability of the PSF.

PMID:
42454340
Bibliographic data and abstract were imported from PubMed on 15 Jul 2026.

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