Abstract

Polydimethylsiloxane(PDMS) based segmented polyether urethanes (SiPEUs) suffer from poor adhesion between apolar PDMS and polar hard domains, which results in inferior mechanical properties and inadequate stability in long-term implantation. To regulate the interfacial miscibility, three chain extenders attached with different dangling side chains (fluorinated diol FDO, silicone-based diol SDO, and hexyl-based diol HDO) were used in two-step synthesis to modify the polarity of hard segments. Thermal analysis demonstrated a higher glass transition temperature of PDMS and PTMO (poly (tetramethylene oxide)) domain in SDO modified SiPEU(SSPEU) in contrast to the samples extended with FDO and HDO. Fourier transform infrared spectroscopy (FT-IR), small-angel x-ray scattering (SAXS), and dissipative particle dynamics (DPD) simulation further proved that SSPEU was achieved with optimal interfacial miscibility compared with SPEU. The intermediate layers were proposed to be functionally percolated composed of PDMS, PTMO, MDI-SDO, and MDI-BDO units, which promoted oxidative stability under accelerated test in vitro without mechanical compromise.

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