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© 2021 American Chemical Society.Hydrophobicity of hybrid polyhydroxyurethane (HPHU), via sol/gel curing of a PHU made from diglycerol dicarbonate (DGC) and a poly(propylene glycol) (PPG)–based diamine, is increased by reacting the carbonate–terminated PHU with diamines based on poly(dimethylsiloxane) (PDMS) and the fatty acid–derived Priamine 1074. The modified PHUs were end–capped with silane moisture–curing agents, and swelling of the HPHUs was studied in water and other solvents over 1 week. These films exhibited a drop in the water swelling index (4%) compared to the original poly(DGC–PPG) HPHUs (75%). The PDMS–modified HPHU has a dominant PDMS phase, due to its comparatively longer chain length relative to the PHU, thereby increasing water repellency. Besides an increase in hydrophobicity, the Priamine 1074–modified HPHU revealed a higher storage modulus that is at least 12 times higher than that of the original films. Consequently, Priamine 1074 is regarded as a promising biobased reactive additive when formulating hydrophobic PHU resins.
