Inorganic–organic hybrid materials with tunable chemical and physical properties were prepared from mono epoxy terminated polydimethylsiloxane (PDMS) macromonomer and gelatin for improving their flexibility and hydrophobicity. Sodium dodecyl sulfate (SDS) and sodium dodecyl benzene sulfonate (SDBS) were used to enhance the compatibility of two polymers phases. Measurement of grafting density indicated that anionic surfactants played a crucial role in deciding the detailed microstructure of PDMS-E grafted gelatin (PGG) polymers in alkaline solution. The interaction between gelatin and SDS/SDBS was investigated by viscosity and SEM. Viscosity analysis showed a regular increase in SDS system and a steeper change in the case of SDBS. SEM micrographs displayed a series of structural transitions (spherical, spindle, irregular granular and spherical aggregates) with the increase of SDS concentration, but spindle and granular aggregates appeared alternately as varying SDBS concentrations. The results demonstrated that both the electrostatic and hydrophobic interactions between anionic surfactant and gelatin controlled the aggregate structure of gelatin–SDS/SDBS, which affected the compatibility between gelatin and PDMS. Thermal properties of PGG polymers had changed with the modification of polymer microstructure. The results above revealed that microstructure transformation of PGG polymers was determined by the compatibility of two polymers in anionic surfactant aqueous solution and the chemical nature of their monomers.
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