Hybrid reinforced sodium silicate/polyurethane (SS/PU) composites mainly derived from low-cost SS and polyisocyanate are produced by a one-step method based on the addition of 3-chloropropyltrimethoxysilane (CTS). The wettability of SS on PU substrate surface is much improved as CTS content increases from 0.0 to 3.5 wt%. Furthermore, with 2.5 wt% of CTS optimal addition, the fracture surface morphology and elemental composition of the resulting SS/PU composites are characterized, as well as mechanical properties, chemical structure and thermal properties. The results indicate that the CTS forms multiple physical and chemical interactions with the SS/PU composites to induce an optimized organic–inorganic hybrid network structure thus achieving simultaneous improvement of compressive strength, flexural strength, flexural modulus and fracture toughness of the SS/PU composites, with the improvement of 12.9%, 6.6%, 17.5% and 9.7%, respectively. Moreover, a reasonable mechanism explanation for CTS modified SS/PU composites is confirmed. Additionally, the high interface areas of the organic–inorganic phase and the active crosslinking effect of the CTS are the main factors to determine the curing process of the SS/PU composites.
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