Polydimethylsiloxane (PDMS) are known as a class of efficient modifiers for epoxy thermosets, but the simultaneous improvement in thermal stability, thermomechanical and mechanical properties remain a challenge. Herein, we report a cycloaliphatic epoxy-functionalized polydimethylsiloxane (PDMS-CE) with a designed epoxy value for comprehensive modifications of diglycidyl ether of bisphenol A (DGEBA)/methylhexahydrophthalic anhydride (MeHHPA) thermosets. Compared to neat epoxy thermoset, the 4 wt% PDMS-CE modified epoxy thermoset showed a 79 %, 120 % and 503 % increase in flexural strength, impact strength and fracture toughness, respectively, as well as a slight increase in the initial thermal decomposition temperature (Td5%) and glass transition temperature (Tg), and a desirable decrease in the dielectric constant and water absorption rate. This comprehensive modification performance was caused by the combined effects of crosslinking density improvement, rigid cycloaliphatic structure, as well as the flexible PDMS chains.
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