Gallic acid is a renewable plant phenolic resource, and the polyphenolic bio‐based epoxy resin prepared from it can be used as a substitute for bisphenol A epoxy resin in certain fields. However, bio‐based epoxy resins used in the field of high‐performance composite material matrices often require modification. In this paper, firstly, γ‐(2,3‐epoxypropoxy)propyl trimethoxysilane (KH560) was used as the raw material to prepare epoxy‐based cage silsesquioxanes (E‐POSS). Then, E‐POSS was grafted onto γ‐aminopropyltriethoxysilane (KH550) modified halloysite nanotubes (m‐HNTs) to prepare a novel hybrid nanoparticle HNTs‐e‐POSS. Experimental analysis shows that ring opening reactions of amino and epoxy groups can occur between m‐HNTs and E‐POSS, forming a hybrid nanoparticle system of POSS aggregates on the surface of HNTs. Bio‐based nanocomposites were prepared by adding different mass fractions of hybrid nanoparticles HNTs‐e‐POSS into polyphenol type gallic acid epoxy resin matrix (GAER) and using methyltetrahydrophthalic anhydride as curing agent. The properties and micromorphology of the composite were analyzed and characterized. The research showed that with the addition of HNTs‐e‐POSS nanoparticles, the strength and toughness of the composite resin system show a pattern of first increasing and then decreasing, while the storage modulus(E′), glass transition temperature (Tg), and thermal stability of the composite material increased. Mechanical performance analysis shows that the introduction of 0.5 wt% HNTs‐e‐POSS would increase the tensile strength of the composite by 25.46%, while adding 0.75 wt% HNTs‐e‐POSS can increase the impact strength by 15%. The E′(30°C) increased by 24.2% and Tg increased by 7.7°C when the HNTs‐e‐POSS addition was 0.25 wt%.Highlights
Prepared hybrid nanoparticle HNTs‐e‐POSS by grafting POSS onto the HNTs surface.
Application of HNTs‐e‐POSS in modification of bio‐based gallic acid epoxy resin.
HNTs‐e‐POSS can co‐cured with epoxy matrix to increase the crosslinking degree.
The strength, toughness, and modulus of gallic acid epoxy resin are improved.
Tg and thermal stability of gallic acid epoxy resin are enhanced.