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Phosphorus- and silicon-modified graphene oxide was prepared to improve the thermal stability and flame retardancy properties of epoxy resin. 9,10-Dihydro-9-oxa-10-phosphaphenanthrene-10-oxide (DOPO) and vinyltriethoxysilane (VTES) were successfully grafted onto the surface of graphene oxide (GO) through solvothermal synthesis and hydrolysis-condensation reaction, respectively. Subsequently, the functionalized graphene oxide grafted by DOPO and VTES (DOPO-VTES-GO) was incorporated into the epoxy resin by the solution blending method. The effect of DOPO-VTES-GO on the thermal stability and flame-retardant properties of epoxy resin was systematically studied. Thermogravimetric analysis showed that the thermal stability and char residue yield of DOPO-VTES-GO/epoxy were increased obviously compared with those of pure epoxy resin and DOPO-GO/epoxy. Cone calorimeter test results showed that DOPO-VTES-GO/epoxy had better flame retardancy than pure epoxy resin and DOPO-GO/epoxy on reducing the peak of heat release rate, total heat release, and total smoke production. Furthermore, the char residue after the cone calorimeter tests was investigated by scanning electron microscopy-energy-dispersive X-ray spectrometry, Raman spectroscopy, and Fourier transform infrared measurements. These results demonstrated that the DOPO-VTES-GO can enhance the graphitization degree of char residues and promote the formation of the thermally stable char. In addition, the mechanism of flame retardancy was proposed, and DOPO-VTES-GO exerts the synergistic effect mainly by means of catalytic charring in the condensed phase and capturing hydroxyl or hydrogen radicals from thermal decomposition of epoxy resin in the gas phase. This work provides novel insights into the preparation of phosphorus-silicon-graphene oxide ternary synergistic flame retardants for thermosetting polymer materials.

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Thermal Stability and Flame Retardancy Properties of Epoxy Resin Modified with Functionalized Graphene Oxide Containing Phosphorus and Silicon Elements