The influence of functionalization of cyclohexyl diamine onto the graphene surface via diazonium reaction on the cure kinetics as well as morphology, mechanical, thermal and physical properties of natural rubber (NR)/graphene nanocomposite foam was investigated. The surface functionalization of graphene was confirmed by Fourier transform infrared spectroscopy, Raman spectroscopy, and thermogravimetric analysis (TGA). Without an addition of blowing agent, the vulcanized NR composites containing cyclohexyl amine‐treated graphene showed not obvious different dispersion of graphene nanoplatelets than those containing untreated graphene as confirmed by transmission electron microscopy micrographs. Although the addition of untreated graphene could accelerate the sulfur vulcanization rate of NR nanocomposite foam due to the high thermal conductivity of graphene particle, and the remaining oxygen functional groups on the surface of graphene, the amines from cyclohexyl diamine on the treated graphene could react with carboxylic and epoxide group on the surface of graphene leading to a reduction of reactive oxygen functional groups on graphene surface and in turn slowed vulcanization rate. The fast vulcanization rate in untreated graphene system led to small bubble size in the NR nanocomposite foams. In contrast, the treated graphene system showed high tensile strength and low thermal expansion coefficient owing to low cell density. Finally, the defect on the graphene surface after functionalization was detected by Raman spectroscopy; this resulted in poor thermal conductivity for the treated graphene composite system. POLYM. COMPOS., 40:E1766–E1776, 2019. © 2018 Society of Plastics Engineers
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