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A novel method for the templated synthesis of the multi-layer graphene nanosheets in the curling layered nanostructure of halloysite nanotubes (HNTs) was developed. The intercalation of acrylamide in the layered nanostructure of HNTs was successfully achieved by the second-step substitution method. The formation of polymer precursor as carbon source exploited the in-situ polymerization of acrylamide in the layered nanostructure. A series of characterizations such as XRD, FT-IR, Raman, XPS, UV–vis, SEM, TEM and HRTEM were used to determine the formation of graphene nanosheets in the curling layered nanostructure of HNTs. The results indicated that the as-synthesized plane-like graphene nanosheets were originated from the unfolding of the spiral spring-like graphene formed in the curling layered nanostructure of HNTs.

In this work, graphene nanosheets (GN) have been successfully prepared under lower carbonization temperature by using the layered compounds CoAl-LDH. A series of characterizations such as XRD, FTIR, Raman TEM, SEM, EDX, XPS and UV–vis were used to verify the formation of graphene nanosheets in the layered structure of CoAl-LDH. It can be concluded that the Co element of layered double hydroxide acted as the catalytic centers in the formation of graphene nanosheets.