The interfacial asymmetric post-functionalization of graphene nanosheets and their self-assembly into superstructures is presented. By performing two sequential functionalizations, graphene nanosheets lying in the interface of a biphasic aqueous-organic system become amphiphilic, thereby generating an organophilic side and a hydrophilic side. The as-prepared Janus type amphiphilic graphene nanosheets are then self-assembled to generate different interesting superstructures, depending on the nature of the solvent in which they are dispersed.
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