Synthesis, decoration and properties of three-dimensional graphene-based macrostructures: A review

• This review summarizes the synthesis, decoration and properties of 3D GBMs.
• Self-assembly, template-directed method and other novel approaches are introduced.
• Decoration operation includes doped graphene, co-construction, and incorporation.
• The structure and properties of 3D GBM are illustrated and emphasized.
• Provides theoretical guidance to design 3D GBM for applications in various fields.

As the first two-dimensional atomic crystal, graphene possesses many superior physical and chemical properties and justifies its nickname of “miracle material”. The assembly of two-dimensional (2D) graphene nanosheets into three-dimensional (3D) macrostructures has gained great attention in the last four years, mainly due to their unique structures and superior properties. An increasing number of 3D graphene-based macrostructures (3D GBMs) with excellent functions has been reported for different applications. This review aims to provide an overview to summarize the structures and properties of 3D GBMs derived from diverse synthesis methods and decoration types. In the synthesis method section, the self-assembly method, template-directed method and other novel approaches are introduced according to the classification. We generalized the second part on decoration into three aspects, including doped graphene sheets within 3D GBMs, 3D GBMs co-constructed with other carbonaceous materials, and incorporation of metal (oxides/sulfides) nanoparticles into 3D GBMs, all of which endow 3D GBMs with new physiochemical properties. This work will provide theoretical guidance for the special design and synthesis of 3D GBM for applications in various fields, such as electronics, photonics, sensors and metrology, bioapplications, and environmental pollutant management.

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