3D Graphene Materials: From Understanding to Design and Synthesis Control

Carbon materials, with their diverse allotropes, have played significant roles in our daily life and the development of material science. Following 0D C₆₀ and 1D carbon nanotube, 2D graphene materials, with their distinctively fascinating properties, have been receiving tremendous attention since 2004. To fulfill the efficient utilization of 2D graphene sheets in applications such as energy storage and conversion, electrochemical catalysis, and environmental remediation, 3D structures constructed by graphene sheets have been attempted over the past decade, giving birth to a new generation of graphene materials called 3D graphene materials. This review starts with the definition, classifications, brief history, and basic synthesis chemistries of 3D graphene materials. Then a critical discussion on the design considerations of 3D graphene materials for diverse applications is provided. Subsequently, after emphasizing the importance of normalized property characterization for the 3D structures, approaches for 3D graphene material synthesis from three major types of carbon sources (GO, hydrocarbons and inorganic carbon compounds) based on GO chemistry, hydrocarbon chemistry, and new alkali-metal chemistry, respectively, are comprehensively reviewed with a focus on their synthesis mechanisms, controllable aspects, and scalability. At last, current challenges and future perspectives for the development of 3D graphene materials are addressed.