Three‐Dimensional Graphene‐Based Macrostructures for Electrocatalysis

Electrochemical energy storage and conversion is an effective strategy to relieve the increasing energy and environment crisis. The sluggish reaction kinetics in the related devices is one of the major obstacles for them to realize practical applications. More efforts should be devoted to searching for high‐efficiency electrocatalysts and enhancing the electrocatalytic performance. 3D graphene macrostructures (3D GMs) are one kind of porous crystalline materials with 3D structures at both micro‐ and macro‐scale. The unique structure can achieve large accessible surface area, expose many active sites, promote fast mass/electron transport, and provide wide room for further functional modification. All these features make them promising candidates for electrocatalysis. In this review, the authors focus on the latest progress of 3D GMs for electrocatalysis. First, the preparation methods of 3D GMs are introduced followed by the strategies for functional modifications. Then, their electrocatalytic performances are discussed in detail including monofunctional and bifunctional electrocatalysis. The electrocatalytic processes involve oxygen reduction reaction, oxygen evolution reaction, hydrogen evolution reaction, and carbon dioxide reduction reaction. Finally, the challenges and perspectives are presented to offer a guideline for the exploration of excellent 3D GM‐based electrocatalysts. The latest progress of 3D graphene‐based macrostructures is discussed systematically to promote the exploration of high‐efficiency electrocatalysts for energy storage and conversion. Materials preparation and functional modification are first introduced followed by their electrocatalytic performance for important electrochemical energy conversion reactions. Key issues are analyzed to guide the further research in future.