Advances in Subcritical Hydro‐/Solvothermal Processing of Graphene Materials

Many promising graphene‐based materials are kept away from mainstream applications due to problems of scalability and environmental concerns in their processing. Hydro‐/solvothermal techniques overwhelmingly satisfy both the aforementioned criteria, and have matured as alternatives to wet‐chemical methods with advances made over the past few decades. The insolubility of graphene in many solvents poses considerable difficulties in their processing. In this context hydro‐/solvothermal techniques present an ideal opportunity for processing of graphenic materials with their versatility in manipulating the physical and thermodynamic properties of the solvent. The flexibility in hydro‐/solvothermal techniques for manipulation of solvent composition, temperature and pressure provides numerous handles to manipulate graphene‐based materials during synthesis. This review provides a comprehensive look at the subcritical hydro‐/solvothermal synthesis of graphene‐based functional materials and their applications. Several key synthetic strategies governing the morphology and properties of the products such as temperature, pressure, and solvent effects are elaborated. Advances in the synthesis, doping, and functionalization of graphene in hydro‐/solvothermal media are highlighted together with our perspectives in the field. The subcritical hydro‐/solvothermal synthesis method is a very promising green alternative to many conventional synthesis methods of graphene and its associated materials. This review elaborates on important developments in subcritical hydro‐/solvothermal syntheses of graphene‐based functional materials and classifies their application.