Advances in Ice-Templated Graphene Aerogels: Fabrication, Properties, and Applications

Graphene has been one of the most widely explored two-dimensional (2D) assemblies due to its outstanding mechanical, electrical, and thermal properties resulting from its unique characteristics of high anisotropy and strong carbon-carbon bonds. Aerogels, characterized by their ultralow density and ultrahigh specific surface area, stand out as leading porous materials. Therefore, the integration of graphene and aerogels would boost the development of multifunctional porous materials. Among the various methods for the fabrication of aerogels, ice-templating has received significant interest due to its ecofriendly nature as a physical process, its broad applicability across material systems, and its proficiency in constructing abundant structures for multifunctionalities. Consequently, ice-templating has become a prevalent technique for the efficient assembly of graphene nanosheets into aerogels with the inherited properties of graphene, the multifunctionality derived from diverse constituents, and the well-controlled architecture. In this review, we systematically summarize the development and progress of ice-templated graphene-based aerogels. Initially, we introduce the fabrication process of these aerogels, elaborating each step from precursor preparation to freezing, drying, and post-treatment. Subsequently, we demonstrate the multifunctional applications of ice-templated graphene aerogels with various macroarchitectures and microstructures. Finally, this review concludes with a straightforward summary, highlighting the challenges and opportunities associated with the ice-templated fabrication of graphene-based aerogels. This systematic review of graphene aerogels aims to offer new insights into the design and ice-templated fabrication of innovative aerogels with multiscale architecture and multifunctionalities, which are crucial for a variety of engineering applications.