Graphene-based aerogels have attracted considerable interest in recent years for their ability to remove toxic pollutants, due to their attractive properties, which include a sufficient number of anchor positioning points, arbitrarily changing shapes, and adjustable functional groups and pore sizes. The potential methods for adsorption, degradation, and reduction of water and atmospheric pollutants using graphene-based aerogels have been thoroughly investigated. Firstly, this review introduced the current research on the application of graphene-based aerogels as environmentally efficient materials for removing water and atmospheric contaminants, including heavy metal ions, organic dyes, nitrogen oxides (NOx), and volatile organic compounds (VOCs). Secondly, the important role in promoting adsorption and catalysis and the types of modifications of graphene aerogels are discussed in depth. Finally, this review summarized the great potential of graphene-based aerogels as environmentally functional materials and put forward the challenges and prospects, aiming to promote the development and industrial application of graphene-based aerogels.

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