Abstract
The integration of graphene or graphene oxide nanosheets into three-dimensional (3D) graphene-based macromolecular assemblies (GMAs), in the form of sponges, beads, fibres, films, and crumpled nanosheets, has greatly advanced their environmental remediation applications. This is attributed to the outstanding physicochemical characteristics and superlative mechanical features of 3D GMAs, including precise and physically linked permeable networks, enormous surface area, profound porosity, and high-class sturdiness, amongst others. In this review, the recent advancements towards the exploration of 3D GMAs as an exciting new class of high-performance adsorbents, for eliminating toxic heavy metal ions from both wastewater and freshwater, are systematically summarized and discussed, from both fundamental and applied perspectives. In particular, the numerous surface modification techniques that are actively pursued to enrich the metal adsorption capacity of 3D GMAs, are comprehensively examined. Additionally, associated challenges are pointed out and tactical research strategies and improvements are proposed, with an eye on the conceivable future.