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Graphene-based functional materials have gained extensive research attention as promising adsorbents in wastewater remediation due to their eco-friendliness and suitable physicochemical characteristics, i.e., high surface area, strong π-interactions, adjustable surface modification, switchable structure, and immense availability of chemical moieties. In particular, engineered multidimensional graphene-based macrostructures (GBMs) have shown remarkable potential for remediating various water pollutants, including heavy metals, dyes, pharmaceuticals, antibiotics, phenols, and polycyclic aromatic hydrocarbons. Given the swift advancement of GBMs, this chapter provides a valuable forum to consolidate prior explorations, ongoing progress, and prospective avenues related to the use of GBMs in wastewater treatment. A comprehensive overview of different GBMs and their applications in the removal of contaminants with diverse charge states, water solubilities, complexities, and emerging pollutants is provided. The major focus of this chapter encompasses the synthetic pathways, structural characteristics, engineering, and adsorption efficiency of GBMs, and their industrial implementation. By elucidating the potential of GBMs for water purification, this chapter aims to provide valuable insights and guidance into the quest for sustainable and efficient wastewater treatment solutions.

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