Geopolymer composite spheres derived from potassium-activated graphene-modified slag/fly ash powder were produced in a polyethylene glycol (PEG 400) solvent. The effect of graphene type (graphene oxide (GO) and few-layered graphene (GNP)) on the pore structure and lead ions (Pb) removal performance of the spheres were evaluated. The results showed that the composite spheres modified with GOs (0.1-0.4 wt%) and GNPs (1-4 wt%) could be spheroidized with an improved performance to adsorb Pb in solution. The graphene-containing spheres reached a maximum BET surface area of 68.85 m/g. Pseudo-second-order and Langmuir isotherm models could express the adsorption process, which was controlled by both monolayer adsorption and chemisorption. The obtained spheres also showed high adsorption capacities for Ni, Cu, Zn and Cd ions. Chemical, physical, electrostatic, ion exchange and cation-π interaction were attributed to the adsorption mechanism of the spheres. The spheres showed good cycling ability compared to those without graphene, which had potential application in heavy metal wastewater treatment.
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