Efficient Removal of Heavy Metals from Polluted Water with High Selectivity for Mercury(II) by 2-Imino-4-thiobiuret–Partially Reduced Graphene Oxide (IT-PRGO)

A novel chelating adsorbent, based on the chemical modification of graphene oxide by functionalization amidinothiourea to form 2-imino-4-thiobiuret-partially reduced graphene oxide (IT-PRGO), is used for the effective extraction of the toxic metal ions Hg(II), Cu(II), Pb(II), Cr(VI), and As(V) from wastewater. FTIR and Raman spectroscopy, XRD, and XPS confirm the successful incorporation of the amidinothiourea groups within the partially reduced GO nanosheets through nucleophilic substitution reactions with the acyl chloride groups in the chemically modified GO. The IT-PRGO adsorbent shows exceptional selectivity for the extraction of Hg(II) with a capacity of 624 mg/g, placing it among the top of carbon-based materials known for the high capacity of Hg(II) removal from aqueous solutions. The maximum sorption capacities for As(V), Cu(II), Cr(VI), and Pb(II) are 19.0, 37.0, 63.0, and 101.5 mg/g, respectively. The IT-PRGO displays a 100% removal of Hg(II) at concentrations up to 100 ppm with 90%, 95%, and 100% removal within 15, 30, and 90 min, respectively, at 50 ppm concentration. In a mixture of six heavy metal ions containing 10 ppm of each ion, the IT-PRGO shows a removal of 3% Zn(II), 4% Ni(II), 9% Cd(II), 21% Cu(II), 63% Pb(II), and 100% Hg(II). A monolayer adsorption behavior is suggested based on the excellent agreement of the experimental sorption isotherms with the Langmuir model. The sorption kinetics can be fitted well to a pseudo-second-order kinetic model which suggests a chemisorption mechanism via the amidinothiourea groups grafted on the reduced graphene oxide nanosheets. Desorption studies demonstrate that the IT-PRGO is easily regenerated with the desorption of the metal ions Hg(II), Cu(II), Pb(II), Cr(VI), and As(V) reaching 96%, 100%, 100%, 96%, and 100%, respectively, from their maximum sorption capacities using different eluents. The IT-PRGO is proposed as a top performing remediation adsorbent for the extraction of heavy metals from waste and polluted water.