Engineering of amine-based binding chemistry on functionalized graphene oxide/alginate hybrids for simultaneous and efficient removal of trace heavy metals: Towards drinking water

Engineering of versatile binding chemistry on graphene oxide surface using nucleophilic substitution/amidation reactions for highly efficient adsorption of Cd (II), Cu (II) and Pb (II) is herein proposed. Graphene oxide (GO) was used as a precursor for covalent bonding of hexamethylenediamine (HMDA) molecules via the nucleophilic substitution/amidation reactions on epoxy (C-O-C) and carboxyl (-COOH) groups to yield hexamethylenediamine functionalized graphene oxide (GO-HMDA) with multiple binding chemistries such as oxygen and nitrogen. Afterwards, GO-HMDA was encapsulated in alginate hydrogel beads with different loadings 5, 10, 15 and 20 wt% to produce Alg/GO-HMDA hybrid adsorbents for the removal of trace heavy metal ions from aqueous solution. Batch adsorption studies showed remarkable adsorption rates reaching 100% for Pb (II), 98.18% for Cu (II) and 95.19 for Cd (II) (similar to 1 mg L-1) with only 15 wt% of GO-HMDA incorporated into the alginate beads. Moreover, Alg/GOHMDA showed high removal efficiencies of heavy metals from tap water with a removal order of (Pb > Cu > Cd) similar to that observed in single aqueous solution. In Addition, the Alg/GO-HMDA adsorbents displayed excellent regeneration ability for six consecutive adsorption-desorption cycles confirming the high performance and potential of these adsorbents, for real heavy metals remediation in environment and in drinking waters in both single and multiple systems. Finally, the adsorption mechanism of traces heavy metals resulted from several phenomena including the electrostatic interactions occurring between the -COOH groups of Alginate and the GO-HMDA surface groups as well as, through chelation interactions occurring between the metal cations and amino-functionalized groups of Alg/GO-HMDA 15 hybrid adsorbent. (C) 2021 Elsevier Inc. All rights reserved.

Automated summary

A versatile binding chemistry was engineered on the surface of graphene oxide using nucleophilic substitution/amidation reactions to efficiently adsorb Cd (II), Cu (II), and Pb (II). The hybrid adsorbents showed high removal efficiencies for heavy metal ions in aqueous solutions and tap water, with excellent regeneration ability for multiple adsorption-desorption cycles. The adsorption mechanism involved electrostatic and chelation interactions between alginate and functionalized graphene oxide.