Understanding the adsorption mechanism of Ni(II) on graphene oxides by batch experiments and density functional theory studies

The graphene oxides (GOs) have attracted multidisciplinary study because of their special physicochemical properties. The high surface area and large amounts of oxygen-containing functional groups make GOs suitable materials for the efficient elimination of heavy metal ions from aqueous solutions. Herein the sorption of Ni(II) on GOs was studied using batch experiments, and the results showed that the sorption of Ni(II) is strongly dependent on pH and ionic strength at pH<8, and independent of ionic strength at pH>8. The sorption of Ni(II) is mainly dominated by outer-sphere surface complexation and ion exchange at low pH, and by inner-sphere surface complexation at high pH. The interaction of Ni(II) with GOs was also investigated by theoretical density functional theory (DFT) calculations, and the results show that the sorption of Ni(II) on GOs is mainly attributed to the–COH and–COC groups and the DFT calculations show that Ni(II) forms stable GO_Ni_triplet structure with the binding energy of -39.44 kcal/mol, which is in good agreement with the batch sorption experimental results. The results are important for the application of GOs as adsorbents in the efficient removal of Ni(II) from wastewater in environmental pollution cleanup.