Antimonate adsorption onto Mg-Fe layered double hydroxides in aqueous solutions at different pH values: Coupling surface complexation modeling with solid-state analyses

Abstract

In this study, the importance of Sb behavior under different pH conditions has been addressed with respect to its stabilization in aqueous solutions using Mg-Fe layered double hydroxides (LDHs). The Sb(V) adsorption onto Mg-Fe LDHs was performed at different initial Sb(V) concentrations and pH values (pH 5.5, 6.5 and 7.5). The removal rate and the maximal adsorbed amount increased with decreasing pH values. Moreover, the surface complexation modeling (SCM) predicted preferable formation of monodentate mononuclear and bidentate binuclear complexes on the Mg-Fe LDH surface. Spectroscopic (X-ray diffraction analysis, Fourier transform infrared spectroscopy, X-ray photoelectron spectroscopy) and microscopic (scanning electron microscopy and energy-dispersive X-ray spectroscopy) techniques were used to further specify the adsorption mechanisms. The influence of chemical adsorption, surface-induced precipitation of brandholzite Mg[Sb(OH)6]2·6H2O, formation of brandholzite-like phases and/or anion exchange was observed. Moreover, Sb(V) was nonhomogeneously distributed on the Mg-Fe LDH surface at all pH values. The surface complexation modeling supported by solid-state analyses provided a strong tool to investigate the binding arrangements of Sb(V) on the Mg-Fe LDH surface. Such a complex mechanistic/modeling approach has not previously been presented and enables prediction of the Sb(V) adsorption behavior onto Mg-Fe LDHs under different conditions, evaluating their possible use in actual applications.