Dissolution, Stability and Solubility of Tooeleite [Fe6(AsO3)4(SO4)(OH)4·4H2O] at 25–45 °C and pH 2–12
Tooeleite [Fe6(AsO3)4(SO4)(OH)4·4H2O] was synthesized and characterized to investigate its possible immobilization for arsenic in acidic and alkali environments by a long-term dissolution of 330 d. The synthetic tooeleite was platy crystallites of ~1μm across, giving the lattice parameters of a = 6.4758 Å, b = 19.3737 Å and c = 8.9170 Å. For the tooeleite dissolution, the dissolved arsenic concentration showed the lowest value of 427.3~435.8 mg/L As at initial pH 12 (final pH 5.54). The constituents were dissolved preferentially in the sequence of SO42− > AsO33− > Fe3+ in the aqueous medium at initial pH 2–12. The dissolved iron, arsenite and sulfate existed mainly as FeSO4+/Fe3+, H3AsO30 and SO42− at initial pH 2, and in the form of Fe(OH)30/Fe(OH)2+, H3AsO30 and SO42− at initial pH 12, respectively. The tooeleite dissolution was characterized by the preferential releases of SO42− anions from solid surface into aqueous medium, which was fundamentally controlled by the Fe-O/OH bond breakages and the outer OH− group layers. From the data of the dissolution at 25 °C and initial pH 2 for 270–330 d, the ion-activity product [logˍIAP], which equaled the solubility product [Ksp] at the dissolution equilibrium, and the Gibbs free energy of formation [ΔGfo] were estimated as −200.28 ± 0.01 and −5180.54 ± 0.07 kJ/mol for the synthetic tooeleite, respectively.