Co-oxidation of arsenic(III) and iron(II) ions by pressurized oxygen in acidic solutions

Abstract

The co-oxidation of As(III) and Fe(II) in acidic solutions by pressured oxygen was studied under an oxygen pressure between 0.5 and 2.0 MPa at a temperature of 150°C. It was confirmed that without Fe(II) ions, As(III) ions in the solutions are virtually non-oxidizable by pressured oxygen even at a temperature as high as 200°C and an oxygen pressure up to 2.0 MPa. Fe(II) ions in the solutions did have a catalysis effect on the oxidation of As(III), possibly attributable to the production of such strong oxidants as hydroxyl free radicals (OH·) and Fe(IV) in the oxidation process of Fe(II). The effects of such factors as the initial molar ratio of Fe(II)/As(III), initial pH value of the solution, oxygen pressure, and the addition of radical scavengers on the oxidation efficiencies of As(III) and Fe(II) were studied. It was found that the oxidation of As(III) was limited in the co-oxidation process due to the accumulation of the As(III) oxidation product, As(V), in the solutions.

Keywords

co-oxidation / As / As(III) oxidation / Fe(II) / pressured oxygen / radical scavenger

References

[1] Nazari AM, Radzinski R, Ghahreman A. Review of arsenic metallurgy: Treatment of arsenical minerals and the immobilization of arsenic. Hydrometallurgy, 2017, 174, 258.

[2] Smedley PL, Kinniburgh DG. A review of the source, behaviour and distribution of arsenic in natural waters. Appl. Geochem., 2002, 17(5): 517.

[3] Filippou D, Demopoulos GP. Arsenic immobilization by controlled scorodite precipitation. JOM, 1997, 49(12): 52.

[4] Safarzadeh MS, Moats MS, Miller JD. An update to “Recent trends in the processing of enargite concentrates”. Miner. Process. Extr. Metall. Rev., 2014, 35(6): 390.

[5] Fernández MA, Segarra M, Espiell F. Selective leaching of arsenic and antimony contained in the anode slimes from copper refining. Hydrometallurgy, 1996, 41(2–3): 255.

[6] Molnár LU, Virčíkova E, Lech P. Experimental study of As(III) oxidation by hydrogen peroxide. Hydrometallurgy, 1994, 35(1): 1.

[7] Sun LH, Liu RP, Xia SJ, Yang YL, Li GB. Enhanced As(III) removal with permanganate oxidation, ferric chloride precipitation and sand filtration as pretreatment of ultrafiltration. Desalination, 2009, 243(1–3): 122.

[8] Sorlini S, Gialdini F. Conventional oxidation treatments for the removal of arsenic with chlorine dioxide, hypochlorite, potassium permanganate and monochloramine. Water Res., 2010, 44(19): 5653.

[9] Dodd MC, Vu ND, Ammann A, Le VC, Kissner R, Pham HV, Cao TH, Berg M, von Gunten U. Kinetics and mechanistic aspects of As(III) oxidation by aqueous chlorine, chloramines, and ozone: relevance to drinking water treatment. Environ. Sci. Technol., 2006, 40(10): 3285.

[10] Khuntia S, Majumder SK, Ghosh P. Oxidation of As(III) to As(V) using ozone microbubbles. Chemosphere, 2014, 97, 120.

[11] Loegager T, Holcman J, Sehested K, Pedersen T. Oxidation of ferrous ions by ozone in acidic solutions. Inorg. Chem., 1992, 31(17): 3523.

[12] Bissen M, Frimmel FH. Arsenic—a review. part II: oxidation of arsenic and its removal in water treatment. Acta Hydroch. Hydrob., 2003, 31(2): 97.

[13] S.L. Shumlas, S. Singireddy, A.C. Thenuwara, N.H. Attanayake, R.J. Reeder, and D.R. Strongin, Oxidation of arsenite to arsenate on birnessite in the presence of light, Geochem. Trans., 17(2016), art No. 5.

[14] Manning BA, Fendorf SE, Bostick B, Suarez DL. Arsenic(III) oxidation and arsenic(V) adsorption reactions on synthetic birnessite. Environ. Sci. Technol., 2002, 36(5): 976.

[15] Li YH, Liu ZH, Liu FP, Li QH, Liu ZY, Zeng L. Promotion effect of KMnO₄ on the oxidation of As(III) by air in alkaline solution. J. Hazard. Mater., 2014, 280, 315.

[16] Bhandari N, Reeder RJ, Strongin DR. Photoinduced oxidation of arsenite to arsenate in the presence of goethite. Environ. Sci. Technol., 2012, 46(15): 8044.

[17] Woods R, Kolthoff IM, Meehan EJ. Arsenic(IV) as an intermediate in the induced oxidation of arsenic(III) by the iron(II)-persulfate reaction and the photoreduction of iron(III). I. absence of oxygen. J. Am. Chem. Soc., 1963, 85(16): 2385.

[18] Fujita T, Taguchi R, Abumiya M, Matsumoto M, Shibata E, Nakamura T. Novel atmospheric scorodite synthesis by oxidation of ferrous sulfate solution. Part I. Hdrometallurgy, 2008, 90(2–4): 92.

[19] Fujita T, Taguchi R, Abumiya M, Matsumoto M, Shibata E, Nakamura T. Novel atmospheric scorodite synthesis by oxidation of ferrous sulfate solution. Part II. Effect of temperature and air. Hydrometallurgy, 2008, 90(2–4): 85.

[20] Rönnholm MR, Wärnå J, Salmi T, Turunen I, Luoma M. Kinetics of oxidation of ferrous sulfate with molecular oxygen. Chem. Eng. Sci., 1999, 54(19): 4223.

[21] Wang Y, Otsuka K, Ebitani K. In situ FTIR study on the active oxygen species for the conversion of methane to methanol. Catal. Lett., 1995, 35(3–4): 259.

[22] Wink DA, Nims RW, Desrosiers MF, Ford PC, Keefer LK. A kinetic investigation of intermediates formed during the Fenton reagent mediated degradation of N-nitrosodimethylamine: evidence for an oxidative pathway not involving hydroxyl radical. Chem. Res. Toxicol., 1991, 4(5): 510.

[23] Bossmann SH, Oliveros E, Göb S, Siegwart S, Dahlen EP, Payawan L, Straub M, Wörner M, Braun AM. New evidence against hydroxyl radicals as reactive intermediates in the thermal and photochemically enhanced Fenton reactions. J. Phys. Chem. A, 1998, 102(28): 5542.

[24] Hug SJ, Leupin O. Iron-catalyzed oxidation of arsenic(III) by oxygen and by hydrogen peroxide: pH-dependent formation of oxidants in the Fenton reaction. Environ. Sci. Technol., 2003, 37(12): 2734.

[25] Wang ZH, Bush RT, Liu JS. Arsenic(III) and iron(II) co-oxidation by oxygen and hydrogen peroxide: Divergent reactions in the presence of organic ligands. Chemosphere, 2013, 93(9): 1936.

[26] Fujita T, Taguchi R, Abumiya M, Matsumoto M, Shibata E, Nakamura T. Effect of pH on atmospheric scorodite synthesis by oxidation of ferrous ions: Physical properties and stability of the scorodite. Hydrometallurgy, 2009, 96(3): 189.

[27] Monhemius AJ, Swash PM. Removing and stabilizing as from copper refining circuits by hydrothermal processing. JOM, 1999, 51(9): 30.

[28] Müller J. Determination of inorganic arsenic(III) in ground water using hydride generation coupled to ICP-AES (HG-ICP-AES) under variable sodium boron hydride (NaBH₄) concentrations. Fresenius J. Anal. Chem., 1999, 363(5–6): 572.

[29] Yang XW, He AP, Yuan BZ. Handbook of Thermodynamic Calculation for High Temperature Aqueous Solutions, 1983, Beijing, Metallurgical Industry Press 34.

[30] Rush JD, Bielski BHJ. Pulse radiolysis studies of alkaline iron(III) and iron(VI) solutions. Observation of transient iron complexes with intermediate oxidation states. J. Am. Chem. Soc., 1986, 108(3): 523.

[31] Klaening UK, Bielski BHJ, Sehested K. Arsenic(IV). A pulse-radiolysis study. Inorg. Chem., 1989, 28(14): 2717.

[32] Bielski BHJ, Cabelli DE. Foote CS, Valentine JS, Greenberg A, Liebman JF. Superoxide and hydroxyl radical chemistry in aqueous solution. Active Oxygen in Chemistry. Structure Energetics and Reactivity in Chemistry Series (SEARCH Series), Vol 2, 1995, Dordrecht, Springer 70.