Abstract
Iron and arsenic have been found to coexist in a water environment and the fate of arsenite in the aquatic system is influenced by iron. Goethite is a form of iron hydroxide, which is commonly found in sediments. In previous studies, we have used iron complexes to degrade organic pollutants. Results have shown that some organic pollutants could be totally degraded by iron complexes and our work indicated that iron might cause conversion of arsenic when irradiated. This work attempts to investigate the conversion of arsenite [As(III)] using natural goethite, as the iron source, to quantify the effect of various factors on photooxidation. We also consider the possible mechanism for photooxidation of As(III) using a suspension of natural goethite. The As(III) concentration variation under illumination was compared with the one in the dark to quantify the contribution of light to As(III) oxidation to As(V) in goethite suspended solution. The experiments under N2 and air atmosphere confirmed the participation of dissolved oxygen. The photooxidation efficiency of As(III) under different conditions was compared to determine the effect of different environmental factors such as pH value, goethite concentration, and humic acid concentration on the photooxidation reaction. In the solution containing 100 μg L−1 arsenite and 0.1 g L−1 suspended goethite at pH 3.0, nearly 80 % of As(III) was photooxidized after irradiation by a 250-W metal halogen lamp (λ ≥ 313 nm) after 6 h. The effects of initial pH and goethite concentration and humic acid concentration were all examined. The results show that the greatest efficiency of photooxidation of As(III) was at pH 3.0. The extent of photooxidation decreased with increasing goethite concentration and fell sharply in the presence of humic acid under the conditions in this work. Although about 80 % of As(III) was photooxidized after irradiation by a 250-W halogen lamp at pH 3.0 in the presence of goethite suspension, photooxidation was also affected by factors such as pH, concentration of goethite, and presence of humic acid. The scavenger experiments showed that the HO• radical and photogenerated hole are the predominant oxidants in this system responsible for 87.1 % oxidation of As(III), while HO •2 /O •−2 is responsible for 12.9 % oxidation of As(III).
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References
Ahmann D, Roberts AL, Krumholz LR, Morel FM (1994) Microbe grows by reducing arsenic. Nature 371:750
Amstaetter K, Borch T, Casanova PL, Kappler A (2010) Redox transformation of arsenic by Fe(II)-activated goethite (α-FeOOH). Environ Sci Technol 44:102–108
Bhandari N, Reeder RJ, Strongin DR (2011) Photoinduced oxidation of arsenite to arsenate on ferrihydrite. Environ Sci Technol 45:2783–2789
Buschmann J, Canonica S, Lindauer U, Hug SJ, Sigg L (2005) Photoirradiation of dissolved humic acid induces arsenic(III) oxidation. Environ Sci Technol 39:9541–9546
Buxton GV, Greenstock CL, Helman WP, Ross AB (1988) Critical review of rate constants for reactions of hydrated electrons, hydrogen atoms and hydroxyl radicals (•OH/•O−) in aqueous solution. J Phys Chem Ref Data 17:513–886
Christl I, Metzger A, Heidmann I, Kretzschmar R (2005) Effect of humic and fulvic acid concentrations and ionic strength on copper and lead binding. Environ Sci Technol 39:5319–5326
DeSesso JM, Jacobson CF, Scialli AR, Farr CH, Holson JF (1998) An assessment of the developmental toxicity of inorganic arsenic. Reprod Toxicol 12:385–433
Dutta PK, Pehkonen SO, Sharma VK, Ray AK (2005) Photocatalytic oxidation of arsenic(III): evidence of hydroxyl radicals. Environ Sci Technol 39:1827–1834
Elliot AJ, McCracken DR, Buxton GV, Wood ND (1990) Estimation of rate constants for near-diffusion-controlled reactions in water at high temperatures. J Chem Soc, Faraday Trans 86:1539–1547
Emett MT, Khoe GH (2001) Photochemical oxidation of arsenic by oxygen and iron in acidic solutions. Water Res 35:649–656
Faust BC, Hoigne J (1990) Photolysis of Fe(III)-hydroxy complexes as sources of OH radicals in clouds, fog and rain. Atmos Environ 24A:79–89
Goldberg S (2002) Competitive adsorption of arsenate and arsenite on oxides and clay minerals. Soil Sci Soc Am J 66:413–421
Greenstock CL, Miller RW (1975) The oxidation of tiron by superoxide anion. Kinetics of the reaction in aqueous solution and in chloroplasts. Biochimica et Biophysica Acta (BBA) –. Bioenergetics 396:11–16
Harbour PJ, Dixon DR, Scales PJ (2007) The role of natural organic matter in suspension stability. 1. Electrokinetic–rheology relationships. Colloids Surfaces A: Physicochem Eng Aspects 295:38–48
Hug SJ, Canonica L, Weglin M, Gechter D, Gunten UV (2001) Solar oxidation and removal of arsenic at circumneutral pH in iron-containing waters. Environ Sci Technol 35:2114–2121
Hughes MF (2002) Arsenic toxicity and potential mechanism of action. Toxicol Lett 133:1–16
Hwang S, Huling SG, Ko S (2010) Fenton-like degradation of MTBE: effects of iron counter anion and radical scavengers. Chemosphere 78:563–568
Johnston SG, Keene AF, Burton ED, Bush RT, Sullivan LA (2011) Iron and arsenic cycling in intertidal surface sediments during wetland remediation. Environ Sci Technol 45:2179–2185
Langner H, Inskeep WP (2000) Microbial reduction of arsenate in the presence of ferrihydrite. Environ Sci Technol 34:3131–3136
Lee H, Choi W (2002) Photocatalytic oxidation of arsenite in TiO2 suspension: kinetics and mechanisms. Environ Sci Technol 36:3872–3878
Manning BA, Hunt ML, Amrhein C, Yarmoff JA (2002) Arsenic(III) and arsenic(V) reactions with zerovalent iron corrosion products. Environ Sci Technol 36:5455–5461
Masscheleyn PH, Delaune RD, Patrick WH Jr (1991) Effect of redox potential and pH on arsenic speciation and solubility in a contaminated soil. Environ Sci Technol 25:1414–1419
Millero FJ, Sotolongo S (1989) The oxidation of Fe(II) with H2O2 in seawater. Geochim Cosmochim Acta 53:1867–1873
Pettine M, Campanella L, Millero FJ (1999) Arsenite oxidation by H2O2 in aqueous solutions. Geochim Cosmochim Acta 63:2727–2735
Philip B (2005) Arsenic-free water still a pipedream. Nature 436:313
Ren C, Peng H, Huang WY, Wang YJ, Wu F (2011) Speciation of inorganic As(V)/As(III) in water and soil by hydride generation—atomic fluorescence spectrometry. Fresen Environ Bull 20:1069–1074
Rush JD, Bielski BHJ (1985) Pulse radiolytic studies of the reaction of perhydroxyl/superoxide HO •2 /O •−2 with iron(II)/iron(III) ions. The reactivity of HO2/O −2 with ferric ions and its implication on the occurrence of the Haber–Weiss reaction. J Phys Chem 89:5062–5066
Sracek O, Bhattacharya P, Jacks G, Gustafsson JP, Brömssen MV (2004) Behavior of arsenic and geochemical modeling of arsenic enrichment in aqueous environments. Appl Geochem 19:169–180
Sulzberger B, Laubscher H-U, Karametaxas G (1994) Photoredox reactions at the surface of iron(III) (hydr)oxides. Aquatic and surface photochemistry. Lewis, Ann Arbor, pp 53–73
Thoral S, Rose J, Garnier JM, Geen AV, Refait P, Traverse A, Fonda E, Nahon D, Bottero JY (2005) XAS study of iron and arsenic speciation during Fe(II) oxidation in the presence of As(III). Environ Sci Technol 39:9478–9485
Voegelin A, Hug SJ (2003) Catalyzed oxidation of arsenic (III) by hydrogen peroxide on the surface of ferrihydrite: an in situ ATR–FTIR study. Environ Sci Technol 37:972–978
Voelker BM, Morel FMM, Sulzberger B (1997) Iron redox cycling in surface waters: effects of humic substances and light. Environ Sci Technol 31:1004–1011
Woods R, Kolthoff IM, Meehan EJ (1963a) 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 85:2385–2390
Woods R, Kolthoff IM, Meehan EJ (1963b) Arsenic(IV) as an intermediate in the induced oxidation of arsenic(III) by the iron(II) persulfate reaction and the photoreduction of iron(III). II. Presence of oxygen. J Am Chem Soc 85:3334–3337
Woods R, Kolthoff IM, Meehan EJ (1964) Arsenic(IV) as an intermediate in the induced oxidation of arsenic(III) by the iron(II)-hydrogen peroxide reaction. J Am Chem Soc 86:1698–1700
Wu F, Deng NS (2000) Photochemistry of hydrolytic iron(III) species and photoinduced degradation of organic compounds. A minireview. Chemosphere 41:1137–1147
Xing BS et al (2011) Biophysico-chemical processes of anthropogenic organic compound in environmental systems. Wiley, New Jersey, pp 1986–1990
Yang JK, Barnett MO, Jardine PM, Basta NT, Casteel SW (2002) Adsorption, sequestration, and bioaccessibility of As(V) in soils. Environ Sci Technol 36:4562–4569
Yoon SH, Lee JH (2005) Oxidation mechanism of As(III) in the UV/TiO2 system: evidence for a direct hole oxidation mechanism. Environ Sci Technol 39:9695–9701
Acknowledgments
This work was supported by the Natural Science Foundation of China (No. 21077080), the Specialized Research Fund for the Doctoral Program of Higher Education of China (No.20100141110046), and the Natural Science Foundation of Hubei Province (No. 2008CDB379). Comments from the anonymous reviewers are also appreciated.
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Wang, Y., Xu, J., Zhao, Y. et al. Photooxidation of arsenite by natural goethite in suspended solution. Environ Sci Pollut Res 20, 31–38 (2013). https://doi.org/10.1007/s11356-012-1079-6
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DOI: https://doi.org/10.1007/s11356-012-1079-6