Arsenic in Porewaters of the Unsaturated Zone of an Argentinean Watershed: Adsorption and Competition with Carbonate as Important Processes that Regulate its Concentration
- 203 Downloads
- 4 Citations
Abstract
The arsenic (As) concentration in porewaters of the unsaturated (vadose) zone of a watershed located in the Chaco-Pampean Plain of Argentina was investigated. A water displacement method using carbon tetrachloride was applied to the sediments in order to obtain the water samples, which could not be obtained by a simple high-speed centrifugation method. The CD-MUSIC surface complexation model was applied to calculate arsenate adsorption on sediments, arsenate concentration in porewaters in contact with the sediments and effects of carbonate. Ferrihydrite was considered to represent the active adsorbing material in the sediments. Therefore, proton adsorption (surface charge) data and arsenate adsorption isotherms obtained with a synthetic ferrihydrite were used to calibrate the CD-MUSIC model. Arsenate and carbonate concentrations in the studied porewaters were positively correlated. The model was able to predict As concentration within a factor of two in most samples. Carbonate affects As concentration by competing with arsenate species for adsorption sites on the mineral surface. As it occurs with groundwater samples of the saturated zone in many aquifers, this article shows for the first time that adsorption–desorption processes also seem to control As concentration in oxic porewaters of the unsaturated zone.
Keywords
Arsenate Aquifer Surface complexation model Arsenic control Vadose zoneNotes
Acknowledgments
This work was financed by CONICET, SECyT-Argentina and SECyT-UNS. Olga Pieroni is thanked for her help with infrared measurement. MA and FL are members of CONICET.
Supplementary material
References
- Anawar HM, Akai J, Komaki K, Terao H, Yoshioka T, Ishizuka T, Safiullah S, Kato K (2003) Geochemical occurrence of arsenic in groundwater of Bangladesh: sources and mobilization processes. J Geochem Explor 77:109–131CrossRefGoogle Scholar
- Anawar HM, Akai J, Sakugawa H (2004) Mobilization of arsenic from subsurface sediments by effect of bicarbonate ions in groundwater. Chemosphere 54:753–762CrossRefGoogle Scholar
- Antelo J, Avena M, Fiol S, López R, Arce F (2005) Effects of pH and ionic strength on the adsorption of phosphate and arsenate at the goethite–water interface. J Colloid Interface Sci 285:476–486CrossRefGoogle Scholar
- Antelo J, Fiol S, Pérez C, Mariño S, Arce F, Gondar D, López R (2010) Analysis of phosphate adsorption onto ferrihydrite using the CD-MUSIC model. J Colloid Interface Sci 347:112–119CrossRefGoogle Scholar
- Appelo CAJ, Van der Weiden MJJ, Tournassat C, Charlet L (2002) Surface complexation of ferrous iron and carbonate on ferrihydrite and the mobilization of arsenic. Environ Sci Technol 36:3096–3103CrossRefGoogle Scholar
- Arai Y, Sparks DL (2001) ATR–FTIR spectroscopic investigation on phosphate adsorption mechanisms at the ferrihydrite–water interface. J Colloid Interface Sci 241:317–326CrossRefGoogle Scholar
- Bargar JR, Kubicki JD, Reitmeyer R, Davis JA (2005) ATR–FTIR spectroscopic characterization of coexisting carbonate surface complexes on hematite. Geochim Cosmochim Acta 69:1527–1542CrossRefGoogle Scholar
- Biswas A, Gustafsson JP, Neidhardt H, Halder D, Kundu AK, Chatterjee D, Berner Z, Bhattacharya P (2014) Role of competing ions in the mobilization of arsenic in groundwater of Bengal Basin: insight from surface complexation modeling. Water Res 55:30–39CrossRefGoogle Scholar
- Bravo O, Blanco M, Amiotti N (2007) Control factors in the segregation of Mollisols and Aridisols of the semiarid–arid transition of Argentina. Catena 70:220–228CrossRefGoogle Scholar
- Charlet L, Chakraborty S, Appelo CAJ, Roman-Ross G, Nath B, Ansari AA, Lanson M, Chatterjee D, Basu Mallik S (2007) Chemodynamics of an arsenic “hotspot” in a West Bengal aquifer: a field and reactive transport modeling study. Appl Geochem 22:1273–1292CrossRefGoogle Scholar
- Cornell RM, Schwertmann U (1996) The iron oxides: structure, properties, reactions, occurrence and uses. Wiley, WeinheimGoogle Scholar
- Dzombak DA, Morel FMM (1990) Surface complexation modeling. hydrous ferric oxide. Wiley, New YorkGoogle Scholar
- Frau F, Biddau R, Fanfani L (2008) Effect of major anions on arsenate desorption from ferrihydrite-bearing natural samples. Appl Geochem 23:1451–1466CrossRefGoogle Scholar
- Gustafsson JP (2001) Modelling competitive anion adsorption on oxide minerals and an allophane-containing soil. Eur J Soil Sci 52:639–653CrossRefGoogle Scholar
- Gustafsson JP (2006) Arsenate adsorption to soils: modelling the competition from humic substances. Geoderma 136:320–330CrossRefGoogle Scholar
- Hammarlund L, Piñones J (2009) Arsenic in geothermal waters of Costa Rica. Master Thesis. Royal Institute of Technology (KTH), Sweden. http://www2.lwr.kth.se/Publikationer/PDF_Files/LWR_EX_09_02.pdf
- Harrington R, Hausner DB, Bhandari N, Strongin DR, Chapman KW, Chupas PJ, Middlemiss DS, Grey CP, Parise JB (2010) Investigation of surface structures by powder diffraction: a differential pair distribution function study on arsenate sorption on ferrihydrite. Inorg Chem 49:325–330CrossRefGoogle Scholar
- Hausner DB, Bhandari N, Pierre-Louis AM, Kubicki JD, Strongin DR (2009) Ferrihydrite reactivity toward carbon dioxide. J Colloid Interface Sci 337:492–500Google Scholar
- Hiemstra T, Van Riemsdijk WH (1996) A surface structural approach to ion adsorption: the charge distribution (CD) model. J Colloid Interface Sci 179:488–508CrossRefGoogle Scholar
- Hiemstra T, Van Riemsdijk WH (1999) Surface structural ion adsorption modeling of competitive binding of oxyanions by metal (hydr)oxides. J Colloid Interface Sci 210:182–193CrossRefGoogle Scholar
- Hiemstra T, Van Riemsdijk WH (2006) On the relationship between charge distribution, surface hydration and the structure of the interface of metal hydroxides. J Colloid Interface Sci 301:1–18CrossRefGoogle Scholar
- Hiemstra T, Van Riemsdijk WH (2009) A surface structural model for ferrihydrite: I. Sites related to primary charge, molar mass and mass density. Geochim Cosmochim Acta 73:4423–4436CrossRefGoogle Scholar
- Hiemstra T, Rahnemaie R, Van Riemsdijk WH (2004) Surface complexation of carbonate on goethite: IR spectroscopy, structure and charge distribution. J Colloid Interface Sci 278:282–290CrossRefGoogle Scholar
- Hiemstra T, Antelo J, Rahnemaie R, Van Riemsdijk WH (2010) Nanoparticles in natural systems I: the effective reactive surface area of the natural oxide fraction in field samples. Geochim Cosmochim Acta 74:41–58Google Scholar
- Hofmann A, Van Beinum W, Meeussen JCL, Kretzschmar R (2005) Sorption kinetics of strontium in porous hydrous ferric oxide aggregates II. Comparison of experimental results and model predictions. J Colloid Interface Sci 283:29–40CrossRefGoogle Scholar
- Jessen S, Postma D, Larsen F, Nhan PQ, Hoa LQ, Trang PTK, Long TV, Viet PH, Jakobsen R (2012) Surface complexation modeling of groundwater arsenic mobility: results of a forced gradient experiment in a Red River flood plain aquifer, Vietnam. Geochim Cosmochim Acta 98:186–201CrossRefGoogle Scholar
- Keizer MG, Van Riemsdijk WH (1998) ECOSAT: Equilibrium calculation of speciation and transport, technical report. Department Soil Science and Plant Nutrition. Wageningen Agricultural University, WageningenGoogle Scholar
- Kosmulski M (2011a) Compilation of PZC and IEP of sparingly soluble metal oxides and hydroxides from literature. Adv Colloid Interface Sci 152:14–25CrossRefGoogle Scholar
- Kosmulski M (2011b) The pH-dependent surface charging and points of zero charge V. Update. J Colloid Interface Sci 353:1–15CrossRefGoogle Scholar
- Kubicki J (2005) Comparison of As(III) and As(V) complexation onto Al and Fe-hydroxides. In: O’Day P, Vlassopoulos D, Benning L (eds) Advances in arsenic research: Integration of experimental and observational studies and implications for mitigation, ACS Symposium Series 915. American Chemical Society, WashingtonGoogle Scholar
- Lenoble V, Deluchat V, Serpaud B, Bollinger J-C (2003) Arsenite oxidation and arsenate determination by the molybdene blue method. Talanta 61:267–276CrossRefGoogle Scholar
- Loring JS, Sandström MH, Norén K, Persson P (2009) Rethinking arsenate coordination at the surface of goethite. Chem Eur J 15:5063–5072CrossRefGoogle Scholar
- Luengo C, Puccia V, Avena M (2011) Arsenate adsorption and desorption kinetics on a Fe(III)-modified montmorillonite. J Hazard Mater 186:1713–1719CrossRefGoogle Scholar
- Martínez-Villegas N, Briones-Gallardo R, Ramos-Leal JA, Avalos-Borja M, Castañón-Sandoval AD, Razo-Flores E, Villalobos M (2013) Arsenic mobility controlled by solid calcium arsenates: a case study in Mexico showcasing a potentially widespread environmental problem. Environ Pollut 176:114–122CrossRefGoogle Scholar
- McLaren SJ, Kim ND (1995) Evidence for a seasonal fluctuation of arsenic in New Zealand’s longest river and the effect of treatment on concentrations in drinking water. Environ Pollut 90:67–73CrossRefGoogle Scholar
- Mubarak A, Olsen RA (1976) Immiscible displacement of the soil solution by centrifugation. Soil Sci Soc Am J 40:329–331CrossRefGoogle Scholar
- Muller K, Ciminelli VST, Dantas MSS, Willscher S (2010) A comparative study of As(III) and As(V) in aqueous solutions and adsorbed on iron oxy-hydroxides by Raman spectroscopy. Water Res 44:5660–5672CrossRefGoogle Scholar
- Murphy J, Riley JP (1962) A modified single solution method for the determination of phosphate in natural waters. Anal Chim Acta 27:31–36CrossRefGoogle Scholar
- Nickson RT, McArthur JM, Ravenscroft P, Burgess WG, Ahmed KM (2000) Mechanism of arsenic release to groundwater, Bangladesh and West Bengal. Appl Geochem 15:403–413CrossRefGoogle Scholar
- Nimick DA, Moore JN, Dalby CE, Savka MW (1998) The fate of geothermal arsenic in the Madison and Missouri Rivers, Montana and Wyoming. Water Resour Res 34:3051–3067CrossRefGoogle Scholar
- Postma D, Larsen F, Hue NTM, Duc MT, Viet PH, Nhan PQ, Jessen S (2007) Arsenic in groundwater of the Red River floodplain, Vietnam: controlling geochemical processes and reactive transport modelling. Geochim Cosmochim Acta 71:5054–5071CrossRefGoogle Scholar
- Robinson B, Outred H, Brooks R, Kirkman J (1995) The distribution and fate of arsenic in the Waikato River System, North Island, New Zealand. Chem Speciat Bioavail 7:89–96Google Scholar
- Schwertmann U, Cornell RM (2000) Iron oxides in the laboratory: preparation and characterization. Wiley, WeinheimCrossRefGoogle Scholar
- Smedley PL, Kinniburgh DG (2002) A review of the source, behaviour, and distribution of arsenic in natural waters. Appl Geochem 17:517–568CrossRefGoogle Scholar
- Smedley PL, Nicolli HB, Macdonald DMJ, Barros AJ, Tullio JO (2002) Hydrogeochemistry of arsenic and other inorganic constituents in groundwaters from La Pampa, Argentina. Appl Geochem 17:259–284CrossRefGoogle Scholar
- Smedley PL, Kinniburgh DG, Macdonald DMJ, Nicolli HB, Barros AJ, Tullio JO, Pearce JM, Alonso MS (2005) Arsenic associations in sediments from the loess aquifer of La Pampa, Argentina. Appl Geochem 20:989–1016CrossRefGoogle Scholar
- Stachowicz M (2007) Solubility of arsenic in multi-component systems. From the microscopic to the macroscopic scale. Ph.D. Thesis. Wageningen University, WageningenGoogle Scholar
- Stachowicz M, Hiemstra T, Van Riemsdijk WH (2006) Surface speciation of As(III) and As(V) in relation to charge distribution. J Colloid Interface Sci 302:62–75CrossRefGoogle Scholar
- Stachowicz M, Hiemstra T, Van Riemsdijk WH (2007) Arsenic-bicarbonate interaction on goethite particles. Environ Sci Technol 41:5620–5625CrossRefGoogle Scholar
- Stachowicz M, Hiemstra T, Van Riemsdijk WH (2008) Multi-competitive interaction of As(III) and As(V) oxyanions with Ca2+, Mg2+, PO4 3−, and CO3 2− ions on goethite. J Colloid Interface Sci 320:400–414CrossRefGoogle Scholar
- Stollenwerk KG (2002) Geochemical processes controlling transport of arsenic in groundwater: a review of adsorption. In: Welch AH, Stollenwerk AG (eds) Arsenic in ground water. Geochemistry and occurrence. Springer, New York, pp 67–100Google Scholar
- Stollenwerk KG, Breit GN, Welch AH, Yount JC, Whitney JW, Foster AL, Uddin MN, Majumder RK, Ahmed N (2007) Arsenic attenuation by oxidized aquifer sediments in Bangladesh. Sci Total Environ 379:133–150CrossRefGoogle Scholar
- Swartz CH, Blute NK, Badruzzman B, Ali A, Brabander D, Jay J, Besancon J, Islam S, Hemond HF, Harvey CF (2004) Mobility of arsenic in a Bangladesh aquifer: inferences from geochemical profiles, leaching data, and mineralogical characterization. Geochim Cosmochim Acta 68:4539–4557CrossRefGoogle Scholar
- Villalobos M, Leckie JO (2000) Carbonate adsorption onto goethite under closed and open CO2 conditions. Geochim Cosmochim Acta 64:3787–3802CrossRefGoogle Scholar
- Waychunas GA, Davis JA, Fuller CC (2005) Geometry of sorbed arsenate on ferrihydrite and crystalline FeOOH: re-evaluation of EXAFS results and topological factors in predicting sorbate geometry and evidence for monodentate complexes. Geochim Cosmochim Acta 59:3655–3661CrossRefGoogle Scholar
- Zeng H, Fisher B, Giammar D (2008) Individual and competitive adsorption of arsenate and phosphate to a high surface-area iron oxide-based sorbent. Environ Sci Technol 42:147–152CrossRefGoogle Scholar