Inorganic arsenic and iron(II) distributions in sediment porewaters investigated by a combined DGT–colourimetric DET technique
William W. Bennett A , Peter R. Teasdale A C , David T. Welsh A , Jared G. Panther A , Ryan R. Stewart A , Helen L. Price B and Dianne F. Jolley B
+ Author Affiliations
- Author Affiliations
A Environmental Futures Centre, Griffith University, Gold Coast campus, QLD 4222, Australia.
B School of Chemistry, University of Wollongong, Wollongong, NSW 2522, Australia.
C Corresponding author. Email: p.teasdale@griffith.edu.au
Environmental Chemistry 9(1) 31-40 https://doi.org/10.1071/EN11074
Submitted: 25 July 2011 Accepted: 2 August 2011 Published: 23 November 2011
Environmental context. Contamination of aquatic ecosystems with inorganic arsenic is a concern for both environmental and human health. Sediments are an important sink for dissolved arsenic, but they may also act as a source of arsenic because of human-induced changes in aquatic systems. This paper describes a new approach for investigating the status of inorganic arsenic in sediments, based on recent developments in diffusion-based sediment sampling techniques.
Abstract. A new approach for investigating the biogeochemistry of inorganic arsenic and iron(II) in freshwater, estuarine and marine sediments is reported. The recently developed Metsorb diffusive gradients in thin films (DGT) technique for the measurement of total inorganic arsenic and the colourimetric diffusive equilibration in thin films (DET) technique for the measurement of iron(II), were utilised in combination to determine co-located depth profiles of both solutes in sediment porewaters. DGT-measured porewater arsenic concentrations were typically less than 40 nM, whereas iron(II) concentrations reached up to 704 µM. Statistically significant (P < 0.0002) correlations between porewater arsenic and iron(II) profiles were observed (R > 0.92) in mesocosms of each sediment type. This approach to investigating arsenic and iron geochemistry in sediments allows the in-situ determination of arsenic and iron species at exactly the same location in the sediment at 3-mm resolution for arsenic and 1-mm resolution for iron(II). The technique was capable of detecting very low concentrations of arsenic, with a detection limit of 0.27 nM (0.02 µg L–1) for a 48-h deployment time. Porewater iron(II), which is often present over a wide range of concentrations, was detectable up to 2000 µM. This study shows the application of these recently developed DGT and DET techniques for the in-situ investigation of inorganic arsenic and iron biogeochemistry in sediments. This approach has the potential to enable simple, yet highly representative assessment of the biogeochemical status of arsenic and iron in a variety of natural sediments, including groundwater sediments where mobilised arsenic is responsible for significant human health risks.
References
[1] H. Zhang, W. Davison, S. Miller, W. Tych, In situ high resolution measurements of fluxes of Ni, Cu, Fe, and Mn and concentrations of Zn and Cd in porewaters by DGT. Geochim. Cosmochim. Acta 1995, 59, 4181.| In situ high resolution measurements of fluxes of Ni, Cu, Fe, and Mn and concentrations of Zn and Cd in porewaters by DGT.Crossref | GoogleScholarGoogle Scholar | 1:CAS:528:DyaK2MXovFCrtrc%3D&md5=a5d9ae7b419973b839d8f82dda2b21bdCAS |
[2] W. Davison, G. Fones, M. Harper, P. Teasdale, H. Zhang, J. Buffle, G. Horvai, Dialysis, DET, and DGT: in situ diffusional techniques for studying water, sediments and soils, in In Situ Monitoring of Aquatic Systems: Chemical Analysis and Speciation (Eds J. Buffle, G. Horvai) 2000, pp. 495–569 (Wiley: Chichester, UK).
[3] H. Zhang, W. Davison, R. J. G. Mortimer, M. D. Krom, P. J. Hayes, I. M. Davies, Localised remobilization of metals in a marine sediment. Sci. Total Environ. 2002, 296, 175.
| Localised remobilization of metals in a marine sediment.Crossref | GoogleScholarGoogle Scholar | 1:CAS:528:DC%2BD38XmvVGrtb4%3D&md5=a2c3d0a9a5eec0d657e633e84823efadCAS |
[4] M. P. Harper, W. Davison, W. Tych, Temporal, spatial, and resolution constraints for in situ sampling devices using diffusional equilibration: dialysis and DET. Environ. Sci. Technol. 1997, 31, 3110.
| Temporal, spatial, and resolution constraints for in situ sampling devices using diffusional equilibration: dialysis and DET.Crossref | GoogleScholarGoogle Scholar | 1:CAS:528:DyaK2sXmt1emsL4%3D&md5=8d17b7f1113e449153d495de3ee8c0c9CAS |
[5] M. P. Harper, W. Davison, W. Tych, Estimation of pore water concentrations from DGT profiles: a modelling approach. Aquat. Geochem. 1999, 5, 337.
| Estimation of pore water concentrations from DGT profiles: a modelling approach.Crossref | GoogleScholarGoogle Scholar | 1:CAS:528:DC%2BD3cXivVCmtA%3D%3D&md5=34aa47d6b049f2a07b0fcaef6629de86CAS |
[6] D. W. Sochaczewski, H. Zhang, W. Tych, Understanding small-scale features in DGT measurements in sediments. Environ. Chem. 2009, 6, 477.
| 1:CAS:528:DC%2BC3cXhslGjsbs%3D&md5=a626c07876f8d4b3627ca15d046971f7CAS |
[7] W. W. Bennett, P. R. Teasdale, J. G. Panther, D. T. Welsh, D. F. Jolley, New diffusive gradients in a thin film technique for measuring inorganic arsenic and selenium(IV) using a titanium dioxide based adsorbent. Anal. Chem. 2010, 82, 7401.
| New diffusive gradients in a thin film technique for measuring inorganic arsenic and selenium(IV) using a titanium dioxide based adsorbent.Crossref | GoogleScholarGoogle Scholar | 1:CAS:528:DC%2BC3cXpvVGmt78%3D&md5=2626102c675037bb5b4d253e48787b16CAS |
[8] P. Smedley, D. Kinniburgh, A review of the source, behaviour and distribution of arsenic in natural waters. Appl. Geochem. 2002, 17, 517.
| A review of the source, behaviour and distribution of arsenic in natural waters.Crossref | GoogleScholarGoogle Scholar | 1:CAS:528:DC%2BD38XhvVSmur0%3D&md5=bee6f2503e0bc328db084535a5edadb4CAS |
[9] N. Belzile, A. Tessier, Interactions between arsenic and iron oxyhydroxides in lacustrine sediments. Geochim. Cosmochim. Acta 1990, 54, 103.
| Interactions between arsenic and iron oxyhydroxides in lacustrine sediments.Crossref | GoogleScholarGoogle Scholar | 1:CAS:528:DyaK3cXhtVagt7w%3D&md5=b9af36ecccf7ec55fd9a7695a7e0aa67CAS |
[10] P. Bose, A. Sharma, Role of iron in controlling speciation and mobilization of arsenic in subsurface environment. Water Res. 2002, 36, 4916.
| Role of iron in controlling speciation and mobilization of arsenic in subsurface environment.Crossref | GoogleScholarGoogle Scholar | 1:CAS:528:DC%2BD38XoslSqsLw%3D&md5=01aae13267b04d072296d3f5f788563eCAS |
[11] W. Maher, E. Butler, Arsenic in the marine environment. Appl. Organomet. Chem. 1988, 2, 191.
| Arsenic in the marine environment.Crossref | GoogleScholarGoogle Scholar | 1:CAS:528:DyaL1MXkvFWr&md5=6d98b33f9ecf662ce3ebfb4664123c6aCAS |
[12] S. Dixit, J. G. Hering, Comparison of arsenic(V) and arsenic(III) sorption onto iron oxide minerals: implications for arsenic mobility. Environ. Sci. Technol. 2003, 37, 4182.
| Comparison of arsenic(V) and arsenic(III) sorption onto iron oxide minerals: implications for arsenic mobility.Crossref | GoogleScholarGoogle Scholar | 1:CAS:528:DC%2BD3sXmtFOltr8%3D&md5=b6bb932a6234219a8c9e6896fef761fdCAS |
[13] P. A. O’Day, D. Vlassopoulos, R. Root, N. Rivera, The influence of sulfur and iron on dissolved arsenic concentrations in the shallow subsurface under changing redox conditions. Proc. Natl. Acad. Sci. USA 2004, 101, 13703.
| The influence of sulfur and iron on dissolved arsenic concentrations in the shallow subsurface under changing redox conditions.Crossref | GoogleScholarGoogle Scholar | 1:CAS:528:DC%2BD2cXotVygtrk%3D&md5=7f97e5e978c3eb19a1d0bf04ef1826bbCAS |
[14] S. S. Chow, M. Taillefert, Effect of arsenic concentration on microbial iron reduction and arsenic speciation in an iron-rich freshwater sediment. Geochim. Cosmochim. Acta 2009, 73, 6008.
| Effect of arsenic concentration on microbial iron reduction and arsenic speciation in an iron-rich freshwater sediment.Crossref | GoogleScholarGoogle Scholar | 1:CAS:528:DC%2BD1MXhtFWltL7F&md5=95fb7bcfd73bb7ab7307ba1b7f547466CAS |
[15] M. L. Polizzotto, B. D. Kocar, S. G. Benner, M. Sampson, S. Fendorf, Near-surface wetland sediments as a source of arsenic release to ground water in Asia. Nature 2008, 454, 505.
| Near-surface wetland sediments as a source of arsenic release to ground water in Asia.Crossref | GoogleScholarGoogle Scholar | 1:CAS:528:DC%2BD1cXovV2mtLs%3D&md5=1e07eb7e8150658ee5259b543b1df918CAS |
[16] A. Horneman, A. van Geen, D. V. Kent, P. E. Mathe, Y. Zheng, R. K. Dhar, S. O’Connell, M. A. Hoque, Z. Aziz, M. Shamsudduha, A. A. Seddique, K. M. Ahmed, Decoupling of As and Fe release to Bangladesh groundwater under reducing conditions. Part I: evidence from sediment profiles. Geochim. Cosmochim. Acta 2004, 68, 3459.
| Decoupling of As and Fe release to Bangladesh groundwater under reducing conditions. Part I: evidence from sediment profiles.Crossref | GoogleScholarGoogle Scholar | 1:CAS:528:DC%2BD2cXmvVGju7o%3D&md5=16f4e873cb81d793ff01b58034b8df81CAS |
[17] A. van Geen, J. Rose, S. Thoral, J. M. Garnier, Y. Zheng, J. Y. Bottero, Decoupling of As and Fe release to Bangladesh groundwater under reducing conditions. Part II: evidence from sediment incubations. Geochim. Cosmochim. Acta 2004, 68, 3475.
| Decoupling of As and Fe release to Bangladesh groundwater under reducing conditions. Part II: evidence from sediment incubations.Crossref | GoogleScholarGoogle Scholar | 1:CAS:528:DC%2BD2cXmvVGju7g%3D&md5=2408f3509672c68e7fa579f262e0c870CAS |
[18] S. Fendorf, H. A. Michael, A. van Geen, Spatial and temporal variations of groundwater arsenic in South and Southeast Asia. Science 2010, 328, 1123.
| Spatial and temporal variations of groundwater arsenic in South and Southeast Asia.Crossref | GoogleScholarGoogle Scholar | 1:CAS:528:DC%2BC3cXmsVGjtrc%3D&md5=ffc798d07dcbc5ad89a4332ad98e30a1CAS |
[19] D. Robertson, P. R. Teasdale, D. T. Welsh, A novel gel-based technique for the high resolution, two-dimensional determination of iron(II) and sulfide in sediment. Limnol. Oceanogr. Methods 2008, 6, 502.
| A novel gel-based technique for the high resolution, two-dimensional determination of iron(II) and sulfide in sediment.Crossref | GoogleScholarGoogle Scholar | 1:CAS:528:DC%2BD1MXhtVWqs77M&md5=bb0c9d0a5431489339278fc182b35b3fCAS |
[20] D. Robertson, D. T. Welsh, P. R. Teasdale, Investigating biogenic heterogeneity in coastal sediments with two-dimensional measurements of iron(II) and sulfide. Environ. Chem. 2009, 6, 60.
| Investigating biogenic heterogeneity in coastal sediments with two-dimensional measurements of iron(II) and sulfide.Crossref | GoogleScholarGoogle Scholar | 1:CAS:528:DC%2BD1MXnsVSmtrk%3D&md5=1061021d07b8924d838e916f0c3a3a19CAS |
[21] R. Dunn, D. Welsh, M. Jordan, P. Teasdale, C. Lemckert, Influence of natural amphipod (Victoriopisa australiensis) (Chilton, 1923) population densities on benthic metabolism, nutrient fluxes, denitrification and DNRA in sub-tropical estuarine sediment. Hydrobiologia 2009, 628, 95.
| Influence of natural amphipod (Victoriopisa australiensis) (Chilton, 1923) population densities on benthic metabolism, nutrient fluxes, denitrification and DNRA in sub-tropical estuarine sediment.Crossref | GoogleScholarGoogle Scholar | 1:CAS:528:DC%2BD1MXls12gtb8%3D&md5=68cb58eac404f298e8fc96eedab4efe4CAS |
[22] M. A. Jordan, D. T. Welsh, R. J. K. Dunn, P. R. Teasdale, Influence of Trypaea australiensis population density on benthic metabolism and nitrogen dynamics in sandy estuarine sediment: a mesocosm simulation. J. Sea Res. 2009, 61, 144.
| Influence of Trypaea australiensis population density on benthic metabolism and nitrogen dynamics in sandy estuarine sediment: a mesocosm simulation.Crossref | GoogleScholarGoogle Scholar | 1:CAS:528:DC%2BD1MXhsFKnt7o%3D&md5=682f57a0027462e0f66f80e6b6b6f33fCAS |
[23] O. Heiri, A. F. Lotter, G. Lemcke, Loss on ignition as a method for estimating organic and carbonate content in sediments: reproducibility and comparability of results. J. Paleolimnol. 2001, 25, 101.
| Loss on ignition as a method for estimating organic and carbonate content in sediments: reproducibility and comparability of results.Crossref | GoogleScholarGoogle Scholar |
[24] K. Reimer, J. Thompson, Arsenic speciation in marine interstitial water. The occurrence of organoarsenicals. Biogeochemistry 1988, 6, 211.
| Arsenic speciation in marine interstitial water. The occurrence of organoarsenicals.Crossref | GoogleScholarGoogle Scholar | 1:CAS:528:DyaL1MXhtVWgtr4%3D&md5=05d43f1ab07b0dc90ede5d3d4666e2f0CAS |
[25] L. Ebdon, A. P. Walton, G. E. Millward, M. Whitfield, Methylated arsenic species in estuarine porewaters. Appl. Organomet. Chem. 1987, 1, 427.
| Methylated arsenic species in estuarine porewaters.Crossref | GoogleScholarGoogle Scholar | 1:CAS:528:DyaL1cXmt1Sruw%3D%3D&md5=513612a3aea767c34c8528957671a35eCAS |
[26] A. Huerga, I. Lavilla, C. Bendicho, Speciation of the immediately mobilisable AsIII, AsV, MMA and DMA in river sediments by high performance liquid chromatography-hydride generation-atomic fluorescence spectrometry following ultrasonic extraction. Anal. Chim. Acta 2005, 534, 121.
| Speciation of the immediately mobilisable AsIII, AsV, MMA and DMA in river sediments by high performance liquid chromatography-hydride generation-atomic fluorescence spectrometry following ultrasonic extraction.Crossref | GoogleScholarGoogle Scholar | 1:CAS:528:DC%2BD2MXis1ChsLg%3D&md5=1bfc536a9f9e787a080841b40c01bbc2CAS |
[27] B. C. Sander, J. Kalff, Factors controlling bacterial production in marine and freshwater sediments. Microb. Ecol. 1993, 26, 79.
| Factors controlling bacterial production in marine and freshwater sediments.Crossref | GoogleScholarGoogle Scholar |
[28] P. E. Kneebone, P. A. O’Day, N. Jones, J. G. Hering, Deposition and fate of arsenic in iron- and arsenic-enriched reservoir sediments. Environ. Sci. Technol. 2002, 36, 381.
| Deposition and fate of arsenic in iron- and arsenic-enriched reservoir sediments.Crossref | GoogleScholarGoogle Scholar | 1:CAS:528:DC%2BD38XhsVWitQ%3D%3D&md5=a0c09873db4e682ebcf7ce81987ec95bCAS |
[29] G. R. Fones, W. Davison, G. W. Grime, Development of constrained DET for measurements of dissolved iron in surface sediments at sub-mm resolution. Sci. Total Environ. 1998, 221, 127.
| Development of constrained DET for measurements of dissolved iron in surface sediments at sub-mm resolution.Crossref | GoogleScholarGoogle Scholar | 1:CAS:528:DyaK1cXmsFygtrY%3D&md5=ffa221b23b7e6ed73f721abb9a4016a5CAS |
[30] A. Mucci, L.-F. Richard, M. Lucotte, C. Guignard, The differential geochemical behavior of arsenic and phosphorus in the water column and sediments of the Saguenay Fjord Estuary, Canada. Aquat. Geochem. 2000, 6, 293.
| The differential geochemical behavior of arsenic and phosphorus in the water column and sediments of the Saguenay Fjord Estuary, Canada.Crossref | GoogleScholarGoogle Scholar | 1:CAS:528:DC%2BD3cXnsFCis70%3D&md5=b7f240f666901a3af6e7dcdcd729093dCAS |
[31] D. E. Canfield, Reactive iron in marine sediments. Geochim. Cosmochim. Acta 1989, 53, 619.
| Reactive iron in marine sediments.Crossref | GoogleScholarGoogle Scholar | 1:CAS:528:DyaL1MXitlCmt7k%3D&md5=c7f2e83151e005c1c657d4f3bb99277cCAS |
[32] P. Teasdale, S. Hayward, W. Davison, In situ, high-resolution measurement of dissolved sulfide using diffusive gradients in thin films with computer-imaging densitometry. Anal. Chem. 1999, 71, 2186.
| In situ, high-resolution measurement of dissolved sulfide using diffusive gradients in thin films with computer-imaging densitometry.Crossref | GoogleScholarGoogle Scholar | 1:CAS:528:DyaK1MXisFGls7w%3D&md5=3586026e6215af22968225ffc7ccc8ebCAS |
[33] G. Pokrovski, R. Gout, J. Schott, A. Zotov, J.-C. Harrichoury, Thermodynamic properties and stoichiometry of AsIII hydroxide complexes at hydrothermal conditions. Geochim. Cosmochim. Acta 1996, 60, 737.
| Thermodynamic properties and stoichiometry of AsIII hydroxide complexes at hydrothermal conditions.Crossref | GoogleScholarGoogle Scholar | 1:CAS:528:DyaK28XhsVSqsbw%3D&md5=f24c7317e9ce8642985d165f0392468dCAS |
[34] P. Atkins, The Elements of Physical Chemistry 2001 (Oxford University Press: Oxford).
[35] M. P. Harper, W. Davison, H. Zhang, W. Tych, Kinetics of metal exchange between solids and solutions in sediments and soils interpreted from DGT measured fluxes. Geochim. Cosmochim. Acta 1998, 62, 2757.
| Kinetics of metal exchange between solids and solutions in sediments and soils interpreted from DGT measured fluxes.Crossref | GoogleScholarGoogle Scholar | 1:CAS:528:DyaK1cXnslOjs7k%3D&md5=608da5f52e771a6cdc54d14c53c46237CAS |
[36] A. Stockdale, W. Davison, H. Zhang, J. Hamilton-Taylor, The association of cobalt with iron and manganese (oxyhydr) oxides in marine sediment. Aquat. Geochem. 2010, 16, 575.
| The association of cobalt with iron and manganese (oxyhydr) oxides in marine sediment.Crossref | GoogleScholarGoogle Scholar | 1:CAS:528:DC%2BC3cXotVOrsL0%3D&md5=7be3a6e36ba814407d1b53a51df78a69CAS |
[37] S. M. Shuttleworth, W. Davison, J. Hamilton-Taylor, Two-dimensional and fine structure in the concentrations of iron and manganese in sediment pore-waters. Environ. Sci. Technol. 1999, 33, 4169.
| Two-dimensional and fine structure in the concentrations of iron and manganese in sediment pore-waters.Crossref | GoogleScholarGoogle Scholar | 1:CAS:528:DyaK1MXmvFCktr4%3D&md5=cb1eb14157c0b854ad40bc8f281d6b4dCAS |
[38] M. P. Harper, W. Davison, W. Tych, One-dimensional views of three-dimensional sediments. Environ. Sci. Technol. 1999, 33, 2611.
| One-dimensional views of three-dimensional sediments.Crossref | GoogleScholarGoogle Scholar | 1:CAS:528:DyaK1MXjvFGht74%3D&md5=6ef7e68a6e45786d03aa6ea52d346886CAS |
[39] G. R. Fones, W. Davison, J. Hamilton-Taylor, The fine-scale remobilization of metals in the surface sediment of the North-east Atlantic. Cont. Shelf Res. 2004, 24, 1485.
| The fine-scale remobilization of metals in the surface sediment of the North-east Atlantic.Crossref | GoogleScholarGoogle Scholar |
[40] W. Davison, G. Fones, G. Grime, Dissolved metals in surface sediment and a microbial mat at 100-m resolution. Nature 1997, 387, 885.
| Dissolved metals in surface sediment and a microbial mat at 100-m resolution.Crossref | GoogleScholarGoogle Scholar | 1:CAS:528:DyaK2sXkt1Gktrs%3D&md5=32ec065bfdbcbb0036c9a71bd35b9072CAS |
[41] T. Fenchel, G. M. King, T. H. Blackburn, Bacterial Biogeochemistry: The Ecophysiology of Mineral Cycling 1998 (Elsevier Academic Press: London).
[42] M. T. Madigan, J. M. Martinko, J. Parker, T. D. Brock, Brock Biology of Microorganisms 2009 (Pearson Benjamin Cummings: San Francisco, CA).
[43] R. R. Christian, W. J. Wiebe, Three experimental regimes in the study of sediment microbial ecology, in Methodology for Biomass Determination and Microbial Activities in Sediments (Eds C. D. Litchfield, P. L. Seyfried) 1979, pp. 148–55 (American Society for Testing and Materials: West Conshohocken, PA).
[44] E. T. Porter, M. S. Owens, J. C. Cornwell, Effect of sediment manipulation on the biogeochemistry of experimental sediment systems. J. Coast. Res. 2006, 226, 1539.
| Effect of sediment manipulation on the biogeochemistry of experimental sediment systems.Crossref | GoogleScholarGoogle Scholar |
[45] J. G. Panther, P. R. Teasdale, W. W. Bennett, D. T. Welsh, H. Zhao, Titanium dioxide-based DGT technique for in situ measurement of dissolved reactive phosphorus in fresh and marine waters. Environ. Sci. Technol. 2010, 44, 9419.
| Titanium dioxide-based DGT technique for in situ measurement of dissolved reactive phosphorus in fresh and marine waters.Crossref | GoogleScholarGoogle Scholar | 1:CAS:528:DC%2BC3cXhsVGkt7jP&md5=b4d623e3269ebcb9e35a18bd5a160d07CAS |
[46] J. G. Panther, P. R. Teasdale, W. W. Bennett, D. T. Welsh, H. Zhao, Comparing dissolved reactive phosphorus measured by DGT with ferrihydrite and titanium dioxide adsorbents: anionic interferences, adsorbent capacity and deployment time. Anal. Chim. Acta 2011, 698, 20.
| Comparing dissolved reactive phosphorus measured by DGT with ferrihydrite and titanium dioxide adsorbents: anionic interferences, adsorbent capacity and deployment time.Crossref | GoogleScholarGoogle Scholar | 1:CAS:528:DC%2BC3MXntFCqtb8%3D&md5=004dd690b04e007b2210ca60d8141cafCAS |
[47] O. Garmo, O. Royset, E. Steinnes, T. Flaten, Performance study of diffusive gradients in thin films for 55 elements. Anal. Chem. 2003, 75, 3573.
| Performance study of diffusive gradients in thin films for 55 elements.Crossref | GoogleScholarGoogle Scholar | 1:CAS:528:DC%2BD3sXks1Krs7o%3D&md5=be1078b4ccd411c05410382016ae1138CAS |
