Abstract
Arsenic concentrations in a drinking water reservoir system in the Eastern Ore mountains (Osterzgebirge, Germany) were observed over a 17-year period. The region experienced an environmental change during the past 20 years with decreasing acid, sulphur and nitrogen deposition and a recovering vitality of forested catchment sites. An increase of the arsenic content in the reservoir waters during that change was observed. This was caused by a diminished nitrate supply leading to lower redox potential in the sediments favouring sediment arsenic release. The recent annual cycle in the Altenberg reservoir water arsenic concentration was found to be independent from artificial aeration of the hypoxic hypolimnion during the summer stratification. However, we found a strong seasonal dependent change in water As concentration, with a maximum in autumn and a minimum in spring. The low productive system is driven by peat derived organic matter. For the recent arsenic catchment yield coherencies to dissolved organic carbon export and runoff intensity were found, indicating rising arsenic loads due to climate-related soil organic matter destabilization. Thus, in the reservoir system, both dry and wet climate conditions can increase the water As concentrations due to an internal arsenic release and a catchment arsenic import.
Similar content being viewed by others
References
Anesio, A. M., & Graneli, W. (2004). Photochemical mineralization of dissolved organic carbon in lakes of differing pH and humic content. Archiv Fur Hydrobiologie, 160, 105–116.
APHA. (1992). Standard methods for examination of water and wastewater. Washington, DC: Association APH.
Armbruster, M., Abiy, M., & Feger, K. H. (2003). The biogeochemistry of two forested catchments in the black Forest and the eastern Ore Mountains (Germany). Biogeochemistry, 65, 341–368.
Azcue, J. M., & Nriagu, J. O. (1995). Impact of abandoned mine tailings on the arsenic concentrations in Moira Lake, Ontario. Journal of Geochemical Exploration, 52, 81–89.
Bauer, M., & Blodau, C. (2006). Mobilization of arsenic by dissolved organic matter from iron oxides, soils and sediments. The Science of the Total Environment, 354, 179–190.
Bauer, M., & Blodau, C. (2009). Arsenic distribution in the dissolved, colloidal and particulate size fraction of experimental solutions rich in dissolved organic matter and ferric iron. Geochimica et Cosmochimica Acta, 73, 529–542.
Bernhofer, C., Franke, J., Fischer, S., Kirsten, L., Körner, P., Kostrowski, D., Prasse, H., Schaller, A., & Donix, T. (2015). Analyse der Klimaentwicklung in Sachsen (analysis of climate development in Saxony). Schriftenreihe des LfULG. 3–2015. Dresden: Sächsisches Landesamt für Umwelt, Landwirtschaft und Geologie.
Curtis, C. J., & Simpson, G. L. (2014). Trends in bulk deposition of acidity in the UK, 1988–2007, assessed using additive models. Ecological Indicators, 37, 274–286.
D’Arcy, P., & Carignan, R. (1997). Influence of catchment topography on water chemistry in southeastern Quebec shield lakes. Canadian Journal of Fisheries and Aquatic Sciences, 54, 2215–2227.
Dixit, S., & Hering, J. G. (2003). Comparison of arsenic (V) and arsenic (III) sorption onto iron oxide minerals: Implications for arsenic mobility. Environmental Science & Technology, 37, 4182–4189.
Dousova, B., Erbanova, L., & Novak, M. (2007). Arsenic in atmospheric deposition at the Czech-polish border: Two sampling campaigns 20 years apart. The Science of the Total Environment, 387, 185–193.
EN-ISO-15587-2. (2002). Water quality - digestion for the determination of selected elements in water - part 2: Nitric acid digestion. German version EN ISO 15587–2:2002. Berlin: Deutsches Institut für Normung.
EN-ISO-17294-2. (2004). Water quality - application of inductively coupled plasma mass spectrometry (ICP-MS) - part 2: Determination of 62 elements. German version EN ISO 17294–2:2004. Berlin: Deutsches Institut für Normung.
Erbanova, L., Novak, M., Fottova, D., & Dousova, B. (2008). Export of arsenic from forested catchments under easing atmospheric pollution. Environmental Science & Technology, 42, 7187–7192.
Gachter, R., & Wehrli, B. (1998). Ten years of artificial mixing and oxygenation: No effect on the internal phosphorus loading of two eutrophic lakes. Environmental Science & Technology, 32, 3659–3665.
Hasegawa, H., Rahman, M. A., Kitahara, K., Itaya, Y., Maki, T., & Ueda, K. (2010). Seasonal changes of arsenic speciation in lake waters in relation to eutrophication. The Science of the Total Environment, 408, 1684–1690.
Hebbel H. Analyse „stetigkeitsbasierter“ Methoden zur Bestimmung von Stofffrachten in Fließgewässern. Umweltwissenschaften und Schadstoff-Forschung 2009; 21: 527–538.
Hemond, H. F., & Lin, K. (2010). Nitrate suppresses internal phosphorus loading in an eutrophic lake. Water Research, 44, 3645–3650.
Huang, J. H., & Matzner, E. (2007). Biogeochemistry of organic and inorganic arsenic species in a forested catchment in Germany. Environmental Science & Technology, 41, 1564–1569.
IPCC. Climate change 2014: Synthesis report. Contribution of working groups I, II and III to the fifth assessment report of the intergovernmental panel on climate change Core Writing Team, R.K. Pachauri and L.A. Meyer (eds.) IPCC, Geneva, 151 pp. 2014.
Jay, J. A., Blute, N. K., Lin, K., Senn, D. B., Hemond, H. F., & Durant, J. L. (2005). Controls on arsenic speciation and solid-phase partitioning in the sediments of a two-basin lake. Environmental Science & Technology, 39, 9174–9181.
Kalbitz, K., Solinger, S., Park, J. H., Michalzik, B., & Matzner, E. (2000). Controls on the dynamics of dissolved organic matter in soils: A review. Soil Science, 165, 277–304.
Kandler, O., & Innes, J. L. (1995). Air pollution and forest decline in Central Europe. Environmental Pollution, 90, 171–180.
Kleeberg, A., & Dudel, E. G. (1997). Changes in extent of phosphorus release in a shallow lake (lake grosser Muggelsee; Germany, Berlin) due to climatic factors and load. Marine Geology, 139, 61–75.
Kuhn, A., & Sigg, L. (1993). Arsenic cycling in eutrophic lake Greifen, Switzerland - influence of seasonal redox processes. Limnology and Oceanography, 38, 1052–1059.
Lehmann, J., & Präger, F. (1992). Reliefentwicklung und periglaziäre Schuttdecken im oberen Erzgebirge. In K. Billwitz, K. D. Jäger, & W. Janke (Eds.), Jungquartäre Landschaftsräume: Aktuelle Forschungen zwischen Atlantik und Tienschan (pp. 110–126). Berlin and Heidelberg: Springer.
Leise S, Zimmermann F, Matschullat J. Unter künftigen‚ Normalbedingungen zu erwartende chemische, größenfraktionierte Aerosol- und Feinstaub-Charakteristik einschließlich Herkunft, Transport, Deposition. In: Renner E, editor. Entwicklung und Erprobung eines Integrierten Regionalen Klimaanpassungsprogramms für die Modellregion Dresden (RegKlam, TP 2.2c). Rhombos-Verlag, Berlin, 2013.
LfULG. Digitale Bodenkarte des Freistaates Sachsen 1:50.000, http://www.umwelt.sachsen.de/umwelt/infosysteme/weboffice101/synserver?project=boden-bka&language=de&view=bka, last Access on 14 Oct 2015. Sächsisches Landesamt für Umwelt, Landwirtschaft und Geologie, 2012.
Liu, R. B., Yang, C. L., Li, S. Y., Sun, P. S., Shen, S. L., Li, Z. Y., & Liu, K. (2014). Arsenic mobility in the arsenic-contaminated Yangzonghai Lake in China. Ecotoxicology and Environmental Safety, 107, 321–327.
Martin, A. J., & Pedersen, T. F. (2002). Seasonal and interannual mobility of arsenic in a lake impacted by metal mining. Environmental Science & Technology, 36, 1516–1523.
Matschullat, J., Maenhaut, W., Zimmermann, F., & Fiebig, J. (2000). Aerosol and bulk deposition trends in the 1990’s, eastern Erzgebirge, Central Europe. Atmospheric Environment, 34, 3213–3221.
Mikutta, C., & Kretzschmar, R. (2011). Spectroscopic evidence for ternary complex formation between arsenate and ferric iron complexes of humic substances. Environmental Science & Technology, 45, 9550–9557.
Monteith, D. T., Evans, C. D., Henrys, P. A., Simpson, G. L., & Malcolm, I. A. (2014). Trends in the hydrochemistry of acid-sensitive surface waters in the UK 1988–2008. Ecological Indicators, 37, Part B, 287–303.
Nebe, W., Abiy, M., Hofmann, W., & Weiske, A. (1998). Standorte der Experimentalflächen. In W. Nebe, A. Roloff, & M. Vogel (Eds.), In: Untersuchungen von Waldökosystemen im Erzgebirge als Grundlage für einen ökologisch begründeten Waldumbau. In: Forstwissenschaftliche Beiträge Tharandt, 4 (pp. 19–27). TU Dresden, Tharandt: Fachrichtung Forstwesen.
Oremland, R. S., Stolz, J. F., & Hollibaugh, J. T. (2004). The microbial arsenic cycle in mono Lake, California. FEMS Microbiology Ecology, 48, 15–27.
Oulehle, F., Chuman, T., Majer, V., & Hruska, J. (2013). Chemical recovery of acidified bohemian lakes between 1984 and 2012: The role of acid deposition and bark beetle induced forest disturbance. Biogeochemistry, 116, 83–101.
Oulehle, F., McDowell, W. H., Aitkenhead-Peterson, J. A., Kram, P., Hruska, J., Navratil, T., Buzek, F., & Fottova, D. (2008). Long-term trends in stream nitrate concentrations and losses across watersheds undergoing recovery from acidification in the Czech Republic. Ecosystems, 11, 410–425.
Planer-Friedrich, B., London, J., McCleskey, R. B., Nordstrom, D. K., & Wallschlager, D. (2007). Thioarsenates in geothermal waters of yellowstone national park: Determination, preservation, and geochemical importance. Environmental Science & Technology, 41, 5245–5251.
Rahman, M. A., & Hasegawa, H. (2012). Arsenic in freshwater systems: Influence of eutrophication on occurrence, distribution, speciation, and bioaccumulation. Applied Geochemistry, 27, 304–314.
R-Development-Core-Team. R: A language and environment for statistical computing. R Foundation for Statistical Computing, Vienna, Austria. ISBN 3–900051–07-0. URL http://www.R-project.org/. 2011.
Rothwell, J. J., Taylor, K. G., Ander, E. L., Evans, M. G., Daniels, S. M., & Allott, T. E. H. (2009). Arsenic retention and release in ombrotrophic peatlands. The Science of the Total Environment, 407, 1405–1417.
Schaller, J., Brackhage, C., Mkandawire, M., & Dudel, G. (2011). Metal/metalloid accumulation/remobilization during aquatic litter decomposition in freshwater: A review. The Science of the Total Environment, 409, 4891–4898.
Scheithauer, J. (2006). Umweltwandel im Erzgebirge: eine vergleichende Analyse und Bewertung geoökologischer Prozesse in bewaldeten Einzugsgebieten von Trinkwassertalsperren der oberen Berglagen. Berlin: Rhombos-Verlag.
Schmidt, P. A. (1993). Changes of Flora and Vegetation of forests under the influence of atmospheric depositions. Forstwissenschaftliches Centralblatt, 112, 213–224.
Senn, D. B., Gawel, J. E., & Jay, J. A. (2007). Long-term fate of a pulse arsenic input to a eutrophic lake. Environmental Science & Technology, 41, 3062–3068.
Senn, D. B., & Hemond, H. F. (2002). Nitrate controls on iron and arsenic in an urban lake. Science, 296, 2373–2376.
Senn, D. B., & Hemond, H. F. (2004). Particulate arsenic and iron during anoxia in a eutrophic, urban lake. Environmental Toxicology and Chemistry, 23, 1610–1616.
Seyler, P., & Martin, J. M. (1989). Biogeochemical processes affecting arsenic species distribution in a permanently stratified lake. Environmental Science & Technology, 23, 1258–1263.
Smedley, P. L., & Kinniburgh, D. G. (2002). A review of the source, behaviour and distribution of arsenic in natural waters. Applied Geochemistry, 17, 517–568.
Stoddard, J. L., Jeffries, D. S., Lukewille, A., Clair, T. A., Dillon, P. J., Driscoll, C. T., Forsius, M., Johannessen, M., Kahl, J. S., Kellogg, J. H., Kemp, A., Mannio, J., Monteith, D. T., Murdoch, P. S., Patrick, S., Rebsdorf, A., Skjelkvale, B. L., Stainton, M. P., Traaen, T., van Dam, H., Webster, K. E., Wieting, J., & Wilander, A. (1999). Regional trends in aquatic recovery from acidification in North America and Europe. Nature, 401, 575–578.
Suhendrayatna, O. A., Kuroiwa, T., & Maeda, S. (1999). Arsenic compounds in the freshwater green microalga Chlorella vulgaris after exposure to arsenite. Applied Organometallic Chemistry, 13, 127–133.
Tanner, C. C., & Clayton, J. S. (1990). Persistence of arsenic 24 years after sodium arsenite herbicide application to Lake Rotoroa, Hamilton, new-Zealand. New Zealand Journal of Marine and Freshwater Research, 24, 173–179.
Ulrich, K. U., Paul, L., & Meybohm, A. (2006). Response of drinking-water reservoir ecosystems to decreased acidic atmospheric deposition in SE Germany: Trends of chemical reversal. Environmental Pollution, 141, 42–53.
Vinogradov, A. P. (1962). Average contents of chemical elements in the principal types of igneous rocks of the Earth’s crust. (in Russian). Geokhimiya, 7, 641–664.
Wallstedt, T., Bjorkvald, L., & Gustafsson, J. P. (2010). Increasing concentrations of arsenic and vanadium in (southern) Swedish streams. Applied Geochemistry, 25, 1162–1175.
Weinhold, G. (2002). Die Zinnerz-Lagerstätte Altenberg/Osterzgebirge (The Tin ore deposit Altenberg/East Ore Mountains). Freiberg: Sächsisches Landesamt für Umwelt und Geologie.
Weiske, A., Schaller, J., Hegewald, T., Kranz, U., Feger, K. H., Werner, I., & Dudel, E. G. (2013a). Changes in catchment conditions lead to enhanced remobilization of arsenic in a water reservoir. The Science of the Total Environment, 449, 63–70.
Weiske, A., Schaller, J., Hegewald, T., Machill, S., Werner, I., & Dudel, E. G. (2013b). High mobilization of arsenic, metals and rare earth elements in seepage waters driven by respiration of old allochthonous organic carbon. Environmental Science: Processes and Impacts, 15, 2297–2303.
Wetzel, R. G. (2001). Limnology: Lake and river ecosystems. Chapter 21: Sediments and Microflora. San Diego: Academic Press.
Wood, S. N. (2011). Fast stable restricted maximum likelihood and marginal likelihood estimation of semiparametric generalized linear models. Journal of the Royal Statistical Society, Series B: Statistical Methodology, 73, 3–36.
Worrall, F., Burt, T., & Adamson, J. (2004). Can climate change explain increases in DOC flux from upland peat catchments? The Science of the Total Environment, 326, 95–112.
Acknowledgements
The experimental studies were funded by the State Reservoir Administration of Saxony. We thank the Paulsdorf and Tharandt laboratory staffs for sampling and analysis. Special thanks to Gunter Ilgen (BayCEER, Bayreuth, Germany) and Britta Planer-Friedrich (Bayreuth University, Germany) for methylated and thiolated speciation analysis and to Britta Planer-Friedrich for comments to the manuscript. We thank Silke Neu for language proofreading.
Author information
Authors and Affiliations
Corresponding author
Additional file
Additional file 1
Table S1: Spearman correlations of water parameters in the waters of the reservoir system, analyzed in biweekly values between May 2008 and September 2014. a) Spearman correlations of water parameters in Quergraben tributary. b) Spearman correlations of water parameters in Neugraben tributary. c) Spearman correlations of water parameters in Galgenteich water (transfer flow to Altenberg reservoir). d) Spearman correlations of water parameters in Altenberg reservoir water, depth profile 12.5 m deep. (DOC 109 kb)
Rights and permissions
About this article
Cite this article
Weiske, A., Hegewald, T., Werner, I. et al. Enhanced Arsenic Mobility in a Dystrophic Water Reservoir System After Acidification Recovery. Water Air Soil Pollut 228, 285 (2017). https://doi.org/10.1007/s11270-017-3434-1
Received:
Accepted:
Published:
DOI: https://doi.org/10.1007/s11270-017-3434-1