Abstract
Historical gold mining operations in Nova Scotia, Canada, resulted in numerous deposits of publicly accessible, arsenic (As)-rich mine waste that has weathered in situ for 75–150 years, resulting in a wide range of As-bearing secondary minerals. The geochemical heterogeneity of this mine waste creates a challenge for identifying a single remediation approach that will limit As mobility. A 30-cm-thick, low-organic content soil cover was evaluated in a laboratory leaching experiment where, to simulate natural conditions, the equivalent of 2 years of synthetic rainwater was leached through each column and two dry seasons were incorporated into the leaching protocol. Each column was a stratigraphic representation of the four major tailings types found at the historical Montague and Goldenville gold mine districts: hardpan tailings, oxic tailings, wetland tailings, and high Ca tailings. Hardpan tailings released acidic, As-rich waters (max 12 mg/L) under the soil cover but this acidity was buffered by surrounding oxic tailings. Leachate from the oxic tailings was circumneutral, with average As concentrations between 4.4 and 9.7 mg/L throughout the experiment. The presence of carbonates in the high Ca tailings resulted in near-neutral to weakly alkaline leachate pH values and average As concentrations between 2.1 and 6.1 mg/L. Oxidation of sulfides in the wetland tailings led to acidic leachate over time and a decrease in As concentrations to values that were generally less than 1 mg/L. This study shows that the use of a low-organic content soil cover does not create reducing conditions that would destabilize oxidized, As-bearing secondary phases in these tailings. However, oxygen penetration through the cover during dry seasons would continue to release As to tailings pore waters via sulfide oxidation reactions.
Similar content being viewed by others
References
Adu-Wusu C, Yanful EK (2007) Post-closure investigation of engineered test covers on acid-generating waste rock at Whistle Mine, Ontario. Can Geotech J 44:496–506
Asta MP, Pérez-López R, Román-Ross G, Illera V, Cama J, Cotte M, Tucoulou R (2013) Analysis of the iron coatings formed during marcasite and arsenopyrite oxidation at neutral-alkaline conditions. Geol Acta 11:465–481
Aubertin M, Bussière B, Barbera J-M, Chapuis RP, Monzon M, Aachib M (1997) Construction and instrumentation of in situ test plots to evaluate covers built with clean tailings. In: Proceedings of the 4th international conference on acid rock drainage, Vancouver, B.C., 31 May–6 June 1997, vol 2, pp 715–730
Bluteau M-C, Demopoulos GP (2007) The incongruent dissolution of scorodite: solubility, kinetics and mechanism. Hydrometallurgy 87:163–177
Bluteau M-C, Becze L, Demopoulos GP (2009) The dissolution of scorodite in gypsum-saturated waters: evidence of Ca–Fe–AsO4 mineral formation and its impact on arsenic retention. Hydrometallurgy 97:221–227
Bouazza A, Rahman F (2007) Oxygen diffusion through partially hydrated geosynthetic clay liners. Géotechnique 57:767–772
Canadian Council of Ministers of the Environment (CCME) (2001a) Canadian soil quality guidelines for the protection of environmental and human health: Arsenic (inorganic) (1997). Updated In: Canadian environmental quality guidelines, 1999, Canadian Council of Ministers of the Environment, Winnipeg
Canadian Council of Ministers of the Environment (CCME) (2001b) Canadian water quality guidelines for the protection of aquatic life: Arsenic. Updated In: Canadian environmental quality guidelines, 1999, Canadian Council of Ministers of the Environment, Winnipeg
Corriveau MC, Jamieson HE, Parsons MB, Hall GEM (2011) Mineralogical characterization of arsenic in gold mine tailings from three sites in Nova Scotia. Geochem Explor Environ Anal 11:179–192
Craw D, Falconer D, Youngson JH (2003) Environmental arsenopyrite stability and dissolution: theory, experiment, and field observations. Chem Geol 199:71–82
Demers I, Bussière B, Mbonimpa M, Benzaazoua M (2009) Oxygen diffusion and consumption in low-sulphide tailings covers. Can Geotech J 46:454–469
DeSisto SL (2014) Hydrogeochemical evaluation and impact of remediation design on arsenic mobility at historical gold mine sites. Ph.D. Thesis, Queen’s University, Kingston, ON. https://qspace.library.queensu.ca/handle/1974/12227
DeSisto SL, Jamieson HE, Parsons MB (2011) Influence of hardpan layers on arsenic mobility in historical gold mine tailings. Appl Geochem 26:2004–2018
DeSisto SL, Jamieson HE, Parsons MB (2016) Subsurface variations in arsenic mineralogy and geochemistry following long-term weathering of gold mine tailings. Appl Geochem 73:81–97
Dove PM, Rimstidt JD (1985) The solubility and stability of scorodite, FeAsO4·2H2O. Am Mineral 70:838–844
Environment Canada (2011) The Canadian National Atmospheric Chemistry (NAtChem) database and analysis system. https://www.ec.gc.ca/natchem/. Accessed 10 Mar 2011
Environment Canada (2012) National Climate Data & Information Archive Canadian Climate Normals. http://climate.weather.gc.ca/climate_normals/index_e.html. Accessed 25 Sept 2012
Filippi M, Doušová B, Machovič V (2007) Mineralogical speciation of arsenic in soil above the Mokrsko-west gold deposit, Czech Republic. Geoderma 139:154–170
Filippou D, Demopoulos GP (1997) Arsenic immobilization by controlled scorodite precipitation. JOM 49:52–55
Flemming RL, Salzsauler KA, Sherriff BL, Sidenko NV (2005) Identification of scorodite in fine-grained, high-sulfide, arsenopyrite mine-waste using micro X-ray diffraction (μXRD). Can Mineral 43:1243–1254
Fukushi K, Sasaki M, Yanase N, Amano H, Ikeda H (2003) A natural attenuation of arsenic in drainage from an abandoned arsenic mine dump. Appl Geochem 18:1267–1278
Hallberg RO, Granhagen JR, Liljemark A (2005) A fly ash/biosludge dry cover for the mitigation of AMD at the falun mine. Chem Erde Geochem 65:43–63
Health Canada (2017) Guidelines for Canadian drinking water quality—summary table. Water and Air Quality Bureau, Healthy Environments and Consumer Safety Branch, Health Canada, Ottawa
Herlin B (2008) Kam Kotia Project Case Study: geocomposite cover for sulfide tailings at mine site in Ontario. Geosynthetics 26:32–39
Hosney MS, Rowe RK (2013) Changes in geosynthetic clay liner (GCL) properties after 2 years in a cover over arsenic-rich tailings. Can Geotech J 50:326–342
Jia Y, Demopoulos GP (2008) Coprecipitation of arsenate with iron (III) in aqueous sulfate media: effect of time, lime as base and co-ions on arsenic retention. Water Res 42:661–668
Kavalench JL (2010) Effect of tailings mineralogy and infiltration water chemistry on arsenic release from historic gold mine tailings. M.Sc. Thesis, Queen’s University, Kingston, ON
Krause E, Ettel VA (1988) Solubility and stability of scorodite, FeAsO4·2H2O: new data and further discussion. Am Mineral 73:850–854
Krause E, Ettel VA (1989) Solubilities and stabilities of ferric arsenate compounds. Hydrometallurgy 22:311–337
Lange K, Rowe RK, Jamieson H (2009) Diffusion of metals in geosynthetic clay liners. Geosynth Int 16:11–27
Lengke MF, Temple RN (2003) Natural realgar and amorphous AsS oxidation kinetics. Geochim Cosmochim Acta 67:859–871
Lengke MF, Temple RN (2005) Geochemical modeling of arsenic sulfide oxidation kinetics in a mining environment. Geochim Cosmochim Acta 69:341–356
Lindberg RD, Runnels DD (1984) Ground water redox reactions: an analysis of equilibrium state applied to Eh measurements and geochemical modeling. Science 225:925–927
Lindsay MBJ, Blowes DW, Condon PD, Ptacek CJ (2011) Organic carbon amendments for passive in situ treatment of mine drainage: field experiments. Appl Geochem 26:1169–1183
Mylona E, Xenidas A, Csövári M, Németh G (2007) Application of dry covers for the closure of tailings facilities. Land Contam Reclam 15:163–182
Nicholson RV, Gillham RW, Cherry JA, Reardon EJ (1989) Reduction of acid generation in mine tailings through the use of moisture-retaining cover layers as oxygen barriers. Can Geotech J 26:1–8
Paktunc D (2013) Mobilization of arsenic from mine tailings through reductive dissolution of goethite influenced by organic cover. Appl Geochem 36:49–56
Paktunc D, Foster A, Laflamme G (2003) Speciation and characterization of arsenic in Ketza River mine tailings using X-ray absorption spectroscopy. Environ Sci Technol 37:2067–2074
Paktunc D, Foster A, Heald S, Laflamme G (2004) Speciation and characterization of arsenic in gold ores and cyanidation tailings using X-ray absorption spectroscopy. Geochim Cosmochim Acta 68:969–983
Parsons MB, LeBlanc KWG, Hall GEM, Sangster AL, Vaive JE, Pelchat P (2012) Environmental geochemistry of tailings, sediments and surface waters collected from 14 historical gold mining districts in Nova Scotia; Geological Survey of Canada. Open File. doi:10.4095/291923
Patrick WH, Gambrell RP, Faulkner SP (1996) Chapter 42, Redox measurements of soils. In: Sparks DL, Page AL, Helmke PA, Loeppert RH, Soltanpour PN, Tabatabai MA, Johnston CT, Sumner ME (eds) Soil science society of America book series 5—methods of soil analysis, part 3 chemical methods, pp 1255–1274
Peppas A, Komnitsas K, Halikia I (2000) Use of organic covers for acid mine drainage control. Miner Eng 13:563–574
Price WA (2009) Prediction manual for drainage chemistry from sulphidic geologic materials. MEND Report 1.20.1. Chapter 19, p 19-6
Renken K, Yanful EK, Mchaina DM (2005) Effective oxygen diffusion coefficient and field oxygen concentrations below a geosynthetic clay liner (GCL) covering mine tailings. In: Waste containment and remediation, geo-frontiers congress 2005, pp 1–15
Rimstidt JD, Chermak JA, Gagen PA (1994) Rates of reaction of galena, sphalerite, chalcopyrite, and arsenopyrite with Fe(III) in acidic solution. In: Alpers CN, Blowes DW (eds) Environmental chemistry of sulfide oxidation, vol 550, ACS symposium series, pp 2–13
Rochette EA, Li GC, Fendorf SE (1998) Stability of arsenate minerals in soil under biotically generated reducing conditions. Soil Sci Soc Am J 62:1530–1537
Salzsauler KA, Sidenko NV, Sherriff BL (2005) Arsenic mobility in alteration products of sulfide-rich, arsenopyrite-bearing mine wastes, Snow Lake, Manitoba, Canada. Appl Geochem 20:2303–2314
Surour AA, Ahmed AH, Harbi HM (2013) Yukonite-like alteration products (Ca-Fe arsenate and As-rich Fe-oxyhydroxide) formed by in situ weathering in granodiorite, Bi’r Tawilah gold prospect, Saudi Arabia. Eur J Mineral 25:61–70
USEPA (1994) Method 1312: synthetic precipitation leaching procedure. In: Test methods for evaluating solid waste, physical/chemical methods. SW-846, 3rd edn. http://www.epa.gov/epawaste/hazard/testmethods/sw846/online/index.htm
Walker FP, Schreiber ME, Rimstidt JD (2006) Kinetics of arsenopyrite oxidative dissolution by oxygen. Geochim Cosmochim Acta 70:1668–1676
Walker SR, Parsons MB, Jamieson HE, Lanzirotti A (2009) Arsenic mineralogy of near-surface tailings and soils: influences on arsenic mobility and bioaccessibility in the Nova Scotia gold mining districts. Can Mineral 47:533–556
Yanful EK, Aubé BC, Woyshner M, St-Arnaud LC (1994) Field and laboratory performance of engineered covers on the Waite Amulet tailings. In: International land reclamation and mine drainage conference and the third international conference on the abatement of acidic drainage, Pittsburgh, PA, April 24–29, pp 138–147
Yanful EK, Simms PH, Payant SC (1999) Soil covers for controlling acid generation in mine tailings: a laboratory evaluation of the physics and geochemistry. Water Air Soil Poll 114:347–375
Acknowledgements
We thank the three reviewers who offered helpful comments that improved this manuscript. We appreciate field assistance from Cirisse Stephen and Matt Corriveau and analytical assistance from Mary Andrews (ASU, Queen’s University) and Bill LeBlanc (GSC-Atlantic). This project was initially made possible through financial support from the NSERC Metals in the Human–Environment Strategic Network (MITHE-SN) with subsequent funding by NSERC Strategic Grant (364927) to Heather Jamieson, Michael Parsons, Dirk Wallschläger, Danielle Fortin, and Kerry Rowe. Partial funding for the study was also provided through the Environmental Geoscience Program (2009–2014) of the Earth Sciences Sector at Natural Resources Canada. This is contribution number 20170113 of Natural Resources Canada.
Author information
Authors and Affiliations
Corresponding author
Rights and permissions
About this article
Cite this article
DeSisto, S.L., Jamieson, H.E. & Parsons, M.B. Arsenic mobility in weathered gold mine tailings under a low-organic soil cover. Environ Earth Sci 76, 773 (2017). https://doi.org/10.1007/s12665-017-7041-7
Received:
Accepted:
Published:
DOI: https://doi.org/10.1007/s12665-017-7041-7