A field and reactive transport model study of arsenic in a basaltic rock aquifer

Bergur Sigfusson, Sigurdur R. Gislason, Andrew A. Meharg

Research output: Contribution to journalArticle

11 Citations (Scopus)

Abstract

The use of geothermal energy as a source for electricity and district heating has increased over recent decades. Dissolved As can be an important constituent of the geothermal fluids brought to the Earth's surface. Here the field application of laboratory measured adsorption coefficients of aqueous As species on basaltic glass surfaces is discussed. The mobility of As species in the basaltic aquifer in the Nesjavellir geothermal system, Iceland was modelled by the one-dimensional (1D) reactive transport model PHREEQC ver. 2, constrained by a long time series of field measurements with the chemical composition of geothermal effluent fluids, pH, Eh and, occasionally, Fe- and As-dissolved species measurements. Di-, tri- and tetrathioarsenic species (As(OH)S-2(2-), AsS33-, AsS33- and As(SH)(4)(-)) were the dominant form of dissolved As in geothermal waters exiting the power plant (2.556 mu M total As) but converted to some extent to arsenite (H3AsO3) and arsenate HAsO42- oxyanions coinciding with rapid oxidation of S-2(-) to S2O32- and finally to SO42- during surface runoff before feeding into a basaltic lava field with a total As concentration of 0.882 mu M following dilution with other surface waters.

A continuous 25-a data set monitoring groundwater chemistry along a cross section of warm springs on the Lake Thingvallavatn shoreline allowed calibration of the 1D model. Furthermore, a series of ground water wells located in the basaltic lava field, provided access along the line of flow of the geothermal effluent waters towards the lake. The conservative ion Cl- moved through the basaltic lava field (4100 m) in less than 10 a but As was retarded considerably due to surface reactions and has entered a groundwater well 850 m down the flow path as arsenate in accordance to the prediction of the 1D model. The 1D model predicted a complete breakthrough of arsenate in the year 2100. In a reduced system arsenite should be retained for about 1 ka. (C) 2011 Elsevier Ltd. All rights reserved.

Original languageEnglish
Pages (from-to)553-564
Number of pages12
JournalApplied Geochemistry : Journal of the International Association of Geochemistry and Cosmochemistry
Volume26
Issue number4
Early online date7 Jan 2011
DOIs
Publication statusPublished - Apr 2011

Keywords

  • natural-waters
  • ion chromatography
  • geothermal waters
  • sulfidic waters
  • volcanic gases
  • speciation
  • Iceland
  • Thingvallavatn
  • thioarsenates
  • spectrometry

Cite this

A field and reactive transport model study of arsenic in a basaltic rock aquifer. / Sigfusson, Bergur; Gislason, Sigurdur R.; Meharg, Andrew A.

In: Applied Geochemistry : Journal of the International Association of Geochemistry and Cosmochemistry , Vol. 26, No. 4, 04.2011, p. 553-564.

Research output: Contribution to journalArticle

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N2 - The use of geothermal energy as a source for electricity and district heating has increased over recent decades. Dissolved As can be an important constituent of the geothermal fluids brought to the Earth's surface. Here the field application of laboratory measured adsorption coefficients of aqueous As species on basaltic glass surfaces is discussed. The mobility of As species in the basaltic aquifer in the Nesjavellir geothermal system, Iceland was modelled by the one-dimensional (1D) reactive transport model PHREEQC ver. 2, constrained by a long time series of field measurements with the chemical composition of geothermal effluent fluids, pH, Eh and, occasionally, Fe- and As-dissolved species measurements. Di-, tri- and tetrathioarsenic species (As(OH)S-2(2-), AsS33-, AsS33- and As(SH)(4)(-)) were the dominant form of dissolved As in geothermal waters exiting the power plant (2.556 mu M total As) but converted to some extent to arsenite (H3AsO3) and arsenate HAsO42- oxyanions coinciding with rapid oxidation of S-2(-) to S2O32- and finally to SO42- during surface runoff before feeding into a basaltic lava field with a total As concentration of 0.882 mu M following dilution with other surface waters.A continuous 25-a data set monitoring groundwater chemistry along a cross section of warm springs on the Lake Thingvallavatn shoreline allowed calibration of the 1D model. Furthermore, a series of ground water wells located in the basaltic lava field, provided access along the line of flow of the geothermal effluent waters towards the lake. The conservative ion Cl- moved through the basaltic lava field (4100 m) in less than 10 a but As was retarded considerably due to surface reactions and has entered a groundwater well 850 m down the flow path as arsenate in accordance to the prediction of the 1D model. The 1D model predicted a complete breakthrough of arsenate in the year 2100. In a reduced system arsenite should be retained for about 1 ka. (C) 2011 Elsevier Ltd. All rights reserved.

AB - The use of geothermal energy as a source for electricity and district heating has increased over recent decades. Dissolved As can be an important constituent of the geothermal fluids brought to the Earth's surface. Here the field application of laboratory measured adsorption coefficients of aqueous As species on basaltic glass surfaces is discussed. The mobility of As species in the basaltic aquifer in the Nesjavellir geothermal system, Iceland was modelled by the one-dimensional (1D) reactive transport model PHREEQC ver. 2, constrained by a long time series of field measurements with the chemical composition of geothermal effluent fluids, pH, Eh and, occasionally, Fe- and As-dissolved species measurements. Di-, tri- and tetrathioarsenic species (As(OH)S-2(2-), AsS33-, AsS33- and As(SH)(4)(-)) were the dominant form of dissolved As in geothermal waters exiting the power plant (2.556 mu M total As) but converted to some extent to arsenite (H3AsO3) and arsenate HAsO42- oxyanions coinciding with rapid oxidation of S-2(-) to S2O32- and finally to SO42- during surface runoff before feeding into a basaltic lava field with a total As concentration of 0.882 mu M following dilution with other surface waters.A continuous 25-a data set monitoring groundwater chemistry along a cross section of warm springs on the Lake Thingvallavatn shoreline allowed calibration of the 1D model. Furthermore, a series of ground water wells located in the basaltic lava field, provided access along the line of flow of the geothermal effluent waters towards the lake. The conservative ion Cl- moved through the basaltic lava field (4100 m) in less than 10 a but As was retarded considerably due to surface reactions and has entered a groundwater well 850 m down the flow path as arsenate in accordance to the prediction of the 1D model. The 1D model predicted a complete breakthrough of arsenate in the year 2100. In a reduced system arsenite should be retained for about 1 ka. (C) 2011 Elsevier Ltd. All rights reserved.

KW - natural-waters

KW - ion chromatography

KW - geothermal waters

KW - sulfidic waters

KW - volcanic gases

KW - speciation

KW - Iceland

KW - Thingvallavatn

KW - thioarsenates

KW - spectrometry

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DO - 10.1016/j.apgeochem.2011.01.013

M3 - Article

VL - 26

SP - 553

EP - 564

JO - Applied Geochemistry : Journal of the International Association of Geochemistry and Cosmochemistry

JF - Applied Geochemistry : Journal of the International Association of Geochemistry and Cosmochemistry

SN - 0883-2927

IS - 4

ER -