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Mineral control of arsenic content in thermal waters from volcano-hosted hydrothermal systems: insights from island of Ischia and Phlegrean Fields (Campanian Volcanic Province, Italy)
Author(s)
Language
English
Status
Published
Peer review journal
Yes
Title of the book
Issue/vol(year)
/229 (2006)
Publisher
Elsevier
Pages (printed)
313–330
Issued date
2006
Alternative Location
Abstract
This paper documents arsenic concentrations in 157 groundwater samples from the island of Ischia and the Phlegrean Fields,
two of the most active volcano-hosted hydrothermal systems from the Campanian Volcanic Province (Southern Italy), in an attempt
to identify the environmental conditions and mineral-solution reactions governing arsenic aqueous cycling. On Ischia and in the
Phlegrean Fields, groundwaters range in composition from NaCl brines, which we interpret as the surface discharge of deep
reservoir fluids, to shallow-depth circulating fluids, the latter ranging from acid-sulphate steam-heated to hypothermal, cold,
bicarbonate groundwaters. Arsenic concentrations range from 1.6 to 6900 μg·l−1 and from 2.6 to 3800 μg·l−1 in the Phlegrean
Fields and on Ischia, respectively. They increase with increasing water temperature and chlorine contents, and in the sequence
bicarbonate groundwatersbsteam-heated groundwatersbNaCl brines. According to thermochemical modeling, we propose that
high As concentrations in NaCl brines form after prolonged water–rock interactions at reservoir T, fO2 and fH2S conditions, and
under the buffering action of an arsenopyrite+pyrite+pyrrhotite rock assemblage. On their ascent toward the surface, NaCl brines
become diluted by As-depleted meteoric-derived bicarbonate groundwaters, giving rise to hybrid water types with intermediate to
low As contents. Steam-heated groundwaters give their intermediate to high As concentrations to extensive rock leaching promoted
by interaction with As-bearing hydrothermal steam.
two of the most active volcano-hosted hydrothermal systems from the Campanian Volcanic Province (Southern Italy), in an attempt
to identify the environmental conditions and mineral-solution reactions governing arsenic aqueous cycling. On Ischia and in the
Phlegrean Fields, groundwaters range in composition from NaCl brines, which we interpret as the surface discharge of deep
reservoir fluids, to shallow-depth circulating fluids, the latter ranging from acid-sulphate steam-heated to hypothermal, cold,
bicarbonate groundwaters. Arsenic concentrations range from 1.6 to 6900 μg·l−1 and from 2.6 to 3800 μg·l−1 in the Phlegrean
Fields and on Ischia, respectively. They increase with increasing water temperature and chlorine contents, and in the sequence
bicarbonate groundwatersbsteam-heated groundwatersbNaCl brines. According to thermochemical modeling, we propose that
high As concentrations in NaCl brines form after prolonged water–rock interactions at reservoir T, fO2 and fH2S conditions, and
under the buffering action of an arsenopyrite+pyrite+pyrrhotite rock assemblage. On their ascent toward the surface, NaCl brines
become diluted by As-depleted meteoric-derived bicarbonate groundwaters, giving rise to hybrid water types with intermediate to
low As contents. Steam-heated groundwaters give their intermediate to high As concentrations to extensive rock leaching promoted
by interaction with As-bearing hydrothermal steam.
References
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Treuil, M., Valenza, M., 2000. Mobility and fluxes of major, minor
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(Sicily). Geochim. Cosmochim. Acta 64, 1827–1841.
Aiuppa, A., D'Alessandro,W., Federico, C., Palumbo, B., Valenza, M.,
2003. The aquatic geochemistry of arsenic in volcanic groundwaters
from southern Italy. Appl. Geochem. 18, 1283–1296.
Aiuppa, A., Federico, C., Allard, P., Gurrieri, S., Valenza, M., 2005.
Trace metal modelling of groundwater–gas–rock interactions in a
volcanic aquifer: Mount Vesuvius, Southern Italy. Chem. Geol.
2163-4, 289–311.
Allard, P., Maiorani, A., Tedesco, D., Cortecci, G., Turi, B., 1991.
Isotopic study of the origin of sulfur and carbon in Solfatara
fumaroles, Campi Flegrei Caldera. J. Volcanol. Geotherm. Res. 48,
139–159.
Ballantyne, J.M., Moore, J.N., 1988. Arsenic geochemistry in
geothermal systems. Geochim. Cosmochim. Acta 52, 475–483.
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springs, geysers, and streams in yellowstone national Park,
Wyoming, 1999–2000. Open-File Rep. U.S. Geolo. Surv. 02-382
(112 pp.).
Barberi, F., Hill, D.P., Innocenti, F., Luongo, G., Treuil, M. (Eds.),
1984. The 1982–1984 Bradyseismic Crisis at Phlegrean Fields-
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dissolved carbon isotope composition of thermal waters of the
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surveillance. J. Volcanol. Geotherm. Res. 90, 219–240.
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signature of the basement rocks from the Campi Flegrei
geothermal field (Naples, southern Italy): inferences about the origin and evolution of its hydrothermal fluids. J. Volcanol.
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in the Phlegrean Fields from 1970 to 1990. Boll. Soc. Geol. Ital.
111, 409–422.
Chiodini, G., Marini, L., 1998. Hydrothermal gas equilibria: the H2O–
H2–CO2–CO–CH4 system. Geochim. Cosmochim. Acta 62,
2673–2687.
Chiodini, G., Comodi, P., Giaquinto, S., 1988. Ammonia and boric
acid in steam and water. Experimental data from geothermal
wells in the Phlegrean Fields, Naples, Italy. Geothermics 17,
711–718.
Chiodini, G., Frondini, F., Cardellini, C., Granieri, D., Marini, L.,
Ventura, G., 2001. CO2 degassing and energy release at Solfatara
Volcano, Campi Flegrei, Italy. J. Geophys. Res. 106 (B8),
16213–16221.
Chiodini, G., Todesco, M., Caliro, S., Del Gaudio, C., Macedonio, G.,
Russo, M., 2003. Magma degassing as a trigger of bradyseismic
events: the case of the Phlegrean Fields (Italy). Geophys. Res. Lett.
30 (8), 1434, doi:10.1029/2002GL016790.
Chiodini, G., Avino, R., Brombach, T., Caliro, S., Cardellini, C., De
Vita, S., Frondini, F., Granieri, D., Marotta, E., Ventura, G., 2004.
Fumarolic and diffuse soil degassing west of Mount Epomeo,
Ischia, Italy. J. Volcanol. Geotherm. Res. 133, 291–309.
Cidu, R., Fanfani, L., Lattanzi, P. (Eds.), 2003. Arsenic GeochemistryAppl.
Geochem. Spec., pp. 18–19.
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indicator of heat transfer at Solfatara fumaroles, Phlegrean Fields
(Italy). Bull. Volcanol. 47, 295–302.
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the As–S system: a case study for geothermal As transport. Appl.
Geochem. 18, 1325–1345.
Criaud, A., Fouillac, C., 1989. The distribution of arsenic(III) and
arsenic(V) in geothermal waters: examples from the Massif Central
of France, the island of Dominica in the Leeward Islands of the
Caribbean, the Valles Caldera of New Mexico, USA, and
southwest Bulgaria. Chem. Geol. 76, 259–269.
D'Amore, F., Panichi, C., 1980. Evaluation of deep temperatures of
hydrothermal systems by a new gas geothermometer. Geochim.
Cosmochim. Acta 44, 549–556.
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Geochemistry of thermal waters on the Island of Ischia.
(Campania, Italy). Geothermics 13, 361–374.
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geothermal system: a fluid inclusion study of the Mofete and
San Vito fields. J. Volcanol. Geotherm. Res. 36, 303–326.
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Academic Press, New York.
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Parello, F., Valenza, M., 2002. Magmatic gas–water interactions
at Vesuvius volcano: major, minor and trace element composition
of the volcanic aquifer. Geochim. Cosmochim. Acta 66,
963–981.
Giggenbach, W.F., 1988. Geothermal solute equilibria. Derivation of
Na–K–Mg–Ca geoindicators. Geochim. Cosmochim. Acta 52,
2749–2763.
Giggenbach, W.F., 1991. Chemical techniques in geothermal
exploration. In: D'Amore, F. (Ed.), Applications of Geochemistry
in Geothermal Reservoir Development. UNITAR/UNDP,
pp. 119–144.
Gillot, P.Y., Chiesa, S., Pasquarè, G., Vezzoli, L., 1982. b33,000 yr K–
Ar dating of the volcano-tectonic horst of the isle of Ischia, Gulf of
Naples. Nature 229, 242–244.
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(Ed.), Encyclopaedia of Volcanoes. Academic Press.
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781–790.
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formation of hydrothermal ore deposits. Nature 370, 519–527.
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the hydrothermal chemistry of arsenic, and their significance for
the paragenic sequence of some cassirite-arsenopyrite-base metal
sulphide deposits. Econ. Geol. 81, 511–529.
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Aiuppa, A., D'Alessandro,W., Federico, C., Palumbo, B., Valenza, M.,
2003. The aquatic geochemistry of arsenic in volcanic groundwaters
from southern Italy. Appl. Geochem. 18, 1283–1296.
Aiuppa, A., Federico, C., Allard, P., Gurrieri, S., Valenza, M., 2005.
Trace metal modelling of groundwater–gas–rock interactions in a
volcanic aquifer: Mount Vesuvius, Southern Italy. Chem. Geol.
2163-4, 289–311.
Allard, P., Maiorani, A., Tedesco, D., Cortecci, G., Turi, B., 1991.
Isotopic study of the origin of sulfur and carbon in Solfatara
fumaroles, Campi Flegrei Caldera. J. Volcanol. Geotherm. Res. 48,
139–159.
Ballantyne, J.M., Moore, J.N., 1988. Arsenic geochemistry in
geothermal systems. Geochim. Cosmochim. Acta 52, 475–483.
Ball, J.W., McCleskey, R.B., Nordstrom, D.K., Holloway, J.M.,
Verplanck, P.L., 2002. Water-chemistry data for selected
springs, geysers, and streams in yellowstone national Park,
Wyoming, 1999–2000. Open-File Rep. U.S. Geolo. Surv. 02-382
(112 pp.).
Barberi, F., Hill, D.P., Innocenti, F., Luongo, G., Treuil, M. (Eds.),
1984. The 1982–1984 Bradyseismic Crisis at Phlegrean Fields-
Bull. Volcanol. Special Issue, vol. 74.
Barnes, H.L. (Ed.), 1997. Geochemistry of Hydrothermal Ore
Deposits. John Wiley & Sons.
Barton Jr., P.B., Skinner, B.J., 1979. Sulfide mineral stabilities, In:
Barnes, H.L. (Ed.), Geochemistry of Hydrothermal Ore Deposits,
second edition. John Wiley & Sons, New York, pp. 278–403.
Brondi, M., Dall'Aglio, M., Ghiara, E., 1986. Elementi in traccia di
interesse geochimico e tossicologico nei fluidi termali e geotermici
dei Campi Flegrei e di Larderello. Acqua Aria 10, 1103–1111.
Caliro, S., Panichi, C., Stanzione, D., 1999. Variation in the total
dissolved carbon isotope composition of thermal waters of the
Island of Ischia (Italy) and its implications for volcanic
surveillance. J. Volcanol. Geotherm. Res. 90, 219–240.
Caprarelli, G., Tsutsumi, M., Turi, B., 1997. Chemical and isotopic
signature of the basement rocks from the Campi Flegrei
geothermal field (Naples, southern Italy): inferences about the origin and evolution of its hydrothermal fluids. J. Volcanol.
Geotherm. Res. 76, 63–82.
Celico, P., Dall'Aglio, M., Ghiara, M.R., Stanzione, D., Brondi, M.,
Prosperi, M., 1992. Geochemical monitoring of the thermal fluids
in the Phlegrean Fields from 1970 to 1990. Boll. Soc. Geol. Ital.
111, 409–422.
Chiodini, G., Marini, L., 1998. Hydrothermal gas equilibria: the H2O–
H2–CO2–CO–CH4 system. Geochim. Cosmochim. Acta 62,
2673–2687.
Chiodini, G., Comodi, P., Giaquinto, S., 1988. Ammonia and boric
acid in steam and water. Experimental data from geothermal
wells in the Phlegrean Fields, Naples, Italy. Geothermics 17,
711–718.
Chiodini, G., Frondini, F., Cardellini, C., Granieri, D., Marini, L.,
Ventura, G., 2001. CO2 degassing and energy release at Solfatara
Volcano, Campi Flegrei, Italy. J. Geophys. Res. 106 (B8),
16213–16221.
Chiodini, G., Todesco, M., Caliro, S., Del Gaudio, C., Macedonio, G.,
Russo, M., 2003. Magma degassing as a trigger of bradyseismic
events: the case of the Phlegrean Fields (Italy). Geophys. Res. Lett.
30 (8), 1434, doi:10.1029/2002GL016790.
Chiodini, G., Avino, R., Brombach, T., Caliro, S., Cardellini, C., De
Vita, S., Frondini, F., Granieri, D., Marotta, E., Ventura, G., 2004.
Fumarolic and diffuse soil degassing west of Mount Epomeo,
Ischia, Italy. J. Volcanol. Geotherm. Res. 133, 291–309.
Cidu, R., Fanfani, L., Lattanzi, P. (Eds.), 2003. Arsenic GeochemistryAppl.
Geochem. Spec., pp. 18–19.
Cioni, R., Corazza, E., Marini, L., 1984. Gas steam ratio as an
indicator of heat transfer at Solfatara fumaroles, Phlegrean Fields
(Italy). Bull. Volcanol. 47, 295–302.
Cleverley, J.S., Benning, L.G., Moutain, B.W., 2003. Reaction path in
the As–S system: a case study for geothermal As transport. Appl.
Geochem. 18, 1325–1345.
Criaud, A., Fouillac, C., 1989. The distribution of arsenic(III) and
arsenic(V) in geothermal waters: examples from the Massif Central
of France, the island of Dominica in the Leeward Islands of the
Caribbean, the Valles Caldera of New Mexico, USA, and
southwest Bulgaria. Chem. Geol. 76, 259–269.
D'Amore, F., Panichi, C., 1980. Evaluation of deep temperatures of
hydrothermal systems by a new gas geothermometer. Geochim.
Cosmochim. Acta 44, 549–556.
De Gennaro, M., Ferreri, M., Ghiara, M.R., Stanzione, D., 1984.
Geochemistry of thermal waters on the Island of Ischia.
(Campania, Italy). Geothermics 13, 361–374.
De Vivo, B., Belkin, H.E., Barbieri, M., Chelini, W., Lattanzi, P.,
Lima, A., Tolomeo, L., 1989. The Campi Flegrei (Italy)
geothermal system: a fluid inclusion study of the Mofete and
San Vito fields. J. Volcanol. Geotherm. Res. 36, 303–326.
Ellis, A.J., Mahon,W.A.J., 1977. Chemistry and Geothermal Systems.
Academic Press, New York.
Federico, C., Aiuppa, A., Allard, P., Bellomo, S., Michel, A.,
Parello, F., Valenza, M., 2002. Magmatic gas–water interactions
at Vesuvius volcano: major, minor and trace element composition
of the volcanic aquifer. Geochim. Cosmochim. Acta 66,
963–981.
Giggenbach, W.F., 1988. Geothermal solute equilibria. Derivation of
Na–K–Mg–Ca geoindicators. Geochim. Cosmochim. Acta 52,
2749–2763.
Giggenbach, W.F., 1991. Chemical techniques in geothermal
exploration. In: D'Amore, F. (Ed.), Applications of Geochemistry
in Geothermal Reservoir Development. UNITAR/UNDP,
pp. 119–144.
Gillot, P.Y., Chiesa, S., Pasquarè, G., Vezzoli, L., 1982. b33,000 yr K–
Ar dating of the volcano-tectonic horst of the isle of Ischia, Gulf of
Naples. Nature 229, 242–244.
Goff, F., Janik, C.J., 2000. Geothermal systems. In: Sugurdsson, H.
(Ed.), Encyclopaedia of Volcanoes. Academic Press.
Guglielminetti, M., 1986. Mofete geothermal fields. Geothermics 15,
781–790.
Hedenquist, J.W., Lowenstern, J.B., 1994. The role of magmas in the
formation of hydrothermal ore deposits. Nature 370, 519–527.
Heinrich, C.A., Eadington, P.E., 1986. Thermodynamic predictions of
the hydrothermal chemistry of arsenic, and their significance for
the paragenic sequence of some cassirite-arsenopyrite-base metal
sulphide deposits. Econ. Geol. 81, 511–529.
Henley, R.W., Truesdell, A.H., Barton, P.B., 1984. Fluid mineral
equilibria in hydrothermal systems. Rev. Econ. Geol. 1 (Society of
Economic Geology).
Hockstein, M.P., Browne, P.R.L., 2000. Surface manifestations of
geothermal systems with volcanic heat sources. In: Sugurdsson, H.
(Ed.), Encyclopaedia of Volcanoes. Academic Press.
Kretschmar, U., Scott, SD., 1976. Phase relations involving arsenopyrite
in the system Fe–As–S and their application. Can. Mineral.
14, 364–386.
Inguaggiato, S., Pecoraino, G., D'Amore, F., 2000. Chemical and
isotopic characterisation of fluid manifestations of Ischia Island. J.
Volcanol. Geotherm. Res. 99, 151–178.
Lima, A., Cicchella, D., Di Francia, S., 2003. Natural contribution of
harmful elements in thermal groundwaters of Ischia Island
(Southern Italy). Environ. Geol. 43, 930–940.
Maest, A.S., Pasilis, S.P., Miller, L.G., Nordstrom, D.K., 1992.
Redox geochemistry of arsenic and iron in Mono Lake,
California, USA. In: Kharaka, Y.K., Maest, A.S. (Eds.), Proc.
7th Internat. Symp. Water–Rock Interaction. A.A. Balkema,
Rotterdam, pp. 507–511.
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