Skip to main content
Article
Licensed
Unlicensed Requires Authentication

Diffusion of F and Cl in dry rhyodacitic melt

  • EMAIL logo , and
Published/Copyright: November 2, 2019
Become an author with De Gruyter Brill

Abstract

Chemical diffusion of F and Cl has been experimentally determined in a rhyodacitic melt obtained from remelting a sample of Hekla pumice (Iceland). Diffusion couple experiments were conducted in a vertical tube furnace over a temperature range of 750–950 °C and in air for durations of 1 to 35 days. Concentration profiles of F and Cl were obtained for the quenched samples using an electron microprobe.

Fluorine and chlorine exhibit Arrhenian behavior over the range of temperature investigated here. The pre-exponential factors of F and Cl are D0(F) = 4.3 × 10-4 and D0(Cl) = 1.6 × 10-5 m2/s. Fluorine diffusion coefficients vary in the order of 1 × 10-15 to 1 × 10-13 m2/s, whereas Cl diffusivity is up to two orders of magnitude slower. The activation energies for F and Cl diffusivities are equal within error at 223 ± 31 and 229 ± 52 kJ/mol, respectively.

The difference in diffusivity between F and Cl is particularly pronounced in the melt of our study, compared to results obtained for other magmatic melt compositions. This means that the potential for diffusive fractionation exists and may occur especially under conditions of magma ascent and bubble growth, as this would favor partitioning of the relatively fast-diffusing halogens into growing bubbles, due to H2O exsolution. A dependence of diffusivity on atomic radius observed here is enhanced over that observed in more basic, less viscous melts, indicating that diffusive fractionation is more likely to be pronounced in more silicic, more viscous systems. A proper parameterization and modeling of diffusive fractionation of halogens in actively degassing volcanic systems thus holds the potential of serving as a tool for quantifying the processes responsible for volcanic unrest.

Acknowledgments

We thank B. Scheu, U. Küppers, and K.-U. Hess for their assistance during sample preparation and N. Groschopf and S. Buhre for their assistance with electron microprobe analyses. B. Watson, H. Balcone-Boissard, and one anonymous reviewer are thanked for their insightful comments that helped to improve this paper.

  1. Funding

    This research is part of the Ph.D. thesis of Y. Feisel and is supported a fellowship of the Gutenberg Research College of the Johannes Gutenberg-University of Mainz to D.B. Dingwell. Additional support was provided by the VAMOS research center of the Johannes Gutenberg-University.

References cited

Aiuppa, A., Bonfanti, P., Brusca, L., D’Alessandro, W., Federico, C., and Parello, F. (2001) Evaluation of the environmental impact of volcanic emissions from the chemistry of rainwater: Mount Etna area (Sicily). Applied Geochemistry, 16, 985–1000.10.1016/S0883-2927(00)00075-5Search in Google Scholar

Aiuppa, A., Baker, D.R., and Webster, J.D. (2009) Halogens in volcanic systems. Chemical Geology, 263, 1–18.10.1016/j.chemgeo.2008.10.005Search in Google Scholar

Alletti, M., Baker, D.R., and Freda, C. (2007) Halogen diffusion in a basaltic melt. Geochimica et Cosmochimica Acta, 71, 3570–3580.10.1016/j.gca.2007.04.018Search in Google Scholar

Baasner, A., Schmidt, B.C., and Webb, S.L. (2013) Compositional dependence of the rheology of halogen (F, Cl) bearing aluminosilicate melts. Chemical Geology, 346, 172–183.10.1016/j.chemgeo.2012.09.020Search in Google Scholar

Bai, T.B., and Koster van Groos, A.F. (1994) Diffusion of chlorine in granitic melts. Geochimica et Cosmochimica Acta, 58, 113–123.10.1016/0016-7037(94)90450-2Search in Google Scholar

Baker, D.R., and Alletti, M. (2012) Fluid saturation and volatile partitioning between melts and hydrous fluids in crustal magmatic systems: The contribution of experimental measurements and solubility models. Earth-Science Reviews, 114, 298–324.10.1016/j.earscirev.2012.06.005Search in Google Scholar

Baker, D.R., and Balcone-Boissard, H. (2009) Halogen diffusion in magmatic systems: Our current state of knowledge. Chemical Geology, 263, 82–88.10.1016/j.chemgeo.2008.10.010Search in Google Scholar

Balcone-Boissard, H., Baker, D.R., Villemant, B., and Boudon, G. (2009) F and Cl diffusion in phonolitic melts: Influence of the Na/K ratio. Chemical Geology, 263, 89–98.10.1016/j.chemgeo.2008.08.018Search in Google Scholar

Bobrowski, N., Hönninger, G., Galle, B., and Platt, U. (2003) Detection of bromine monoxide in a volcanic plume. Nature, 423, 273–276.10.1038/nature01625Search in Google Scholar PubMed

Bobrowski, N., von Glasow, R., Aiuppa, A., Inguaggiato, S., Louban, I., Ibrahim, O.W., and Platt, U. (2007) Reactive halogen chemistry in volcanic plumes. Journal of Geophysical Research Atmospheres, 112.10.1029/2006JD007206Search in Google Scholar

Böhm, A., and Schmidt, B.C. (2013) Fluorine and chlorine diffusion in phonolitic melt. Chemical Geology, 346, 162–171.10.1016/j.chemgeo.2012.09.005Search in Google Scholar

Boichu, M., Oppenheimer, C., Roberts, T.J., Tsanev, V., and Kyle, P.R. (2011) On bromine, nitrogen oxides and ozone depletion in the tropospheric plume of Erebus volcano (Antarctica). Atmospheric Environment, 45, 3856–3866.10.1016/j.atmosenv.2011.03.027Search in Google Scholar

Boudon, G., Balcone-Boissard, H., Villemant, B., and Morgan, D.J. (2015) What factors control superficial lava dome explosivity? Scientific Reports, 5.10.1038/srep14551Search in Google Scholar

Carroll, M.R., and Webster, J.D. (1994) Solubilities of sulfur, noble gases, nitrogen, chlorine, and fluorine in magmas. In M.R. Carroll and J.R. Holloway, Eds., Volatiles in Magmas, 30, p. 231–279. Reviews in Mineralogy, Mineralogical Society of America, Chantilly, Virginia.10.1515/9781501509674-013Search in Google Scholar

Castro, J.M., Cordonnier, B., Schipper, C.I., Tuffen, H., Baumann, T.S., and Feisel, Y. (2016) Rapid laccolith intrusion driven by explosive volcanic eruption. Nature Communications, 7.10.1038/ncomms13585Search in Google Scholar

Crank, J. (1975) The Mathematics of Diffusion. Clarendon-Oxford, London.Search in Google Scholar

Dingwell, D.B. (1990) Effects of structural relaxation on cationic tracer diffusion in silicate melts. Chemical Geology, 82, 209–216.10.1016/0009-2541(90)90082-ISearch in Google Scholar

Dingwell, D.B., and Hess, K.U. (1998) Melt viscosities in the system Na-Fe-Si-OF-Cl; contrasting effects of F and Cl in alkaline melts. American Mineralogist, 83, 1016–1021.10.2138/am-1998-9-1009Search in Google Scholar

Dingwell, D.B., and Scarfe, C.M. (1984) Chemical diffusion of fluorine in jadeite melt at high pressure. Geochimica et Cosmochimica Acta, 48, 2517–2525.10.1016/0016-7037(84)90302-8Search in Google Scholar

Dingwell, D.B., and Scarfe, C.M. (1985) Chemical diffusion of fluorine in melts in the system Na2O-Al2O3- SiO2 Earth and Planetary Science Letters, 73, 377–384.10.1016/0012-821X(85)90085-8Search in Google Scholar

Dingwell, D.B., and Webb, S.L. (1990) Relaxation in silicate melts. European Journal of Mineralogy, 2, 427–449.10.1127/ejm/2/4/0427Search in Google Scholar

Dingwell, D.B., Scarfe, C.M., and Cronin, D.J. (1985) The effect of fluorine on viscosities in the system sodium monoxide-aluminum oxide-silicon dioxide: implications for phonolites, trachytes and rhyolites. American Mineralogist, 70, 80–87.Search in Google Scholar

Fortin, M.A., Watson, E.B., and Stern, R. (2017) The isotope mass effect on chlorine diffusion in dacite melt, with implications for fractionation during bubble growth. Earth and Planetary Science Letters, 480, 15–24.10.1016/j.epsl.2017.09.042Search in Google Scholar

Giordano, D., and Dingwell, D.B. (2003) Non-Arrhenian multicomponent melt viscosity: A model. Earth and Planetary Science Letters, 208, 337–349.10.1016/S0012-821X(03)00042-6Search in Google Scholar

Giordano, D., Russell, J.K., and Dingwell, D.B. (2008) Viscosity of magmatic liquids: A model. Earth and Planetary Science Letters, 271, 123–134.10.1016/j.epsl.2008.03.038Search in Google Scholar

Glasstone, S., Laidler, K.J., and Eyring, H. (1941) The Theory of Rate Processes. McGraw-Hill.Search in Google Scholar

Gonnermann, H.M., and Manga, M. (2007) The fluid mechanics inside a volcano. Annual Review of Fluid Mechanics, 39, 321–356.10.1146/annurev.fluid.39.050905.110207Search in Google Scholar

Henderson, P., Nolan, J., Cunningham, G.C., and Lowry, R.K. (1985) Structural controls and mechanisms of diffusion in natural silicate melts. Contributions to Mineralogy and Petrology, 89, 263–272.10.1007/BF00379459Search in Google Scholar

Jambon, A., and Semet, M.P. (1978) Lithium diffusion in silicate glasses of Albite, Orthoclase, and Obsidian composition: an ion-microprobe determination. Earth and Planetary Science Letters, 37, 445–450.10.1016/0012-821X(78)90060-2Search in Google Scholar

Liang, Y., Richter, F.M., Davis, A.M., and Watson, E.B. (1996) Diffusion in silicate melts: I. Self diffusion in CaO-Al2O3-SiO2 at 1500° C and 1 GPa. Geochimica et Cosmochimica Acta, 60, 4353–4367.10.1016/S0016-7037(96)00288-8Search in Google Scholar

Lowenstern, J.B., Bleick, H., Vazquez, J.A., Castro, J.M., and Larson, P.B. (2012) Degassing of Cl, F, Li, and Be during extrusion and crystallization of the rhyolite dome at Volcán Chaitén, Chile during 2008 and 2009. Bulletin of Volcanology, 74, 2303–2319.10.1007/s00445-012-0663-4Search in Google Scholar

Lowry, R.K., Hender, P., and Nolan, J. (1982) Tracer diffusion of some alkali, alkaline-earth and transition element ions in a basaltic and an andesitic melt, and the implications concerning melt structure. Contributions to Mineralogy and Petrology, 80, 254–261.10.1007/BF00371355Search in Google Scholar

Lux, G. (1987) The behavior of noble gases in silicate liquids: Solution, diffusion, bubbles and surface effects, with applications to natural samples. Geochimica et Cosmochimica Acta, 51, 1549–1560.10.1016/0016-7037(87)90336-XSearch in Google Scholar

Manning, D.A.C. (1981) The effect of fluorine on liquidus phase relationships in the system Qz–Ab–Or with excess water at 1 kb. Contributions to Mineralogy and Petrology, 76, 206–215.10.1007/BF00371960Search in Google Scholar

Margaritz, M., and Hofmann, A.W. (1978) Diffusion of Sr, Ba and Na in obsidian. Geochimica et Cosmochimica Acta, 42, 595–605.10.1016/0016-7037(78)90004-2Search in Google Scholar

Mysen, B.O. (1988) Structure and Properties of Silicate Melts. Elsevier, Amsterdam.Search in Google Scholar

Roberts, T. (2018) Ozone depletion in tropospheric volcanic plumes: From halogen-poor to halogen-rich emissions. Geosciences, 8, 68.10.3390/geosciences8020068Search in Google Scholar

Schipper, C.I., Castro, J.M., Tuffen, H., Wadsworth, F.B., Chappell, D., Pantoja, A.E., Simpson, M.P., and Le Ru, E.C. (2015) Cristobalite in the 2011–2012 Cordón Caulle eruption (Chile). Bulletin of Volcanology, 77, 34.10.1007/s00445-015-0925-zSearch in Google Scholar

Schipper, I.C., Mandon, C., Maksimenko, A., Castro, J.M., Conway, C.E., Hauer, P., Kirilova, M., and Kilgour, G. (2017) Vapor-phase cristobalite as a durable indicator of magmatic pore structure and halogen degassing: an example from White Island volcano (New Zealand). Bulletin of Volcanology, 79, 74.10.1007/s00445-017-1157-1Search in Google Scholar

Schipper, C.I., Castro, J., Kennedy, B., Christenson, B., Aiuppa, A., Alloway, B., Forte, P., Seropian, G., and Tuffen, H. (2019) Halogen (Cl, F) release during explosive, effusive, and intrusive phases of the 2011 rhyolitic eruption at Cordón Caulle volcano (Chile). Volcanica, 2, 73–90.10.30909/vol.02.01.7390Search in Google Scholar

Shimizu, N., and Kushiro, I. (1984) Diffusivity of oxygen in jadeite and diopside melts at high pressures. Geochimica et Cosmochimica Acta, 48, 1295–1303.10.1016/0016-7037(84)90063-2Search in Google Scholar

Spilliaert, N., Métrich, N., and Allard, P. (2006) S-Cl-F degassing pattern of water-rich alkali basalt: Modelling and relationship with eruption styles on Mount Etna volcano. Earth and Planetary Science Letters, 248, 772–786.10.1016/j.epsl.2006.06.031Search in Google Scholar

Surl, L., Donohoue, D., Aiuppa, A., Bobrowski, N., and Von Glasow, R. (2015) Quantification of the depletion of ozone in the plume of Mount Etna. Atmospheric Chemistry and Physics, 15, 2613–2628.10.5194/acp-15-2613-2015Search in Google Scholar

Sverrisdottir, G. (2007) Hybrid magma generation preceding Plinian silicic eruptions at Hekla, Iceland: Evidence from mineralogy and chemistry of two zoned deposits. Geological Magazine, 144, 643–659.10.1017/S0016756807003470Search in Google Scholar

Symonds, R.B., Rose, W.I., Bluth, G.J.S., and Gerlach, T.M. (1994) Volcanic-gas studies: methods, results, and applications. In M.R. Carroll and J.R. Holloway, Eds., Volatiles in Magmas, vol. 30, p. 1–66. Reviews in Mineralogy, Mineralogical Society of America, Chantilly, Virginia.10.1515/9781501509674-007Search in Google Scholar

Thordarson, T., and Larsen, G. (2007) Volcanism in Iceland in historical time: Volcano types, eruption styles and eruptive history. Journal of Geodynamics, 43, 118–152.10.1016/j.jog.2006.09.005Search in Google Scholar

von Glasow, R., Bobrowski, N., and Kern, C. (2009) The effects of volcanic eruptions on atmospheric chemistry. Chemical Geology, 263, 131–142.10.1016/j.chemgeo.2008.08.020Search in Google Scholar

Watson, E.B. (2017) Diffusive fractionation of volatiles and their isotopes during bubble growth in magmas. Contributions to Mineralogy and Petrology, 172.10.1007/s00410-017-1384-7Search in Google Scholar

Watson, E.B., and Bender, J.F. (1980) Diffusion of cesium, samarium, strontium, and chlorine in molten silicate at high temperatures and pressures. Geological Society of America, Abstracts with Programs, 12, 545.Search in Google Scholar

Weber, G., and Castro, J.M. (2017) Phase petrology reveals shallow magma storage prior to large explosive silicic eruptions at Hekla volcano, Iceland. Earth and Planetary Science Letters, 466, 168–180.10.1016/j.epsl.2017.03.015Search in Google Scholar

Webster, J.D., and Duffield, W.A. (1994) Extreme halogen abundances in tin-rich magma of the Taylor Creek rhyolite, New Mexico. Economic Geology, 89, 849–850.10.2113/gsecongeo.89.4.840Search in Google Scholar

Webster, J.D., Baker, D.R., and Aiuppa, A. (2018) Halogens in mafic and intermediate-silica content magmas. In D.E. Harlov and L.Y. Aranovich, Eds., The Role of Halogens in Terrestrial and Extraterrestrial Geochemical Processes, pp. 307–430. Springer-Verlag.10.1007/978-3-319-61667-4_6Search in Google Scholar

Yoshimura, S. (2018) Chlorine diffusion in rhyolite under low-H2O conditions. Chemical Geology, 483, 619–630.10.1016/j.chemgeo.2018.03.032Search in Google Scholar

Zhang, Y., Ni, H., and Chen, Y. (2010) Diffusion data in silicate melts. In Y. Zhang and D.J. Cherniak, Eds., Diffusion in Minerals and Melts, 72, p. 311–408. Reviews in Mineralogy and Geochemistry, Mineralogical Society of America, Chantilly, Virginia.10.1515/9781501508394-009Search in Google Scholar

Received: 2019-05-02
Accepted: 2019-07-27
Published Online: 2019-11-02
Published in Print: 2019-11-26

© 2019 Walter de Gruyter GmbH, Berlin/Boston

Downloaded on 21.4.2026 from https://www.degruyterbrill.com/document/doi/10.2138/am-2019-7095/html
Scroll to top button