Abstract
Natural occurrence of chrysotile, a rock-forming serpentine mineral, is largely associated with fluid-rich environments, thus making the fluid chemistry an important factor governing chrysotile growth and stability. Paper examines the effect of alkali chlorides, lowering the H2O activity in fluid, on chrysotile stability at high pressure. The behavior of natural chrysotile (Thetford) in the presence of concentrated NaCl-H2O fluids was studied up to 5 GPa and 400 °C using in-situ Raman spectroscopy and X-ray diffraction combined with resistively heated diamond anvil cell. Reference experiments were also performed on salt-free samples. In salt-free H2O-saturated conditions, chrysotile is stable within the whole temperature range at 1.5–5 GPa. The presence of NaCl in the fluid at XNaCl = mole NaCl/(NaCl+H2O) ≈ 0.1–0.15 strongly suppresses the temperature of chrysotile dehydration at 2–4 GPa to 380 °C, which is about 170 °C lower compared to the equilibrium data for H2O-saturated salt-free system. Talc/talc-like phase only crystallizes at HP-HT conditions as product of the reaction “chrysotile → forsterite + talc”, whereas forsterite appears after the P,T release. This indicates an enhanced solubility of forsterite in supercritical NaCl-H2O fluid at HP-HT conditions. Chrysotile shows disordering/amorphization at unusually low temperature of 150 °C. The shift of the chrysotile dehydration to lower temperatures in saline environment makes this process more operable in natural metamorphic processes in serpentinites. This effect can be extended to other serpentine minerals, including antigorite, a common participant of HP-HT metamorphic reactions in subduction zones.
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Acknowledgements
We thank anonymous reviewers for their profound and constructive criticisms, which helped to improve the manuscript, as well as Prof. L.K. Kazantseva for discussion of the results and Dr. A. Pan for providing us with the chrysotile sample. Diffraction experiments were carried out at the shared research center SSTRC on the basis of the Novosibirsk VEPP-4 - VEPP-2000 complex at BINP SB RAS, using equipment supported by project RFMEFI62119X0022.
Funding
This work is performed on state assignment of IGM SB RAS and is supported by the RFBR project # 18–05-00312.
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Suppl Fig. 1
HP-HT Raman spectra of Ctl, added with 5 wt.% of Tlc + Fo, in the presence of saturated NaCl-H2O fluid (run #2s) collected on P,T increase (a) and on P,T release (b). Ctl bands are numerated with smaller letters, the minor bands of seed Tlc (Tlc-s) and Fo (Fo-s), as well as the bands of new-formed Tlc are numerated with larger letters. Circles mark the bands of a tungstate phase produced by the oxidation of W gasket (the most similar spectrum in RRUFF database #R050139.3). Long vertical arrow in Fig.(a) indicates the run time. (PNG 1289 kb)
Suppl Fig. 1b
(PNG 545 kb)
Suppl Fig. 2
HP-HT Raman spectra of Ctl, added with 5 wt.% of Tlc + Fo, in the presence of saturated NaCl-H2O fluid (run #3s). Ctl bands are numerated with smaller letters, the minor bands of seed Tlc (Tlc-s) and Fo (Fo-s) are numerated with larger letters. (PNG 771 kb)
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Likhacheva, A.Y., Goryainov, S.V., Rashchenko, S.V. et al. In situ observation of chrysotile decomposition in the presence of NaCl-bearing aqueous fluid up to 5 GPa and 400 °C. Miner Petrol 115, 213–222 (2021). https://doi.org/10.1007/s00710-020-00731-x
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DOI: https://doi.org/10.1007/s00710-020-00731-x