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Natural Distillation of Solutions and Opal Formation in Closed Vapor–Liquid Hydrothermal Systems

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Abstract

The experiments were performed with water (0.5 g) saturated with silica relative to quartz (10.3 mmol/kg) in sealed platinum ampoules at 300°C. After quenching, the solutions were analyzed by ICP‑AES and photometry, while the ampoule walls and solid phases were analyzed by scanning electron microscopy, X-ray energy-dispersion analysis, atomic force microscopy, and profilometry. In the new ampoules with smooth inner walls, the molality of silica in liquid solution (m) did not change over time, which is consistent with the stability of quartz under these conditions. In the same ampoules, but with rough inner walls, the m value decreased over time to 0.06 mmol/kg, and metastable opal-A was deposited on the ampoule walls above the liquid water level. The decrease in m over time obeyed an exponential law that described the gradual replacement of the solution with vapor condensate. This unusual behavior of silica was explained by natural distillation supported by the predominant evaporation of a thin water film on the rough walls. The evaporation (distillation) rate was 0.1–0.8 g/day and depended on the roughness parameters and the direction of small temperature gradient on the autoclave surface. Distillation modeling based on the equations of lifting the solution film along the rough wall, transfer and deposition of silica, allowed us to calculate the supersaturation in the fluid film, the deposition/dissolution rates of the opal, and its effective thickness and particle size depending on the time and height above the solution level. The results of modeling and experiments were consistent with each other and led to the conclusion that the permanent mass transfer of silica between water, vapor and opal maintained a non-equilibrium steady state of the system. Distillation of solutions can occur also in natural cavities containing various minerals when water–vapor interface and rough hydrophilic walls are presented. As a result, cavities can migrate downwards and recrystallize large volumes of rock.

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ACKNOWLEDGMENTS

The authors thank I.N. Gromyak for the analysis of experimental solutions with low silica content by ICP-AES and A.A. Burmistrov for the study of solid phases in a scanning electron microscope. The authors thank Associate Editor Lawrence Anovitz and three anonymous reviewers for their critical comments and useful suggestions. V. Balashov acknowledges support from the Penn State Earth and Environmental Systems Institute (Director S.L. Brantley). The experimental part of the work was carried out within the framework of the state task 0137-2019-0016 of the Vernadsky Institute of Geochemistry and Analytical Chemistry and was financially supported by the Russian Foundation for Basic Research, project no. 06-05-64110.

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  1. Vernadsky Institute of Geochemistry and Analytical Chemistry, Russian Academy of Sciences, 119991, Moscow, Russia

    V. A. Alekseyev & L. S. Medvedeva

  2. Earth and Environmental Systems Institute, Pennsylvania State University University Park, 16802, Building, 2217 EES, PA, United States

    V. N. Balashov

  3. Shubnikov Institute of Crystallography, Russian Academy of Sciences, 119333, Moscow, Russia

    A. M. Opolchentsev

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  1. V. A. Alekseyev
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Alekseyev, V.A., Balashov, V.N., Medvedeva, L.S. et al. Natural Distillation of Solutions and Opal Formation in Closed Vapor–Liquid Hydrothermal Systems. Geochem. Int. 60, 1393–1414 (2022). https://doi.org/10.1134/S0016702922130031

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