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Quantifying the concurrent changes in rock volume and fluid composition during serpentinization remains a major challenge in assessing its physicochemical effects during continental rifting, seafloor spreading, and subduction. Here we conducted a series of 11 hydrothermal laboratory experiments where cylindrical cores of natural dunite, harzburgite, and pyroxenite were reacted with an aqueous solution at 300 °C and 35 MPa for up to 18 months. Using three-dimensional microcomputed tomography and thermogravimetry, we show that rock volume systematically increased with time and extent of reaction, leading to a volume increase of 44% (±8%) in altered rock domains after 10–18 months of serpentinization. The volume expansion was accompanied by Mg-Ca exchange between fluid and rock, while Fe and Si were largely conserved. We find that the protolith composition (olivine/orthopyroxene ratio) plays a significant role in controlling the fluid chemistry and the proportions of hydrous secondary minerals during serpentinization. Agreement between alteration mineralogy, composition of reacting fluids, and measured volume changes suggests that serpentinization under static conditions is a volume-increasing process in spite of demonstrable mass transfer. Volume expansion implies an increased water carrying capacity and buoyancy force of serpentinite per unit mass of protolith, while Mg-Ca exchange during serpentinization may affect the Mg/Ca ratio of seawater on Earth and possibly other ocean worlds.
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Formation of mixed-layer sulfide-hydroxide minerals from the Tochilinite-Valleriite group during experimental serpentinization of olivine
Abstract We report the formation of minerals from the tochilinite-valleriite group (TVG) during laboratory serpentinization experiments conducted at 300 and 328 °C. Minerals in the TVG are composed of a mixture of sulfide and hydroxide layers that can contain variable proportions of Fe, Mg, Cu, Ni, and other cations in both layers. Members of this group have been observed as accessory minerals in several serpentinites, and have also been observed in association with serpentine minerals in meteorites. To our knowledge, however, TVG minerals have not previously been identified as reaction products during laboratory simulation of serpentinization. The serpentinization experiments reacted olivine with artificial seawater containing 34S-labeled sulfate, with a small amount of solid FeS also added to the 300 °C experiment. In both experiments, the predominant reaction products were chrysotile serpentine, brucite, and magnetite. At 300 °C, these major products were accompanied by trace amounts of the Ni-bearing TVG member haapalaite, Ni,Fe-sulfide (likely pentlandite), and anhydrite. At 328 °C, valleriite occurs rather than haapalaite and the accompanying Ni,Fe-sulfide is proportionally more enriched in Ni. Reduction of sulfate by H2 produced during serpentinization evidently provided a source of reduced S that contributed to formation of the TVG minerals and Ni,Fe-sulfides. The results provide new constraints on the conditions that allow precipitation of tochilinite-valleriite group minerals in natural serpentinites.
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- Award ID(s):
- 2153786
- PAR ID:
- 10488191
- Publisher / Repository:
- Mineralogical Society of America
- Date Published:
- Journal Name:
- American Mineralogist
- Volume:
- 109
- Issue:
- 1
- ISSN:
- 0003-004X
- Page Range / eLocation ID:
- 61 to 72
- Format(s):
- Medium: X
- Sponsoring Org:
- National Science Foundation
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Quantifying the concurrent changes in rock volume and fluid composition during serpentinization remains a major challenge in assessing its physicochemical effects during continental rifting, seafloor spreading, and subduction. Here we conducted a series of 11 hydrothermal laboratory experiments where cylindrical cores of natural dunite, harzburgite, and pyroxenite were reacted with an aqueous solution at 300 °C and 35 MPa for up to 18 months. Using three-dimensional microcomputed tomography and thermogravimetry, we show that rock volume systematically increased with time and extent of reaction, leading to a volume increase of 44% (±8%) in altered rock domains after 10–18 months of serpentinization. The volume expansion was accompanied by Mg-Ca exchange between fluid and rock, while Fe and Si were largely conserved. We find that the protolith composition (olivine/orthopyroxene ratio) plays a significant role in controlling the fluid chemistry and the proportions of hydrous secondary minerals during serpentinization. Agreement between alteration mineralogy, composition of reacting fluids, and measured volume changes suggests that serpentinization under static conditions is a volume-increasing process in spite of demonstrable mass transfer. Volume expansion implies an increased water carrying capacity and buoyancy force of serpentinite per unit mass of protolith, while Mg-Ca exchange during serpentinization may affect the Mg/Ca ratio of seawater on Earth and possibly other ocean worlds.more » « less
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Accepted Manuscript1.0
- Journal Article:
- https://doi.org/10.2138/am-2022-8625
