The Samail ophiolite in Oman is undergoing modern hydration and carbonation of peridotite and may host a deep subsurface biosphere. Previous investigations of hyperalkaline fluids in Oman have focused on fluids released at surface seeps, which quickly lose their reducing character and precipitate carbonates upon contact with the O 2 /CO 2-rich atmosphere. In this work, geochemical analysis of rocks and fluids from the subsurface provides new insights into the operative reactions in serpentinizing aquifers. Serpentinite rock and hyperalkaline fluids (pH >10), which exhibit millimolar concentrations of Ca 2+ , H 2 and CH 4, as well as variable sulfate and nitrate, were accessed from wells situated in mantle peridotite near Ibra and studied to investigate their aqueous geochemistry, gas concentrations, isotopic signatures, mineralogy, Fe speciation and microbial community composition. The bulk mineralogy of drill cuttings is dominated by olivine, pyroxene, brucite, serpentine and magnetite. At depth, Fe-bearing brucite is commonly intermixed with serpentine, whereas near the surface, olivine and brucite are lost and increased magnetite and serpentine is detected. Micro-Raman spectroscopy reveals at least two distinct generations of serpentine present in drill cuttings recovered from several depths from two wells. Fe K-edge x-ray absorption near-edge spectroscopy (XANES) analysis of the lizardite shows a strong tetrahedral Fe coordination, suggesting a mixture of both Fe(II) and Fe(III) in the serpentine. Magnetite veins are also closely associated with this second generation serpentine, and 2-10µm magnetite grains overprint all minerals in the drill cuttings. Thus we propose that the dissolved H 2 that accumulates in the subsurface hyperalkaline fluids was evolved through low temperature oxidation and hydration of relict olivine, as well as destabilization of pre-existing brucite present in the partially serpentinized dunites and harzburgites. In particular, we hypothesize that Fe-bearing brucite is currently reacting with dissolved silica in the aquifer fluids to generate late-stage magnetite, additional serpentine and dissolved H 2. Dissolved CH 4 in the fluids exhibits the most isotopically heavy carbon in CH 4 reported in the literature thus far. The CH 4 may have formed through abiotic reduction of dissolved CO 2 or through biogenic pathways under extreme carbon limitation. The methane isotopic composition may have also been modified by significant methane oxidation. 16S rRNA sequencing of DNA recovered from filtered hyperalkaline well fluids reveals an abundance of Meiothermus, Thermodesulfovibrionaceae (sulfate-reducers) and Clostridia (fermenters). The fluids also contain candidate phyla OP1 and OD1, as well as Methanobacterium (methanogen) and Methylococcus sp. (methanotroph). The composition of these microbial communities suggests that low-temperature hydrogen and methane generation, coupled with the presence of electron acceptors such as nitrate and sulfate, sustains subsurface microbial life within the O...

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Serpentinization can generate highly reduced fluids replete with hydrogen (H2) and methane (CH4), potent reductants capable of driving microbial methanogenesis and methanotrophy, respectively. However, CH4 in serpentinized waters is thought to be primarily abiogenic, raising key questions about the relative importance of methanogens and methanotrophs in the production and consumption of CH4 in these systems. Herein, we apply molecular approaches to examine the functional capability and activity of microbial CH4 cycling in serpentinization-impacted subsurface waters intersecting multiple rock and water types within the Samail Ophiolite of Oman. Abundant 16S rRNA genes and transcripts affiliated with the methanogenic genus, Methanobacterium, were recovered from the most alkaline (pH > 10), H2- and CH4-rich subsurface waters. Additionally, 16S rRNA genes and transcripts associated with the aerobic methanotrophic genus, Methylococcus, were detected in wells that spanned varied fluid geochemistry. Metagenomic sequencing yielded genes encoding homologs of proteins involved in the hydrogenotrophic pathway of microbial CH4 production and in microbial CH4 oxidation. Transcripts of several key genes encoding methanogenesis/methanotrophy enzymes were identified, predominantly in communities from the most hyperalkaline waters. These results indicate active methanogenic and methanotrophic populations in waters with hyperalkaline pH in the Samail Ophiolite thereby supporting a role for biological CH4 cycling in aquifers that undergo low temperature serpentinization. Importance Serpentinization of ultramafic rock can generate conditions favorable for microbial methane (CH4) cycling, including the abiotic production of H2 and possibly CH4. Systems of low-temperature serpentinization are geobiological targets due to their potential to harbor microbial life and ubiquity throughout Earth's history. Biomass in fracture waters collected from the Samail Ophiolite of Oman, a system undergoing modern serpentinization, yielded DNA and RNA signatures indicative of active microbial methanogenesis and methanotrophy. Intriguingly, transcripts for proteins involved in methanogenesis were most abundant in the most highly-reacted waters that have hyperalkaline pH and elevated concentrations of H2 and CH4. These findings suggest active biological methane cycling in serpentinite-hosted aquifers, even under extreme conditions of high pH and carbon limitation. These observations underscore the potential for microbial activity to influence the isotopic composition of CH4 in these systems, information that could help in identifying biosignatures of microbial activity on other planets.

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Reactions that occur during the hydration and aqueous alteration of ultramafic rocks (collectively, serpentinization reactions) are important where fluids circulate in seafloor oceanic crust and uplifted mantle rocks on Earth. Evidence of serpentinization has also been found in carbonaceous chondrite meteorites (Velbel et al., 2012), and serpentine minerals have been detected spectrally on a variety of rocky bodies in the solar system (Mars,

Cite this article: Templeton AS, Ellison ET. 2020 Formation and loss of metastable brucite: does Fe(II)-bearing brucite support microbial activity in serpentinizing ecosystems?. Phil. Trans. R. Soc. A 378: 20180423. http://dx.One contribution of 11 to a discussion meeting issue 'Serpentinite in the Earth system'.

The Oman Drilling Project established an "Active Alteration" multi-borehole observatory in peridotites undergoing low-temperature serpentinization in the Samail Ophiolite. The highly serpentinized rocks are in contact with strongly reducing fluids. Distinct hydrological regimes, governed by differences in rock porosity and fracture density, give rise to steep redox (Eh +200 to −750 mV) and pH (pH range 8.5-11.2) gradients within the 300-400 m deep boreholes. The serpentinites and fluids host an active subsurface ecosystem. Microbial cell abundances in serpentinite vary at least six orders of magnitude, from ≤3.5 × 10 1 to 2.9 × 10 7 cells/g. Low levels of biological sulfate reduction (2-1,000 fmol/ cm 3 /day) can be detected in rock cores, particularly in rocks in contact with reduced groundwaters with pH < 10.5. Thermodesulfovibrio is the predominant sulfate reducer identified via metagenomic sequencing of adjacent groundwater communities. We infer that transport and reaction of microbially generated sulfide with the serpentine and brucite assemblages gives rise to optical darkening and sulfide overprinting, including the formation of tochilinite-vallerite group minerals, potentially serving as an indicator that this system is inhabited by microbial life. Olivine mesh-cores replaced with ferroan brucite and minor awaruite, abundant veins containing hydroandradite garnet and polyhedral serpentine, and late-stage carbonate veins are suggested as targets for future spatially resolved life-detection investigations. The high-quality whole-round core samples that have been preserved can be further probed to define how life distributes itself and functions within a system where chemical disequilibria are sustained by lowtemperature water/rock interaction, and how biosignatures of in situ microbial activity are generated.Plain Language Summary Ultramafic rocks undergoing water/rock interaction, and storing fluids that are far from chemical equilibrium, may be one of the most common habitats in our solar system. Through the Oman Drilling Project we collected >1 km of intact serpentinite in contact with groundwaters. These cores capture parts of the rock-hosted biosphere and show how cells are distributed within serpentinites that vary in their mineralogical, physical and chemical properties. The cores are also biologically active, enabling us to detect specific metabolisms, such as when microorganisms combine hydrogen as reductant and sulfate as an oxidant to fuel their metabolism. Although the distribution of microbial cells in the rock cores is very heterogeneous, there are many intervals where the abundance of cells constitutes robust biomass. In the deeper cores, slow, albeit detectable, microbial sulfate reduction proceeds. We suggest that this pervasive biological activity releases byproducts such as sulfide that can react with the serpentinite and change the optical and chemical properties of the rocks. The feedbacks between the rock alteration and microbial activity produce markers that enable us to focus our sea...