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In hyperalkaline ((Formula presented.)) fluids that have participated in low-temperature (

High Mg# andesites and dacites (Mg# = molar Mg/Mg + Fe) from western Aleutian seafloor volcanoes carry high concentrations of Sr (>1000 ppm) that is unradiogenic (87Sr/86Sr < 0.7029) compared to lavas from emergent volcanoes throughout the arc (200–800 ppm Sr, 87Sr/86Sr >0.7030). Data patterns in plots of 87Sr/86Sr vs Y/Sr and Nd/Sr imply the existence of an eclogite-melt source component – formed by partial melting of MORB eclogite in the subducting Pacific Plate – which is most clearly expressed in the compositions of western Aleutian andesites and dacites (Nd/Sr and Y/Sr < 0.02) and which dominates the source budget for Sr in volcanic rocks throughout the arc. When viewed in combination with inversely correlated εNd and 87Sr/86Sr, these patterns rule out aqueous fluids as an important source of Sr because mixtures of fluids from altered oceanic crust with depleted mantle and sediment produce compositions with 87Sr/86Sr higher than in common Aleutian rocks. The unradiogenic nature of Sr in the western Aleutian andesite–dacite end-member may be understood if H2O required to drive melting of the subducting oceanic crust is transported in fluids containing little Sr. Mass balance demonstrates that such fluids may be produced by dewatering of serpentinite in the mantle section of the subducting plate. If the eclogite-melt source component is present throughout the Aleutian arc, melting of the subducting plate must extend into minimally altered parts of the sheeted dike section or upper gabbros, at depths >2 km below the paleo-seafloor. Oxygen isotopes in western Aleutian seafloor lavas, which fall within a narrow range of MORB-like values (δ18O=5.1–5.7), are also consistent with this model. These results indicate that the subducting Pacific lithosphere beneath the Aleutian arc is significantly hotter than indicated my most thermal models.

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 O2/CO2-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 Ca2+, H2 and CH4, 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 2-10 μm magnetite grains overprint all minerals in the drill cuttings. Thus we propose that the dissolved H2 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 H2. Dissolved CH4 in the fluids exhibits the most isotopically heavy carbon in CH4 reported in the literature thus far. The CH4 may have formed through abiotic reduction of dissolved CO2 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 Oman ophiolite.

Carbon fluxes in subduction zones can be better constrained by including new estimates of carbon concentration in subducting mantle peridotites, consideration of carbonate solubility in aqueous fluid along subduction geotherms, and diapirism of carbon-bearing metasediments. Whereas previous studies concluded that about half the subducting carbon is returned to the convecting mantle, we find that relatively little carbon may be recycled. If so, input from subduction zones into the overlying plate is larger than output from arc volcanoes plus diffuse venting, and substantial quantities of carbon are stored in the mantle lithosphere and crust. Also, if the subduction zone carbon cycle is nearly closed on time scales of 5-10 Ma, then the carbon content of the mantle lithosphere + crust + ocean + atmosphere must be increasing. Such an increase is consistent with inferences from noble gas data. Carbon in diamonds, which may have been recycled into the convecting mantle, is a small fraction of the global carbon inventory.