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1. Slab-derived sulfate generates oxidized basaltic magmas in the southern Cascade arc (California, USA)

   https://doi.org/10.1130/G48759.1  

   Muth, Michelle J.; Wallace, Paul J. (June 2021, Geology)

   Abstract Whether and how subduction increases the oxidation state of Earth's mantle are two of the most important unresolved questions in solid Earth geochemistry. Using data from the southern Cascade arc (California, USA), we show quantitatively for the first time that increases in arc magma oxidation state are fundamentally linked to mass transfer of isotopically heavy sulfate from the subducted plate into the mantle wedge. We investigate multiple hypotheses related to plate dehydration and melting and the rise and reaction of slab melts with mantle peridotite in the wedge, focusing on electron balance between redox-sensitive iron and sulfur during these processes. These results show that unless slab-derived silicic melts contain much higher dissolved sulfur than is indicated by currently available experimental data, arc magma generation by mantle wedge melting must involve multiple stages of mantle metasomatism by slab-derived oxidized and sulfur-bearing hydrous components. 

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2. The origin of sulfur in Canary Island magmas and its implications for Earth’s deep sulfur cycle

   https://doi.org/10.1073/pnas.2416070122  

   Taracsák, Zoltán; Hartley, Margaret E; Burgess, Ray; Edmonds, Marie; Longpré, Marc-Antoine; Monteleone, Brian D; Tartèse, Romain; Turchyn, Alexandra V (March 2025, Proceedings of the National Academy of Sciences)

   The global sulfur cycle plays a critical role in the redox evolution of Earth’s surface and upper mantle, yet the distribution and origin of sulfur in the mantle remains largely unconstrained. El Hierro is a volcanic island in the Canary archipelago that is fed by sulfur-rich magmas. To constrain the origin of sulfur in these melts, we combine in situ sulfur isotope analyses with regression modeling. We calculate that undegassed El Hierro melts have δ34S values of 0 ± 2‰. The average δ34S of undegassed El Hierro melts is 0.3‰ to 1‰ higher than magmas erupting at mid-ocean ridges. Mass balance calculations reveal that El Hierro’s mantle source contains 310 ± 120 μg/g sulfur and that on average 60% of sulfur in the source is of recycled origin. This recycled material should contain >1,800 μg/g sulfur to satisfy isotopic constraints on its mass fraction in the mantle source. The sulfur and oxygen isotopic signature in serpentinites and sediments deviate significantly from the upper mantle, making them unsuitable candidates for the recycled material. An oxidized partial melt of recycled oceanic crust that retained one third of its sulfur budget after subduction zone processing can explain excess sulfur in the Canary Island mantle. Recycled oceanic crust is expected to contain sulfur as sulfide, which is not capable of oxidizing the mantle. The presence of ferric iron in the recycled component is necessary to produce metasomatic melts that are oxidizing enough to carry sufficient sulfur into the mantle source of ocean island basalts. 

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3. Effects of H2O–CO2 Fluids, Temperature, and Peridotite Fertility on Partial Melting in Mantle Wedges and Generation of Primary Arc Basalts

   https://doi.org/10.1093/petrology/egad047  

   Lara, Michael; Dasgupta, Rajdeep (July 2023, Journal of Petrology)

   Abstract Many lines of evidence from high P–T experiments, thermodynamic models, and natural observations suggest that slab-derived aqueous fluids, which flux mantle wedges contain variable amounts of dissolved carbon. However, constraints on the effects of H2O–CO2 fluids on mantle melting, particularly at mantle wedge P–T conditions, are limited. Here, we present new piston cylinder experiments on fertile and depleted peridotite compositions with 3.5 wt.% H2O and XCO2 [= molar CO2 / (CO2 + H2O)] of 0.04–0.17. Experiments were performed at 2–3 GPa and 1350°C to assess how temperature, peridotite fertility, and XCO2 of slab-derived fluid affects partial melting in mantle wedges. All experiments produce olivine + orthopyroxene +7 to 41 wt.% partial melt. Our new data, along with previous lower temperature data, show that as mantle wedge temperature increases, primary melts become richer in SiO2, FeO*, and MgO and poorer CaO, Al2O3, and alkalis when influenced by H2O–CO2 fluids. At constant P–T and bulk H2O content, the extent of melting in the mantle wedge is largely controlled by peridotite fertility and XCO2 of slab-fluid. High XCO2 depleted compositions generate ~7 wt.% melt, whereas, at identical P–T, low XCO2 fertile compositions generate ~30 to 40 wt.% melt. Additionally, peridotite fertility and XCO2 have significant effects on peridotite partial melt compositions. At a constant P–T–XCO2, fertile peridotites generate melts richer in CaO and Al2O3 and poorer in SiO2, MgO + FeO, and alkalis. Similar to previous experimental studies, at a constant P–T fertility condition, as XCO2 increases, SiO2 and CaO of melts systematically decrease and increase, respectively. Such distinctive effects of oxidized form of dissolved carbon on peridotite partial melt compositions are not observed if the carbon-bearing fluid is reduced, such as CH4-bearing. Considering the large effect of XCO2 on melt SiO2 and CaO concentrations and the relatively oxidized nature of arc magmas, we compare the SiO2/CaO of our experimental melts and melts from previous peridotite + H2O ± CO2 studies to the SiO2/CaO systematics of primitive arc basalts and ultra-calcic, silica-undersaturated arc melt inclusions. From this comparison, we demonstrate that across most P–T–fertility conditions predicted for mantle wedges, partial melts from bulk compositions with XCO2 ≥ 0.11 have lower SiO2/CaO than all primitive arc melts found globally, even when correcting for olivine fractionation, whereas partial melts from bulk compositions with XCO2 = 0.04 overlap the lower end of the SiO2/CaO field defined by natural data. These results suggest that the upper XCO2 limit of slab-fluids influencing primary arc magma formation is 0.04 < XCO2 < 0.11, and this upper limit is likely to apply globally. Lastly, we show that the anomalous SiO2/CaO and CaO/Al2O3 signatures observed in ultra-calcic arc melt inclusions can be reproduced by partial melting of either CO2-bearing hydrous fertile and depleted peridotites with 0 < XCO2 < 0.11 at 2–3 GPa, or from nominally CO2-free hydrous fertile peridotites at P > 3 GPa. 

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4. Highly oxidized intraplate basalts and deep carbon storage

   https://doi.org/10.1126/sciadv.adm8138  

   Dong, Xu-Han; Wang, Shui-Jiong; Wang, Wenzhong; Huang, Shichun; Li, Qiu-Li; Liu, Chengshuai; Gao, Ting; Li, Shuguang; Wu, Shitou (August 2024, Science Advances)

   Deep carbon cycle is crucial for mantle dynamics and maintaining Earth’s habitability. Recycled carbonates are a strong oxidant in mantle carbon-iron redox reactions, leading to the formation of highly oxidized mantle domains and deep carbon storage. Here we report high Fe³⁺/∑Fe values in Cenozoic intraplate basalts from eastern China, which are correlated with geochemical and isotopic compositions that point to a common role of carbonated melt with recycled carbonate signatures. We propose that the source of these highly oxidized basalts has been oxidized by carbonated melts derived from the stagnant subducted slab in the mantle transition zone. Diamonds formed during the carbon-iron redox reaction were separated from the melt due to density differences. This would leave a large amount of carbon (about four times of preindustrial atmospheric carbon budget) stored in the deep mantle and isolated from global carbon cycle. As such, the amounts of subducted slabs stagnated at mantle transition zone can be an important factor regulating the climate. 

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5. Recycled calcium carbonate is an efficient oxidation agent under deep upper mantle conditions

   https://doi.org/10.1038/s43247-021-00116-8  

   Tao, Renbiao; Fei, Yingwei (February 2021, Communications Earth & Environment)

   Abstract Observations of high ferric iron content in diamond garnet inclusions and mantle plume melts suggest a highly heterogeneous distribution of ferric iron in the mantle. Recycling of oxidized materials such as carbonates from Earth’s surface by subduction could explain the observed variations. Here we present high-pressure high-temperature multi-anvil experiments to determine the redox reactions between calcium-, magnesium-, or iron-carbonate and ferrous iron-bearing silicate mineral (garnet or fayalite) at conditions representative of subduction zones with intermediate thermal structures. We show that both garnet and fayalite can be oxidized to ferric iron-rich garnets accompanied by reduction of calcium carbonate to form graphite. The ferric iron content in the synthetic garnets increases with increasing pressure, and is correlated with the Ca content in the garnets. We suggest that recycled sedimentary calcium carbonate could influence the evolution of the mantle oxidation state by efficiently increasing the ferric iron content in the deep upper mantle. 

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