—Modeling the compositions, properties, and conditions of generation of natural agents of mantle metasomatism is one of the most topical subjects in experimental petrology. Particular attention is paid to the study of C- and S-bearing metasomatic agents and their role in the global carbon and sulfur cycles and in the processes of natural diamond formation. Experimental studies aimed at the estimation of sulfur solubility in carbonate melts under lithospheric mantle conditions were carried out on a multianvil high-pressure apparatus of the “split-sphere” type (BARS) in the carbonate–sulfur ((Mg,Ca)CO3–S) and carbonate–pyrite ((Mg,Ca)CO3–FeS2) systems at 6.3 GPa and 1050–1550 °C for 20–60 h. It has been experimentally established that the main processes occurring in the carbonate–sulfur system are the recrystallization of carbonate in a sulfur melt (1050–1350 °C) and the generation of a high-calcium carbonate melt with dissolved sulfur (5.0–6.5 wt.%) (1450–1550 °C) as well as graphite recrystallization and the initial stage of diamond growth (1550 °C) in this melt. The work demonstrates that the carbonate–pyrite interaction is accompanied by the recrystallization of carbonates and pyrite (1050–1250 °C) and the generation of two immiscible melts (sulfide one with dissolved oxygen and carbonate one with dissolved sulfur (1.7–2.5 wt.%) (1350–1550 °C)) along with the formation of graphite and the growth of diamond on seed crystals (1550 °C). It has been found that the solubility of sulfur in carbonate melts increases with temperature, which goes together with a decrease in CaO (±FeO) concentrations and an increase in MgO concentrations. The present study has shown for the first time that melts of alkaline-earth carbonates are capable of dissolving up to 6.5 wt.% sulfur and they are probable sulfur concentrators under the conditions of the lithospheric mantle.

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