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The geological conundrum of sulfur excess refers to the finding thatpredicted amounts of sulfur, in the form of SO2, discharged in volcaniceruptions much exceeds the sulfur available for degassing from the eruptedmagma. Exploring the source of the excess sulfur has been the subject ofconsiderable interest. Here, from a systematic computational investigation ofsulfur-oxygen compounds under pressure, a hitherto unknown S3O4 compoundcontaining a mixture of sulfur oxidation states +II and +IV emerges and ispredicted to be stabilized above a pressure of 79 GPa. We predict that S3O4 canbe produced via multiple redox reactions involving subducted S-bearing minerals(e.g., sulfates and sulfides) at high pressure conditions relevant to the deeplower mantle, and conversely be decomposed into SO2 and S at shallow depths ofEarth. Therefore, S3O4 can be considered as a key intermediate compound topromote the decomposition of sulfates to release SO2, which offers analternative source of the excess sulfur released during explosive eruptions.These findings provide a possible resolution to the geological paradox ofexcess sulfur degassing and a viable mechanism for the understanding of Sexchange between surface and the lower mantle for the deep sulfur cycle.

Stabilization of S3O4 at High Pressure-Implications for the Sulfur Excess Paradox