Uncovering and quantifying the subduction zone sulfur cycle from the slab perspective.

Abstract

Sulfur belongs among H₂O, CO₂, and Cl as one of the key volatiles in Earth's chemical cycles. High oxygen fugacity, sulfur concentration, and δ³⁴S values in volcanic arc rocks have been attributed to significant sulfate addition by slab fluids. However, sulfur speciation, flux, and isotope composition in slab-dehydrated fluids remain unclear. Here, we use high-pressure rocks and enclosed veins to provide direct constraints on subduction zone sulfur recycling for a typical oceanic lithosphere. Textural and thermodynamic evidence indicates the predominance of reduced sulfur species in slab fluids; those derived from metasediments, altered oceanic crust, and serpentinite have δ³⁴S values of approximately -8‰, -1‰, and +8‰, respectively. Mass-balance calculations demonstrate that 6.4% (up to 20% maximum) of total subducted sulfur is released between 30-230 km depth, and the predominant sulfur loss takes place at 70-100 km with a net δ³⁴S composition of -2.5 ± 3‰. We conclude that modest slab-to-wedge sulfur transport occurs, but that slab-derived fluids provide negligible sulfate to oxidize the sub-arc mantle and cannot deliver ³⁴S-enriched sulfur to produce the positive δ³⁴S signature in arc settings. Most sulfur has negative δ³⁴S and is subducted into the deep mantle, which could cause a long-term increase in the δ³⁴S of Earth surface reservoirs.