The role of scapolite-bearing granulites in sequestering and releasing sulfur: Implications for S isotope signatures of crustal fluids during lower-crustal exhumation

To understand sulfur and carbon sequestration and release within the continental crust, scapolite minerals from a variety of granulite facies rocks were analyzed for their elemental composition and S isotope signatures. These high-grade scapolites host significant amounts of SO₃ and CO₂, up to approximately 5 wt% and 3 wt%, respectively, with δ³⁴S_VCDT from −3 to +10 ‰, and formed in relatively oxidizing environments characterized by low aH₂O in which scapolite may form as a primary igneous mineral or via metamorphic reactions involving sulfides and silicates. The range of scapolite sulfur isotope compositions mirrors those observed in mantle xenoliths, suggesting transport of S from the mantle into the lower crust via fluids and melts. Although scapolite’s contribution to the global S and C cycles may be modest, it is significant in the context of sulfur fluxing from the mantle to the lower crust, particularly in its oxidized form. We estimate that at least 10 % of lower crustal sulfur is sequestered within scapolite. The exhumation of scapolite-bearing lower crustal rocks can therefore liberate substantial quantities of sulfur species and CO₂, which may serve to both supply and compositionally buffer retrograde metamorphic fluids. These fluids may exhibit a range of S isotope compositions from mantle-like (δ³⁴S_VCDT ≈ 0 ‰) to relatively ³⁴S-enriched signatures. Consequently, retrograde fluids may have S isotope signatures indistinguishable from those of mantle fluids, even in the absence of direct mantle S input during fluid formation. Exhumation of scapolite-bearing lower crust may facilitate element mobilization through S and Cl complexing, particularly with respect to base metals, within exhumed lower crustal sections, thus providing sources of metals and fluids in mid- to high-grade metamorphic rocks. Globally, scapolite-bearing lower crust may help balance the global sulfur cycle through catch-and-release from scapolite.