Metamorphic devolatilization of subducted marine sediments and the transport of volatiles into the Earth's mantle

Volatiles, most notably CO2, are recycled back into the Earth's interior at subduction zones(1,2). The amount of CO2 emitted from arc volcanism appears to be less than that subducted, which implies that a significant amount of CO2 either is released before reaching the depth at which arc magmas are generated or is subducted to deeper depths. Few high-pressure experimental studies(3-5) have addressed this problem and therefore metamorphic decarbonation in subduction zones remains largely unquantified, despite its importance to arc magmatism, palaeoatmospheric CO2 concentrations and the global carbon cycle(6). Here we present computed phase equilibria to quantify the evolution of CO2 and H2O through the subduction-zone metamorphism of carbonate-bearing marine sediments (which are considered to be a major source for CO2 released by arc volcanoes(6)). Our analysis indicates that siliceous limestones undergo negligible devolatilization under subduction-zone conditions. Along high-temperature geotherms clay-rich marls completely devolatilize before reaching the depths at which arc magmatism is generated, but along low-temperature geotherms, they undergo virtually no devolatilization. And from 80 to 180 km depth, little devolatilization occurs for all carbonate-bearing marine sediments. Infiltration of H2O-rich fluids therefore seems essential to promote subarc decarbonation of most marine sediments. In the absence of such infiltration, volatiles retained within marine sediments may explain the apparent discrepancy between subducted and volcanic volatile fluxes and represent a mechanism for return of carbon to the Earth's mantle.