Tetracarbonates in silicate melts may be at the origin of a deep carbon reservoir in the deep Earth

Abstract

Much of Earth’s carbon may have been stripped away from the silicate mantle by dense metallic-iron during core formation. However, at deep magma ocean conditions carbon becomes less siderophile and thus large amounts of it may be stranded instead in the deep mantle. Here, we describe the structure and compaction mechanisms of carbonate glass to deep mantle pressures. Our results, based on non-resonant inelastic X-ray scattering, X-ray diffraction and ab initio calculations, demonstrate a pressure-induced change in hybridization of carbon from sp2 to sp3 starting at 40 GPa, due to the conversion of [3]CO32- groups into [4]CO44- units, which is completed at ~112 GPa. The pressure-induced change of carbon coordination number from three to four increases possibilities for carbon-oxygen interactions with lower mantle silicate melts. sp3 hybridized carbon provides a mechanism for changing the presumed siderophile nature of deep carbon, becoming a possible source for carbon-rich emissions registered at the surface in intra-plate and near-ridge hot spots.