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A hallmark of the rapid and massive release of carbon during the Palaeocene–Eocene Thermal Maximum is the global negative carbon isotope excursion. The delayed recovery of the carbon isotope excursion, however, indicates that CO2inputs continued well after the initial rapid onset, although there is no consensus about the source of this secondary carbon. Here we suggest this secondary input might have derived partly from the oxidation of remobilized sedimentary fossil carbon. We measured the biomarker indicators of thermal maturation in shelf records from the US Mid-Atlantic coast, constructed biomarker mixing models to constrain the amount of fossil carbon in US Mid-Atlantic and Tanzania coastal records, estimated the fossil carbon accumulation rate in coastal sediments and determined the range of global CO2release from fossil carbon reservoirs. This work provides evidence for an order of magnitude increase in fossil carbon delivery to the oceans that began ~10–20 kyr after the event onset and demonstrates that the oxidation of remobilized fossil carbon released between 102and 104PgC as CO2during the body of the Palaeocene–Eocene Thermal Maximum. The estimated mass is sufficient to have sustained the elevated atmospheric CO2levels required by the prolonged global carbon isotope excursion. Even after considering uncertainties in the sedimentation rates, these results indicate that the enhanced erosion, mobilization and oxidation of ancient sedimentary carbon contributed to the delayed recovery of the climate system for many thousands of years.

Mitigating climate change requires transformational advances for carbon dioxide removal, including geologic carbon sequestration in reactive subsurface environments. The Wallula Basalt Carbon Storage Pilot Project demonstrated that CO2injected into >800 m deep Columbia River Basalt Group flow top reservoirs mineralizes on month-year timescales. Herein, we present new optical petrography, micro-computed X-ray tomography, and electron microscopy results obtained from sidewall cores collected two years after CO2injection. As no other anthropogenic carbonates from geologic carbon storage field studies have been recovered, this world-unique sample suite provides unparalleled insight for subsurface carbon mineralization products and paragenesis. Chemically zoned nodules with Ca/Mn-rich cores and Fe-dominant outer rims are prominent examples of the neoformed carbonate assemblages with ankerite–siderite compositions and exotic divalent cation correlations. Paragenetic insights for the timing of aragonite, silica, and fibrous zeolites are clarified based on mineral texture and spatial relationships, along with time-resolved downhole fluid sampling. Collectively, these results clarify the mineralogy, chemistry, and paragenesis of carbon mineralization, providing insight into the ultimate fate and transport of CO2in reactive mafic–ultramafic reservoirs.