Reactive transport experiments of coupled carbonation and serpentinization in a natural serpentinite. Implication for hydrogen production and carbon geological storage

Serpentinization and carbonation of ultramafic formations is a ubiquitous phenomenon, which deeply influences the biogeochemical cycles of water, hydrogen, carbon…while supporting the particular biosphere around the oceanic hydrothermal vents. Carbonation of peridotites and other mafic and ultramafic rocks is also a hot topic in the current energy landscape as the engineered sequestration of mineral CO2 in these formations could help reduce the atmospheric emissions and cope with climate change. In this study, we present two reactive percolation experiments performed on a natural serpentinite dredged from the ultraslow South-West Indian Oceanic Ridge. The serpentinite cores (length 3-4 cm and dia. 5.6 mm) were subjected for about 10 days to the continuous injection of a NaHCO3-saturated brine at respectively 160°C and 280°C. Petrographic and petrophysical results as well as outlet fluid compositions were compared to numerical batch simulations performed with the PHREEQC open software allowing to reconstruct the mineralogical evolution of both cores. The most striking observation is the fast and dramatic decrease of the permeability for both experiments principally due to the precipitation of carbonates. On the contrary, serpentine was found to be less impacting as it precipitates in low-flow zones, out of the main percolation paths. In total, about 5.6% of the total injected CO2 was retained in the core, at 280°C. In the same time, hydrogen was consistently produced with a total recovered H2 corresponding to 0.8% of the maximum H2 possible. The global behavior of the cores is interpreted as the result from an interplay between interacting spatio-temporal lengthscales controlled by the Damköhler number.