Subsurface dissolution reduces the efficiency of mineral-based open-ocean alkalinity enhancement

Carbon dioxide removal (CDR) from the atmosphere will likely be required to offset hard-to-abate emissions and limit global warming to well below 2 °C, in line with the Paris Agreement. Among proposed CDR strategies, ocean alkalinity enhancement (OAE) is increasingly discussed because it offers high carbon sequestration potential, long storage timescales, and potentially mitigates ocean acidification. OAE is often envisioned to occur in the open ocean through the dissolution of alkaline mineral powders, such as forsterite, the most abundant form of olivine. Fine-grained powders dissolve near the surface, where the added alkalinity can efficiently enhance oceanic carbon uptake, whereas coarser grains sink and dissolve at depth. Most modeling studies assume complete surface dissolution, leaving the impact of subsurface dissolution on ocean carbon uptake poorly understood. Here, we develop idealized vertical mineral dissolution profiles that vary with environmental conditions and grain size. These profiles are implemented in a comprehensive Earth system model to assess the capture efficiency of OAE, defined as the additional carbon taken up by the ocean per alkalinity added. We find that the efficiency is very sensitive to grain size and may decrease by more than 75 % when grain size doubles, as larger grains release the alkalinity at deeper depth. Efficiency further decreases when particles are not uniformly sized but follow a particle size distribution with the same mean particle volume. In addition, efficiency is time-dependent: it is lower in the first decades of OAE and increases as alkalinity previously released in the ocean interior eventually resurfaces, often far from deployment sites. For forsterite particles with diameter 3.4 µm, the efficiency is less than one-fourth of that achieved with surface alkalinity addition over the first decade, less than one-third over the first 30 years, and less than half over 175 years. Our results indicate that forsterite grain sizes would need to be around 1.7 µm to achieve effective open-ocean alkalinity enhancement and that monitoring, reporting, and verification would be challenged by delayed and spatially dispersed carbon uptake, questioning the suitability of olivine. Minerals with faster dissolution rates may present more viable alternatives when mineral particle properties are closely controlled.