Various recent studies have shown that basalt formations have the capacity for long-term secure CO₂ storage through carbon mineralization. Many of these studies have demonstrated extremely rapid rates of mineralization, but the underlying mechanism enabling these elevated reaction rates, and their relation to the processes occurring in proposed basaltic reservoirs, remain poorly constrained. In this work, a 3D micro-continuum reactive transport model was designed to investigate the impact of alkalinity on basalt interactions with CO₂-rich fluids. Reactive transport models were developed in PFLOTRAN based on 3D imaging data from high-temperature, high-pressure flow-through experiments (Luhmann et al. (2017) Chemical Geology, Water Resources Research). Mineral reactive surface areas in the model were adjusted to produce agreement with chemistry of output fluids sampled during the experiments. The benchmarked model showed that no considerable carbonate was formed during interaction with the relatively low alkalinity, low pH solutions, regardless of the enrichment of basalt-derived Na⁺, Mg²⁺, and Fe²⁺ ions in the reactant fluid. Increasing the alkalinity of the injected fluids consistently yielded higher rates of carbon mineralization. Similarly, introducing a small initial volume fraction of carbonate minerals into the system contributed to increased carbon mineralization, because of the increased fluid alkalinity. These results thus reinforce a conceptual understanding of carbonate mineralization in basalt-hosted CO₂ storage reservoirs that emphasizes the importance of aquifer fluid alkalinity, and caution against extrapolating results from elevated-alkalinity CO₂ storage reservoirs and experiments to others where this is less likely to be representative.