A system and method for recovering lithium carbonate from lithium-bearing aqueous solutions using controlled droplet-phase carbonation. An alkaline lithium-bearing solution is atomized to form liquid droplets that are introduced into a reaction chamber containing a controlled carbon dioxide-rich gas flow. Carbon dioxide diffuses into the suspended droplets and reacts with dissolved lithium species to nucleate and precipitate lithium carbonate within the droplets while the droplets remain suspended in the gas environment and prior to substantial deposition on internal reactor surfaces. The reaction occurs outside of any bulk liquid bath. Partial evaporation of water may occur during droplet suspension. Resulting lithium carbonate particles are separated from the gas stream using a particulate separation system. The system may operate in a continuous flow configuration and may include optional pretreatment, gas recycling, spatially differentiated gas regions, and thermal management components configured to remove water vapor and recover thermal energy. By coordinating gas-liquid mass transfer, droplet suspension, and precipitation timing, the system enables controlled in-air carbonation and continuous lithium recovery.