Investigations were conducted to purify crude Li2CO3 via direct carbonation with CO2-water solutions at atmospheric pressure. The experiments were carried out in a slurry bubble column reactor with 0.05 m inner diameter and 1.0 m height. Parameters that may affect the dissolution of Li2CO3 in the CO2-water solutions such as CO2-bubble perforation diameter, CO2 partial pressure, CO2 gas flow rate, Li2CO3 particle size, solid concentration in the slurry, reaction temperature, slurry height in the column and so on were investigated. It was found that the increases of CO2 partial pressure, and CO2 flow rate were favorable to the dissolution of Li2CO3, which had the opposite effects with Li2CO3 particle size, solid concentration, slurry height in the column and temperature. On the other hand, in order to get insight into the mechanism of the refining process, reaction kinetics was studied. The results showed that the kinetics of the carbonation process can be properly represented by 1.3(1.X)2/3+2(1.X)=kt+b, and the rate-determining step of this process under the conditions studied was product layer diffusion. Finally, the apparent activation energy of the carbonation reaction was obtained by calculation. This study will provide theoretical basis for the reactor design and the optimization of the process operation.