AbstractCalcium looping processes for capturing CO2 from large emissions sources are based on the use of CaO particles as sorbent in circulating fluidized‐bed (CFB) reactors. A continuous flow of CaO from an oxyfired calciner is fed into the carbonator and a certain inventory of active CaO is expected to capture the CO2 in the flue gas. The circulation rate and the inventory of CaO determine the CO2 capture efficiency. Other parameters such as the average carrying capacity of the CaO circulating particles, the temperature, and the gas velocity must be taken into account. To investigate the effect of these variables on CO2 capture efficiency, we used a 6.5 m height CFB carbonator connected to a twin CFB calciner. Many stationary operating states were achieved using different operating conditions. The trends of CO2 capture efficiency measured are compared with those from a simple reactor model. This information may contribute to the future scaling up of the technology. © 2010 American Institute of Chemical Engineers AIChE J, 57: 000–000, 2011