Calcination and carbonation behaviour of dolomite has been studied in a pressurised thermo balance at pressures in the range of 1.1 to 2.3 MPa and for temperatures ranging from 730 to 840 degrees C. The atmosphere consisted of nitrogen containing up to 20 vol.-% carbon dioxide. The calcination of dolomite has been studied as a function of temperature, particle size, and P-CO2. An investigation concerning possible mass transfer restrictions for the experimental system and a model investigation of the calcination rate in CO2 atmosphere has been made. Further, the effect of calcination on the BET surface and the BET surface including the surface structure due to successive temperature cycles has been studied. The temperature for the initialisation of calcination of dolomite in CO2 atmosphere was independent of both P-CO2 and the particle size. No conclusive indications on mass transfer restrictions have been detected for the experimental system. A significant difference in calcination rate as a function of particle size existed for decomposition in CO2 atmosphere. A model for homogeneously progressing chemical reaction parallel with a shrinking core chemical reaction together with a mass transfer control mechanism was found to describe the calcination rate in CO2 atmosphere most accurately.