AbstractA heterogeneous model is developed to account for noncatalytic gas‐solid reactions in a vertical pneumatic transport reactor. The model takes into consideration both the positive and negative variations of the solid porosity and the variation of the gas diffusivity with the reaction. The method of lines utilizing the second order centered finite difference scheme for the spatial discretization is employed to obtain the model solution.Experiments utilizing a vertical pneumatic transport reactor of a laboratory scale are performed to study the reaction between limestone and sulfur dioxide generated from coal combustion. The reactor is of 16.2 cm ID and 610 cm in length. The experimental data for sulfur retention are reported for various superficial gas velocities and calcium‐sulfur molar ratios. Verification of the model with experimental data is conducted. The agreement between the model prediction and experimental data is satisfact