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The influence of operating parameters on the morphology of particles prepared by spray pyrolysis was investigated using a temperature-graded laminar flow aerosol reactor. Experimentally, zirconia particles were prepared by spray pyrolysis using an aqueous solution of zirconyl hydroxide chloride. Hollow particles were formed if the reactor temperature was high, the temperature gradient was too large, the flow rate of carrier gas was high, and the initial solute concentration was low. A numerical simulation of the pyrolysis process was developed using a combination of two previous models. The simulation results compared well with the experimental results.