It has been shown previously that pulse-response experiments on single catalyst pellets can provide a simple, rapid method for determining effective diffusivities and adsorption equilibrium constants. Assumptions were made about boundary conditions in the earlier work in order to simplify the mathematical treatment. In this paper a more rigorous development is presented in order to evaluate the magnitude of likely errors in the simplified approach. By using large flow rates, small chamber volumes, and for catalyst pellets of moderate or low porosity, the error in using the approximate equations should be small (less than 10%). For short diffusion paths (short pellets) of highly porous catalysts, the error can be large. © 1979.