The importance of the wall effect on packed beds in the adsorption and desorption of carbon dioxide, nitrogen, and water on molecular sieve 5A of 0.127 cm radius is examined experimentally and with one-dimensional computer simulations. Experimental results are presented for a 22.5-cm long by 4.5-cm diameter cylindrical column with concentration measurements taken at various radial locations. The set of partial differential equations is solved using finite differences and Newmans＇s method. Comparison of test data with the axial-dispersed, nonisothermal, linear driving force model suggests that a two-dimensional model (submitted to Separation Science and Technology) is required for accurate simulation of the average column breakthrough concentration. Additional comparisons of test data with the model provided information on the interactive effects of carrier gas coadsorption with CO2 as well as CO2-H2O interactions.