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Developments intended to improve system efficiency and reliability for water and carbon dioxide separation systems to be used on crewed vehicles combine sub-scale systems testing and multiphysics simulations. This paper describes the development of COMSOL Multiphysics® simulations in support of the Atmosphere Revitalization Recovery and Environmental Monitoring (ARREM) project within NASA's Advanced Exploration Systems (AES) program. The transport of a concentrated species, water or carbon dioxide in a carrier gas, namely nitrogen, was modeled as free and porous media flow through a bed of silica gel pellets. Using COMSOL to model the bulk desiccant process has resulted in a favorable match to temperature and concentration data for a range of inlet dew points, initial conditions, and flow rates.