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To support manned lunar and Martian exploration, NASA/JSC and LESC are conducting an extensive evaluation of air revitalization subsystems. The major operations under study include regenerative CO2 removal and reduction; O2 and N2 production, storage, and distribution; humidity and temperature control; and trace contaminant control. This paper describes the ongoing analysis of air revitalization subsystems, including ASPEN PLUS™ modeling and breadboard test stand operation. A comprehensive analysis program based on a generalized block flow model is currently being developed to facilitate the evaluation of various processes and their interactions. Future plans for the development of this simulation will be discussed. ASPEN PLUS™ has been used to model a variety of the subsystems described above; application of this package in modeling CO2 removal and reduction will be discussed.