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Closed-loop inhabited spacecraft, including a space suit, require removal of carbon dioxide from the breathing atmosphere. A membrane device that separates CO2 from breathing air can effectively control CO2 levels in the breathing loop by venting the carbon dioxide directly to the vacuum of space. Such a membrane device requires no regeneration and, therefore, imposes no limitations on mission length. Systematic studies have expanded our knowledge of the parameters most critical to the successful development of a membrane carbon dioxide removal system. The membrane type disclosed in this paper is an immobilized liquid membrane (ILM) in which the liquid is engineered to facilitate the transport of carbon dioxide while inhibiting the progress of oxygen. Selectivity superior to that achieved in previously published studies has been demonstrated and has approached values desired for an Extravehicular Mobility Unit (EMU) system.