CARBONIC ANHYDRASES (CA) ARE METALLOENZYMES THAT CATALYZE THE HYDRATION OF CARBON DIOXIDE TO BICARBONATE AT RATES APPROACHING ONE MILLION PER SECOND. THE ACTIVE SITE RESPONSIBLE FOR THIS FAST CHEMICAL REACTION CONTAINS A TETRAHEDRAL ZINC ION BEARING A TERMINAL HYDROXIDE LIGAND. RECENT EVIDENCE SUGGESTS THAT POROUS MATERIALS CONTAINING TERMINAL TRANSITION METAL HYDROXIDE (M OH) GROUPS CAN ACT AS FUNCTIONAL MIMICS OF THE CA ACTIVE SITE PAVING THE WAY FOR DEVELOPMENT OF A NEW CLASS OF HIGHLY SELECTIVE CARBON DIOXIDE ADSORBENTS. METAL-ORGANIC FRAMEWORKS (MOFS) ARE POROUS POLYMERS THAT SELF-ASSEMBLE BY COORDINATION OF ORGANIC LINKERS TO METAL IONS OR CLUSTERS. THESE MATERIALS EXCEL IN GAS STORAGE AND SEPARATION APPLICATIONS OWING TO THE AVAILABILITY OF AN ESSENTIALLY INFINITE POOL OF ORGANIC AND INORGANIC BUILDING BLOCKS THAT CAN BE USED TO VARY STRUCTURE AND POROSITY AS WELL AS TO INTRODUCE CHEMICALLY REACTIVE FUNCTIONAL GROUPS. THE PROPOSED RESEARCH IS BASED ON THE HYPOTHESIS THAT NUCLEOPHILIC M OH GROUPS INCORPORATED IN MOFS WILL MIMIC THE CARBON DIOXIDE FIXATION MECHANISM OF CA ACTIVE SITES RESULTING IN FAST AND SELECTIVE CARBON DIOXIDE CAPTURE FROM AMBIENT AIR. THE RESEARCH WILL PURSUE POSTSYNTHETIC MODIFICATION OF BOTH THE METAL CLUSTER (DIRECTION 1) AND ORGANIC LINKER (DIRECTION 2) BUILDING UNITS OF MOFS TO GENERATE TERMINAL M OH GROUPS THAT ARE POISED TO REACT WITH CARBON DIOXIDE GUEST MOLECULES. THE SYNTHETIC INVESTIGATION WILL INCLUDE MOFS OF DIFFERENT TOPOLOGIES AND EXPLORE THE GENERATION OF REACTIVE M OH GROUPS WITH A RANGE OF ABUNDANT TRANSITION METALS. THIS DIVERSITY WILL ALLOW FOR SYSTEMATIC STUDIES THAT ENABLE THE DEVELOPMENT OF STRUCTURE-FUNCTION AND COMPOSITION-FUNCTION RELATIONSHIPS. THE RESULTS OF THESE STUDIES WILL GUIDE OPTIMIZATION OF THIS NEW CLASS OF MOF ADSORBENTS FOR LOW PRESSURE CARBON DIOXIDE CAPTURE APPLICATIONS. IN PARTICULAR THE MATERIALS DEVELOPED IN THIS RESEARCH ARE ANTICIPATED TO BE GOOD CANDIDATE ADSORBENTS FOR USE IN THE CARBON DIOXIDE REMOVAL ASSEMBLY (CDRA) OF THE ATMOSPHERE REVITALIZATION SYSTEMS (ARS) IN NASA SPACECRAFT. THIS ASSESSMENT IS BASED ON THE GOOD CHEMICAL AND THERMAL STABILITY AND STRONGLY EXOTHERMIC CARBON DIOXIDE CHEMISORPTION MECHANISM EXPECTED FOR THE MOF ADSORBENTS. THE ABSENCE OF VOLATILE COMPONENTS WILL PROVIDE GOOD RELIABILITY AND LONG-TERM PERFORMANCE. IN ADDITION A THEORETICAL ANALYSIS OF THE CARBON DIOXIDE UPTAKE CAPACITIES SUGGESTS THAT THE TARGET MOFS SHOULD BE COMPETITIVE WITH OR EXCEED THE ABILITIES OF CURRENT STATE OF THE ART ADSORBENTS.