Journal
NATURE MATERIALS
Volume 16, Issue 5, Pages 526-+Publisher
NATURE PUBLISHING GROUP
DOI: 10.1038/NMAT4825
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Funding
- MSIP (Ministry of Science, ICT and Future Planning) [CRC-14-1-KRICT]
- NST (National Research Council of Science & Technology) of Republic of Korea
- Global Frontier Center for Hybrid Interface Materials (GFHIM) [NRF-2013M3A6B1078879]
- CNRS (Centre National de la Recherche Scientifique)
- DRC Program - NST (National Research Council of Science & Technology) of Korea [SKM-1503]
- Institut Universitaire de France
- National Research Foundation of Korea - Korean Government [NRF-2016M3D1A1021147]
- National Research Council of Science & Technology (NST), Republic of Korea [CRC-14-1-KRICT] Funding Source: Korea Institute of Science & Technology Information (KISTI), National Science & Technology Information Service (NTIS)
- National Research Foundation of Korea [10Z20130011056, 2013M3A6B1078879] Funding Source: Korea Institute of Science & Technology Information (KISTI), National Science & Technology Information Service (NTIS)
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Selective dinitrogen binding to transition metal ions mainly covers two strategic domains: biological nitrogen fixation catalysed by metalloenzyme nitrogenases(1-3), and adsorptive purification of natural gas and air(4-6). Many transition metal-dinitrogen complexes have been envisaged for biomimetic nitrogen fixation to produce ammonia(3). Inspired by this concept, here we report mesoporous metal-organic framework materials containing accessible Cr(III) sites, able to thermodynamically capture N-2 over CH4 and O-2. This fundamental study integrating advanced experimental and computational tools confirmed that the separation mechanism for both N-2/CH4 and N-2/O-2 gas mixtures is driven by the presence of these unsaturated Cr(III) sites that allows a much stronger binding of N-2 over the two other gases. Besides the potential breakthrough in adsorption-based technologies, this proof of concept could open new horizons to address several challenges in chemistry, including the design of heterogeneous biomimetic catalysts through nitrogen fixation.
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