Journal
CHEMISTRY-A EUROPEAN JOURNAL
Volume 21, Issue 46, Pages 16525-16531Publisher
WILEY-V C H VERLAG GMBH
DOI: 10.1002/chem.201502532
Keywords
carbon dioxide capture; manganese; metal-organic frameworks; microporous materials; N,O ligands
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Funding
- NSFC [21471124, 21371142, 21531007, 21001088]
- NSF of Shannxi Province [2013KJXX-26, 13JS114, 2014JQ2049]
- Australian Research Council [FT12010072]
- Open Foundation of Key Laboratory of Synthetic and Natural Functional Molecule Chemistry of Ministry of Education [338080060]
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The reaction of N-rich pyrazinyl triazolyl carboxyl ligand 3-(4-carboxylbenzene)-5-(2-pyrazinyl)-1H-1,2,4-triazole (H(2)cbptz) with MnCl2 afforded 3D cationic metal-organic framework (MOF) [Mn-2(Hcbptz)(2)(Cl)(H2O)]ClDMF0.5CH(3)CN (1), which has an unusual (3,4)-connected 3,4T1 topology and 1D channels composed of cavities. MOF 1 has a very polar framework that contains exposed metal sites, uncoordinated N atoms, narrow channels, and Cl- basic sites, which lead to not only high CO2 uptake, but also remarkably selective adsorption of CO2 over N-2 and CH4 at 298-333K. The multiple CO2-philic sites were identified by grand canonical Monte Carlo simulations. Moreover, 1 shows excellent stability in natural air environment. These advantages make 1 a very promising candidate in post-combustion CO2 capture, natural-gas upgrading, and landfill gas-purification processes.
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