期刊
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
卷 138, 期 10, 页码 3371-3381出版社
AMER CHEMICAL SOC
DOI: 10.1021/jacs.5b12312
关键词
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资金
- EPSRC (U.K. Sustainable Hydrogen Energy Consortium)
- University of Nottingham
- EPSRC
- ERC
- Joint Center of Excellence in Integrated Nano Systems (JCIN) at King Abdul-Aziz City for Science and Technology (KACST) and Northwestern University (NU) [94-938]
- Marie Curie Cofund Action
- Swiss National Science Foundation
- GENCI-IDRIS [x2015087069, x2016087069]
- EPSRC [EP/P001386/1, EP/I011870/2, EP/I020942/1, EP/I011870/1, EP/K038869/1] Funding Source: UKRI
- Engineering and Physical Sciences Research Council [EP/C528964/1, EP/K038869/1, EP/I011870/1, EP/I011870/2, EP/P001386/1, EP/I020942/1] Funding Source: researchfish
Two metal organic framework materials, MFM-130 and MFM-131 (MFM = Manchester Framework Material), have been synthesized using two oligoparaxylene (OPX) tetracarboxylate linkers containing four and five aromatic rings, respectively. Both fof-type non-interpenetrated networks contain Kagome lattice layers comprising [Cu-2(COO)(4)] paddlewheel units and isophthalates, which are pillared by the OPX linkers. Desolvated MFM-130, MFM-130a, shows permanent porosity (BET surface area of 2173 m(2)/g, pore volume of 1.0 cm(3)/g), high H-2 storage capacity at 77 K (5.3 wt% at 20 bar and 2.2 wt% at 1 bar), and a higher CH4 adsorption uptake (163 cm(3)(STP)/cm(3) (35 bar and 298 K)) compared with its structural analogue, NOTT-103. MFM-130a also shows impressive selective adsorption of C2H2, C2H4, and C2H6 over CH4 at room temperature, indicating its potential for separation of C-2 hydrocarbons from CH4. The single-crystal structure of MFM-131 confirms that the methyl substituents of the paraxylene units block the windows in the Kagome lattice layer of the framework, effectively inhibiting network interpenetration in MFM-131. This situation is to be contrasted with that of the doubly interpenetrated oligophenylene analogue, NOTT-104. Calculation of the mechanical properties of these two MOFs confirms and explains the instability of MFM-131 upon desolvation in contrast to the behavior of MFM-130. The incorporation of paraxylene units, therefore, provides an efficient method for preventing network interpenetration as well as accessing new functional materials with modified and selective sorption properties for gas substrates.
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