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Furukawa H Go YB Ko N Park YK Uribe-Romo FJ Kim J O'Keeffe M Yaghi OM 《Inorganic chemistry》2011,50(18):9147-9152
The concept and occurrence of isoreticular (same topology) series of metal-organic frameworks (MOFs) is reviewed. We describe the preparation, characterization, and crystal structures of three new MOFs that are isoreticular expansions of known materials with the tbo (Cu(3)(4,4',4'-(benzene-1,3,5-triyl-tris(benzene-4,1-diyl))tribenzoate)(2), MOF-399) and pto topologies (Cu(3)(4,4',4'-(benzene-1,3,5-triyl-tribenzoate)(2), MOF-143; Cu(3)(4,4',4'-(triazine-2,4,6-triyl-tris(benzene-4,1-diyl))tribenzoate)(2), MOF-388). One of these materials (MOF-399) has a unit cell volume 17 times larger than that of the first reported material isoreticular to it, and has the highest porosity (94%) and lowest density (0.126 g cm(-3)) of any MOFs reported to date. 相似文献
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The dihydrogen adsorption isotherms of eight metal-organic frameworks (MOFs), measured at 77 K up to a pressure of 1 atm, have been examined for correlations with their structural features. All materials display approximately Type I isotherms with no hysteresis, and saturation was not reached for any of the materials under these conditions. Among the six isoreticular MOFs (IRMOFs) studied, the catenated materials exhibit the largest capacities on a molar basis, up to 9.8 H(2) per formula unit. The addition of functional groups (-Br, -NH(2), -C(2)H(4)-) to the phenylene links of IRMOF-1 (MOF-5), or their replacement with thieno[3,2-b]thiophene moieties in IRMOF-20, altered the adsorption behavior by a minor amount despite large variations in the pore volumes of the resulting materials. In contrast, replacement of the metal oxide units with those containing coordinatively unsaturated metal sites resulted in greater H(2) uptake. The enhanced affinities of these materials, MOF-74 and HKUST-1, were further demonstrated by calculation of the isosteric heats of adsorption, which were larger across much of the range of coverage examined, compared to those of representative IRMOFs. The results suggest that under low-loading conditions, the H(2) adsorption behavior of MOFs can be improved by imparting larger charge gradients on the metal oxide units and adjusting the link metrics to constrict the pore dimensions; however, a large pore volume is still a prerequisite feature. 相似文献
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Saturation H2 uptake in a series of microporous metal-organic frameworks (MOFs) has been measured at 77 K. Saturation pressures vary between 25 and 80 bar across the series, with MOF-177 showing the highest uptake on a gravimetric basis (7.5 wt %) and IRMOF-20 showing the highest uptake on a volumetric basis at 34 g/L. These results demonstrate that maximum H2 storage capacity in MOFs correlates well to surface area, and that feasible volumetric uptakes can be realized even in highly porous materials. 相似文献