Abstract
Metal–organic frameworks (MOFs) are a promising class of porous materials because it is possible to mutually control their porous structure, composition and functionality. However, it is still a challenge to predict the network topology of such framework materials prior to their synthesis. Here we use a new rare earth (RE) nonanuclear carboxylate-based cluster as an 18-connected molecular building block to form a gea-MOF (gea-MOF-1) based on a (3,18)-connected net. We then utilized this gea net as a blueprint to design and assemble another MOF (gea-MOF-2). In gea-MOF-2, the 18-connected RE clusters are replaced by metal–organic polyhedra, peripherally functionalized so as to have the same connectivity as the RE clusters. These metal–organic polyhedra act as supermolecular building blocks when they form gea-MOF-2. The discovery of a (3,18)-connected MOF followed by deliberate transposition of its topology to a predesigned second MOF with a different chemical system validates the prospective rational design of MOFs.
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Acknowledgements
Research reported in this publication was supported by the King Abdullah University of Science and Technology (KAUST).
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V.G. and M.E. contributed to the conceptual approach to designing the material synthetic experiments; V.G. carried out the synthetic experiments; V.G., Ł.W. and K.A. conducted and interpreted the crystallographic experiments; V.G. performed the topological analysis; Y.B. and A.J.C. conducted and interpreted low- and high-pressure sorption experiments and IAST models (Y.B.); V.D. designed, conducted and interpreted catalysis experiments; V.G., M.E. and Ł.J.W. envisioned, designed and synthesized (Ł.J.W.) the organic hexacarboxylic ligand; V.G., Y.B. and M.E. wrote the manuscript.
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Crystallographic data for compound gea-MOF-1 (CIF 22 kb)
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Crystallographic data for compound gea-MOF-2 (CIF 39 kb)
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Crystallographic data for compound Tb(III) hexanuclear cluster (CIF 22 kb)
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Guillerm, V., Weseliński, Ł., Belmabkhout, Y. et al. Discovery and introduction of a (3,18)-connected net as an ideal blueprint for the design of metal–organic frameworks. Nature Chem 6, 673–680 (2014). https://doi.org/10.1038/nchem.1982
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DOI: https://doi.org/10.1038/nchem.1982
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