Direct Observation of Molecular‐Level Template Action Leading to Self‐Assembly of a Porous Framework |
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| Authors: | Sneha R Bajpe Christine E?A Kirschhock Prof Alexander Aerts Dr Eric Breynaert Dr Gregory Absillis Tatjana N Parac‐Vogt Prof Lars Giebeler Dr Johan A Martens Prof |
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| Institution: | 1. Centre for Surface Science and Catalysis, Department of Microbial and Molecular Systems, K. U. Leuven, Kasteelpark Arenberg 23, Leuven B‐3001 (Belgium), Fax: (+32)?16‐321062;2. Molecular Design and Synthesis, Department of Chemistry, K. U. Leuven, Celestijnenlaan 200?F, Leuven B‐3001 (Belgium) |
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| Abstract: | The molecular steps involved in the self‐assembly of Cu3(BTC)2 (BTC=1,3,5‐benzenetricarboxylic acid) metal–organic frameworks that enclose Keggin‐type H3PW12O40 heteropolyacid molecules were unraveled by using solution 17O, 31P, and 183W NMR spectroscopy, small‐angle X‐ray scattering, near‐IR spectroscopy, and dynamic light scattering. In aqueous solution, complexation of Cu2+ ions with Keggin‐type heteropolyacids was observed. Cu2+ ions are arranged around the Keggin structure so that linking through benzenetricarboxylate groups results in the formation of the Cu3(BTC)2 MOF structure HKUST‐1. This is a unique instance in which a templating mechanism that relies on specific molecular‐level matching and leads to explicit nanoscale building units can be observed in situ during formation of the synthetic nanoporous material. |
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| Keywords: | keggin heteropolyacids NMR spectroscopy polyoxometalates metal– organic frameworks template synthesis |
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