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This consists of an organic\u2013inorganic hybrid hydrogen\u2010bonded nanoporous framework, the internal surface of which acts as a template for the three\u2010dimensional (3D) clustering of water molecules. The structure and molecular dynamics of this material are characterised by single\u2010crystal X\u2010ray diffraction, thermogravimetric analysis, Raman (H\/D isotopic substitution) spectroscopy, and <jats:sup>2<\/jats:sup>H solid\u2010state (wide\u2010line and MAS) NMR spectroscopy. Material <jats:bold>1<\/jats:bold> is shown to be unusual because 1) few nanoporous materials exhibit a well\u2010organised 3D framework of water molecules, 2) it provides a unique opportunity to follow experimentally and to rationalise the deconstruction of a 3D water framework and 3) despite the fact that the hybrid framework is a supramolecular salt, the structure does not collapse after dehydration and the final material is crystalline.<\/jats:p>","DOI":"10.1002\/chem.201000431","type":"journal-article","created":{"date-parts":[[2010,6,11]],"date-time":"2010-06-11T12:46:16Z","timestamp":1276260376000},"page":"7741-7749","source":"Crossref","is-referenced-by-count":14,"title":["3D\u20132D\u20130D Stepwise Deconstruction of a Water Framework Templated by a Nanoporous Organic\u2013Inorganic Hybrid Host"],"prefix":"10.1002","volume":"16","author":[{"given":"Jo\u00e3o","family":"Rocha","sequence":"first","affiliation":[]},{"given":"Fa\u2010Nian","family":"Shi","sequence":"additional","affiliation":[]},{"given":"Filipe\u2005A. 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