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Compounds <jats:bold>1<\/jats:bold> and <jats:bold>2<\/jats:bold> have been characterized by elemental analyses, IR, <jats:sup>1<\/jats:sup>H and <jats:sup>13<\/jats:sup>C{<jats:sup>1<\/jats:sup>H} NMR spectroscopy, and FAB<jats:sup>+<\/jats:sup> mass spectrometry, while their slow recrystallization in air from organic solvents revealed a high affinity for water and resulted in the formation of the derived compounds [Ni{HN=C(3\u2010py)NC(3\u2010py)=NH}<jats:sub>2<\/jats:sub>]<jats:bold>\u00b7<\/jats:bold>6H<jats:sub>2<\/jats:sub>O (<jats:bold>1\u2032<\/jats:bold>) and [Ni{HN=C(3\u2010py)N(H)<jats:sub>0.5<\/jats:sub>C(3\u2010py)=NH}<jats:sub>2<\/jats:sub>]Cl<jats:bold>\u00b7<\/jats:bold>2H<jats:sub>2<\/jats:sub>O (<jats:bold>2\u2032<\/jats:bold>). Single\u2010crystal X\u2010ray diffraction analyses allowed the identification of discrete hexameric water or hybrid water\u2013chloride clusters hosted by the crystal matrixes of <jats:bold>1\u2032<\/jats:bold> and <jats:bold>2\u2032<\/jats:bold>, respectively. Both the (H<jats:sub>2<\/jats:sub>O)<jats:sub>6<\/jats:sub> and [(H<jats:sub>2<\/jats:sub>O)<jats:sub>4<\/jats:sub>(Cl)<jats:sub>2<\/jats:sub>]<jats:sup>2\u2013<\/jats:sup> clusters possess similar geometries and consist of cyclic planar tetranuclear (H<jats:sub>2<\/jats:sub>O)<jats:sub>4<\/jats:sub> or [(H<jats:sub>2<\/jats:sub>O)<jats:sub>2<\/jats:sub>(Cl)<jats:sub>2<\/jats:sub>]<jats:sup>2\u2013<\/jats:sup> cores with two dangling water molecules. These water associates occupy voids in the crystal cells and display extensive H\u2010bonding interactions with monomeric nickel\u2013organic units, thus playing a key role in the formation of 3D hydrogen\u2010bonded supramolecular assemblies. (\u00a9 Wiley\u2010VCH Verlag GmbH &amp; Co. KGaA, 69451 Weinheim, Germany, 2007)<\/jats:p>","DOI":"10.1002\/ejic.200700462","type":"journal-article","created":{"date-parts":[[2007,8,15]],"date-time":"2007-08-15T08:17:41Z","timestamp":1187165861000},"page":"4621-4627","update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":67,"title":["Identification of Hexameric Water and Hybrid Water\u2013Chloride Clusters Intercalated in the Crystal Hosts of (Imidoylamidine)nickel(II) Complexes"],"prefix":"10.1002","volume":"2007","author":[{"given":"Maximilian N.","family":"Kopylovich","sequence":"first","affiliation":[]},{"given":"Ekaterina A.","family":"Tronova","sequence":"additional","affiliation":[]},{"given":"Matti","family":"Haukka","sequence":"additional","affiliation":[]},{"given":"Alexander M.","family":"Kirillov","sequence":"additional","affiliation":[]},{"given":"Vadim Yu.","family":"Kukushkin","sequence":"additional","affiliation":[]},{"given":"Jo\u00e3o J. 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