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Reactions of <jats:bold>2<\/jats:bold> with a series of linear aromatic diamines results in the formation of polycrystalline frameworks [Zn<jats:sub>4<\/jats:sub>(dipp)<jats:sub>4<\/jats:sub>(<jats:bold>L<\/jats:bold>)<jats:sub>2<\/jats:sub>]<jats:sub><jats:italic>n<\/jats:italic><\/jats:sub> (<jats:bold>3<\/jats:bold>\u2013<jats:bold>6<\/jats:bold>) (<jats:bold>L<\/jats:bold>=<jats:bold>L<jats:sup>1<\/jats:sup><\/jats:bold> to <jats:bold>L<jats:sup>4<\/jats:sup><\/jats:bold>, diimines formed by condensation of 4\u2010pyridine carboxaldehyde with diamines). Employing an alternative synthetic strategy, through a diffusion\u2010controlled slow reaction of <jats:bold>2<\/jats:bold> with the pre\u2010synthesized 4,4\u2018\u2010bispyridyl bisimine (<jats:bold>L<jats:sup>3<\/jats:sup><\/jats:bold>), [Zn<jats:sub>4<\/jats:sub>(dipp)<jats:sub>4<\/jats:sub>(<jats:bold>L<jats:sup>3<\/jats:sup><\/jats:bold>)<jats:sub>2<\/jats:sub>]<jats:sub><jats:italic>n<\/jats:italic><\/jats:sub> (<jats:bold>5\u2032<\/jats:bold>) has been obtained as single crystals. Complex <jats:bold>5\u2032<\/jats:bold> is a 3D\u2010framework, exhibiting a rare eightfold interpenetrated diamondoid network. The long spacer length (19.6\u2005\u00c5) results in extensive entanglement in <jats:bold>5\u2032<\/jats:bold>. Powder diffraction data suggest that these compounds are isoreticular 3D\u2010frameworks. To study the effect of the relative position of pyridyl donors with respect to the central benzidine moiety, 3,3\u2018\u2010bispyridyl bisimine (<jats:bold>L<jats:sup>5<\/jats:sup><\/jats:bold>) was investigated as the spacer. A slow reaction of <jats:bold>1\u2009b<\/jats:bold> with <jats:bold>L<jats:sup>5<\/jats:sup><\/jats:bold> leads to the isolation of a 2D\u2010boxed\u2010sheet coordination polymer [Zn<jats:sub>4<\/jats:sub>(dipp)<jats:sub>4<\/jats:sub>(<jats:bold>L<jats:sup>5<\/jats:sup><\/jats:bold>)<jats:sub>2<\/jats:sub>]<jats:sub><jats:italic>n<\/jats:italic><\/jats:sub> (<jats:bold>7<\/jats:bold>). Selective formation of 3D\u2010framework <jats:bold>5\u2032<\/jats:bold> from <jats:bold>L<jats:sup>3<\/jats:sup><\/jats:bold> and the 2D\u2010framework <jats:bold>7<\/jats:bold> from <jats:bold>L<jats:sup>5<\/jats:sup><\/jats:bold> is due to the angles created by the coordination of <jats:italic>para<\/jats:italic>\u2010 and <jats:italic>meta<\/jats:italic>\u2010pyridyl nitrogen centers at the zinc centers of the D4R cubane. Compound <jats:bold>5\u2032<\/jats:bold> has been utilized as a catalyst for Knoevenagel condensation.<\/jats:p>","DOI":"10.1002\/chem.201800149","type":"journal-article","created":{"date-parts":[[2018,3,22]],"date-time":"2018-03-22T19:31:10Z","timestamp":1521747070000},"page":"6178-6190","update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":21,"title":["A [4+2] Condensation Strategy to Imine\u2010Linked Single\u2010Crystalline Zeolite\u2010Like Zinc Phosphate Frameworks"],"prefix":"10.1002","volume":"24","author":[{"given":"Ritambhara","family":"Jangir","sequence":"first","affiliation":[{"name":"Department of Chemistry Institution Institute of Technology Bombay, Powai  Mumbai- 400076 India"}],"role":[{"role":"author","vocabulary":"crossref"}]},{"given":"Alok Ch.","family":"Kalita","sequence":"additional","affiliation":[{"name":"Department of Chemistry Institution Institute of Technology Bombay, Powai  Mumbai- 400076 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