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Here we demonstrate the self\u2010assembly of two simple organic molecules with Cd<jats:sup>II<\/jats:sup> and Pt<jats:sup>II<\/jats:sup> into a giant heterometallic supramolecular cube which is capable of binding a variety of mono\u2010 and dianionic guests within an enclosed cavity greater than 4200\u2005\u00c5<jats:sup>3<\/jats:sup>. Its structure was established by X\u2010ray crystallography and cryogenic transmission electron microscopy. This cube is the largest discrete abiological assembly that has been observed to bind guests in solution; cavity enclosure and coulombic effects appear to be crucial drivers of host\u2013guest chemistry at this scale. The degree of cavity occupancy, however, appears less important: the largest guest studied, bound the most weakly, occupying only 11\u2009% of the host cavity.<\/jats:p>","DOI":"10.1002\/anie.201501892","type":"journal-article","created":{"date-parts":[[2015,4,14]],"date-time":"2015-04-14T19:28:30Z","timestamp":1429039710000},"page":"5636-5640","source":"Crossref","is-referenced-by-count":81,"title":["Designed Enclosure Enables Guest Binding Within the 4200\u2005\u00c5<sup>3<\/sup> Cavity of a Self\u2010Assembled Cube"],"prefix":"10.1002","volume":"54","author":[{"given":"William J.","family":"Ramsay","sequence":"first","affiliation":[],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Filip T.","family":"Szczypi\u0144ski","sequence":"additional","affiliation":[],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Haim","family":"Weissman","sequence":"additional","affiliation":[],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Tanya K.","family":"Ronson","sequence":"additional","affiliation":[],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Maarten M. 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