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Here, we report a retrospective design strategy for octahedral cages using a dibenzo[a,e]cyclooctene (DBCOT)-based nonaromatic tetratopic vertex that satisfies the required angular geometry. Coupling these vertices with linear ditopic linkers via imine condensation affords a series of isoreticular [6 + 12] cages. Their intrinsic insolubility precludes conventional crystallization and solution-phase characterization. Thermodynamically controlled in situ crystallization using polar aromatic solvents, Lewis acid catalysis, and slow cooling affords single crystals up to \u223c 1 mm and enables direct structure determination using a laboratory X-ray diffractometer. Directional edge-to-edge packing of the cages generates hierarchical pore networks that remain accessible after activation. Notably, this packing propagates the octahedral molecular geometry across length scales into the macroscopic octahedral crystal habit, revealing molecular-to-crystal shape transference. These findings establish a general platform for designing structurally rare higher-connectivity cages with geometry-programmed assembly across length scales.<\/jats:p>","DOI":"10.1021\/jacs.6c10786","type":"journal-article","created":{"date-parts":[[2026,8,31]],"date-time":"2026-08-31T18:58:10Z","timestamp":1788202690000},"page":"37056-37068","source":"Crossref","is-referenced-by-count":0,"title":["Symmetry-Encoded [6\n+ 12] Octahedral Organic Cages\nEnabled by Retrospective Design"],"prefix":"10.1021","volume":"148","author":[{"ORCID":"https:\/\/orcid.org\/0000-0002-5662-6569","authenticated-orcid":true,"given":"Shayan","family":"Karak","sequence":"first","affiliation":[{"name":"Indian Institute of Science Education and Research , , , ,","place":["Kolkata, Mohanpur, India, 741246"]},{"name":"Indian Institute of Science Education and Research , , , ,","place":["Kolkata, Mohanpur, India, 741246"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0009-0007-1056-5346","authenticated-orcid":true,"given":"Soubhik","family":"Khata","sequence":"additional","affiliation":[{"name":"Indian Institute of Science Education and Research , , , ,","place":["Kolkata, Mohanpur, India, 741246"]},{"name":"Indian Institute of Science Education and Research , , , ,","place":["Kolkata, Mohanpur, India, 741246"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Ekta","family":"Nehra","sequence":"additional","affiliation":[{"name":"JEOL Ltd , , ,","place":["Akishima, Tokyo, Japan, 196\u22128558"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0001-7136-1127","authenticated-orcid":true,"given":"Yusuke","family":"Nishiyama","sequence":"additional","affiliation":[{"name":"JEOL Ltd , , ,","place":["Akishima, Tokyo, Japan, 196\u22128558"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Naomi","family":"Watanabe","sequence":"additional","affiliation":[{"name":"JEOL Ltd , , ,","place":["Akishima, Tokyo, Japan, 196\u22128558"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Christian","family":"Go\u0308b","sequence":"additional","affiliation":[{"name":"Rigaku Asia Pacific Pte. Ltd ., 10 Anson Road, #22-04, International Plaza , ,","place":["Singapore, Singapore, 079903"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0002-3547-4746","authenticated-orcid":true,"given":"Rahul","family":"Banerjee","sequence":"additional","affiliation":[{"name":"Indian Institute of Science Education and Research , , , ,","place":["Kolkata, Mohanpur, India, 741246"]},{"name":"Indian Institute of Science Education and Research , , , ,","place":["Kolkata, Mohanpur, India, 741246"]},{"name":"Korea University , , ,","place":["Seoul, Korea, 02841"]}],"role":[{"vocabulary":"crossref","role":"author"}]}],"member":"316","published-online":{"date-parts":[[2026,8,24]]},"reference":[{"issue":"48","key":"2026090312101048900_cit1","doi-asserted-by":"publisher","first-page":"15507","DOI":"10.1021\/jacs.6b11821","article-title":"Reticular\nChemistry: Construction, Properties, and Precision Reactions of Frameworks","volume":"138","author":"Yaghi","year":"2016","journal-title":"J. Am. Chem. Soc."},{"issue":"5751","key":"2026090312101048900_cit2","doi-asserted-by":"publisher","first-page":"1166","DOI":"10.1126\/science.1120411","article-title":"Porous,\nCrystalline, Covalent Organic\nFrameworks","volume":"310","author":"Co\u0302te\u0301","year":"2005","journal-title":"Science"},{"issue":"6941","key":"2026090312101048900_cit3","doi-asserted-by":"publisher","first-page":"705","DOI":"10.1038\/nature01650","article-title":"Reticular\nsynthesis and the design of new materials","volume":"423","author":"Yaghi","year":"2003","journal-title":"Nature"},{"issue":"8","key":"2026090312101048900_cit4","doi-asserted-by":"publisher","first-page":"1295","DOI":"10.1021\/acscentsci.9b00750","article-title":"Reticular\nChemistry in All Dimensions","volume":"5","author":"Yaghi","year":"2019","journal-title":"ACS Cent. 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Soc."},{"issue":"30","key":"2026090312101048900_cit49","doi-asserted-by":"publisher","first-page":"5042","DOI":"10.1002\/anie.201000443","article-title":"Shape-Persistent\nOrganic Cage Compounds by Dynamic Covalent Bond Formation","volume":"49","author":"Mastalerz","year":"2010","journal-title":"Angew. Chem., Int. Ed."},{"issue":"16","key":"2026090312101048900_cit50","doi-asserted-by":"publisher","first-page":"6634","DOI":"10.1039\/c3cs60044k","article-title":"Recent advances in dynamic covalent\nchemistry","volume":"42","author":"Jin","year":"2013","journal-title":"Chem. Soc. Rev."},{"issue":"98","key":"2026090312101048900_cit51","doi-asserted-by":"publisher","first-page":"11948","DOI":"10.1039\/c2cc36602a","article-title":"Porous organic cage\ncrystals: characterising the porous\ncrystal surface","volume":"48","author":"Bojdys","year":"2012","journal-title":"Chem. 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Ed."}],"container-title":["Journal of the American\nChemical Society"],"original-title":[],"language":"en","link":[{"URL":"https:\/\/pubs.acs.org\/doi\/pdf\/10.1021\/jacs.6c10786","content-type":"application\/pdf","content-version":"vor","intended-application":"unspecified"},{"URL":"https:\/\/pubs.acs.org\/jacsat\/article-pdf\/148\/34\/37056\/67385056\/jacs.6c10786.pdf","content-type":"application\/pdf","content-version":"vor","intended-application":"syndication"},{"URL":"https:\/\/pubs.acs.org\/jacsat\/article-pdf\/148\/34\/37056\/67385056\/jacs.6c10786.pdf","content-type":"unspecified","content-version":"vor","intended-application":"similarity-checking"}],"deposited":{"date-parts":[[2026,9,3]],"date-time":"2026-09-03T16:22:22Z","timestamp":1788452542000},"score":1,"resource":{"primary":{"URL":"https:\/\/pubs.acs.org\/jacsat\/article\/148\/34\/37056\/5327623\/Symmetry-Encoded-6-12-Octahedral-Organic-Cages"}},"subtitle":[],"short-title":[],"issued":{"date-parts":[[2026,8,24]]},"references-count":52,"journal-issue":{"issue":"34","published-online":{"date-parts":[[2026,8,24]]},"published-print":{"date-parts":[[2026,9,2]]}},"URL":"https:\/\/doi.org\/10.1021\/jacs.6c10786","relation":{},"ISSN":["0002-7863","1520-5126"],"issn-type":[{"value":"0002-7863","type":"print"},{"value":"1520-5126","type":"electronic"}],"subject":[],"published":{"date-parts":[[2026,8,24]]}}}