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dc.contributor.authorAlezi, Dalal
dc.contributor.authorPeedikakkal, Abdul Malik P.
dc.contributor.authorWeselinski, Lukasz Jan
dc.contributor.authorGuillerm, Vincent
dc.contributor.authorBelmabkhout, Youssef
dc.contributor.authorCairns, Amy
dc.contributor.authorChen, Zhijie
dc.contributor.authorWojtas, Lukasz
dc.contributor.authorEddaoudi, Mohamed
dc.date.accessioned2015-04-12T06:32:35Z
dc.date.available2015-04-12T06:32:35Z
dc.date.issued2015-04-17
dc.identifier.citationQuest for Highly-connected MOF Platforms: Rare-Earth Polynuclear Clusters Versatility Meets Net Topology Needs. 2015:150407200837004 Journal of the American Chemical Society
dc.identifier.issn0002-7863
dc.identifier.issn1520-5126
dc.identifier.pmid25851127
dc.identifier.doi10.1021/jacs.5b00450
dc.identifier.urihttp://hdl.handle.net/10754/528236
dc.description.abstractGaining control over the assembly of highly porous rare-earth (RE) based metal-organic frameworks (MOFs) remains challenging. Here we report the latest discoveries on our continuous quest for highly-connected nets. The topological exploration based on the non-compatibility of 12-connected RE polynuclear carboxylate-based cluster, points of extension matching the 12 vertices of the cuboctahedron (cuo), with 3-connected organic ligands led to the discovery of two fascinating and highly-connected minimal edge-transitive nets, pek and aea. The reduced symmetry of the employed triangular tricarboxylate ligand, as compared to the prototype highly symmetrical 1,3,5-benzene(tris)benzoic acid guided the concurrent occurrence of nonanuclear [RE9(μ3-OH)12(μ3-O)2(O2C–)12] and hexanuclear [RE6(OH)8(O2C–)8] carboxylate-based clusters as 12-connected and 8-connected molecular building blocks in the structure of a 3-periodic pek-MOF based on a novel (3,8,12)-c trinodal net. The use of a tricarboxylate ligand with modified angles between carboxylate moieties led to the formation of a second MOF containing solely nonanuclear clusters and exhibiting once more a novel and a highly-connected (3,12,12)-c trinodal net with aea topology. Notably, it is the first time that RE-MOFs with double six-membered ring (d6R) secondary building units are isolated, representing therefore a critical step forward toward the design of novel and highly coordinated materials using the supermolecular building layer approach while considering the d6Rs as building pillars. Lastly, the potential of these new MOFs for gas separation/storage was investigated by performing gas adsorption studies of various probe gas molecules over a wide range of pressures. Noticeably, pek-MOF-1 showed excellent volumetric CO2 and CH4 uptakes at high pressures.
dc.publisherAmerican Chemical Society (ACS)
dc.relation.urlhttp://pubs.acs.org/doi/abs/10.1021/jacs.5b00450
dc.rightsThis document is the Accepted Manuscript version of a Published Work that appeared in final form in Journal of the American Chemical Society, copyright © American Chemical Society after peer review and technical editing by the publisher. To access the final edited and published work see http://pubs.acs.org/doi/abs/10.1021/jacs.5b00450.
dc.titleQuest for Highly-connected MOF Platforms: Rare-Earth Polynuclear Clusters Versatility Meets Net Topology Needs.
dc.typeArticle
dc.contributor.departmentAdvanced Membranes and Porous Materials Research Center
dc.contributor.departmentChemical Science Program
dc.contributor.departmentFunctional Materials Design, Discovery and Development (FMD3)
dc.contributor.departmentPhysical Science and Engineering (PSE) Division
dc.identifier.journalJournal of the American Chemical Society
dc.eprint.versionPost-print
dc.contributor.institutionDepartment of Chemistry, University of South Florida, 4202 East Fowler Avenue, Tampa, Florida 33620, United States
kaust.personWeselinski, Lukasz Jan
kaust.personGuillerm, Vincent
kaust.personBelmabkhout, Youssef
kaust.personCairns, Amy
kaust.personEddaoudi, Mohamed
kaust.personAlezi, Dalal
kaust.personPuthan Peedikakkal, Abdul Malik
kaust.personChen, Zhijie
dc.relation.issupplementedbyDOI:10.5517/cc1jc298
dc.relation.issupplementedbyDOI:10.5517/cc1jc2b9
dc.relation.issupplementedbyDOI:10.5517/cc1jc2cb
dc.relation.issupplementedbyDOI:10.5517/cc1jc2dc
dc.relation.issupplementedbyDOI:10.5517/cc1jc2fd
refterms.dateFOA2016-04-07T00:00:00Z
display.relations<b> Is Supplemented By:</b> <br/> <ul><li><i>[Dataset]</i> <br/> Alezi, D., Peedikakkal, A. M. P., Weseliński, Ł. J., Guillerm, V., Belmabkhout, Y., Cairns, A. J., … Eddaoudi, M. (2015). CCDC 1410819: Experimental Crystal Structure Determination [Data set]. Cambridge Crystallographic Data Centre. https://doi.org/10.5517/cc1jc298. DOI: <a href="https://doi.org/10.5517/cc1jc298">10.5517/cc1jc298</a> HANDLE: <a href="http://hdl.handle.net/10754/624447">10754/624447</a></li><li><i>[Dataset]</i> <br/> Alezi, D., Peedikakkal, A. M. P., Weseliński, Ł. J., Guillerm, V., Belmabkhout, Y., Cairns, A. J., … Eddaoudi, M. (2015). CCDC 1410820: Experimental Crystal Structure Determination [Data set]. Cambridge Crystallographic Data Centre. https://doi.org/10.5517/cc1jc2b9. DOI: <a href="https://doi.org/10.5517/cc1jc2b9">10.5517/cc1jc2b9</a> HANDLE: <a href="http://hdl.handle.net/10754/624448">10754/624448</a></li><li><i>[Dataset]</i> <br/> Alezi, D., Peedikakkal, A. M. P., Weseliński, Ł. J., Guillerm, V., Belmabkhout, Y., Cairns, A. J., … Eddaoudi, M. (2015). CCDC 1410821: Experimental Crystal Structure Determination [Data set]. Cambridge Crystallographic Data Centre. https://doi.org/10.5517/cc1jc2cb. DOI: <a href="https://doi.org/10.5517/cc1jc2cb">10.5517/cc1jc2cb</a> HANDLE: <a href="http://hdl.handle.net/10754/624449">10754/624449</a></li><li><i>[Dataset]</i> <br/> Alezi, D., Peedikakkal, A. M. P., Weseliński, Ł. J., Guillerm, V., Belmabkhout, Y., Cairns, A. J., … Eddaoudi, M. (2015). CCDC 1410822: Experimental Crystal Structure Determination [Data set]. Cambridge Crystallographic Data Centre. https://doi.org/10.5517/cc1jc2dc. DOI: <a href="https://doi.org/10.5517/cc1jc2dc">10.5517/cc1jc2dc</a> HANDLE: <a href="http://hdl.handle.net/10754/624450">10754/624450</a></li><li><i>[Dataset]</i> <br/> Alezi, D., Peedikakkal, A. M. P., Weseliński, Ł. J., Guillerm, V., Belmabkhout, Y., Cairns, A. J., … Eddaoudi, M. (2015). CCDC 1410823: Experimental Crystal Structure Determination [Data set]. Cambridge Crystallographic Data Centre. https://doi.org/10.5517/cc1jc2fd. DOI: <a href="https://doi.org/10.5517/cc1jc2fd">10.5517/cc1jc2fd</a> HANDLE: <a href="http://hdl.handle.net/10754/624451">10754/624451</a></li></ul>
dc.date.published-online2015-04-17
dc.date.published-print2015-04-29


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