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    Quest for Highly-connected MOF Platforms: Rare-Earth Polynuclear Clusters Versatility Meets Net Topology Needs.

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    Type
    Article
    Authors
    Alezi, Dalal cc
    Peedikakkal, Abdul Malik P.
    Weselinski, Lukasz Jan cc
    Guillerm, Vincent cc
    Belmabkhout, Youssef cc
    Cairns, Amy
    Chen, Zhijie cc
    Wojtas, Lukasz
    Eddaoudi, Mohamed cc
    KAUST Department
    Advanced Membranes and Porous Materials Research Center
    Chemical Science Program
    Functional Materials Design, Discovery and Development (FMD3)
    Physical Science and Engineering (PSE) Division
    Date
    2015-04-17
    Online Publication Date
    2015-04-17
    Print Publication Date
    2015-04-29
    Permanent link to this record
    http://hdl.handle.net/10754/528236
    
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    Show full item record
    Abstract
    Gaining 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.
    Citation
    Quest for Highly-connected MOF Platforms: Rare-Earth Polynuclear Clusters Versatility Meets Net Topology Needs. 2015:150407200837004 Journal of the American Chemical Society
    Publisher
    American Chemical Society (ACS)
    Journal
    Journal of the American Chemical Society
    DOI
    10.1021/jacs.5b00450
    PubMed ID
    25851127
    Additional Links
    http://pubs.acs.org/doi/abs/10.1021/jacs.5b00450
    Relations
    Is Supplemented By:
    • [Dataset]
      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: 10.5517/cc1jc298 HANDLE: 10754/624447
    • [Dataset]
      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: 10.5517/cc1jc2b9 HANDLE: 10754/624448
    • [Dataset]
      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: 10.5517/cc1jc2cb HANDLE: 10754/624449
    • [Dataset]
      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: 10.5517/cc1jc2dc HANDLE: 10754/624450
    • [Dataset]
      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: 10.5517/cc1jc2fd HANDLE: 10754/624451
    ae974a485f413a2113503eed53cd6c53
    10.1021/jacs.5b00450
    Scopus Count
    Collections
    Articles; Advanced Membranes and Porous Materials Research Center; Physical Science and Engineering (PSE) Division; Functional Materials Design, Discovery and Development (FMD3); Chemical Science Program

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