Reticular Chemistry at Its Best: Directed Assembly of Hexagonal Building Units into the Awaited Metal-Organic Framework with the Intricate Polybenzene Topology, pbz-MOF

Handle URI:
http://hdl.handle.net/10754/621097
Title:
Reticular Chemistry at Its Best: Directed Assembly of Hexagonal Building Units into the Awaited Metal-Organic Framework with the Intricate Polybenzene Topology, pbz-MOF
Authors:
Alezi, Dalal; Spanopoulos, Ioannis; Tsangarakis, Constantinos; Shkurenko, Aleksander; Adil, Karim; Belmabkhout, Youssef; O'Keeffe, Michael; Eddaoudi, Mohamed ( 0000-0003-1916-9837 ) ; Trikalitis, Pantelis N.
Abstract:
The ability to direct the assembly of hexagonal building units offers great prospective to construct the awaited and looked-for hypothetical polybenzene (pbz) or “cubic graphite” structure, described 70 years ago. Here, we demonstrate the successful use of reticular chemistry as an appropriate strategy for the design and deliberate construction of a zirconium-based metal–organic framework (MOF) with the intricate pbz underlying net topology. The judicious selection of the perquisite hexagonal building units, six connected organic and inorganic building blocks, allowed the formation of the pbz-MOF-1, the first example of a Zr(IV)-based MOF with pbz topology. Prominently, pbz-MOF-1 is highly porous, with associated pore size and pore volume of 13 Å and 0.99 cm3 g–1, respectively, and offers high gravimetric and volumetric methane storage capacities (0.23 g g–1 and 210.4 cm3 (STP) cm–3 at 80 bar). Notably, the pbz-MOF-1 pore system permits the attainment of one of the highest CH4 adsorbed phase density enhancements at high pressures (0.15 and 0.21 g cm–3 at 35 and 65 bar, respectively) as compared to benchmark microporous MOFs.
KAUST Department:
Advanced Membranes and Porous Materials Research Center; Functional Materials Design, Discovery and Development (FMD3); Physical Sciences and Engineering (PSE) Division
Citation:
Alezi D, Spanopoulos I, Tsangarakis C, Shkurenko A, Adil K, et al. (2016) Reticular Chemistry at Its Best: Directed Assembly of Hexagonal Building Units into the Awaited Metal-Organic Framework with the Intricate Polybenzene Topology, pbz-MOF. Journal of the American Chemical Society 138: 12767–12770. Available: http://dx.doi.org/10.1021/jacs.6b08176.
Publisher:
American Chemical Society (ACS)
Journal:
Journal of the American Chemical Society
Issue Date:
5-Oct-2016
DOI:
10.1021/jacs.6b08176
Type:
Article
ISSN:
0002-7863; 1520-5126
Sponsors:
This research has been cofinanced by the European Union and Greek national funds through the Operational Program “Education and Lifelong Learning” of the National Strategic Reference Framework, Research Funding Program: ARISTEIA II - 4862. Financial support by King Abdullah University of Science and Technology is gratefully acknowledged.
Is Supplemented By:
Alezi, D., Spanopoulos, I., Tsangarakis, C., Shkurenko, A., Adil, K., Belmabkhout, Y., … Trikalitis, P. N. (2016). CCDC 1497835: Experimental Crystal Structure Determination [Data set]. Cambridge Crystallographic Data Centre. https://doi.org/10.5517/ccdc.csd.cc1m8m8s; DOI:10.5517/ccdc.csd.cc1m8m8s; HANDLE:http://hdl.handle.net/10754/624593
Additional Links:
http://pubs.acs.org/doi/full/10.1021/jacs.6b08176
Appears in Collections:
Articles; Advanced Membranes and Porous Materials Research Center; Physical Sciences and Engineering (PSE) Division; Functional Materials Design, Discovery and Development (FMD3)

Full metadata record

DC FieldValue Language
dc.contributor.authorAlezi, Dalalen
dc.contributor.authorSpanopoulos, Ioannisen
dc.contributor.authorTsangarakis, Constantinosen
dc.contributor.authorShkurenko, Aleksanderen
dc.contributor.authorAdil, Karimen
dc.contributor.authorBelmabkhout, Youssefen
dc.contributor.authorO'Keeffe, Michaelen
dc.contributor.authorEddaoudi, Mohameden
dc.contributor.authorTrikalitis, Pantelis N.en
dc.date.accessioned2016-10-20T11:52:19Z-
dc.date.available2016-10-20T11:52:19Z-
dc.date.issued2016-10-05en
dc.identifier.citationAlezi D, Spanopoulos I, Tsangarakis C, Shkurenko A, Adil K, et al. (2016) Reticular Chemistry at Its Best: Directed Assembly of Hexagonal Building Units into the Awaited Metal-Organic Framework with the Intricate Polybenzene Topology, pbz-MOF. Journal of the American Chemical Society 138: 12767–12770. Available: http://dx.doi.org/10.1021/jacs.6b08176.en
dc.identifier.issn0002-7863en
dc.identifier.issn1520-5126en
dc.identifier.doi10.1021/jacs.6b08176en
dc.identifier.urihttp://hdl.handle.net/10754/621097-
dc.description.abstractThe ability to direct the assembly of hexagonal building units offers great prospective to construct the awaited and looked-for hypothetical polybenzene (pbz) or “cubic graphite” structure, described 70 years ago. Here, we demonstrate the successful use of reticular chemistry as an appropriate strategy for the design and deliberate construction of a zirconium-based metal–organic framework (MOF) with the intricate pbz underlying net topology. The judicious selection of the perquisite hexagonal building units, six connected organic and inorganic building blocks, allowed the formation of the pbz-MOF-1, the first example of a Zr(IV)-based MOF with pbz topology. Prominently, pbz-MOF-1 is highly porous, with associated pore size and pore volume of 13 Å and 0.99 cm3 g–1, respectively, and offers high gravimetric and volumetric methane storage capacities (0.23 g g–1 and 210.4 cm3 (STP) cm–3 at 80 bar). Notably, the pbz-MOF-1 pore system permits the attainment of one of the highest CH4 adsorbed phase density enhancements at high pressures (0.15 and 0.21 g cm–3 at 35 and 65 bar, respectively) as compared to benchmark microporous MOFs.en
dc.description.sponsorshipThis research has been cofinanced by the European Union and Greek national funds through the Operational Program “Education and Lifelong Learning” of the National Strategic Reference Framework, Research Funding Program: ARISTEIA II - 4862. Financial support by King Abdullah University of Science and Technology is gratefully acknowledged.en
dc.publisherAmerican Chemical Society (ACS)en
dc.relation.urlhttp://pubs.acs.org/doi/full/10.1021/jacs.6b08176en
dc.rightsACS Editors' Choice - This is an open access article published under an ACS AuthorChoice License, which permits copying and redistribution of the article or any adaptations for non-commercial purposes.en
dc.rights.urihttp://pubs.acs.org/page/policy/authorchoice_termsofuse.htmlen
dc.titleReticular Chemistry at Its Best: Directed Assembly of Hexagonal Building Units into the Awaited Metal-Organic Framework with the Intricate Polybenzene Topology, pbz-MOFen
dc.typeArticleen
dc.contributor.departmentAdvanced Membranes and Porous Materials Research Centeren
dc.contributor.departmentFunctional Materials Design, Discovery and Development (FMD3)en
dc.contributor.departmentPhysical Sciences and Engineering (PSE) Divisionen
dc.identifier.journalJournal of the American Chemical Societyen
dc.eprint.versionPublisher's Version/PDFen
dc.contributor.institutionDepartment of Chemistry, University of Crete, Voutes 71003 Heraklion, Greeceen
dc.contributor.institutionSchool of Molecular Sciences, Arizona State University, Tempe, Arizona 85287, United Statesen
kaust.authorAlezi, Dalalen
kaust.authorShkurenko, Aleksanderen
kaust.authorAdil, Karimen
kaust.authorBelmabkhout, Youssefen
kaust.authorEddaoudi, Mohameden
dc.relation.isSupplementedByAlezi, D., Spanopoulos, I., Tsangarakis, C., Shkurenko, A., Adil, K., Belmabkhout, Y., … Trikalitis, P. N. (2016). CCDC 1497835: Experimental Crystal Structure Determination [Data set]. Cambridge Crystallographic Data Centre. https://doi.org/10.5517/ccdc.csd.cc1m8m8sen
dc.relation.isSupplementedByDOI:10.5517/ccdc.csd.cc1m8m8sen
dc.relation.isSupplementedByHANDLE:http://hdl.handle.net/10754/624593en
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