Remote stabilization of copper paddlewheel based molecular building blocks in metal-organic frameworks

Handle URI:
http://hdl.handle.net/10754/564111
Title:
Remote stabilization of copper paddlewheel based molecular building blocks in metal-organic frameworks
Authors:
Gao, Wenyang; Cai, Rong; Pham, Tony T.; Forrest, Katherine A.; Hogan, Adam; Nugent, Patrick S.; Williams, Kia R.; Wojtas, Łukasz; Luebke, Ryan ( 0000-0002-1285-3321 ) ; Weselinski, Lukasz Jan ( 0000-0003-4516-2727 ) ; Zaworotko, Michael J.; Space, Brian; Chen, Yusheng; Eddaoudi, Mohamed ( 0000-0003-1916-9837 ) ; Shi, Xiaodong; Ma, Shengqian
Abstract:
Copper paddlewheel based molecular building blocks (MBBs) are ubiquitous and have been widely employed for the construction of highly porous metal-organic frameworks (MOFs). However, most copper paddlewheel based MOFs fail to retain their structural integrity in the presence of water. This instability is directly correlated to the plausible displacement of coordinating carboxylates in the copper paddlewheel MBB, [Cu2(O2C-)4], by the strongly coordinating water molecules. In this comprehensive study, we illustrate the chemical stability control in the rht-MOF platform via strengthening the coordinating bonds within the triangular inorganic MBB, [Cu3O(N4-x(CH)xC-)3] (x = 0, 1, or 2). Remotely, the chemical stabilization propagated into the paddlewheel MBB to afford isoreticular rht-MOFs with remarkably enhanced water/chemical stabilities compared to the prototypal rht-MOF-1. © 2015 American Chemical Society.
KAUST Department:
Functional Materials Design, Discovery and Development (FMD3); Physical Sciences and Engineering (PSE) Division; Chemical Science Program; Advanced Membranes and Porous Materials Research Center
Publisher:
American Chemical Society (ACS)
Journal:
Chemistry of Materials
Issue Date:
24-Mar-2015
DOI:
10.1021/acs.chemmater.5b00084
Type:
Article
ISSN:
08974756
Sponsors:
The authors acknowledge NSF (DMR-1352065) and USF for financial support of this work. B.S. acknowledges the National Science Foundation (Award No. CHE-1152362), the computational resources that were made available by an XSEDE Grant (No. TG-DMR090028), and the use of the services provided by Research Computing at the University of South Florida. X.S. thanks NSF for the financial support (CHE-0844602). The single-crystal X-ray diffraction of rht-MOF-tri and rht-MOF-pyr was carried out at the Advanced Photon Source on beamline 15-ID-B of ChemMatCARS Sector 15, supported by the National Science Foundation under grant number NSF/CHE-1346572. This research used resources of the Advanced Photon Source, a U.S. Department of Energy (DOE) Office of Science User Facility operated for the DOE Office of Science by Argonne National Laboratory under Contract No. DE-AC02-06CH11357. M.E. acknowledges the financial support from King Abdullah University of Science and Technology.
Is Supplemented By:
Gao, W.-Y., Cai, R., Pham, T., Forrest, K. A., Hogan, A., Nugent, P., … Ma, S. (2015). CCDC 884202: Experimental Crystal Structure Determination [Data set]. Cambridge Crystallographic Data Centre. https://doi.org/10.5517/ccyp2nb; DOI:10.5517/ccyp2nb; HANDLE:http://hdl.handle.net/10754/624716; Gao, W.-Y., Cai, R., Pham, T., Forrest, K. A., Hogan, A., Nugent, P., … Ma, S. (2015). CCDC 1061183: Experimental Crystal Structure Determination [Data set]. Cambridge Crystallographic Data Centre. https://doi.org/10.5517/cc14m7qq; DOI:10.5517/cc14m7qq; HANDLE:http://hdl.handle.net/10754/624429
Appears in Collections:
Articles; Advanced Membranes and Porous Materials Research Center; Physical Sciences and Engineering (PSE) Division; Functional Materials Design, Discovery and Development (FMD3); Chemical Science Program

Full metadata record

DC FieldValue Language
dc.contributor.authorGao, Wenyangen
dc.contributor.authorCai, Rongen
dc.contributor.authorPham, Tony T.en
dc.contributor.authorForrest, Katherine A.en
dc.contributor.authorHogan, Adamen
dc.contributor.authorNugent, Patrick S.en
dc.contributor.authorWilliams, Kia R.en
dc.contributor.authorWojtas, Łukaszen
dc.contributor.authorLuebke, Ryanen
dc.contributor.authorWeselinski, Lukasz Janen
dc.contributor.authorZaworotko, Michael J.en
dc.contributor.authorSpace, Brianen
dc.contributor.authorChen, Yushengen
dc.contributor.authorEddaoudi, Mohameden
dc.contributor.authorShi, Xiaodongen
dc.contributor.authorMa, Shengqianen
dc.date.accessioned2015-08-03T12:32:38Zen
dc.date.available2015-08-03T12:32:38Zen
dc.date.issued2015-03-24en
dc.identifier.issn08974756en
dc.identifier.doi10.1021/acs.chemmater.5b00084en
dc.identifier.urihttp://hdl.handle.net/10754/564111en
dc.description.abstractCopper paddlewheel based molecular building blocks (MBBs) are ubiquitous and have been widely employed for the construction of highly porous metal-organic frameworks (MOFs). However, most copper paddlewheel based MOFs fail to retain their structural integrity in the presence of water. This instability is directly correlated to the plausible displacement of coordinating carboxylates in the copper paddlewheel MBB, [Cu2(O2C-)4], by the strongly coordinating water molecules. In this comprehensive study, we illustrate the chemical stability control in the rht-MOF platform via strengthening the coordinating bonds within the triangular inorganic MBB, [Cu3O(N4-x(CH)xC-)3] (x = 0, 1, or 2). Remotely, the chemical stabilization propagated into the paddlewheel MBB to afford isoreticular rht-MOFs with remarkably enhanced water/chemical stabilities compared to the prototypal rht-MOF-1. © 2015 American Chemical Society.en
dc.description.sponsorshipThe authors acknowledge NSF (DMR-1352065) and USF for financial support of this work. B.S. acknowledges the National Science Foundation (Award No. CHE-1152362), the computational resources that were made available by an XSEDE Grant (No. TG-DMR090028), and the use of the services provided by Research Computing at the University of South Florida. X.S. thanks NSF for the financial support (CHE-0844602). The single-crystal X-ray diffraction of rht-MOF-tri and rht-MOF-pyr was carried out at the Advanced Photon Source on beamline 15-ID-B of ChemMatCARS Sector 15, supported by the National Science Foundation under grant number NSF/CHE-1346572. This research used resources of the Advanced Photon Source, a U.S. Department of Energy (DOE) Office of Science User Facility operated for the DOE Office of Science by Argonne National Laboratory under Contract No. DE-AC02-06CH11357. M.E. acknowledges the financial support from King Abdullah University of Science and Technology.en
dc.publisherAmerican Chemical Society (ACS)en
dc.titleRemote stabilization of copper paddlewheel based molecular building blocks in metal-organic frameworksen
dc.typeArticleen
dc.contributor.departmentFunctional Materials Design, Discovery and Development (FMD3)en
dc.contributor.departmentPhysical Sciences and Engineering (PSE) Divisionen
dc.contributor.departmentChemical Science Programen
dc.contributor.departmentAdvanced Membranes and Porous Materials Research Centeren
dc.identifier.journalChemistry of Materialsen
dc.contributor.institutionDepartment of Chemistry, University of South Florida, 4202 East Fowler Avenue, CHE205Tampa, FL, United Statesen
dc.contributor.institutionDepartment of Chemistry, West Virginia UniversityMorgantown, WV, United Statesen
dc.contributor.institutionChemMatCARS, Center for Advanced Radiation Sources, University of Chicago, 9700 S. Cass AvenueArgonne, IL, United Statesen
kaust.authorLuebke, Ryanen
kaust.authorWeselinski, Lukasz Janen
kaust.authorEddaoudi, Mohameden
dc.relation.isSupplementedByGao, W.-Y., Cai, R., Pham, T., Forrest, K. A., Hogan, A., Nugent, P., … Ma, S. (2015). CCDC 884202: Experimental Crystal Structure Determination [Data set]. Cambridge Crystallographic Data Centre. https://doi.org/10.5517/ccyp2nben
dc.relation.isSupplementedByDOI:10.5517/ccyp2nben
dc.relation.isSupplementedByHANDLE:http://hdl.handle.net/10754/624716en
dc.relation.isSupplementedByGao, W.-Y., Cai, R., Pham, T., Forrest, K. A., Hogan, A., Nugent, P., … Ma, S. (2015). CCDC 1061183: Experimental Crystal Structure Determination [Data set]. Cambridge Crystallographic Data Centre. https://doi.org/10.5517/cc14m7qqen
dc.relation.isSupplementedByDOI:10.5517/cc14m7qqen
dc.relation.isSupplementedByHANDLE:http://hdl.handle.net/10754/624429en
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