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dc.contributor.authorThiam, Zeynabou
dc.contributor.authorAbou-Hamad, Edy
dc.contributor.authorDereli, Busra
dc.contributor.authorLiu, Lingmei
dc.contributor.authorEmwas, Abdul-Hamid M.
dc.contributor.authorAhmad, Rafia
dc.contributor.authorJiang, Hao
dc.contributor.authorIsah, Abdulrahman Adamu
dc.contributor.authorNdiaye, Papa Birame
dc.contributor.authorTaoufik, Mostafa
dc.contributor.authorHan, Yu
dc.contributor.authorCavallo, Luigi
dc.contributor.authorBasset, Jean-Marie
dc.contributor.authorEddaoudi, Mohamed
dc.date.accessioned2020-09-16T06:35:43Z
dc.date.available2020-09-16T06:35:43Z
dc.date.issued2020-09-09
dc.identifier.citationThiam, Z., Abou-Hamad, E., Dereli, B., Liu, L., Emwas, A.-H., Ahmad, R., … Eddaoudi, M. (2020). Extension of the Surface Organometallic Chemistry to Metal-Organic Framework: development of well-defined single site [(≡Zr-O-)W(=O)(CH2tBu)3] olefin metathesis catalyst. Journal of the American Chemical Society. doi:10.1021/jacs.0c06925
dc.identifier.issn0002-7863
dc.identifier.issn1520-5126
dc.identifier.doi10.1021/jacs.0c06925
dc.identifier.urihttp://hdl.handle.net/10754/665172
dc.description.abstractWe report here the first step by step anchoring of a W(≡CtBu)(CH2 tBu)3 complex on a highly crystalline and mesoporous MOF, namely Zr-NU-1000, using Surface organometallic Chemistry (SOMC) concept and methodology. SOMC allowed us to selectively graft the complex on the Zr6 clusters and characterize the obtained single site material by using state of the art experimental methods including extensive solid-state NMR techniques and HAADF-STEM imaging. Further FT-IR spectroscopy revealed the presence of a W=O moiety arising from the in situ reaction of the W≡CtBu functionality with the coordinated water coming from the 8-connected hexanuclear Zr6 clusters. All the steps leading to the final grafted molecular complex have been identified by DFT. The obtained material was tested for gas phase and liquid phase olefin metathesis and exhibited higher catalytic activity than the corresponding catalysts synthesized by different grafting methods. This contribution establishes the importance of applying SOMC to MOF chemistry to get well defined single site catalyst on MOF inorganic secondary building units, in particular the in situ synthesis of W=O alkyl complexes from their W carbyne analogues.
dc.description.sponsorshipDr. Karim Adil, Dr. Anissa Bendjeriou and Dr. Youssef Belmabkhout are thanked for fruitful discussions.
dc.description.sponsorshipThe authors gratefully acknowledge financial support from King Abdullah University of Science and Technology (KAUST), Kingdom of Saudi Arabia.
dc.publisherAmerican Chemical Society (ACS)
dc.relation.urlhttps://pubs.acs.org/doi/10.1021/jacs.0c06925
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 https://pubs.acs.org/doi/10.1021/jacs.0c06925.
dc.titleExtension of the Surface Organometallic Chemistry to Metal-Organic Framework: development of well-defined single site [(≡Zr-O-)W(=O)(CH2tBu)3] olefin metathesis catalyst.
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.departmentImaging and Characterization Core Lab
dc.contributor.departmentKAUST Catalysis Center (KCC)
dc.contributor.departmentNMR
dc.contributor.departmentNanostructured Functional Materials (NFM) laboratory
dc.contributor.departmentPhysical Science and Engineering (PSE) Division
dc.identifier.journalJournal of the American Chemical Society
dc.rights.embargodate2021-09-09
dc.eprint.versionPost-print
dc.contributor.institutionFunctional Materials Design, Discovery & Development Research Group (FMD3).
dc.contributor.institutionKing Fahd University of Petroleum & Minerals (KFUPM), Dhahran 31261, Saudi Arabia.
dc.contributor.institutionC2P2 (CNRS-UMR 5265), Université Lyon 1, ESCPE Lyon, 43 Boulevard du 11 Novembre 1918, 69626 Villeurbanne Cedex, France.
kaust.personThiam, Zeynabou
kaust.personThiam, Zeynabou
kaust.personAbou-Hamad, Edy
kaust.personDereli, Busra
kaust.personLiu, Lingmei
kaust.personEmwas, Abdul-Hamid M.
kaust.personAhmad, Rafia
kaust.personJiang, Hao
kaust.personIsah, Abdulrahman Adamu
kaust.personHan, Yu
kaust.personCavallo, Luigi
kaust.personBasset, Jean-Marie
kaust.personEddaoudi, Mohamed
refterms.dateFOA2020-09-16T06:36:42Z
dc.date.published-online2020-09-09
dc.date.published-print2020-09-30


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