Two-dimensional bimetallic hydroxide nanostructures for catalyzing low-temperature aerobic C–H bond activation in alkylarene and alcohol partial oxidation

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buir.contributor.authorSika-Nartey, Abel Tetteh
buir.contributor.authorSahin, Yesim
buir.contributor.authorErcan, Kerem Emre
buir.contributor.authorKap, Zeynep
buir.contributor.authorKocak, Yusuf
buir.contributor.authorErdali, Ayşe Dilay
buir.contributor.authorErdivan, Beyzanur
buir.contributor.authorTürkmen, Yunus Emre
buir.contributor.authorOzensoy, Emrah
buir.contributor.orcidSahin, Yesim|0000-0001-9717-9729
buir.contributor.orcidSika-Nartey, Abel Tetteh|0000-0002-5327-844X
buir.contributor.orcidErcan, Kerem Emre|0000-0003-4650-7977
buir.contributor.orcidKap, Zeynep|0000-0002-2102-4744
buir.contributor.orcidKocak, Yusuf|0000-0003-4511-1321
buir.contributor.orcidErdali, Ayşe Dilay|0000-0002-5065-1317
buir.contributor.orcidErdivan, Beyzanur|0000-0002-1725-1127
buir.contributor.orcidTürkmen, Yunus Emre|0000-0002-9797-2820
buir.contributor.orcidOzensoy, Emrah|0000-0003-4352-3824
dc.citation.epage18870en_US
dc.citation.issueNumber12en_US
dc.citation.spage18855en_US
dc.citation.volumeNumber5en_US
dc.contributor.authorSika-Nartey, Abel Tetteh
dc.contributor.authorSahin, Yesim
dc.contributor.authorErcan, Kerem Emre
dc.contributor.authorKap, Zeynep
dc.contributor.authorKocak, Yusuf
dc.contributor.authorErdali, Ayşe Dilay
dc.contributor.authorErdivan, Beyzanur
dc.contributor.authorTürkmen, Yunus Emre
dc.contributor.authorOzensoy, Emrah
dc.date.accessioned2023-02-14T13:00:37Z
dc.date.available2023-02-14T13:00:37Z
dc.date.issued2022-12-08
dc.departmentDepartment of Chemistryen_US
dc.description.abstractTwo-dimensional (2D) bimetallic NixMn1–x(OH)y layered double hydroxide (LDH) nanostructures were synthesized and optimized as a remarkably active catalytic platform for low-temperature aerobic C–H bond activation in alkylarenes and partial oxidation of alcohols using a wide substrate (i.e., reactant) and diverse solvent scope. The NixMn1–x(OH)y structure consists of nonprecious and earth-abundant metals that can effectively operate at low catalyst loadings, requiring only molecular oxygen as the stoichiometric oxidant. Structurally diverse alkylarenes as well as primary and secondary alcohols were shown to be competent substrates where oxidation products were obtained in excellent yields (93–99%). Comprehensive catalyst structural characterization via XRD, ATR-IR, TEM, EDX, XPS, BET, and TGA indicated that the ultimately optimized Ni0.6Mn0.4(OH)y-9S catalyst possessed not only particular rotational faults in its β-Ni0.6Mn0.4(OH)y domains but also distinct α/β-Ni0.6Mn0.4(OH)y interstratification disorders, in addition to a relatively high specific surface area of 125 m2/g, a 2D platelet morphology, and an average Mn oxidation state of +3.5, suggesting the presence of both Mn3+ and Mn4+ species in its structure working in a synergistic fashion with the Ni2+/x+ cations (the latter is justified by the lack of catalytic activity in the monometallic LDH catalysts Ni(OH)2 and Mn(OH)2). Kinetic isotope effect studies carried out in the fluorene oxidation reaction (kH/kD = 5.7) revealed that the rate-determining step of the catalytic oxidation reaction directly involved the scission of a C–H bond. Moreover, the optimized catalyst was demonstrated to be reusable through the application of a regeneration protocol, which can redeem the full initial activity of the carbon-poisoned spent catalyst in the fluorene oxidation reaction.en_US
dc.description.provenanceSubmitted by Samet Emre (samet.emre@bilkent.edu.tr) on 2023-02-14T13:00:37Z No. of bitstreams: 1 Two-dimensional_bimetallic_hydroxide_nanostructures_for_catalyzing_low-temperature_aerobic_C–H_bond_activation_in_alkylarene_and_alcohol_partial_oxidation.pdf: 8349829 bytes, checksum: 019f6fad11fe67ce11ce2923fd9d3662 (MD5)en
dc.description.provenanceMade available in DSpace on 2023-02-14T13:00:37Z (GMT). No. of bitstreams: 1 Two-dimensional_bimetallic_hydroxide_nanostructures_for_catalyzing_low-temperature_aerobic_C–H_bond_activation_in_alkylarene_and_alcohol_partial_oxidation.pdf: 8349829 bytes, checksum: 019f6fad11fe67ce11ce2923fd9d3662 (MD5) Previous issue date: 2022-12-08en
dc.identifier.doi10.1021/acsanm.2c04634en_US
dc.identifier.eissn2574-0970
dc.identifier.urihttp://hdl.handle.net/11693/111269
dc.language.isoEnglishen_US
dc.publisherAmerican Chemical Societyen_US
dc.relation.isversionofhttps://pubs.acs.org/doi/pdf/10.1021/acsanm.2c04634en_US
dc.source.titleACS Applied Nano Materialsen_US
dc.subjectAlcohol oxidationen_US
dc.subjectC−H oxidationen_US
dc.subjectLayered double hydroxideen_US
dc.subjectHeterogeneous catalysisen_US
dc.subjectAlkylarene C−H activationen_US
dc.titleTwo-dimensional bimetallic hydroxide nanostructures for catalyzing low-temperature aerobic C–H bond activation in alkylarene and alcohol partial oxidationen_US
dc.typeArticleen_US

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Department of Chemistry
Institute of Materials Science and Nanotechnology (UNAM)