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

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      Author(s)
      Sika-Nartey, Abel Tetteh
      Sahin, Yesim
      Ercan, Kerem Emre
      Kap, Zeynep
      Kocak, Yusuf
      Erdali, Ayşe Dilay
      Erdivan, Beyzanur
      Türkmen, Yunus Emre
      Ozensoy, Emrah
      Date
      2022-12-08
      Source Title
      ACS Applied Nano Materials
      Electronic ISSN
      2574-0970
      Publisher
      American Chemical Society
      Volume
      5
      Issue
      12
      Pages
      18855 - 18870
      Language
      English
      Type
      Article
      Item Usage Stats
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      Abstract
      Two-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.
      Keywords
      Alcohol oxidation
      C−H oxidation
      Layered double hydroxide
      Heterogeneous catalysis
      Alkylarene C−H activation
      Permalink
      http://hdl.handle.net/11693/111269
      Published Version (Please cite this version)
      https://pubs.acs.org/doi/pdf/10.1021/acsanm.2c04634
      Collections
      • Department of Chemistry 707
      • Institute of Materials Science and Nanotechnology (UNAM) 2258
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