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Soluble/MOF-supported palladium single atoms catalyze the ligand-, additive-, and solvent-free aerobic oxidation of benzyl alcohols to benzoic acids
Authors:
Estefanía
Tiburcio
(Universidad de Valencia)
,
Rossella
Greco
(Universitat Politècnica de València−Consejo Superior de Investigaciones Científicas)
,
Marta
Mon
(Universitat Politècnica de València−Consejo Superior de Investigaciones Científicas)
,
Jordi
Ballesteros-Soberanas
(Universitat Politècnica de València−Consejo Superior de Investigaciones Científicas)
,
Jesus
Ferrando-Soria
(Universidad de Valencia)
,
Juan-Carlos
Hernandez-Garrido
(Universidad de Cádiz)
,
Judit
Oliver-Meseguer
(0000-0001-8499-0395)
,
Carlo
Marini
(CELLS−ALBA Synchrotron)
,
Mercedes
Boronat
(Universitat Politècnica de València−Consejo Superior de Investigaciones Científicas)
,
Donatella
Armentano
(Università della Calabria)
,
Antonio
Leyva-Perez
(Universitat Politècnica de València−Consejo Superior de Investigaciones Científicas)
,
Emilio
Pardo
(Universidad de Valencia)
,
Miguel
López-Haro
(Universidad de Cádiz)
Co-authored by industrial partner:
No
Type:
Journal Paper
Journal:
Journal Of The American Chemical Society
State:
Published (Approved)
Published:
February 2021
Diamond Proposal Number(s):
18768
,
22411
Abstract: Metal single-atom catalysts (SACs) promise great rewards in terms of metal atom efficiency. However, the requirement of particular conditions and supports for their synthesis, together with the need of solvents and additives for catalytic implementation, often precludes their use under industrially viable conditions. Here, we show that palladium single atoms are spontaneously formed after dissolving tiny amounts of palladium salts in neat benzyl alcohols, to catalyze their direct aerobic oxidation to benzoic acids without ligands, additives, or solvents. With this result in hand, the gram-scale preparation and stabilization of Pd SACs within the functional channels of a novel methyl-cysteine-based metal−organic framework (MOF) was accomplished, to give a robust and crystalline solid catalyst fully characterized with the help of single-crystal X-ray diffraction (SCXRD). These results illustrate the advantages of metal speciation in ligand-free homogeneous organic reactions and the translation into solid catalysts for potential industrial implementation.
Subject Areas:
Chemistry,
Materials
Instruments:
I19-Small Molecule Single Crystal Diffraction
Other Facilities: CLAESS beamline at ALBA Synchrotron Light Source
Added On:
05/02/2021 09:39
Documents:
jacs.0c12367.pdf
Discipline Tags:
Molecular Complexes
Catalysis
Chemistry
Materials Science
Metal-Organic Frameworks
Metallurgy
Organometallic Chemistry
Technical Tags:
Diffraction
Single Crystal X-ray Diffraction (SXRD)