Publication

Article Metrics

Citations


Online attention

Soluble/MOF-supported palladium single atoms catalyze the ligand-, additive-, and solvent-free aerobic oxidation of benzyl alcohols to benzoic acids

DOI: 10.1021/jacs.0c12367 DOI Help

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

Discipline Tags:

Molecular Complexes Catalysis Chemistry Materials Science Metal-Organic Frameworks Metallurgy Organometallic Chemistry

Technical Tags:

Diffraction Single Crystal X-ray Diffraction (SXRD)