Journal
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
Volume 143, Issue 6, Pages 2581-2592Publisher
AMER CHEMICAL SOC
DOI: 10.1021/jacs.0c12367
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Funding
- Ministero dell'Istruzione, dell'Universita e della Ricerca (Italy)
- MINECO (Spain) [PID2019-104778GB-I00, CTQ 2017-86735-P, RTC-2017-6331-5, SEV-2016-0683, CEX2019-000919-M]
- Fondazione CARIPLO/Economia Circolare: ricerca per un futuro sostenibile 2019 [2019-2090]
- la Caixa Foundation [ID100010434, LCF/BQ/PR19/11700011]
- La Caixa scholarship [100010434, LCF/BQ/DI19/11730029]
- European Research Council under the European Union's Horizon 2020 research and innovation programme/ERC Grant [814804]
- Juan de la Cierva program [IJC2018-036514-I]
- MOCA
- Diamond Light Source
- 2019 Post-doctoral Junior Leader-Retaining Fellowship
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Palladium single atoms can be spontaneously formed in neat benzyl alcohols and used for organic oxidation reactions without additives or solvents. By stabilizing Pd SACs within a metal-organic framework, a solid catalyst was successfully prepared and characterized.
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.
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