期刊
INORGANIC CHEMISTRY
卷 57, 期 12, 页码 6816-6824出版社
AMER CHEMICAL SOC
DOI: 10.1021/acs.inorgchem.8b00034
关键词
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资金
- Department of Science and Technology (DST), India [SR/S2/JCB-09/2011, EMR/2014/000520]
- DST-SERB
- BRNS
- Council for Scientific and Industrial Research, India
- Indian Association for the Cultivation of Science
Electroprotic storage materials, though invaluable in energy-related research, are scanty among non-natural compounds. Herein, we report a zinc(II) complex of the ligand 2,6-bis(phenylazo)pyridine (L), which acts as a multiple electron and proton reservoir during catalytic dehydrogenation of alcohols to aldehydes/ketones. The redox-inactive metal ion Zn(II) serves as an oxophilic Lewis acid, while the ligand behaves as efficient storage of electron and proton. Synthesis, X-ray structure, and spectral characterizations of the catalyst, ZnLCl2 (la) along with the two hydrogenated complexes of la, ZnH2LCl2 (lb), and ZnH4LCl2 (lc) are reported. It has been argued that the reversible azo-hydrazo redox couple of la controls aerobic dehydrogenation of alcohols. Hydrogenated complexes are hyper-reactive and quantitatively reduce O-2 and para-benzoquinone to H2O2 and para-hydroquinone, respectively. Plausible mechanistic pathways for alcohol oxidation are discussed based on controlled experiments, isotope labeling, and spectral analysis of intermediates.
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