Journal
NATURE COMMUNICATIONS
Volume 9, Issue -, Pages -Publisher
NATURE PUBLISHING GROUP
DOI: 10.1038/s41467-018-05351-w
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Funding
- National Natural Science Foundation of China [21476109, U1662107, 21136005, 21303084]
- Specialized Research Fund for the Doctoral Program of Higher Education [20133221120002]
- Project of Priority Academic Program Development of Jiangsu Higher Education Institutions (PAPD)
- Jiangsu National Synergetic Innovation Center for Advanced Materials
- Young Investigator Award from National University of Singapore [R-279-000-464-133]
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Hydroxylation of arenes via activation of aromatic C-sp2-H bond has attracted great attention for decades but remains a huge challenge. Herein, we achieve the ring hydroxylation of various arenes with stoichiometric hydrogen peroxide (H2O2) into the corresponding phenols on a robust heterogeneous catalyst series of V-Si-ZSM-22 (TON type vanadium silicalite zeolites) that is straightforward synthesized from an unusual ionic liquid involved dry-gelconversion route. For benzene hydroxylation, the phenol yield is 30.8% (selectivity >99%). Ring hydroxylation of mono-/di-alkylbenzenes and halogenated aromatic hydrocarbons cause the yields up to 26.2% and selectivities above 90%. The reaction is completed within 30 s, the fastest occasion so far, resulting in ultra-high turnover frequencies (TOFs). Systematic characterization including V-51 NMR and X-ray absorption fine structure (XAFS) analyses suggest that such high activity associates with the unique non-radical hydroxylation mechanism arising from the in situ created diperoxo V(IV) state.
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