期刊
DALTON TRANSACTIONS
卷 49, 期 39, 页码 13829-13839出版社
ROYAL SOC CHEMISTRY
DOI: 10.1039/d0dt02413a
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资金
- CSIR, New Delhi, India [01(2942)/18/EMR-II]
- MHRD, India
- Science and Engineering Research Board (SERB), New Delhi
- Board of Research in Nuclear Science (BRNS), Mumbai
- Council of Scientific and Industrial Research (CSIR), New Delhi [09/114(0224)/19-EMRI]
- UGC
- CSIR
Copper(i) complexes [Cu(tL(1-7))(2)](ClO4) (1-7) of bidentate ligands (L-1-L-7) have been synthesized via spontaneous reduction and characterized as catalysts for aromatic C-H activation using H2O2 as the oxidant. The single crystal X-ray structure of 1 exhibited a distorted tetrahedral geometry. All the copper(i) complexes catalyzed direct hydroxylation of benzene to form phenol with good selectivity up to 98%. The determined kinetic isotope effect (KIE) values, 1.69-1.71, support the involvement of a radical type mechanism. The isotope-labeling experiments using (H2O2)-O-18 showed 92% incorporation of O-18 into phenol and confirm that H2O2 is the key oxygen supplier. Overall, the catalytic efficiencies of the complexes are strongly influenced by the electronic and steric factor of the ligand, which is fine-tuned by the ligand architecture. The benzene hydroxylation reaction possibly proceeded via a radical mechanism, which was confirmed by the addition of radical scavengers (TEMPO) to the catalytic reaction that showed a reduction in phenol formation.
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