期刊
ACS CATALYSIS
卷 4, 期 5, 页码 1617-1625出版社
AMER CHEMICAL SOC
DOI: 10.1021/cs500187q
关键词
cyclohexene; carbon nanotubes; nitrogen; allylic oxidation; aerobic oxidation
资金
- National Science Foundation of China [21133010, 21273079]
- Guangdong Provincial National Science Foundation of China [9251064101000020, S20120011275]
- Program for New Century Excellent Talents in University [NCET-12-0190]
- Fundamental Research Funds for the Central Universities of China [2014ZG0005]
Carbon nanotubes (CNTs) and nitrogen-doped CNTs (NCNTs) were systematically investigated as metal-free catalysts in the selective allylic oxidation of cyclohexene using molecular oxygen as oxidant in the liquid phase. High cyclohexene conversion (up to 59.0%) and 620.1 mmol g(-1) h(-1) mass-normalized activity were obtained for NCNTs, competing with the state-of-the-art metal catalysts. The positive effect of nitrogen dopant on the performance of CNTs was demonstrated, with respect to the aspects of enhancing activity and increasing selectivity of 2-cyclohexen-1-one, allowing for a ketone/alcohol ratio of 3.7 at 59% conversion. The unique catalytic role of NCNTs was attributed to their capability to promote the radical chain propagation via stabilizing peroxyl and cycloxyl radicals, which boosted the further conversion of 2-cyclohexen-1-ol toward 2-cyclohexen-1-one as well.
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