Highly dispersive tetrahedral vanadium species on pure silica ZSM-12 zeolite boosting the selective oxidation of cyclohexane into cyclohexanone

Menglin Xie, Ting Li, Chao Wu, Xiaoling Liu, Jinling Ni, Siqin Yao, Yu Zhou, Shibo Xi, Jun Wang

科研成果: 期刊稿件文章同行评审

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摘要

The selective oxidation of cyclohexane is a promising green route for the production of KA oil (cyclohexanol and cyclohexanone), but remains a huge challenge to design high-performing heterogeneous catalysts under mild conditions. Herein, a pure silica ZSM-12 (MTW topology) zeolite was applied as the support to immobilize highly dispersive tetrahedrally coordinated vanadium (V) species and the constructed catalyst 1%V/SZ-12 exhibited high efficiency in the fast and selective oxidation of cyclohexane into cyclohexanone with H2O2. The reaction completed within 30 s, affording the selectivity of 99% towards cyclohexanone and the extremely high turnover frequency (TOF) of 5,891 h−1. 1%V/SZ-12 was facilely reused with stable activity and feasibly extended to the oxidation of various cyclohexane derivatives. The one-dimensional 12-membered ring microchannels contributed to the formation and accessibility of tetrahedrally coordinated high valent V5+ species as the robust active centers, which activated H2O2 to generate V–O–O·, the active oxygen species for the electrophilic attack on cyclohexane to produce cyclohexanone as the sole product. (Figure presented.)

源语言英语
页(从-至)2206-2214
页数9
期刊Science China Chemistry
67
7
DOI
出版状态已出版 - 7月 2024

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