Selective Oxidation of Cyclohexane to Cyclohexanone Using Chromium Oxide Supported Mesoporous MCM-41 Nanospheres: Probing the Nature of Catalytically Active Chromium Sites

被引:16
作者
Betsy, Kurisingal J. [1 ]
Nayak, Chandrani [2 ]
Lazar, Anish [1 ,3 ]
Krishnan, Athira [1 ]
Bhattacharyya, Dibyendu [2 ]
Jha, Shambhu N. [2 ]
Vinod, Chathakudath P. [1 ,3 ,4 ]
机构
[1] CSIR Natl Chem Lab, Catalysis & Inorgan Chem Div, Dr Homi Bhabha Rd, Pune 411008, Maharashtra, India
[2] Bhabha Atom Res Ctr, Atom & Mol Phys Div, Bombay 400085, Maharashtra, India
[3] Acad Sci & Innovat Res AcSIR, Anusandhan Bhawan, 2 Rafi Marg, New Delhi 110001, India
[4] CSIR Natl Chem Lab, Ctr Excellence Surface Sci, Dr Homi Bhabha Rd, Pune 411008, Maharashtra, India
关键词
chromium; heterogeneous catalysis; nanostructures; oxidation; supported catalysts; SOLVENT-FREE SYSTEM; MOLECULAR-SIEVES; SURFACE-CHEMISTRY; HYDROGEN-PEROXIDE; CARBON MATERIALS; CATALYSTS; DEHYDROGENATION; PROPANE; SILICA; CR-MCM-41;
D O I
10.1002/cctc.201800309
中图分类号
O64 [物理化学(理论化学)、化学物理学];
学科分类号
070304 ; 081704 ;
摘要
Highly dispersed chromium oxide supported mesoporous MCM-41 nanosphere catalysts have been synthesized using a simple wet impregnation method. This work is devoted to a systematic study to reveal the active Cr sites in chromium oxide supported MCM-41 nanosphere catalysts for the selective oxidation of cyclohexane to cyclohexanone. To probe the nature of the active species, we synthesized 0.5-10wt% Cr loaded catalysts and characterized them by using XRD, UV/Vis spectroscopy, Raman spectroscopy, X-ray photoelectron spectroscopy, extended X-ray absorption fine structure analysis, X-ray absorption near edge structure analysis, N-2 sorption analysis, FTIR spectroscopy, (SiNMR)-Si-29 spectroscopy, SEM, and TEM. The liquid-phase oxidation of cyclohexane to cyclohexanone (99% selectivity) was performed under mild reaction conditions, and the results reveal clearly that the 5wt% Cr loaded catalyst was optimum for the reaction. The initial composition of isolated Cr3+ species in the catalyst is the major factor that influences the enhanced activity for cyclohexane oxidation.
引用
收藏
页码:3291 / 3298
页数:8
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