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Volumn 36, Issue 15, 1997, Pages 1639-1642

Designing a Solid Catalyst for the Selective Low-Temperature Oxidation of Cyclohexane to Cyclohexanone

Author keywords

Cobalt; EXAFS spectroscopy; Heterogeneous catalysis; Mesoporosity; Oxidations

Indexed keywords


EID: 0030867380     PISSN: 05700833     EISSN: None     Source Type: Journal    
DOI: 10.1002/anie.199716391     Document Type: Article
Times cited : (92)

References (30)
  • 2
    • 0642275524 scopus 로고
    • a) N. M. Emanuel, Z. K. Maizus, I. P. Skibida, Angew. Chem. 1969, 81, 91; Angew. Chem. Int. Ed. Engl 1969,8,97;
    • (1969) Angew. Chem. Int. Ed. Engl , vol.8 , pp. 97
  • 8
    • 0002990947 scopus 로고
    • Catalytic Selective Oxidation (Eds.: S. T. Oyama, J. W. Hightower)
    • c) W. Partenheimer, R. K. Gipe in Catalytic Selective Oxidation (Eds.: S. T. Oyama, J. W. Hightower), ACS Symp. Ser. 523, 1993, 81.
    • (1993) ACS Symp. Ser. 523 , pp. 81
    • Partenheimer, W.1    Gipe, R.K.2
  • 11
    • 0642367349 scopus 로고    scopus 로고
    • note
    • Mesoporous materials readily permit the combination of organometallic surface chemistry with the principle of shape-selectivity generally associated with microporous zeolites and the results from this initial study of cyclohexane might possibly be extended to applications where shape-selectivity is important.
  • 21
    • 0642367343 scopus 로고    scopus 로고
    • note
    • a) This approach (results were calibrated by using mesitylene as internal standard) was deemed necessary for the in-situ X-ray absorption spectroscopy (XAS) experiments as the TOF using the flow system were anticipated to be low and appropriate chlorinated solvents interfere with the XAS measurements. b) Reaction conditions: TBHP (10 mL), cyclohexane (9.5 mL), mesitylene (0.5 mL; internal standard), catalyst (150mg) stirred in a batch reactor at 70°C under argon. Up to 20 aliquots of 0.1 mL were withdrawn for analysis during a catalysis run. The MCM-41 was initially exposed to a small amount of the reactive dichlorodimethylsilane with the aim of functionalizing the majority of the silanol groups on the external surface, assuming a faster rate of reaction for the external compared to the internal surface. Hence, to ensure that the catalyst was present predominantly on the inside of the MCM-41 channels, the MCM-41 was treated with the various alkyl tethers only after this pretreatment. This procedure has been shown by scanning transmission electron microscopy to yield the desired effect in related systems (unpublished results).
  • 22
    • 0642275522 scopus 로고    scopus 로고
    • The kinetic profile showed no detectable induction period at a resolution of 5 minute time steps and behaved in a typical exponential fashion
    • The kinetic profile showed no detectable induction period at a resolution of 5 minute time steps and behaved in a typical exponential fashion.
  • 23
    • 0642367341 scopus 로고    scopus 로고
    • note
    • From the microanalysis the ratio of bromide tether to tethered cobalt is 100:1, NMR experiments aimed at trying to identify the glycine-derived tether were not sensitive enough to conclusively pick up the glycine-part, as can be expected at such low loadings.
  • 24
    • 0642306050 scopus 로고    scopus 로고
    • note
    • The increase in the selectivity of the catalyst system with time can be explained by the observation that the by-products dicyclohexyl peroxide and cyclohexyl tert-butyl peroxide might both decompose to cyclohexanone and that the by-products might react further, disappearing in the base-line. Due to the solvent-free conditions no full mass balance was attempted.


* 이 정보는 Elsevier사의 SCOPUS DB에서 KISTI가 분석하여 추출한 것입니다.