Silicalite-1 deactivation in vapour phase Beckmann rearrangement of cyclohexanone oxime to caprolactam

Cesana, Alberto; Palmery, Stefano; Buzzoni, R.; Spanò, Guido; Rivetti, Franco; Carnelli, Lino

doi:10.1016/j.cattod.2010.03.038

Cited by 21 publications

(14 citation statements)

References 22 publications

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“…Wojciechowski reported the time on stream theory of catalyst decay. The Wojciechowski model relates the activity decrease with time on stream, and the advantages of the model based on coke deposition theory are usually well established . Since the reason for the deactivation of TS‐1 catalyst in the epoxidation of propylene has been shown by the above characterization results to be the deposition of high molecular weight organic matter on the catalyst, this model is valuable in guiding the kinetics study of the catalyst deactivation.…”

Section: Resultsmentioning

confidence: 99%

Liquid phase propylene epoxidation with H₂O₂on TS-1/SiO₂catalyst in a fixed-bed reactor: experiments and deactivation kinetics

Feng

Wang

et al. 2014

J. Chem. Technol. Biotechnol.

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BACKGROUND The epoxidation of propylene with H2O2 in liquid phase catalyzed by a TS‐1/SiO2 catalyst in a fixed‐bed reactor has been studied. The effects of reaction temperature (313–328 K), methanol concentrations (55–70 wt%) and hydrogen peroxide concentrations (9–15 wt%) on the reaction are investigated. The fresh, deactivated and regenerated catalysts were characterized with XRD, FT‐IR, UV–vis, N2 sorption and TG to study the reasons for catalyst deactivation. In addition, the kinetics of catalyst deactivation was studied by fitting the experimental data. RESULTS The rate of decrease of H2O2 conversion decreases with increasing reaction temperature and methanol concentration, but increases with increasing hydrogen peroxide concentration. The reason for catalyst deactivation is that the bulky organic matter covers the active centers. The study on deactivation kinetics shows that the deactivation reaction order is 2, and an expression for H2O2 conversion as a function of reaction time is obtained. CONCLUSION The operating conditions such as reaction temperature, methanol concentration and hydrogen peroxide concentration remarkably affect the reaction. The kinetic parameters including deactivation reaction order and activation energy are developed by fitting the experimental data based on the Wojciechowski model. © 2014 Society of Chemical Industry

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Section: Resultsmentioning

confidence: 99%

Liquid phase propylene epoxidation with H₂O₂on TS-1/SiO₂catalyst in a fixed-bed reactor: experiments and deactivation kinetics

Feng

Wang

et al. 2014

J. Chem. Technol. Biotechnol.

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“…), are known to provide a spatial fit that confers high selectivity in the vapour-phase Beckmann rearrangement [ 22 , 23 , 29 ]. Due to their potential for industrial implementation, there is significant interest in probing in detail the reaction kinetics and catalyst deactivation processes that operate in these zeolitic systems [ 30 , 31 ].…”

Section: Introductionmentioning

confidence: 99%

The Molecular Design of Active Sites in Nanoporous Materials for Sustainable Catalysis

2017

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At the forefront of global development, the chemical industry is being confronted by a growing demand for products and services, but also the need to provide these in a manner that is sustainable in the long-term. In facing this challenge, the industry is being revolutionised by advances in catalysis that allow chemical transformations to be performed in a more efficient and economical manner. To this end, molecular design, facilitated by detailed theoretical and empirical studies, has played a pivotal role in creating highly-active and selective heterogeneous catalysts. In this review, the industrially-relevant Beckmann rearrangement is presented as an exemplar of how judicious characterisation and ab initio experiments can be used to understand and optimise nanoporous materials for sustainable catalysis.

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“…The shortcomings of this process motivated research toward the development of new processes for the synthesis of -caprolactam [24,25]. Consequently, vapor phase and liquid phase Beckmann rearrangement of cyclohexanone oxime over solid acid catalysts and zeolites have been studied as potential alternatives [26][27][28][29][30][31][32][33][34][35][36]. It was suggested that the strong Brønsted acidity of the zeolite catalyst enhances the formation of -caprolactam [30].…”

Section: Introductionmentioning

confidence: 99%

Amorphous SiO2–Al2O3 supported Co3O4 and its catalytic properties in cyclohexane nitrosation to ɛ-caprolactam: Influences of preparation conditions

Hao

Zhong

Liu

et al. 2012

Journal of Molecular Catalysis A: Chemical

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Silicalite-1 deactivation in vapour phase Beckmann rearrangement of cyclohexanone oxime to caprolactam

Cited by 21 publications

References 22 publications

Liquid phase propylene epoxidation with H₂O₂on TS-1/SiO₂catalyst in a fixed-bed reactor: experiments and deactivation kinetics

Liquid phase propylene epoxidation with H₂O₂on TS-1/SiO₂catalyst in a fixed-bed reactor: experiments and deactivation kinetics

The Molecular Design of Active Sites in Nanoporous Materials for Sustainable Catalysis

Amorphous SiO2–Al2O3 supported Co3O4 and its catalytic properties in cyclohexane nitrosation to ɛ-caprolactam: Influences of preparation conditions

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Silicalite-1 deactivation in vapour phase Beckmann rearrangement of cyclohexanone oxime to caprolactam

Cited by 21 publications

References 22 publications

Liquid phase propylene epoxidation with H2O2on TS-1/SiO2catalyst in a fixed-bed reactor: experiments and deactivation kinetics

Liquid phase propylene epoxidation with H2O2on TS-1/SiO2catalyst in a fixed-bed reactor: experiments and deactivation kinetics

The Molecular Design of Active Sites in Nanoporous Materials for Sustainable Catalysis

Amorphous SiO2–Al2O3 supported Co3O4 and its catalytic properties in cyclohexane nitrosation to ɛ-caprolactam: Influences of preparation conditions

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Liquid phase propylene epoxidation with H₂O₂on TS-1/SiO₂catalyst in a fixed-bed reactor: experiments and deactivation kinetics

Liquid phase propylene epoxidation with H₂O₂on TS-1/SiO₂catalyst in a fixed-bed reactor: experiments and deactivation kinetics