Catalytic hydrodenitrogenation of propionitrile over supported nickel phosphide catalysts as a model reaction for the transformation of pyrolysis oil obtained from animal by-products

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• 作者：Cecília A. Badari ; Ferenc Lónyi ; Sándor Dóbé…
• 关键词：Hydrodenitrogenation ; Ni2P/SiO2 ; Ni2P/Laponite ; Propionitrile ; Operando DRIFTS
• 刊名：Reaction Kinetics, Mechanisms and Catalysis
• 出版年：2015
• 出版时间：June 2015
• 年：2015
• 卷：115
• 期：1
• 页码：217-230
• 全文大小：974 KB
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• 作者单位：Cecília A. Badari (1)
  Ferenc Lónyi (1)
  Sándor Dóbé (1)
  Jen? Hancsók (2)
  József Valyon (1)
  
  1. Institute of Materials and Environmental Chemistry, Research Centre for Natural Sciences, Hungarian Academy of Sciences, Magyar tudósok k?rútja 2, Budapest, 1117, Hungary
  2. Department of Hydrocarbon and Coal Processing, University of Pannonia, Egyetem u. 10, Veszprém, 8200, Hungary
  
• 刊物类别：Chemistry and Materials Science
• 刊物主题：Chemistry
  Catalysis
  Industrial Chemistry and Chemical Engineering
  Physical Chemistry
  
• 出版者：Akad茅miai Kiad贸, co-published with Springer Science+Business Media B.V., Formerly Kluwer Academic
• ISSN：1878-5204

文摘

The catalytic hydroconversion of propionitrile (PN) was studied over supported nickel and nickel phosphide catalysts. PN was used as a model compound of aliphatic nitriles in pyrolysis oil obtained from animal by-products. Silica gel and Laponite were used as supports. The structure and particle size of the supported active phase was characterized by X-ray diffractometry and transmission electron microscopy. Catalytic experiments were carried out using a flow-through tube reactor at temperatures between 200 and 400?°C, total pressure of 30?bar, and H₂/PN molar ratio of 10. High-pressure operando diffuse reflectance infrared Fourier transform spectroscopy experiments were carried out to study the species on the catalyst surface during reaction. The results substantiated that propane-1-imine (PI) is a surface intermediate of propylamine, dipropylamine and tripropylamine formation. The conversion of PN to hydrocarbon and ammonia hardly proceeded below 300?°C but became dominating reaction between 350 and 400?°C. Br?nsted acid sites were not required for the reactions. Supported Ni₂P catalysts catalyzed hydrogenolysis of C–N bonds only, whereas also the C–C bonds suffered significant cleavage over supported Ni catalyst.