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

被引:5
作者
Badari, Cecilia A. [1 ]
Lonyi, Ferenc [1 ]
Dobe, Sandor [1 ]
Hancsok, Jeno [2 ]
Valyon, Jozsef [1 ]
机构
[1] Hungarian Acad Sci, Res Ctr Nat Sci, Inst Mat & Environm Chem, H-1117 Budapest, Hungary
[2] Univ Pannonia, Dept Hydrocarbon & Coal Proc, H-8200 Veszprem, Hungary
关键词
Hydrodenitrogenation; Ni2P/SiO2; Ni2P/Laponite; Propionitrile; Operando DRIFTS; TRANSITION-METAL PHOSPHIDES; BONE MEAL; THIOPHENE HYDRODESULFURIZATION; PHOSPHORIC-ACID; OXIDE CARRIERS; IN-SITU; HYDROGENATION; ACETONITRILE; SILICA; PRECURSORS;
D O I
10.1007/s11144-015-0842-3
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
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 A degrees C, total pressure of 30 bar, and H-2/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 A degrees C but became dominating reaction between 350 and 400 A degrees C. Bronsted 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.
引用
收藏
页码:217 / 230
页数:14
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