Hydrodenitrogenation of quinoline catalyzed by MCM-41-supported nickel phosphides

Mohong Lu, Anjie Wang, Xiang Li, Xinping Duan, Yang Teng, Yao Wang, Chunshan Song, Yongkang Hu

Research output: Contribution to journalArticle

36 Citations (Scopus)

Abstract

A series of MCM-41-supported nickel phosphides with an initial Ni/P atomic ratio of 0.5-2 in the oxidic precursors were prepared by an in situ reduction method and characterized by X-ray diffraction (XRD), CO chemisorption, N2 adsorption, and transmission electron microscopy. Their catalytic performances were evaluated in the hydrodenitrogenation (HDN) of quinoline and compared with MCM-41-supported Ni-Mo sulfide. The supported nickel phosphides with initial Ni/P ratios of 1 or 1.25 exhibited much higher HDN activity than the supported Ni-Mo sulfide. XRD patterns of both high-performance phosphide catalysts revealed that the active phase was Ni2P. It is indicated that the HDN of quinoline on the MCM-41-supported nickel phosphides exclusively proceeds via a pathway, which involves fully saturated intermediates. The cleavage of the C-N bond in the decahydroquinoline is the rate-determining step in the HDN of quinoline on the supported nickel phosphides. In addition, the effects of H2S (CS2 as the precursor) on HDN and the performances of the prepared nickel phosphide catalysts in the simultaneous HDN of quinoline and hydrodesulfurization (HDS) of dibenzothiophene (DBT) were investigated. The presence of H2S dramatically reduced the hydrogenation of 1,2,3,4-tetrahydroquinoline to decahydroquinoline, altering unfavorably the reaction pathways involved in the HDN of quinoline. The simultaneous HDN and HDS indicated that the HDN activity of Ni-Mo sulfide was hardly affected in the presence of DBT. Whereas, the supported nickel phosphide was sensitive to the presence of DBT at low temperatures. It is favorable to perform HDN at high temperatures because the inhibiting effects of H2S and DBT on HDN were dramatically reduced at elevated temperatures.

Original languageEnglish (US)
Pages (from-to)554-560
Number of pages7
JournalEnergy and Fuels
Volume21
Issue number2
DOIs
StatePublished - Mar 1 2007

Fingerprint

Multicarrier modulation
Nickel
Sulfides
Hydrodesulfurization
X ray diffraction
Catalysts
Carbon Monoxide
Chemisorption
Temperature
Diffraction patterns
Hydrogenation
MCM-41
quinoline
Transmission electron microscopy
Adsorption
dibenzothiophene

All Science Journal Classification (ASJC) codes

  • Chemical Engineering(all)
  • Fuel Technology
  • Energy Engineering and Power Technology

Cite this

Lu, M., Wang, A., Li, X., Duan, X., Teng, Y., Wang, Y., ... Hu, Y. (2007). Hydrodenitrogenation of quinoline catalyzed by MCM-41-supported nickel phosphides. Energy and Fuels, 21(2), 554-560. https://doi.org/10.1021/ef060467g
Lu, Mohong ; Wang, Anjie ; Li, Xiang ; Duan, Xinping ; Teng, Yang ; Wang, Yao ; Song, Chunshan ; Hu, Yongkang. / Hydrodenitrogenation of quinoline catalyzed by MCM-41-supported nickel phosphides. In: Energy and Fuels. 2007 ; Vol. 21, No. 2. pp. 554-560.
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abstract = "A series of MCM-41-supported nickel phosphides with an initial Ni/P atomic ratio of 0.5-2 in the oxidic precursors were prepared by an in situ reduction method and characterized by X-ray diffraction (XRD), CO chemisorption, N2 adsorption, and transmission electron microscopy. Their catalytic performances were evaluated in the hydrodenitrogenation (HDN) of quinoline and compared with MCM-41-supported Ni-Mo sulfide. The supported nickel phosphides with initial Ni/P ratios of 1 or 1.25 exhibited much higher HDN activity than the supported Ni-Mo sulfide. XRD patterns of both high-performance phosphide catalysts revealed that the active phase was Ni2P. It is indicated that the HDN of quinoline on the MCM-41-supported nickel phosphides exclusively proceeds via a pathway, which involves fully saturated intermediates. The cleavage of the C-N bond in the decahydroquinoline is the rate-determining step in the HDN of quinoline on the supported nickel phosphides. In addition, the effects of H2S (CS2 as the precursor) on HDN and the performances of the prepared nickel phosphide catalysts in the simultaneous HDN of quinoline and hydrodesulfurization (HDS) of dibenzothiophene (DBT) were investigated. The presence of H2S dramatically reduced the hydrogenation of 1,2,3,4-tetrahydroquinoline to decahydroquinoline, altering unfavorably the reaction pathways involved in the HDN of quinoline. The simultaneous HDN and HDS indicated that the HDN activity of Ni-Mo sulfide was hardly affected in the presence of DBT. Whereas, the supported nickel phosphide was sensitive to the presence of DBT at low temperatures. It is favorable to perform HDN at high temperatures because the inhibiting effects of H2S and DBT on HDN were dramatically reduced at elevated temperatures.",
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Lu, M, Wang, A, Li, X, Duan, X, Teng, Y, Wang, Y, Song, C & Hu, Y 2007, 'Hydrodenitrogenation of quinoline catalyzed by MCM-41-supported nickel phosphides', Energy and Fuels, vol. 21, no. 2, pp. 554-560. https://doi.org/10.1021/ef060467g

Hydrodenitrogenation of quinoline catalyzed by MCM-41-supported nickel phosphides. / Lu, Mohong; Wang, Anjie; Li, Xiang; Duan, Xinping; Teng, Yang; Wang, Yao; Song, Chunshan; Hu, Yongkang.

In: Energy and Fuels, Vol. 21, No. 2, 01.03.2007, p. 554-560.

Research output: Contribution to journalArticle

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T1 - Hydrodenitrogenation of quinoline catalyzed by MCM-41-supported nickel phosphides

AU - Lu, Mohong

AU - Wang, Anjie

AU - Li, Xiang

AU - Duan, Xinping

AU - Teng, Yang

AU - Wang, Yao

AU - Song, Chunshan

AU - Hu, Yongkang

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