WP/γ-Al2O3催化剂的制备、表征及加氢脱硫和加氢脱氮活性

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WP/γ-Al₂O₃催化剂的制备、表征及加氢脱硫和加氢脱氮活性

李翠清^a,b; 孙桂大^b; 李成岳^a; 宋亚娟^b

^a The Key Laboratory of Science and Technology of Controllable Chemical Reactions, Ministry of Education, Beijing University of Chemical Technology, Beijing 100029, China
^b The Green Chemistry and Catalysis Materials Laboratory, Beijing Institute of Petrochemical Technology, Beijing 102617, China

收稿日期:1900-01-01 修回日期:1900-01-01 出版日期:2006-04-28 发布日期:2006-04-28
通讯作者: 李翠清

Preparation, Characterization, Hydrodesulfurization and Hydrode-nitrogenation Activities of Alumina-supported Tungsten Phosphide Catalysts

LI Cuiqing^a,b; SUN Guida^b; LI Chengyue^a; SONG Yajuan^b

^a The Key Laboratory of Science and Technology of Controllable Chemical Reactions, Ministry of Education, Beijing University of Chemical Technology, Beijing 100029, China
^b The Green Chemistry and Catalysis Materials Laboratory, Beijing Institute of Petrochemical Technology, Beijing 102617, China

Received:1900-01-01 Revised:1900-01-01 Online:2006-04-28 Published:2006-04-28
Contact: LI Cuiqing

摘要/Abstract

摘要： Two series of WP/Al2O3 catalyst precursors with WP mass loading in the range 18.5%—37.1% were prepared using the impregnation method and mixing method, respectively, and the catalysts were then obtained by temperature-programmed reduction of supported tungsten phosphate (precursor of WP/Al2O3 catatlysts) in H2 at 650℃ for 4h. The catalysts were characterized by XRD, BET, TG/DTA , XPS and 31P MAS-NMR. The activities of these catalysts were tested in the hydrodenitrogenation (HDN) of pyridine and hydrodesulfurization (HDS) of thiophene at 340℃ and 3.0MPa. The results showed that owing to the stronger interaction of the support with the active species, the precursor of WP/Al2O3 catalyst was more difficultly phosphided and a greater amount of W spe-cies was in a high valence state W6+ on the surface of the catalyst prepared by the impregnation method than that by the mixing method. 31P MAS-NMR results indicated that 31P shift from 85% H3PO4 of 2.55×10－4 for WP and 2.57×10－4 for WP/γ-Al2O3 catalysts prepared by mixing method. Such WP/Al2O3 catalysts showed higher HDN activi-ties and lower HDS activities than those prepared by the impregnation method under the same loading of WP. WP/γ-Al2O3 catalysts with weak interaction between support and active species were favorable for HDN reaction while the WP/γ-Al2O3 catalysts with strong interaction were favorable for HDS reaction.

关键词: hydrodesulfurization;hydrodenitrogenation;tungsten phosphide;pyridine;thiophene

Abstract: Two series of WP/Al2O3 catalyst precursors with WP mass loading in the range 18.5%—37.1% were prepared using the impregnation method and mixing method, respectively, and the catalysts were then obtained by temperature-programmed reduction of supported tungsten phosphate (precursor of WP/Al2O3 catatlysts) in H2 at 650℃ for 4h. The catalysts were characterized by XRD, BET, TG/DTA , XPS and 31P MAS-NMR. The activities of these catalysts were tested in the hydrodenitrogenation (HDN) of pyridine and hydrodesulfurization (HDS) of thiophene at 340℃ and 3.0MPa. The results showed that owing to the stronger interaction of the support with the active species, the precursor of WP/Al2O3 catalyst was more difficultly phosphided and a greater amount of W spe-cies was in a high valence state W6+ on the surface of the catalyst prepared by the impregnation method than that by the mixing method. 31P MAS-NMR results indicated that 31P shift from 85% H3PO4 of 2.55×10－4 for WP and 2.57×10－4 for WP/γ-Al2O3 catalysts prepared by mixing method. Such WP/Al2O3 catalysts showed higher HDN activi-ties and lower HDS activities than those prepared by the impregnation method under the same loading of WP. WP/γ-Al2O3 catalysts with weak interaction between support and active species were favorable for HDN reaction while the WP/γ-Al2O3 catalysts with strong interaction were favorable for HDS reaction.

Key words: hydrodesulfurization, hydrodenitrogenation, tungsten phosphide, pyridine, thiophene

李翠清, 孙桂大, 李成岳, 宋亚娟. WP/γ-Al₂O₃催化剂的制备、表征及加氢脱硫和加氢脱氮活性[J]. , DOI: .

LI Cuiqing, SUN Guida, LI Chengyue, SONG Yajuan. Preparation, Characterization, Hydrodesulfurization and Hydrode-nitrogenation Activities of Alumina-supported Tungsten Phosphide Catalysts[J]. , DOI: .

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WP/γ-Al₂O₃催化剂的制备、表征及加氢脱硫和加氢脱氮活性

Preparation, Characterization, Hydrodesulfurization and Hydrode-nitrogenation Activities of Alumina-supported Tungsten Phosphide Catalysts

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