载体对钒铬氧化物催化剂结构及催化3-甲基吡啶氨氧化反应活性的影响

doi:10.1016/S1872-2067(12)60650-0

催化学报 ›› 2013, Vol. 34 ›› Issue (10): 1833-1838.DOI: 10.1016/S1872-2067(12)60650-0

载体对钒铬氧化物催化剂结构及催化3-甲基吡啶氨氧化反应活性的影响

姜枫^a, 邓生财^b, 牛磊^a, 肖国民^a

a 东南大学化学化工学院, 江苏南京211189;
b 南京大学化学化工学院, 介观化学教育部重点实验室, 江苏省纳米技术重点实验室, 江苏南京210093

收稿日期:2013-06-07 修回日期:2013-07-02 出版日期:2013-09-29 发布日期:2013-09-29
基金资助:
国家自然科学基金(21276050);国家科技支撑计划(2012BAD32B03).

Effect of supports on the structure and activity of vanadium-chromium oxide catalysts for ammoxidation of 3-picoline

Feng Jiang^a, Shengcai Deng^b, Lei Niu^a, Guomin Xiao^a

a School of Chemistry and Chemical Engineering, Southeast University, Nanjing 211189, Jiangsu, China;
b Key Laboratory of Mesoscopic Chemistry of MOE, Jiangsu Provincial Key Laboratory of Nanotechnology, School of Chemistry and Chemical Engineering, Nanjing University, Nanjing 210093, Jiangsu, China

Received:2013-06-07 Revised:2013-07-02 Online:2013-09-29 Published:2013-09-29
Contact: Guomin Xiao
Supported by:
This work was supported by the National Natural Science Foundation of China (21276050) and the National Key Technology R&D Program (2012BAD32B03).

摘要/Abstract

摘要：

通过等体积浸渍法制备了Nb₂O₅,MgF₂,TiO₂和SiO₂负载和未负载的钒铬氧化物催化剂,并应用X射线衍射、N₂吸附-脱附、H₂程序升温还原和NH₃程序升温脱附对催化剂进行了表征. 结果表明,催化剂比表面积较大时有利于CrVO₄-I(单斜)的生成,比表面积较小则有利于CrVO₄-III(斜方)的生成. 在310-400℃下3-甲基吡啶氨氧化制备3-氰基吡啶反应中,具有较高催化活性的催化剂与V物种还原性较高和表面活性位数量较多有关; 而高的3-氰基吡啶选择性则与催化剂表面较低的酸性密切相关. 升高反应温度可大幅度提高催化剂的活性,且其选择性基本不变.

关键词: 氨氧化, 3-甲基吡啶, 3-氰基吡啶, 载体, 钒铬氧化物

Abstract:

Bulk and Nb₂O₅-, MgF₂-, TiO₂-, and SiO₂-supported vanadium-chromium oxide catalysts were prepared by the incipient wetness impregnation method and investigated for the ammoxidation of 3-picoline to nicotinonitrile at 310-400 ℃. The physical and chemical properties of the catalysts were assessed by X-ray diffraction, N₂ adsorption-desorption, H₂-temperature-programmed reduction, and NH₃-temperature-programmed desorption. The surface area of the supports influenced the formation of the active components of the catalysts: high surface area encouraged the formation of monoclinic CrVO₄ whereas low surface area favored the formation of orthorhombic CrVO₄. The high reducibility of vanadium in the catalyst and the large number of surface active sites resulted in higher 3-picoline conversion efficiencies. The high selectivity was attributed to the low surface acidity of the catalysts. Reaction temperature showed a positive effect on the catalytic performance for it could increase 3-picoline conversion and maintain nicotinonitrile selectivity.

Key words: Ammoxidation, 3-Picoline, Nicotinonitrile, Support, Vanadium-chromium oxide

姜枫, 邓生财, 牛磊, 肖国民. 载体对钒铬氧化物催化剂结构及催化3-甲基吡啶氨氧化反应活性的影响[J]. 催化学报, 2013, 34(10): 1833-1838.

Feng Jiang, Shengcai Deng, Lei Niu, Guomin Xiao. Effect of supports on the structure and activity of vanadium-chromium oxide catalysts for ammoxidation of 3-picoline[J]. Chinese Journal of Catalysis, 2013, 34(10): 1833-1838.

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载体对钒铬氧化物催化剂结构及催化3-甲基吡啶氨氧化反应活性的影响

Effect of supports on the structure and activity of vanadium-chromium oxide catalysts for ammoxidation of 3-picoline

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