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化学学报
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化学学报 ›› 2011, Vol. 69 ›› Issue (14): 1622-1626. 上一篇    下一篇

研究论文

助剂对WNx/TiO2-γ-Al2O3催化剂物化性质及加氢脱硫性能影响

刘维桥*,1，周虎1，雷卫宁1，尚通明1，张强2，孙桂大*,2   

  1. (1江苏省贵金属深加工技术及其应用重点实验室 江苏技术师范学院化学与环境工程学院 常州 213001)
    (2北京石油化工学院 北京 102617)
  • 投稿日期:2010-12-08 修回日期:2011-03-08 发布日期:2011-03-24
  • 通讯作者: 刘维桥 E-mail:lwq@jstu.edu.cn
  • 基金资助:

    国家重点基础研究发展规划;国家自然科学基金;江苏省重点建设实验室开放研究课题基金

Physicochemical Properties and Hydrodesulphurization (HDS) Performances of WNx/TiO2-γ-Al2O3 Catalysts with Additives

Liu Weiqiao*,1 Zhou Hu1 Lei Weining1 Shang Tongming1 Zhang Qiang2 Sun Guida*,2   

  1. (1J iangsu Province Key Laboratory of Precious Metal Chemistry and Technology, School of Chemistry & Environmental Engineering, Jiangsu Teachers University of Technology, Changzhou 213001)
    (2 Beijing Institute of Petrochemical Technology, Beijing 102617)
  • Received:2010-12-08 Revised:2011-03-08 Published:2011-03-24
  • Contact: LIU WeiQiao E-mail:lwq@jstu.edu.cn
  • Supported by:

    ;the National Natural Science Foundation of China

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在H2和N2混合气中, 采用程序升温还原氮化反应的方法, 合成了分别含有助剂Ni, Co, P或V的WNx/TiO2- γ-Al2O3催化剂. 通过低温氮物理吸附、氨程序升温脱附、TG-DTA和X光电子能谱技术对所合成的催化剂进行了表征. 实验结果表明, 4种助剂的引入分别使WNx/TiO2-γ-Al2O3催化剂前驱体更易于还原氮化以及比表面积和酸量减小. 其中NiWNx/TiO2-γ-Al2O3催化剂的比表面积和酸量减小幅度相对较小, 其前驱体最易被还原氮化, 而且助剂Ni更有利于活性钨物种的稳定存在. 同时, 利用噻吩加氢脱硫(HDS)评价了催化剂的性能. 结果表明, 4种助剂对WNx/TiO2-γ-Al2O3催化剂的噻吩HDS活性均有促进作用, 其中Ni助剂的作用最为显著.

关键词: 氮化, 钨, 助剂, 加氢脱硫, TiO2-γ-Al2O3

Ni(Co,P,V)WNx/TiO2-γ-Al2O3 catalysts were synthesized by nitriding with N2-H2 mixture in the process of temperature programmed reduction. Nitrogen adsorption, temperature-programmed desorption of ammonia (NH3-TPD), TG-DTA and XPS techniques were employed to analyze the natures of the catalysts. The results show that the reduction-nitriding of the precursors of Ni(Co,P,V)WNx/TiO2-γ-Al2O3 catalysts can be carried out more easily than that of WNx/TiO2-γ-Al2O3 catalyst, and the BET surface areas and acid amounts of Ni(Co,P,V)WNx/TiO2-γ-Al2O3 catalysts are smaller than those of WNx/TiO2-γ-Al2O3 catalyst. Among the Ni(Co,P,V)WNx/TiO2-γ-Al2O3 catalysts, the BET surface area and acid amount of the NiWNx/TiO2-γ-Al2O3 catalyst are relatively larger, and the precursor of the NiWNx/TiO2-γ-Al2O3 catalyst is most easily reduced and nitrided. In addition, the addition of additive Ni is more conducive to the stability of active W species on the WNx/TiO2-γ-Al2O3 catalyst. At last, the activities of thiophene hydrodesulphurization (HDS) over the catalysts were evaluated. The results show that the addition of additives can promote the activities of thiophene HDS over the WNx/TiO2-γ-Al2O3 catalyst, and the NiWNx/TiO2-γ-Al2O3 catalyst has a higher activity of thiophene HDS.

Key words: nitrogenation, tungsten, additives, hydrodesulphurization, TiO2-γ-Al2O3

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