P改性对Mo-Ni/Al<sub>2</sub>O<sub>3</sub>煤焦油加氢脱氮性能的影响

石垒; 张增辉; 邱泽刚; 郭芳; 张伟; 赵亮富

P改性对Mo-Ni/Al₂O₃煤焦油加氢脱氮性能的影响

石垒^1,2,
张增辉^1,2,
邱泽刚^1,,
郭芳^1,2,
张伟¹,
赵亮富¹

1.
中国科学院山西煤炭化学研究所应用催化与绿色化工实验室, 山西太原 030001;
2.
中国科学院大学, 北京 100049

基金项目: 中国科学院战略性先导科技专项课题(XDA07020200).

详细信息

通讯作者:
邱泽刚,Tel:0351-2021169,E-mail:qiuzegang@sxicc.ac.cn.

中图分类号: TQ519
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- 被引次数: 0
出版历程
- 收稿日期: 2014-07-14
- 修回日期: 2014-09-22
- 刊出日期: 2015-01-30

Effect of phosphorus modification on the catalytic properties of Mo-Ni/Al₂O₃ in the hydrodenitrogenation of coal tar

1.
Laboratory of Applied Catalysis and Green Chemical Engineering, Institute of Coal Chemistry, Chinese Academy of Sciences, Taiyuan 030001, China;
2.
University of Chinese Academy of Sciences, Beijing 100049, China

摘要

摘要: 在磷含量1.34%下,采用分步浸渍法按磷添加顺序不同制备了3种改性催化剂:MoP-Ni/Al₂O₃、Mo-NiP/Al₂O₃、Mo-Ni/PAl₂O₃.通过X射线衍射(XRD)、程序升温脱附(NH₃-TPD)、程序升温还原(H₂-TPR)、氮气吸附等技术对催化剂进行了表征.以新疆中低温煤焦油为原料,考察了不同磷改性方式对催化剂加氢脱氮(HDN)性能的影响.结果表明,适宜的磷添加方式能够改变催化剂的酸性分布,提高10~13 nm加氢脱氮有效孔的比例,并且减弱活性组分与载体的相互作用,同时使得活性组分更易被还原,进而提高催化剂加氢脱氮性能.加氢脱氮活性顺序为Mo-Ni/PAl₂O₃(74.36%)>Mo-NiP/Al₂O₃(72.74%)>Mo-Ni/Al₂O₃(71.72%)>MoP-Ni/Al₂O₃(56.13%).
- 磷 /
- 煤焦油 /
- 加氢脱氮 /
- 催化剂
Abstract: Mo-Ni/Al₂O₃ catalysts were modified with phosphorus by using the impregnation method. By changing the addition sequence of phosphorus, three types of catalysts, viz. MoP-Ni/Al₂O₃, Mo-NiP/Al₂O₃ and Mo-Ni/PAl₂O₃, were obtained with a P loading of 1.34%. These catalysts were characterized by X-ray diffraction, temperature-programmed desorption of NH₃, temperature-programmed reduction by H₂ and N₂ sorption experiment. The catalytic properties of these catalysts were investigated with the hydrodenitrogenation (HDN) of low- and middle-temperature coal tar obtained from Xinjiang province. It was shown that appropriate P addition sequence can alter acid site distributions, increase the proportion of effective pores between 10 and 13 nm, weaken the interaction of the support and active metal components and make the reduction of the active components easier, consequently, improving the catalytic performance. The HDN activity of the three types of catalysts decreased in the order of Mo-Ni/PAl₂O₃(74.36%) > Mo-NiP/Al₂O₃(72.74%) > Mo-Ni/Al₂O₃(56.13%) > MoP-Ni/Al₂O₃(71.72%).
- phosphous /
- coal tar /
- hydrodenitrogenation /
- catalyst

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