催化学报

催化学报 ›› 2006, Vol. 27 ›› Issue (7): 624-630.

• 研究论文 • 上一篇    下一篇

器外预硫化型MoNiP/γ-Al2O3催化剂的二苯并噻吩加氢脱硫活性

李彦鹏,刘大鹏,刘晓,柴永明,刘晨光   

  1. 中国石油大学(华东)化学化工学院重质油国家重点实验室, CNPC催化重点实验室, 山东东营 257061
  • 收稿日期:2006-07-25 出版日期:2006-07-25 发布日期:2006-07-25

Hydrodesulfurization of Dibenzothiophene over ex Situ Presulfided MoNiP/γ-Al2O3 Catalyst

LI Yanpeng*, LIU Dapeng, LIU Xiao, CHAI Yongming, LIU Chenguang   

  1. State Key Laboratory of Heavy Oil Processing, CNPC, Key Laboratory of Catalysis, College of Chemistry and Chemical Engineering, China University of Petroleum, Dongying 257061, Shandong, China
  • Received:2006-07-25 Online:2006-07-25 Published:2006-07-25

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摘要： 制备了两种器外预硫化型MoNiP/γ-Al2O3催化剂,并以二苯并噻吩为模型化合物考察了其加氢脱硫(HDS)活性,选择了传统的器内预硫化催化剂作为参比. 采用X射线衍射(XRD)、 高分辨透射电镜(HRTEM)和X射线光电子能谱(XPS)等手段对二者在加氢活性相方面的差别进行了研究. 结果表明,器外预硫化催化剂的HDS活性(最高达到99%)与器内预硫化催化剂相当,但是其加氢能力相对较弱. XRD与HRTEM等研究表明,器外预硫化催化剂所形成的MoS2片晶的堆垛层数相对较低,而Mo与S元素的XPS分析结果则说明相对器内预硫化催化剂,器外预硫化催化剂中不但Mo的硫化度较低,而且MoS2活性相的含量亦较少,而二者活性相之间的这种差异应是导致两类催化剂加氢活性不同的主要原因.

关键词: 器外预硫化, 二苯并噻吩, 加氢脱硫, 钼, 镍, 磷, 氧化铝, 负载型催化剂

Abstract: Two ex situ presulfided MoNiP/γ-Al2O3 catalysts have been prepared, and their hydrodesulfurization performance has been evaluated using dibenzothiophene as the model compound. A conventional in situ presulfided MoNiP/γ-Al2O3 catalyst was selected as the competitor. The differences in the hydrogenation active phases of the two types of presulfided catalysts have been studied by X-ray diffraction (XRD), high-resolution transmission electron icroscopy (HRTEM), and X-ray photoelectron spectroscopy (XPS). The ex situ presulfided catalysts had a similar sulfur removal rate (99%) to the in situ presulfided one, but showed a lower hydrogenation activity. Morphology studies using XRD and HRTEM showed that the ex situ presulfided catalysts had a lower stacking number of MoS2 slabs. The XPS results showed that both the sulphidity of Mo and the content of MoS2 active phase of the ex situ presulfided catalyst were lower than those of the in situ presulfided one. The difference in active phase of the two types of presulfided catalysts led to their different hydrogenation activity.

Key words: ex situ presulfiding, dibenzothiophene, hydrodesulfurization, molybdenum, nickel, phosphorus, alumina, supported catalyst