催化学报 ›› 2009, Vol. 30 ›› Issue (2): 111-118.

• 研究论文 • 上一篇    下一篇

氮气热处理对硫代硫酸铵预硫化的Mo/Al2O3催化剂的影响

葛晖1,2,李学宽1,樊卫斌1,秦张峰1,吕占军1,王建国1   

  1. 1 中国科学院山西煤炭化学研究所煤转化国家重点实验室, 山西太原 030001; 2 太原理工大学化学与化工学院, 山西太原 030024
  • 收稿日期:2009-02-25 出版日期:2009-02-25 发布日期:2012-11-21

Effect of Thermal Treatment under Nitrogen on the Ammonium Thiosulfate-Presulfidized Mo/Al2O3 Catalyst

GE Hui1,2, LI Xuekuan1*, FAN Weibin1, QIN Zhangfeng1, L Zhanjun1, WANG Jianguo1   

  1. 1 State Key Laboratory of Coal Conversion, Institute of Coal Chemistry, The Chinese Academy of Sciences, Taiyuan 030001, Shanxi, China; 2 College of Chemistry and Chemical Engineering, Taiyuan University of Technology, Taiyuan 030024, Shanxi, China
  • Received:2009-02-25 Online:2009-02-25 Published:2012-11-21

摘要: 考察了氮气预处理温度对硫代硫酸铵预硫化的Mo/Al2O3催化剂噻吩加氢脱硫(HDS)活性的影响. 采用X射线衍射、高分辨电镜、光电子能谱、热重质谱和硫分析等方法对催化剂进行了表征. 结果表明,预硫化催化剂经80 ℃低温处理并于200 ℃氢气原位活化后噻吩转化率达到最高. 对于氮气低温预处理或常温干燥的预硫化催化剂,载体氧化铝被硫酸根修饰,减少了Mo与载体的相互作用,使得催化剂活化后硫化程度高, MoS2活性相呈多层的Ⅱ型结构,因而HDS活性高. 高于200 ℃的氮气热处理造成硫代硫酸铵的分解,并有少量的多层MoS2活性相生成,但高温热处理造成硫的流失使得活性金属活化后硫化程度偏低,而且MoS2活性相呈现单层的Ⅰ型结构,因而HDS活性较低.

关键词: 氮气热处理, 硫代硫酸铵, 预硫化, 二硫化钼, 氧化铝, 加氢脱硫

Abstract: The (NH4)2S2O3-presulfidized Mo/Al2O3 catalyst pretreated with N2 at 80 ℃ gave the highest thiophene conversion. This is due to the modification of the Al2O3 support by sulfate ions, forming a highly active Type II MoS2 st ructure. Whereas an increase in the N2-pretreatment temperature above 200 ℃ led to a decomposition of (NH4)2S2O3, forming less active Type I MoS2 structure.

Key words: nitrogen thermal treatment, ammonium thiosulfate, presulfidation, molybdenum disulfide, alumina, hydrodesufurization