物理化学学报 >> 2010, Vol. 26 >> Issue (10): 2691-2698.doi: 10.3866/PKU.WHXB20101006

催化和表面结构 上一篇    下一篇

萘在贵金属Pd、Pt 及Pd-Pt 催化剂上的加氢活性及耐硫性能

张小菲, 邵正锋, 毛国强, 何德民, 张秋民, 梁长海   

  1. 大连理工大学化工学院精细化工国家重点实验室, 辽宁大连116012
  • 收稿日期:2010-05-06 修回日期:2010-07-21 发布日期:2010-09-27
  • 通讯作者: 张秋民, 梁长海 E-mail:qmzhang@chem.dlut.edu.cn, changhai@dlut.edu.cn
  • 基金资助:

    国家自然科学基金(20973029)和中央高校基本科研业务费专项资金资助项目.

Naphthalene Hydrogenation Activity over Pd, Pt and Pd-Pt Catalysts and Their Sulfur Tolerance

ZHANG Xiao-Fei,SHAO Zheng-Feng,MAO Guo-Qiang,HE De-Min, ZHANG Qiu-Min, LIANG Chang-Hai   

  1. State Key Laboratory of Fine Chemicals, School of Chemical Engineering, Dalian University of Technology, Dalian 116012, Liaoning Province, P. R. China
  • Received:2010-05-06 Revised:2010-07-21 Published:2010-09-27
  • Contact: ZHANG Qiu-Min, LIANG Chang-Hai E-mail:qmzhang@chem.dlut.edu.cn, changhai@dlut.edu.cn
  • Supported by:

    The project was supported by the National Natural Science Foundation of China (20973029) and Fundamental Research Funds for the Central Universities, China.

摘要:

采用等体积浸渍法制备了SiO2-Al2O3 负载的Pd、Pt 单金属催化剂及Pd/Pt 摩尔比分别为1:1、1:4、4:1 的双金属催化剂(Pd1Pt1、Pd1Pt4、Pd4Pt1), 对其进行X 射线衍射(XRD) 、透射电镜(TEM) 、CO 化学吸附和X 射线光电子能谱(XPS) 表征, 并详细考察了各催化剂的萘加氢活性和耐硫性能. 结果表明, 在实验考察范围内, Pd4Pt1 催化剂上的萘转化率最高可达98.2%, 全饱和产物十氢萘选择性最高可达93.6%, 十氢萘反/顺生成率之比最高可达7.8, 均高于单金属Pd(97.5%, 59.1%, 4.3) 和Pt(96.8%, 39.9%, 2.9) 催化剂的值. 萘在三种催化剂上的加氢速率顺序为vPd4Pt1>vPd>vPt. 添加二苯并噻吩(DBT) 后Pd4Pt1 上的萘转化率和十氢萘选择性仍然最高, 十氢萘反/顺比在Pt 催化剂上不受影响, 在Pd4Pt1 催化剂上稍有降低, 而在Pd 催化剂上降低明显. 在三种不同Pd/Pt 摩尔比的双金属催化剂中, Pd4Pt1 催化剂上的萘转化率和十氢萘选择性在添加DBT 前后都是最佳的.

关键词: 贵金属, 萘, 加氢, 耐硫性, 十氢萘反/顺生成率之比

Abstract:

Monometallic Pd and Pt as well as bimetallic Pd:Pt catalysts (Pd1Pt1, Pd1Pt4, and Pd4Pt1) with Pd/Pt molar ratios of 1:1, 1:4, and 4:1 supported on SiO2-Al2O3 were prepared by incipient-wetness impregnation and characterized by X-ray diffraction (XRD), transmission electron microscopy (TEM), CO chemisorption, and X-ray photoelectron spectroscopy (XPS). Their catalytic activities toward naphthalene hydrogenation and the sulfur tolerance of these catalysts were investigated. We found that naphthalene conversion, selectivity toward decalin, and the trans-/cis-decalin yieldratio on Pd4Pt1 were 98.2%,93.6%,and 7.8,respectively,which are higher than those on Pd(97.5%,59.1%, 4.3) and Pt (96.8%, 39.9%, 2.9). The rate of naphthalene hydrogenation on the three catalysts increased according to: vPd4Pt1>vPd>vPt. In the presence of dibenzothiophene (DBT), the naphthalene conversion and selectivity toward decalin for Pd4Pt1 were still the highest. The trans-/cis-decalin ratio was not affected on the Pt catalyst, but it did decrease slightly on Pd4Pt1 and it decreased observably on the Pd catalyst. The Pd4Pt1 catalyst also presented the highest naphthalene conversion and selectivity toward decalin among the three bimetallic catalysts studied in the presence and absence of DBT.

 

Key words: Noble metal, Naphthalene, Hydrogenation, Sulfur tolerance, trans-/cis-decalin yield ratio

MSC2000: 

  • O643