石油学报(石油加工) ›› 2015, Vol. 31 ›› Issue (2): 542-549.doi: 10.3969/j.issn.1001-8719.2015.02.035

• 特约报告 • 上一篇    下一篇

以活性炭为载体制备Pd和Pt加氢脱硫催化剂

董超1,李翔1,2,王安杰1,2,陈永英1   

  1. 1. 大连理工大学 精细化工国家重点实验室,辽宁 大连116012;
    2. 辽宁省高校石油化工技术与装备重点实验室,辽宁 大连 116012
  • 收稿日期:2014-12-10 修回日期:2014-12-18 出版日期:2015-04-25 发布日期:2015-05-06
  • 通讯作者: 李翔,副教授,工学博士,从事加氢精制催化剂及介孔分子筛研究;TEl: 0411-84986124;E-mail: lixiang@dlut.edu.cn E-mail:lixiang@dlut.edu.cn
  • 作者简介:第一作者:董超,博士研究生,从事贵金属催化剂加氢脱硫及脱氮研究
  • 基金资助:

    国家自然科学基金项目(20973030,21073022, 和U1162203)、中央高校基本科研业务费专项资金(DUT13LK18)、辽宁省教育厅科学研究项目(L2013023)及中国石油科技创新项目(2014D-5006-0402)资助

Preparation of Pd and Pt Hydrodesulfurization catalysts Supported on Activated Carbons

DONG Chao1,LI Xiang1,2,WANG Anjie1,2,CHEN Yongying1   

  1. 1. State Key Laboratory of Fine Chemical, Dalian University of Technology, Dalian 116012, China; 2. Liaoning Key Laboratory of Petrochemical Technology and Experiment, Dalian 116012, China
  • Received:2014-12-10 Revised:2014-12-18 Online:2015-04-25 Published:2015-05-06

摘要: 别以椰壳活性炭、果壳活性炭和木质活性炭为载体,采用等体积浸渍法制备了Pd/C和Pt/C催化剂。以二苯并噻吩(DBT)为模型含硫化合物,考察了不同种类活性炭负载的贵金属催化剂加氢脱硫(HDS)催化性能。结果表明,增加活性炭表面酸性含氧基团或碱性基团数量都有助于提高Pt和Pd的分散度。DBT在Pd/C和Pt/C催化剂催化下进行HDS反应时,直接脱硫(DDS)路径选择性高于加氢反应路径(HYD)选择性,其中Pt/C催化剂的HDS催化活性和DDS路径选择性都显著高于Pd/C催化剂。Pd/C和Pt/C催化剂的HDS催化性能主要取决于载体表面官能团的种类和分布。Pd和Pt催化剂的HYD反应路径选择性和稳定性都随载体表面酸性含氧基团的增加而增加,但它们断裂C—S的活性却有所降低;增加载体表面碱性基团数量则有助于提高催化剂断裂C—S的活性,但不利于其稳定性。

关键词: 钯, 铂, 活性炭, 加氢脱硫

Abstract:  The Pd and Pt hydrodesulfurization (HDS) catalysts supported on coconut shell activated carbon, nut shell activated carbon, and wood activated carbon were prepared by an incipient wetness impregnation method. The HDS catalytic performances of these noble metal catalysts supported on different activated carbons were investigated by using a model feed containing 0.8 % dibenzothiophene (DBT) in decalin. The results indicated that the dispersion of Pd and Pt could be enhanced by increasing the amounts of either the acidic oxygen-containing groups or the basic groups on the surface of the support. In the HDS of DBT over the Pd/C and Pt/C catalysts, the selectivity toward the direct desulfurization pathway (DDS) was higher than that toward the hydrogenation pathway (HYD). Both the HDS activity and the DDS pathway selectivity of the supported Pt catalysts were significantly higher than those of the supported Pd catalysts. The HDS catalytic performances of the Pt/C and Pd/C catalysts were mainly determined by the surface groups of the support and their distributions. An increase of the surface acidic oxygen-containing groups led to an increase of the HYD selectivity and the stability of the Pd and Pt catalysts, but a decrease in their C-S bond cleavage activity. On the other hand, the basic groups showed a positive effect on the C-S bond cleavage activity of Pd/C and Pt/C and a negative influence on their stability.

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