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噻吩在猝冷骨架Ni上吸附脱硫的XPS研究

谢福中1, 胡华荣1, 乔明华1, 闫世润1, 范康年1, 雷浩2, 谭大力2, 包信和2, 宗保宁3, 张晓昕3
  

    1. 上海市分子催化和创新材料重点实验室, 复旦大学化学系, 上海 200433;
    2. 中国科学院大连化学物理研究所催化基础国家重点实验室, 大连 116023;
    3. 石油化工科学研究院, 北京 100083
  • 收稿日期:2005-09-20 修回日期:1900-01-01 出版日期:2006-09-10 发布日期:2006-09-10
  • 通讯作者: 范康年

XPS Study on Adsorptive Desulfurization of Thiophene over Rapidly Quenched Skeletal Ni

XIE Fu-Zhong1, HU Hua-Rong1, QIAO Ming-Hua1, YAN Shi-Run1, FAN Kang-Nian1, LEI Hao2, TAN Da-Li2, BAO Xin-He2, ZONG Bao-Ning3, ZHANG Xiao-Xin3   

    1. Department of Chemistry, Shanghai Key Laboratory of Molecular Catalysis and Innovative Materials, Fudan University, Shanghai 200433, China;
    2. State Key Laboratory of Catalysis, Dalian Institute of Chemical Physics, Chinese Academy of Sciences, Dalian 116023, China;
    3. Research Institute of Petroleum Processing, Beijing 100083, China
  • Received:2005-09-20 Revised:1900-01-01 Online:2006-09-10 Published:2006-09-10
  • Contact: FAN Kang-Nian

摘要: 采用X射线光电子能谱(XPS)研究了室温下噻吩在猝冷骨架Ni吸附剂上的吸附及受热分解行为. 研究结果表明, 298 K时噻吩首先在吸附剂表面发生C—S键断裂, 生成原子硫及含金属的有机环状化合物. 当吸附剂表面完全被解离物种覆盖后, 发生噻吩的多层物理吸附. 加热至373 K, 大部分物理吸附的噻吩直接脱附, 其余部分在碳物种脱附后暴露的Ni表面上发生解离. 473 K时表面的碳物种消失, 而残留在样品上的硫均转化为硫化镍.

关键词: 猝冷镍, 噻吩, 吸附脱硫, X射线光电子能谱

Abstract: The adsorptive desulfurization of thiophene on rapidly quenched skeletal Ni(RQ Ni) was investigated by XPS. At 298 K, thiophene in direct contact with RQ Ni undergoes C—S bond scission, forming metallocycle-like species and atomic sulfur on metallic nickel. Further exposure to thiophene leads to physisorbed thiophene. At 373 K, most of the physisorbed thiophene desorbs, with a small portion undergoing sulfur abstraction on the newly exposed nickel surface. The existence of alumina and hydrogen may block the further cracking of the metallocycle-like species at higher temperatures, which has been considered to be the dominant reaction pathway on Ni single crystals. At 473 K, the C1s peak disappears, leaving nickel sulfide on the surface.

Key words: Rapidly quenched Ni, Thiophene, Adsorptive desulfurization, XPS

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