催化学报

催化学报 ›› 2011, Vol. 32 ›› Issue (4): 612-617.DOI: 10.3724/SP.J.1088.2011.01016

• 研究论文 • 上一篇    下一篇

Ni/HZSM-5 催化剂的结构及其催化山梨醇水相加氢合成烷烃性能

邱珂 1,2, 章青 1, 江婷 1,2, 马隆龙 1, 王铁军 1, 张兴华 1,2, 丘明煌 1,2   

  1. 1中国科学院广州能源研究所可再生能源与天然气水合物重点实验室, 广东广州 510640; 2中国科学院研究生院, 北京 100049
  • 收稿日期:2010-11-12 修回日期:2011-01-14 出版日期:2011-04-18 发布日期:2014-08-30

Structure of Ni/HZSM-5 Catalyst and Its Catalytic Performance for Aqueous Phase Hydrogenation of Sorbitol to Alkanes

QIU Ke1,2, ZHANG Qing1, JIANG Ting1,2, MA Longlong1, WANG Tiejun1, ZHANG Xinhua1,2, QIU Minghuang1,2   

  1. 1Key Laboratory of Renewable Energy and Gas Hydrate, Guangzhou Institute of Energy Conversion, Chinese Academy of Sciences, Guangzhou 510640, Guangdong, China; 2Graduate University of Chinese Academy of Sciences, Beijing 100049, China
  • Received:2010-11-12 Revised:2011-01-14 Online:2011-04-18 Published:2014-08-30

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被引次数

21

摘要： 采用浸渍法制备了 Ni/HZSM-5 双功能催化剂, 考察了焙烧温度对催化剂结构及其催化山梨醇水相加氢合成 C5~C6 烷烃性能的影响. 结果表明, 在金属中心和酸性载体的协同作用下, 通过山梨醇中 C–O 键加氢和异构化高选择性合成了 C5~C6 烷烃. 经 500oC 焙烧的 Ni/HZSM-5 催化剂上山梨醇水相加氢的活性最高, 山梨醇转化率为 62.0%, 戊烷和己烷的总选择性为 76.4%, 其中异己烷选择性达 45.4%. 对催化剂进行 N2 物理吸附、X-射线衍射、NH3 程序升温脱附和 H2 程序升温还原等表征后发现, 经 500oC 焙烧催化剂的有效比表面积和孔体积均明显增大, HZSM-5 负载的硝酸镍分解成较小晶粒的 NiO, 表面酸量适中, 且 Ni 物种与载体相互作用较强, 较易被 H2 还原, Ni 还原度达 100%. 这是其催化活性最高的原因.

关键词: 镍, HZSM-5 分子筛, 山梨醇, 水相加氢, 烷烃

Abstract: A bifunctional Ni/HZSM-5 catalyst was prepared by the conventional impregnation method. The effects of calcination temperature on the structure properties of the catalyst and its catalytic performance for aqueous phase hydrogenation of sorbitol were studied. The results showed that C5~C6 alkanes were effectively obtained by the hydrogenation of the C–O bond in sorbitol and the following isomerization due to the synergism of the metal center and acid support. Moreover, the catalyst calcined at 500 °C exhibited a maximum value of 62.0% for sorbitol conversion and 76.4% of selectivity for pentane and hexane in comparison with other catalyst samples, wherein the isohexane selectivity was about 45.4%. The catalyst samples were characterized by N2 physical adsorption, X-ray diffraction, NH3 temperature-programmed desorption, and H2 temperature-programmed reduction. It was found that the surface area and pore volume of the catalyst calcined at 500 °C were obviously increased. Smaller grains of NiO can be formed from the decomposition of nickel nitrate on the surface of HZSM-5, which can provide with the appropriate amounts of acid and the interaction between the nickel species and acid support for easier hydrogen reduction with the Ni reducibility of 100%. All these factors are closely related to the highest catalytic performance of Ni/HZSM-5 catalyst for aqueous phase hydrogenation of sorbitol.

Key words: nickel, HZSM-5 zeolite, sorbitol, aqueous phase hydrogenation, alkane