高等学校化学学报 ›› 2019, Vol. 40 ›› Issue (12): 2436-2442.doi: 10.7503/cjcu20190415

• 研究论文: 无机化学 • 上一篇    下一篇

碗状双亲型ZSM-5分子筛负载金纳米粒子的制备及催化性能

孙思齐,王影,孙传胤,王润伟,张震东(),张宗弢(),裘式纶   

  1. 吉林大学化学学院, 无机合成与制备化学国家重点实验室, 长春 130012
  • 收稿日期:2019-07-24 出版日期:2019-10-18 发布日期:2019-10-18
  • 通讯作者: 张震东,张宗弢 E-mail:zzddoc@jlu.edu.cn;zzhang@jlu.edu.cn
  • 基金资助:
    国家自然科学基金(21771081);国家自然科学基金(21390394);国家自然科学基金(20971052);长白山学者奖励计划(2014004);吉林省科技发展计划项目(20180101001JC)

Preparation and Catalytic Performance of Bowl-shaped Amphiphilic ZSM-5 Zeolites Supported Gold Nanoparticles

Siqi SUN,Ying WANG,Chuanyin SUN,Runwei WANG,Zhendong ZHANG(),Zongtao ZHANG(),Shilun QIU   

  1. College of Chemistry, State Key Laboratory of Inorganic Synthesis and Preparative Chemistry, Jilin University, Changchun 130012, China
  • Received:2019-07-24 Online:2019-10-18 Published:2019-10-18
  • Contact: Zhendong ZHANG,Zongtao ZHANG E-mail:zzddoc@jlu.edu.cn;zzhang@jlu.edu.cn
  • Supported by:
    ? Supported by the National Natural Science Foundation of China(21771081);the National Natural Science Foundation of China(21390394);the National Natural Science Foundation of China(20971052);the Changbai Mountain Scholars Program, China(2014004);the Jilin Provincial Scientific and Technological Development Program, China(20180101001JC)

摘要:

通过不对称修饰法制备了一种碗状双亲型的ZSM-5分子筛, 其拥有一个非极性的外表面和一个可修饰的极性内表面; 进一步利用经典的氨基接枝-原位还原过程, 选择性地在其内表面生长金纳米粒子. 通过X射线粉末衍射、 扫描电子显微镜、 透射电子显微镜、 红外光谱和X射线光电子能谱对材料进行了表征, 并考察了其催化硝基苯加氢制苯胺反应的性能. 在非常温和(室温、 水作溶剂及无需氮气保护)以及更低反应物浓度(0.03 mol/L, 低于室温下硝基苯在水中的溶解度)条件下, 该催化剂展现出与其它使用有机溶剂的催化剂相当的催化活性和选择性, 而且其催化性能明显高于其它以水为溶剂的催化剂, 这表明载体的双亲型结构是提升催化性能的主要原因. 该催化剂循环使用6次后, 其催化活性和选择性仍保持在相同等级.

关键词: 金纳米粒子, ZSM-5分子筛, 不对称修饰, 选择催化, 硝基苯

Abstract:

Bowl-shaped amphiphilic ZSM-5 zeolites, which have a lipophilic outer surface and a modified hydrophilic inner surface, were prepared by asymmetric modification via a classical amino graft-in situ reduction process. The gold nanoparticles were selectively grown on the inner surface of the zeolites. The samples were characterized by means of XRD, SEM, TEM, IR and XPS, and their catalytic properties for hydrogenation of nitrobenzene to aniline were investigated. Under very mild conditions(room temperature, water as solvent, without nitrogen protection) and lower reactant concentration(0.03 mol/L, lower than the solubility of nitrobenzene in water at room temperature), the catalyst exhibited the same catalytic activity and selectivity as other catalysts using organic solvents, and was significantly higher than other catalysts using water as catalyst. The amphiphilic structure of the support was proved to be the main reason for improving the catalytic effect. After six cycles, the catalytic activity and selectivity of the catalyst remained at the same level.

Key words: Gold nanoparticles, ZSM-5 zeolite, Asymmetric modification, Selective catalysis, Nitrobenzene

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