催化学报 ›› 2013, Vol. 34 ›› Issue (11): 2057-2065.DOI: 10.1016/S1872-2067(12)60670-6

• 研究论文 • 上一篇    下一篇

Rh(OH)x/TS-1@KCC-1双功能催化剂上一锅反应合成伯酰胺

彭洪根, 王达锐, 徐乐, 吴鹏   

  1. 华东师范大学化学系, 上海市绿色化学与化工过程绿色化重点实验室, 上海200062
  • 收稿日期:2013-06-19 修回日期:2013-07-23 出版日期:2013-10-18 发布日期:2013-10-18
  • 通讯作者: Peng Wu
  • 基金资助:

    国家自然科学基金(220925310,U1162102);高等学校博士学科点专项科研基金(2012007613000);国家重点基础研究发展计划(973计划,2012BAE05B02);上海市教育委员会重点学科建设项目(B409).

One-pot synthesis of primary amides on bifunctional Rh(OH)x/TS-1@KCC-1 catalysts

Honggen Peng, Darui Wang, Le Xu, Peng Wu   

  1. Shanghai Key Laboratory of Green Chemistry and Chemical Processes, Department of Chemistry, East China Normal University, Shanghai 200062, China
  • Received:2013-06-19 Revised:2013-07-23 Online:2013-10-18 Published:2013-10-18
  • Contact: Peng Wu
  • Supported by:

    This work was supported by the National Natural Science Foundation of China (220925310, U1162102), the Specialized Research Fund for the Doctoral of Higher Education (2012007613000), the National Basic Research Program of China (973 Program, 2012BAE05B02), and the Shanghai Leading Academic Discipline Project (B409).

摘要:

在微乳液体系中成功地将花瓣状介孔氧化硅微球(KCC-1)包覆在钛硅分子筛TS-1表面, 得到了一种新型微孔/介孔复合核壳结构材料TS-1@KCC-1. 详细考察了TS-1@KCC-1的合成条件及可能的形成机理. 适宜的合成温度及时间分别为373-393 K和4 h. 壳层厚度可方便地通过改变硅源正硅酸乙酯和TS-1的比例在25-80 nmm间进行调控. 以TS-1@KCC-1为载体负载Rh(OH)x后即得到双功能催化材料Rh(OH)x/TS-1@KCC-1, 该材料同时具有Ti和Rh(OH)x活性中心, 可以高效催化醛、氨水和过氧化氢经一锅串联反应直接制备得到伯酰胺.

关键词: TS-1分子筛, 核壳材料, KCC-1, 伯酰胺, 串联催化剂

Abstract:

A new microporous/mesoporous composite with a core-shell structure, TS-1@KCC-1, was fabricated in a microemulsion system by coating flower-like mesoporous silica (KCC-1) on the crystal surface of TS-1 zeolite. The synthesis conditions and a possible formation mechanism were studied in detail for the TS-1@KCC-1 material. A suitable temperature and assembly time were found to be 373-393 K and 4 h, respectively. The shell thickness of TS-1@KCC-1 was conveniently tuned in the range 25-80 nm. Rh(OH)x species were supported on TS-1@KCC-1, giving rise to a novel bifunctional tandem catalyst Rh(OH)x/TS-1@KCC-1, which effectively catalyzed the one-pot synthesis of primary amides directly from aldehydes, ammonia, and hydrogen peroxide.

Key words: TS-1 zeolite, Core-shell material, KCC-1, Primary amide, Tandem catalyst