| 庞少峰,袁航空,吴亚娟,石峰.Co@N-石墨烯/C催化甲苯衍生物氧化胺化研究[J].分子催化,2017,31(2):105-120 |
| Co@N-石墨烯/C催化甲苯衍生物氧化胺化研究 |
| Co@N-graphene/C Catalyzed Oxidative Amination of Toluene Derivatives |
| 投稿时间：2017-01-05 修订日期：2017-02-16 |
| DOI： |
| 中文关键词: 氧化胺化 碳氢键 sp3-C-H N-烷基化胺 |
| 英文关键词:oxidative amination C-H bond sp3-C-H N-Alkyl amine |
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| 摘要点击次数: 1913 |
| 全文下载次数: 2829 |
| 中文摘要: |
| 核壳结构纳米催化剂的发展一直备受化学家的关注.我们通过热解碳担载乙酸钴和1，10-菲啰啉复合物制备出具有核壳结构的氮掺杂石墨烯包裹钴催化剂，并对其进行了系统的表征和催化性能研究.研究发现，该催化剂在TBHP和H2共存的条件下，在催化硝基苯和甲苯的选择性还原-氧化胺化合成N-烷基化胺反应中展现出较好的催化性能和良好的官能团耐受性.透射电镜表征表明氧化钴纳米颗粒被厚度约1.12~1.87 nm的含氮石墨烯壳包裹.X射线光电子能谱表征发现壳层中的石墨烯氮和作为核的氧化钴纳米颗粒间具有较明显的相互作用.我们对催化体系的普适性以及反应机理也进行了较为系统的研究. |
| 英文摘要: |
| The development of core-shell nanocatalysts has been intensively pursued. Here, we present the preparation, characterization and catalytic performance exploration of Co@N-graphene/C catalysts obtained via pyrolysis of cobalt acetate and phenanthroline. The Co@N-graphene/C catalysts showed high activity in the selectively reductive-oxidative amination of toluene and nitrobenzene for N-alkyl amines syntheses with excellent functional groups tolerance in the co-presence of oxidant and reductant, i.e., TBHP and H2. The generality of the catalyst system, and also the reaction mechanism were investigated. The transmission electron microscopy (TEM) and high resolution transmission electron microscopy (HR-TEM) characterizations indicate that a thickness of graphene shells about 1.12~1.87 nm around nanocobalt oxide particles. Meanwhile, the XPS characterization unravels the electronic interaction between the graphitic N and cobalt oxide nanoparticles. These results might promote the development of efficient heterogeneous catalysts for nitrogen containing fine chemical synthesis. |
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