高等学校化学学报 ›› 2020, Vol. 41 ›› Issue (6): 1262-1268.doi: 10.7503/cjcu20200149

• 物理化学 • 上一篇    下一篇

原子级分散Fe-N-C温和条件下选择性氧化催化特性

熊俊宇,王姗姗,许颜清*(),胡长文*()   

  1. 北京理工大学化学与化工学院, 原子分子簇科学教育部重点实验室, 光电转换材料北京市重点实验室, 北京 100081
  • 收稿日期:2020-03-17 出版日期:2020-06-10 发布日期:2020-04-26
  • 通讯作者: 许颜清,胡长文 E-mail:xyq@bit.edu.cn;cwhu@bit.edu.cn
  • 基金资助:
    国家自然科学基金;国家自然科学基金(21671019);国家自然科学基金(21871026);国家自然科学基金(21271025);国家自然科学基金(11474204)

Selective Oxidation of Atomically Dispersed Fe-N-C Catalyst Under Mild Conditions

XIONG Junyu,WANG Shanshan,XU Yanqing*(),HU Changwen*()   

  1. Key Laboratory of Cluster Science, Ministry of Education of China, Beijing Key Laboratory of Photoelectronic/Electrophotonic Conversion Materials, School of Chemistry and Chemical Engineering, Beijing Institute of Technology, Beijing 100081, China
  • Received:2020-03-17 Online:2020-06-10 Published:2020-04-26
  • Contact: Yanqing XU,Changwen HU E-mail:xyq@bit.edu.cn;cwhu@bit.edu.cn
  • Supported by:
    † National Natural Sciecnce Foundation of China;National Natural Sciecnce Foundation of China(21671019);National Natural Sciecnce Foundation of China(21871026);National Natural Sciecnce Foundation of China(21271025);National Natural Sciecnce Foundation of China(11474204)

摘要:

采用非溶液法制备了原子级分散的Fe-N-C催化剂, 并用于硫醚和二级醇的选择性氧化. 研究结果表明, 这种原子级分散的Fe-N-C催化剂可在温和条件下选择性地将硫醚转化为亚砜, 而不会产生过度氧化的砜. 该工艺具有反应条件温和、 反应速度快、 收率高等优点; 该催化剂对二级醇氧化制酮反应具有较高的催化活性, 产率较高. 作为一种非均相催化剂, Fe-N-C催化剂循环使用5次后活性未见显著下降; 在实验结果和参考文献的基础上还提出了一种可能的自由基反应机理.

关键词: 单原子催化剂, 选择性氧化, 铁氮掺杂碳材料, 非均相催化剂

Abstract:

An atomically dispersed Fe-N-C catalyst prepared by one-pot mechanochemical process was used for selective oxidation of sulfides and secondary alcohols. The results show Fe-N-C catalyst can selectively transform sulfides to sulfoxides under mild conditions without any over-oxidized sulfones. This process has several advantages such as mild reaction conditions, high reaction speed and satisfactory yields. In addition, this catalyst exhibits high catalytic activity in the oxidation of the secondary alcohols to the related ketones with decent yields. As a heterogeneous catalyst, activity of this atomically dispersed Fe-N-C does not significantly decrease after 5 times of circulation.

Key words: Single-atom catalyst, Selective oxidation, Iron-nitrogen-doped carbon, Heterogeneous catalyst

中图分类号: