石油学报(石油加工) ›› 2017, Vol. 33 ›› Issue (5): 941-949.doi: 10.3969/j.issn.1001-8719.2017.05.017

• 研究报道 • 上一篇    下一篇

咖啡渣基新型氮杂化炭材料制备与催化环己基苯氧化

冯洋洋, 单玉华,郑一天,李明时,鲁墨弘   

  1. 常州大学 江苏省先进催化与绿色制造协同创新中心,江苏 常州 213164

  • 收稿日期:2016-10-27 修回日期:2017-02-27 出版日期:2017-09-25 发布日期:2017-11-29
  • 通讯作者: 单玉华,男,教授,博士,从事绿色催化材料研究;Tel: 0519-86330360; E-mail:yhshan@cczu.edu.cn E-mail:565625295@qq.com
  • 作者简介:第一作者:冯洋洋,女,硕士研究生,从事绿色催化材料研究;E-mail:565625295@qq.com
  • 基金资助:
    江苏省绿色催化材料与技术重点实验室项目(BM2012110)、江苏省科技厅前瞻性研究项目(BY2014037-12)资助

Preparation of Nitrogen-Doped Carbon From Waste Coffee Grounds and Its Catalytic Performance in Cyclohexylbenzene Oxidation

FENG Yangyang, SHAN Yuhua, ZHENG Yitian, LI Mingshi, LU Mohong   

  1. Advanced Catalysis and Green Manufacturing Collaborative Innovation Center, Changzhou University, Changzhou 213164, China
  • Received:2016-10-27 Revised:2017-02-27 Online:2017-09-25 Published:2017-11-29

摘要: 将咖啡渣在氨气氛中高温热处理,制备氮杂化炭材料。采用X射线粉末衍射(XRD)、拉曼光谱(Raman)、氮气吸附脱附(BET)、透射电镜(TEM)、红外光谱(FTIR)等方法对其进行表征,采用X射线光电子能谱(XPS)测定其掺氮量,并将其用于催化氧化环己基苯(CHB)合成苯酚和环己酮,考察了咖啡渣的热处理温度和反应条件(O2压力、反应温度和时间)对上述反应的影响。结果表明,700℃氨气氛中制备的咖啡渣基氮杂化炭材料(NC700)具有较好的催化性能,其中所含石墨氮杂化结构对形成催化活性中心起重要作用;以NC700为催化剂,在130℃、09 MPa O2分压下反应4 h,CHB转化率为183%,环己酮和苯酚的选择性分别为818%和707%。NC700循环使用10次,其催化性能没有明显变化。表明NC700是可用于CHB氧化合成苯酚和环己酮的性能稳定、易回收利用、无污染的新型催化剂。

关键词: 咖啡渣;氮掺杂炭材料;环己基苯(CHB), 催化氧化;苯酚;环己酮.

Abstract: A new N-doped carbon material was prepared by thermal treatment of waste coffee grounds under ammonia gas atmosphere, and characterized by XRD, Raman, BET, TEM and FT-IR methods. The amount and nature of doped nitrogenspecies in the asprepared material were examined by Xray photoelectron spectroscopy (XPS). The material was used as a catalyst for cyclohexylbenzene (CHB) oxidation to phenol and cyclohexanone. The effects of thermal treating temperature of waste coffee grounds and reaction conditions (O2 pressure, reaction temperature and time) were investigated. The results show that: the Ndoped carbon material obtained by thermal treatment of waste coffee grounds and NH3 at 700℃ (NC700) exhibits good catalytic performance, and the graphitetype doped nitrogen structures play a significant role for the formation of the catalytic active sites; using NC700 as a catalyst, carrying out the reaction under 09 MPa O2 at 130℃ for 4 h, we converted 183% of CHB into phenol and cyclohexanone with the selectivity of 818% and 707%, respectively. After the catalyst was reused 10 times, no obvious catalytic performance change has been observed. The present results demonstrated that the NC700 is a stable, reusable and clean catalyst for the synthesis of phenol and cyclohexanone from CHB oxidation.

Key words: waste coffee grounds, N-doped carbon material, clohexylbenzene(CHB), catalytic oxidation, phenol, cyclohexanone.