咖啡渣基新型氮杂化炭材料制备与催化环己基苯氧化  

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

作　　者：冯洋洋[1] 单玉华[1] 郑一天 李明时[1] 鲁墨弘[1] 

机构地区：[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

出　　处：《石油学报（石油加工）》2017年第5期941-949,共9页Acta Petrolei Sinica(Petroleum Processing Section)

基　　金：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

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(O2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 O2分压下反应4h,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。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 MPaO_2 at130℃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.

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 

分 类 号：TQ426[化学工程]