氮掺杂碳材料的制备及其催化乙苯氧化制备苯乙酮的性能
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摘要
以蔗糖为碳源,以三聚氰胺为氮掺杂剂和模板剂,采用高温热解法制备了半透明的片状氮掺杂碳材料(NC)。用XRD、XPS和TEM对NC进行表征。结果表明,NC为无定型材料,850℃下热解制备的NC含有较多的石墨N,NC为半透明片状材料。以NC为催化剂,用于叔丁基过氧化氢氧化乙苯制备苯乙酮。在适宜的反应条件下,0.53g(5mmol)乙苯、1.35 g(15 mmol)叔丁基过氧化氢、0.03 g的NC和15 mL去离子水在85℃反应20 h,苯乙酮的收率达76%。催化剂重复使用7次,活性没有明显降低。
A translucent flake nitrogen-doped carbon material(NC) was prepared by pyrolysis at high temperature using sucrose as carbon source, melamine as nitrogen dopant and template. NC was characterized by XRD, XPS and TEM. The results showed that NC was amorphous material. The NC prepared by pyrolysis at 850℃ contained more graphite N, and the NC was translucent sheet material. Acetophenone was prepared by oxidation of ethylbenzene with tert-butyl hydrogen peroxide using NC as catalyst. Under the suitable conditions: 0.53 g(5 mmol) of ethylbenzene, 1.35 g(15 mmol) of tert-butyl hydrogen peroxide, 0.03 g of NC and 15 mL of deionized water reacted at 85℃ for 20 h, the yield of acetophenone was about 76%. The catalyst could be reused 7 times, and its activity did not decrease significantly.
A translucent flake nitrogen-doped carbon material(NC) was prepared by pyrolysis at high temperature using sucrose as carbon source, melamine as nitrogen dopant and template. NC was characterized by XRD, XPS and TEM. The results showed that NC was amorphous material. The NC prepared by pyrolysis at 850℃ contained more graphite N, and the NC was translucent sheet material. Acetophenone was prepared by oxidation of ethylbenzene with tert-butyl hydrogen peroxide using NC as catalyst. Under the suitable conditions: 0.53 g(5 mmol) of ethylbenzene, 1.35 g(15 mmol) of tert-butyl hydrogen peroxide, 0.03 g of NC and 15 mL of deionized water reacted at 85℃ for 20 h, the yield of acetophenone was about 76%. The catalyst could be reused 7 times, and its activity did not decrease significantly.
引文
[1]李贵贤,李亚珍,徐彦铎,等.乙苯液相氧化制备苯乙酮催化剂的研究进展[J].应用化工,2012,41(8):1412-1416.
[2]程亮,徐丽,侯翠红,等.V-SBA-15分子筛的制备及其对乙苯制苯乙酮反应的催化性能[J].精细化工,2014,13(11):1348-1352.
[3]李贵贤,高云艳,张雪梅,等.叔丁基过氧化氢一步氧化乙苯合成苯乙酮[J].石油化工,2011,40(6):599-602.
[4]Du J, Zhang L, Zhang Y, et al. Fe modified mesoporous hollow carbon spheres for selective oxidation of ethylbenzene.Science China Materials, 2017, 60(12):1227-1233.
[5]张德懿,雷龙艳,尚永花.氮掺杂对碳材料性能的影响研究进展[J].化工进展,2016,35(3):831-836.
[6]Tang P, Gao Y, Yang J, et al. Growth mechanism of N-doped graphene materials and their catalytic behavior in the selective oxidation of ethylbenzene. Chinese Journal Catalysts, 2014, 35(6):922-928.
[7]刘振宇.新型多孔碳材料的合成与其应用研究[D].北京:北京化工大学,2013.
[8]徐旋.氮掺杂负载的纳米钯催化剂在催化加氢反应中的应用研究[D].杭州:浙江大学,2014.
[9]杨勇,王言,蓝国钧,等.氮掺杂多孔炭材料的制备及在多相催化中的应用[J].化学通报,2016,79(10):905-913.
[2]程亮,徐丽,侯翠红,等.V-SBA-15分子筛的制备及其对乙苯制苯乙酮反应的催化性能[J].精细化工,2014,13(11):1348-1352.
[3]李贵贤,高云艳,张雪梅,等.叔丁基过氧化氢一步氧化乙苯合成苯乙酮[J].石油化工,2011,40(6):599-602.
[4]Du J, Zhang L, Zhang Y, et al. Fe modified mesoporous hollow carbon spheres for selective oxidation of ethylbenzene.Science China Materials, 2017, 60(12):1227-1233.
[5]张德懿,雷龙艳,尚永花.氮掺杂对碳材料性能的影响研究进展[J].化工进展,2016,35(3):831-836.
[6]Tang P, Gao Y, Yang J, et al. Growth mechanism of N-doped graphene materials and their catalytic behavior in the selective oxidation of ethylbenzene. Chinese Journal Catalysts, 2014, 35(6):922-928.
[7]刘振宇.新型多孔碳材料的合成与其应用研究[D].北京:北京化工大学,2013.
[8]徐旋.氮掺杂负载的纳米钯催化剂在催化加氢反应中的应用研究[D].杭州:浙江大学,2014.
[9]杨勇,王言,蓝国钧,等.氮掺杂多孔炭材料的制备及在多相催化中的应用[J].化学通报,2016,79(10):905-913.