CIESC Journal ›› 2017, Vol. 68 ›› Issue (6): 2344-2351.DOI: 10.11949/j.issn.0438-1157.20161659

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Catalytic performance of CuO/HZSM-5 in aromatic synthesis from CH3Br

CHEN Tan1, CHEN Hao2, FU Jie2, CHEN Kequan1, OUYANG Pingkai1,2   

  1. 1. Biotechnology and Pharmaceutical Engineering, Nanjing Tech University, Nanjing 211800, Jiangsu, China;
    2. Key Laboratory of Biomass Chemical Engineering of Ministry of Education, College of Chemical and Biological Engineering, Zhejiang University, Hangzhou 310027, Zhejiang, China
  • Received:2016-11-24 Revised:2017-03-20 Online:2017-06-05 Published:2017-06-05
  • Contact: 10.11949/j.issn.0438-1157.20161659
  • Supported by:

    supported by the National Natural Science Foundation of China (21436007) and the Natural Science Foundation of Zhejiang Province (LR17B060002)

CuO/HZSM-5催化溴甲烷芳构化制备芳烃

陈坦1, 陈皓2, 傅杰2, 陈可泉1, 欧阳平凯1,2   

  1. 1. 南京工业大学生物与制药工程学院, 江苏 南京 211800;
    2. 浙江大学生物质化工教育部重点实验室, 化学工程与生物工程学院, 浙江 杭州 310027
  • 通讯作者: 傅杰
  • 基金资助:

    国家自然科学基金项目(21436007);浙江省自然科学基金项目(LR17B060002)

Abstract:

CuO/HZSM-5 catalysts with 1%—7% CuO loading, which were prepared by incipient wetness impregnation, were used to study catalytic performance in the conversion of CH3Br to aromatic compounds in a fixed-bed reactor by changing temperature, CH3Br flow rate and CuO loading. Fresh and used catalysts were characterized by SEM, TEM, XRD, XPS, TG, DSC, N2 adsorption and desorption, and NH3-TPD. XRD results showed that CuO was highly dispersed on HZSM-5 and structure of CuO crystals did not change during reaction. NH3-TPD results showed that 3% (mass) CuO loading increased strong acidity of catalyst. XPS results showed that coke deposition on used CuO/HZSM-5 catalyst was mainly graphite. The highest aromatic yield of 22.3% was achieved at condition of 3% (mass) CuO loading, 360℃ temperature and 240 ml·g-1·h-1 GHSV. The 3% (mass) CuO/HZSM-5 maintained stable catalytic activity within 40 h reaction time.

Key words: CuO/HZSM-5, CH3Br, catalysis, fixed-bed, aromatic, stability

摘要:

采用等体积浸渍法制备了不同负载量(1%~7%)的CuO/HZSM-5催化剂,在固定床反应器中研究了不同反应温度、溴甲烷流量以及CuO负载量对溴甲烷芳构化催化性能的影响。采用SEM、XRD、N2吸附脱附、TEM、XPS、TG、DSC、NH3-TPD等技术对反应前后的催化剂进行表征。XRD 结果显示活性组分CuO 在HZSM-5上具有很好的分散性,并且反应后Cu晶型不变。NH3-TPD 结果显示3%的CuO 负载后,催化剂强酸量增加。在CuO 负载量为3%,温度为360℃,反应空速为240 ml·g-1·h-1 条件下得到最高的芳烃收率(22.3%)。XPS 结果显示反应后在催化剂上主要的积炭为石墨碳。催化剂稳定性测试结果表明反应40 h内催化活性没有明显下降。

关键词: CuO/HZSM-5, 溴甲烷, 催化, 固定床, 芳烃, 稳定性

CLC Number: