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

doi:10.11949/j.issn.0438-1157.20161659

Abstract

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:

TQ032

CHEN Tan, CHEN Hao, FU Jie, CHEN Kequan, OUYANG Pingkai. Catalytic performance of CuO/HZSM-5 in aromatic synthesis from CH₃Br[J]. CIESC Journal, 2017, 68(6): 2344-2351.

陈坦, 陈皓, 傅杰, 陈可泉, 欧阳平凯. CuO/HZSM-5催化溴甲烷芳构化制备芳烃[J]. 化工学报, 2017, 68(6): 2344-2351.

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

CuO/HZSM-5催化溴甲烷芳构化制备芳烃

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