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合成气经费托路线直接制芳烃进展

王清俊 孙来芝 陈雷 杨双霞 谢新苹 司洪宇 赵保峰 许美荣 高明杰 李天津 华栋梁

王清俊, 孙来芝, 陈雷, 杨双霞, 谢新苹, 司洪宇, 赵保峰, 许美荣, 高明杰, 李天津, 华栋梁. 合成气经费托路线直接制芳烃进展[J]. 燃料化学学报, 2023, 51(1): 52-66. doi: 10.19906/j.cnki.JFCT.2022066
引用本文: 王清俊, 孙来芝, 陈雷, 杨双霞, 谢新苹, 司洪宇, 赵保峰, 许美荣, 高明杰, 李天津, 华栋梁. 合成气经费托路线直接制芳烃进展[J]. 燃料化学学报, 2023, 51(1): 52-66. doi: 10.19906/j.cnki.JFCT.2022066
WANG Qing-jun, SUN Lai-zhi, CHEN Lei, YANG Shuang-xia, XIE Xin-ping, SI Hong-yu, ZHAO Bao-feng, XU Mei-rong, GAO Ming-jie, LI Tian-jin, HUA Dong-liang. Recent advance in directing synthesis of aromatic hydrocarbons from syngas via Fischer-Tropsch route[J]. Journal of Fuel Chemistry and Technology, 2023, 51(1): 52-66. doi: 10.19906/j.cnki.JFCT.2022066
Citation: WANG Qing-jun, SUN Lai-zhi, CHEN Lei, YANG Shuang-xia, XIE Xin-ping, SI Hong-yu, ZHAO Bao-feng, XU Mei-rong, GAO Ming-jie, LI Tian-jin, HUA Dong-liang. Recent advance in directing synthesis of aromatic hydrocarbons from syngas via Fischer-Tropsch route[J]. Journal of Fuel Chemistry and Technology, 2023, 51(1): 52-66. doi: 10.19906/j.cnki.JFCT.2022066

合成气经费托路线直接制芳烃进展

doi: 10.19906/j.cnki.JFCT.2022066
基金项目: 国家自然科学基金青年基金(21908117),山东省重点研发计划(重大科技创新工程)(2022CXGC010701),山东省高等学校青年创新团队项目(2019KJD002),济南市科研带头人工作室(2021GXRC095)和齐鲁工业大学(山东省科学院)校(院)地产学研协同创新基金(2020-CXY30)资助
详细信息
    通讯作者:

    Tel: 13220597603, E-mail:sunlz@sderi.cn

  • 中图分类号: TQ241;O643.36

Recent advance in directing synthesis of aromatic hydrocarbons from syngas via Fischer-Tropsch route

Funds: The project was supported by the National Natural Science Foundation of China (21908117), Key Research and Development Program of Shandong Province (2022CXGC010701), Youth Innovation Team Project of Colleges and Universities of Shandong Province (2019KJD002), Jinan Research Leader Workshop (2021GXRC095), Collaborative Innovation Fund of Qilu University of Technology (Shandong Academy of Sciences) (2020-CXY30).
  • 摘要: 芳烃作为重要的工业基础化学品,可通过合成气直接或间接法转化制备。与间接转化法相比较,合成气直接制芳烃路线(STA)具有原料转化率高、流程短、产品易分离等优点。本研究主要综述了合成气经费托路线直接制芳烃的研究进展,重点分析了金属氧化物耦合分子筛双功能催化剂中费托活性组分与助剂的选择、分子筛酸性调变、孔道结构调控等对催化反应性能的影响;归纳了反应温度、压力、空速、氢碳比等反应参数对反应性能的影响规律,并基于STA反应机理和失活机理等方面概述探讨如何提高活性和稳定性;总结归纳了合成气经费托路线制芳烃面临的主要问题以及今后研究的方向。
  • 图  1  合成气经CoC/HZSM-5制取芳烃[30]

    Figure  1  Synthesis of aromatic hydrocarbons from syngas by CoC/HZSM-5[30](with permission from ACS Publications)

    图  2  合成气经K/FeZrZn-Ni/HZSM-5制取芳烃[40]

    Figure  2  Synthesis of aromatics from syngas by K/FeZrZn-Ni/HZSM-5[40](with permission from Elsevier)

    图  3  合成气经Na-Zn-Fe/HZSM-5制取芳烃[13]

    Figure  3  Synthesis of aromatic hydrocarbons from syngas via NA-Zn-Fe /HZSM-5 [13](with permission from Elsevier)

    图  4  FeMnK/SiO2和HZSM-5催化剂不同组合方式[59]

    Figure  4  Different combinations of FeMnK/SiO2 and HZSM-5 catalysts[59](with permission from Elsevier)

    图  5  核壳 FeMn@Hollow HZSM-5纳米反应器直接将合成气转化为芳烃[48]

    Figure  5  Core-shell FeMn@Hollow HZSM-5 nanoreactor directly converts syngas to aromatics[48](with permission from ACS Publications)

    图  6  木质生物质合成气在Pd促进的 Fe/HZSM-5催化剂上合成[61]

    Figure  6  Synthesis of aroma-rich gasoline distillates from lignocellulosic biomass syngas over Fe/HZSM-5 catalyst promoted by Pd [61](with permission from ACS Publications)

    图  7  FeNiOxNa/HZSM-5用于合成气直接制芳烃反应途径[27]

    Figure  7  Reaction pathway of FeNiOxNa/HZSM-5 for direct aromatics production from syngas [27](with permission from ACS Publications)

    图  8  HZSM-5芳烃生成路径[63]

    Figure  8  Formation paths of HZSM-5 arenes [63](with permission from Elsevier)

    表  1  不同催化剂上合成气经费托路线一步法制芳烃反应条件和性能

    Table  1  Reaction conditions and performance of aromatics by one-step synthesis gas method on different catalysts

    CatalystReaction conditionsxCO
    /%
    saromatic
    /%
    Ref.
    temperature
    /℃
    pressure
    /MPa
    GHSV
    /h−1
    H2/CO
    Na-FeMnCo/HZSM-5350415001.598.055.0a[25]
    Na-FeMn/nano-HZSM-535041800295.053.0a[22]
    Fe/MnO-ZnZSM-527011600298.153.1a[46]
    FeK + HZSM-530024000027618a[38]
    Fe/Ni-HZSM-533041813299.248.0b[19]
    K-FeMnO/MoNi-ZSM-537041395297.634.1a[39]
    K/FeZrZn20-Ni/ZSM-534042000297.232.1a[40]
    Fe/HZSM-530012264285.030.0a[50]
    Fe/HZSM-5300225 mL/min157.070b[51]
    Fe/HZSM-532024000150.063b[24]
    FeNiOx(5:1)-0.41Na/HZSM-532011800146.399.4b[27]
    Na-Zn-Fe5C2-HZSM-5340210000 mL/(g·h)2.58551b[13]
    K/Zn-FeZr/Ni/HZS-534042000296.8139.48a[40]
    Mo/HZSM-5350360001.3264.497.6b[33]
    Na-Fe-Zro2/HZSM-528032400 mL/(g·h)109422a[23]
    FeNaMg-NiHZSM-537041800296.1951.38b[42]
    Fe3O4@MnO2-Hollow ZSM-5320450 mL/min7073.5b[48]
    CoMnAl-HZSM-527013000 mL/(g·h)0.534.955.5a[30]
    a: selectivity of aromatics in hydrocarbon products; b: selectivity of aromatic hydrocarbons in C5 +
    下载: 导出CSV

    表  2  合成气直接制芳烃反应的主要方程式

    Table  2  Main equations of direct aromatics production from syngas

    Reaction nameNumber of the reaction equationSerial number
    Total reaction$\left(n + 6\right){\rm{CO} } + \left(2n + 9\right){ {\rm{H} } }_{2}\to { {\rm{C} } }_{n + 6}{ {\rm{H} } }_{2n + 6} + \left(n + 6\right){ {\rm{H} } }_{2}{\rm{O}}\left(n > 0\right)$(1)
    Water vapor transformation reaction${\rm{CO}} + {{\rm{H}}}_{2}{\rm{O}}\to {\rm{C}}{{\rm{O}}}_{2} + {{\rm{H}}}_{2}$(2)
    Disproportionation$2{\rm{CO}}\to {\rm{C }}+ {\rm{C}}{{\rm{O}}}_{2}$(3)
    Methanation${\rm{CO}} + 3{{\rm{H}}}_{2}\to {\rm{C}}{{\rm{H}}}_{4} + {{\rm{H}}}_{2}{\rm{O}}$(4)
    Ethane reaction$2{\rm{CO}} + 6{{\rm{H}}}_{2}\to {{\rm{C}}}_{2}{{\rm{H}}}_{8} + 2{{\rm{H}}}_{2}{\rm{O}}$(5)
    Ethylene reaction$2{\rm{CO}} + 4{{\rm{H}}}_{2}\to {{\rm{C}}}_{2}{{\rm{H}}}_{4} + 2{{\rm{H}}}_{2}{\rm{O}}$(6)
    下载: 导出CSV
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出版历程
  • 收稿日期:  2022-05-25
  • 录用日期:  2022-07-14
  • 修回日期:  2022-07-13
  • 网络出版日期:  2022-08-11
  • 刊出日期:  2023-01-10

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