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合成气一步法制备低碳烯烃和液体燃料催化剂研究进展

刘赛赛 姚金刚 陈冠益 易维明 颜蓓蓓 刘静 张庆文 朱磊

刘赛赛, 姚金刚, 陈冠益, 易维明, 颜蓓蓓, 刘静, 张庆文, 朱磊. 合成气一步法制备低碳烯烃和液体燃料催化剂研究进展[J]. 燃料化学学报(中英文), 2023, 51(1): 34-51. doi: 10.19906/j.cnki.JFCT.2022055
引用本文: 刘赛赛, 姚金刚, 陈冠益, 易维明, 颜蓓蓓, 刘静, 张庆文, 朱磊. 合成气一步法制备低碳烯烃和液体燃料催化剂研究进展[J]. 燃料化学学报(中英文), 2023, 51(1): 34-51. doi: 10.19906/j.cnki.JFCT.2022055
LIU Sai-sai, YAO Jin-gang, CHEN Guan-yi, YI Wei-ming, YAN Bei-bei, LIU Jing, ZHANG Qing-wen, ZHU Lei. One-step catalyst for the preparation of light olefins and liquid fuels from syngas[J]. Journal of Fuel Chemistry and Technology, 2023, 51(1): 34-51. doi: 10.19906/j.cnki.JFCT.2022055
Citation: LIU Sai-sai, YAO Jin-gang, CHEN Guan-yi, YI Wei-ming, YAN Bei-bei, LIU Jing, ZHANG Qing-wen, ZHU Lei. One-step catalyst for the preparation of light olefins and liquid fuels from syngas[J]. Journal of Fuel Chemistry and Technology, 2023, 51(1): 34-51. doi: 10.19906/j.cnki.JFCT.2022055

合成气一步法制备低碳烯烃和液体燃料催化剂研究进展

doi: 10.19906/j.cnki.JFCT.2022055
基金项目: 山东省自然科学基金(ZR2020QE205),国家自然科学基金(52006129,51906129)和广东省新能源和可再生能源研究开发与应用重点实验室(E039kf0701,E239kf0401)资助
详细信息
    通讯作者:

    Tel:15695431959,E-mail: yaojingang@sdut.edu.cn

    ljing815@tju.edu.cn

  • 中图分类号: O643.3

One-step catalyst for the preparation of light olefins and liquid fuels from syngas

Funds: The project was supported by the Shandong Provincial Natural Science Foundation (ZR2020QE205), National Natural Science Foundation of China (52006129, 51906129) and Guangdong Provincial Key Laboratory of New and Renewable Energy Research and Development (E039kf0701, E239kf0401).
  • 摘要: 以合成气作为平台化合物一步法制备低碳烯烃和液体燃料是有效利用碳资源的重要路径,具备流程短、能耗低的特点,有着良好的工业应用前景。合成气一步法直接转化制备低碳烯烃和液体燃料包括两条工艺路线:费托合成路线和双功能催化路线。本综述简述了两种路线的反应机理,重点阐述了费托合成路线中采用添加助剂和惰性载体对铁基和钴基催化剂的优化设计,费托金属粒径、反应条件、催化剂界面结构对催化剂性能和反应过程的影响。详细解析了双功能催化路线中,一氧化碳活化组分和酸性分子筛的选择、金属氧化物粒径与元素比例、分子筛酸度与孔径大小以及一氧化碳活化组分和酸性分子筛的耦合方式对于催化剂性能的影响。总结了两条路线所具备的优势和面临的挑战,并对未来高效催化剂的发展方向进行了展望。
  • 图  1  合成气转化制备低碳烯烃和液体燃料示意图

    Figure  1  Schematic diagram of syngas conversion to prepare light olefin and liquid fuel

    图  2  合成气经由二甲醚制汽油串联反应器[7]

    Figure  2  Syngas to gasoline via dimethyl ether tandem reactor[7](with permission from Elsevier)

    图  3  碳化物机理示意图[14]

    Figure  3  Carbide mechanism diagram[14](with permission from Elsevier)

    图  4  ASF分布图[5]

    Figure  4  ASF distribution[5]

    图  5  不同Zn-ZrO2比例催化剂CO转化率及产物选择性[80]

    Figure  5  CO conversion and product selectivity of different Zn-ZrO2 ratio catalysts[80](with permission from RSC Publication)

    图  6  Brønsted酸性位点密度对CO转化率及产物选择性的影响[80]

    Figure  6  Effect of Brønsted acidic site density on CO conversion and product selectivity[80](with permission from RSC Publication)

    图  7  两种组分邻近程度对反应的影响[80]

    Figure  7  Effect of the degree of contact between the two components on the reaction[80](with permission from RSC Publication)

    图  8  核壳结构催化剂[89]

    Figure  8  Core-shell structure catalyst[89](with permission from Spring Nature Publication)

    表  1  费托合成反应

    Table  1  Fischer-Tropsch synthesis reaction

    Reaction typeReaction nameReaction equation
    Main reactionparaffin formation$n{\rm{CO}} + \left(2n + 1\right){{\rm{H}}}_{2}\to {{\rm{C}}}_{n}{{\rm{H}}}_{2n + 2} + n{{\rm{H}}}_{2}{\rm{O}}$
    olefin formation$n{\rm{CO}} + 2n{{\rm{H}}}_{2}\to {{\rm{C}}}_{n}{{\rm{H}}}_{2n} + n{{\rm{H}}}_{2}{\rm{O}}$
    water-gas shift reaction${\rm{CO}} + {{\rm{H}}}_{2}{\rm{O}}\rightleftharpoons {\rm{C}}{{\rm{O}}}_{2} + {{\rm{H}}}_{2}$
    Side reactionalcohol formation$n{\rm{CO}} + 2n{{\rm{H}}}_{2}\to {{\rm{C}}}_{n}{{\rm{H}}}_{2n + 1}{\rm{O}} + \left(n + 1\right){{\rm{H}}}_{2}{\rm{O}}$
    boudard reaction$2{\rm{CO}}\rightleftharpoons {\rm{C}} + {\rm{C}}{\rm{{O}}}_{2}$
    下载: 导出CSV

    表  2  不同CO活化组分与酸性分子筛相结合的双功能催化剂

    Table  2  Bifunctional catalysts with different CO activated components combined with acidic molecular sieves

    CO activation
    components
    ZeoliteCO conv./%Selectivity of hydrocarbonsm/%Reference
    CH4${\rm{C}}_{2}^=-{\rm{C}}_{4}^= $${\rm{C}}_{2}^{0}-{\rm{C}}_{4}^{0}$C5 +
    Rumeso-ZSM-529.6a5.979.0[69]
    Comeso-ZSM-543.0a7.770.0[70]
    FeZSM-548.0a27.051.0[71]
    CoZSM-529.0b15.053.0[72]
    MnOxSAPO-348.5c2.079.212.9[73]
    ZnCrOxSAPO-3417.0d2.080.014.04.0[74]
    Zn-CrSAPO-3430.0e16.038.045.0[67]
    Zn-Al2O3SAPO-344.5f10.477.012.60[68]
    Zn-Cr2O3SAPO-341.8f16.037.246.80[68]
    Zn-ZrO2SAPO-345.3f30.211.258.60[68]
    Zn-CeO2SAPO-342.1f34.455.89.80[68]
    Zr-ZnSAPO-347.5g11.037.048.03.2[75]
    MgAl2O4SAPO-341.0h9.962.033.00.1[76]
    MgGa2O4SAPO-346.8h6.568.018.07.7[76]
    MgCr2O4SAPO-344.2h4.462.033.00.1[76]
    Mn-GaSAPO-3414.0i2.088.08.02.0[77]
    ZnxCe2-yZryO4SAPO-346.0j5.083.04.09.0[78]
    ZnO-ZrO2SAPO-347.0k4.069.025.02.0[79]
    ZnGa2O4SAPO-3430.0l5.077.017.02.0[80]
    a: H2/CO=1.0,360 ℃,2.0 MPa,GHSV=2400 mL/(h·gcat);b: H2/CO=1.0,280 ℃,2.1 MPa,GHSV=1153 mL/(h·gcat);c: H2/CO=2.5, 400 ℃,2.5 MPa,GHSV=4800 mL/(h·gcat);d: H2/CO=2.5,400 ℃,2.5 MPa,GHSV=7714 mL/(h·gcat);e: H2/CO=1.0,400 ℃,2.0 MPa,GHSV=1125 mL/(h·gcat);f: H2/CO=1.0,390 ℃,4.0 MPa,GHSV=1800 mL/(h·gcat);g: H2/CO=2.0,360 ℃,1.0 MPa,GHSV=3600 mL/(h·gcat);h: H2/CO=2.0,400 ℃,3.0 MPa,GHSV=1800 mL/(h·gcat);i: H2/CO=2.0,400 ℃,2.5 MPa,GHSV=4875 mL/(h·gcat);j: H2/CO=2.0,300 ℃,1.0 MPa,GHSV=5400 mL/(h·gcat);k: H2/CO=1.0,360 ℃,2.0 MPa,GHSV=1600 mL/(h·gcat);l: H2/CO=2.0,400 ℃,3.0 MPa,GHSV=3600 mL/(h·gcat);m:Product obtained based on C mole calculations, excluding CO2
    下载: 导出CSV

    表  3  不同比例金属元素与酸性分子筛相结合的双功能催化剂

    Table  3  Bifunctional catalysts with different ratios of metal elements combined with acidic molecular sieves

    Metal oxides (scale)ZeoliteCO conv./%Selectivity of hydrocarbonsc/%Reference
    CH4${\rm{C} }_{2}^= - {\rm{C} }_{4}^=$${\rm{C} }_{2}^{0} - {\rm{C} }_{4}^{0}$C5 +
    ZnOSAPO-343.3a43.08.14.90[75]
    Zr-Zn(1∶1)SAPO-347.5a11.037.048.03.2[75]
    Zr-Zn(2∶1)SAPO-349.5a6.063.029.02.2[75]
    Zr-Zn(4∶1)SAPO-346.8a4.269.025.02.1[75]
    ZrO2SAPO-341.0a4.090.05.51.1[75]
    ZrO2SSZ-133.9a2.080.010.08.0[80]
    Zn-ZrO2(1∶64)SSZ-1318.0b1.875.22.010.0[80]
    Zn-ZrO2(1∶32)SSZ-1321.0b2.074.04.010.0[80]
    Zn-ZrO2(1∶16)SSZ-1323.0b2.075.04.09.0[80]
    Zn-ZrO2(1∶4)SSZ-1326.0b2.066.021.011.0[80]
    Zn-ZrO2(1∶1)SSZ-1328.0b3.059.020.018.0[80]
    Zn-ZrO2(2∶1)SSZ-1328.0b4.054.026.016.0[80]
    Zn-ZrO2(4∶1)SSZ-1322.0b5.035.044.016.0[80]
    ZnOSSZ-136.0b8.024.058.010.0[80]
    a: H2/CO=2,360 ℃,1.0 MPa,GHSV=3600 mL/(h·gcat);b: H2/CO=2,400 ℃,3.0 MPa,GHSV=2700 mL/(h·gcat);c Product obtained based on C mole calculations, excluding CO2
    下载: 导出CSV

    表  4  CO活化组分粒径对反应的影响

    Table  4  Effect of CO activation component particle size on the reaction

    CO activation
    component
    Particle size/ nmZeoliteCO conv.
    /%
    CO2 sel.
    /%
    Selectivity of hydrocarbonsc/%Reference
    CH4${\rm{C}}_{2}^= - {\rm{C}}_{4}^= $${\rm{C}}_{2}^{0} - {\rm{C}}_{4}^{0} $C5–C9C10–C20
    Co4.9Na-meso-Y40.0a12.029.045.0[64]
    Co6.5Na-meso-Y38.0a5.027.047.0[64]
    Co8.4Na-meso-Y34.0a5.018.060.0[64]
    Co14.0Na-meso-Y39.0a5.018.552.0[64]
    Co20.0Na-meso-Y36.0a4.518.351.0[64]
    Co27.0Na-meso-Y30.0a4.018.048.0[64]
    ZnO23.0SAPO-3431.9b42.03.176.715.5[81]
    ZnO24.0SAPO-3433.2b41.03.076.515.9[81]
    ZnO25.0SAPO-3433.5b41.02.976.116.4[81]
    ZnO33.0SAPO-3429.7b41.02.675.617.4[81]
    ZnO40.0SAPO-3424.4b41.02.574.318.9[81]
    ZnO53.0SAPO-3417.4b40.02.467.024.8[81]
    ZnO62.0SAPO-3411.8b37.02.760.030.1[81]
    ZnO79.0SAPO-346.5b32.02.461.028.6[81]
    a: Co/zeolite=0.15∶1 (mass ratio),H2/CO=1,230 ℃,2.0 MPa,GHSV=1800 mL/(h·gcat);b: ZnO/zeolite =2∶1 (mass ratio),H2/CO=2.5,400 ℃,4 MPa,GHSV =1600 mL/(h·gcat);c Product obtained based on C mole calculations, excluding CO2
    下载: 导出CSV

    表  5  双功能催化剂中分子筛结构对合成气催化转化的影响

    Table  5  Effect of zeolite structure in bifunctional catalysts on the catalytic conversion of syngas

    CO activation
    component
    ZeoliteTopologyOrifice structureCO conv.
    /%
    CO2 sel.
    /%
    Selectivity of hydrocarbonsh/%Reference
    CH4${\rm{C}}_{2}^= - {\rm{C}}_{4}^= $${\rm{C}}_{2}^{0} - {\rm{C}}_{4}^{0} $C5 + ${\rm{C}}_{5} - {\rm{C}}_{11}$
    CoSSZ-13CHA3D 8-MR27.4a17.571.1[83]
    CoZSM-22TON1D 10-MR5.0a32.548.5[83]
    CoZSM-11MEL3D 10-MR54.8a15.472.7[83]
    CoZSM-5MFI3D 10-MR56.7a15.671.7[83]
    CoYFAU3D12-MR50.6a15.972.3[83]
    CoMORMOR2D 8&12-MR29.5a14.376.3[83]
    Zn2MnOxZSM-35FER2D 8&10-MR23.0 b48.720.311.7[82]
    Zn2MnOxSAPO-11AEL1D 10-MR20.3b50.02.376.7[82]
    Zn2MnOxZSM-22TON1D 10-MR19.3b48.74.264.2[82]
    Zn2MnOxZSM-12MTW1D 12-MR20.7b48.52.170.2[82]
    Zn2MnOxZSM-5MFI3D 10-MR22.9b48.92.067.4[82]
    Zn2MnOxZSM-11MEL3D 10-MR22.6b48.91.863.5[82]
    Zn-ZrO2ZSM-5MFI3D 10-MR9.3 c39.01.92.913.01.0[66]
    Zn-ZrO2BetaBEA3D12-MR7.5 c41.07.513.073.01.8[66]
    Zn-ZrO2MORMOR2D 8&12-MR9.2c40.09.243.026.04.3[66]
    Zn-ZrO2SAPO-34CHA3D 8-MR7.4 c40.07.461.029.05.5[66]
    Zn-ZrO2SSZ-13CHA3D 8-MR29.0d42.02.077.018.03.0[80]
    ZnCrOxSAPO-34CHA3D 8-MR17.0e41.02.080.014.04.0[74]
    ZnCrOxMORMOR2D 8&12-MR9.0e5.089.05.50.5[73]
    ZnAl2O4SAPO-34CHA3D 8-MR6.9f33.15.577.014.5[84]
    ZnAl2O4MORMOR2D 8&12-MR10.0g44.05.277.012.0[85]
    a: H2/CO=2.0,240 ℃,2.5 MPa,GHSV=7714 mL/(h·gcat);b: H2/CO=1.0,360 ℃,4.0 MPa,GHSV=1000 mL/(h·gcat);c: H2/CO=2.0,400 ℃,3.0 MPa,GHSV=1500 mL/(h·gcat);d: H2/CO=2.0,400 ℃,3.0 MPa,GHSV=2700 mL/(h·gcat);e: H2/CO=2.5,400 ℃,2.0 MPa,GHSV=4000 mL/(h·gcat);f: H2/CO=1.0,390 ℃,4.0 MPa,GHSV=12000 mL/(h·gcat);g: H2/CO=1.0,330 ℃,3.0 MPa,GHSV=1500 mL/(h·gcat);h Product obtained based on C mole calculations, excluding CO2
    下载: 导出CSV
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  • 收稿日期:  2022-05-23
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