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分子筛结构设计及酸性调控在合成气催化转化中的应用研究进展

庹杰 李石擎 徐浩 关业军 吴鹏

庹杰, 李石擎, 徐浩, 关业军, 吴鹏. 分子筛结构设计及酸性调控在合成气催化转化中的应用研究进展[J]. 燃料化学学报(中英文), 2023, 51(1): 1-18. doi: 10.1016/S1872-5813(22)60035-5
引用本文: 庹杰, 李石擎, 徐浩, 关业军, 吴鹏. 分子筛结构设计及酸性调控在合成气催化转化中的应用研究进展[J]. 燃料化学学报(中英文), 2023, 51(1): 1-18. doi: 10.1016/S1872-5813(22)60035-5
TUO Jie, LI Shi-qing, XU Hao, GUAN Ye-jun, WU Peng. Research progress of structure design and acidity tuning of zeolites for the catalytic conversion of syngas[J]. Journal of Fuel Chemistry and Technology, 2023, 51(1): 1-18. doi: 10.1016/S1872-5813(22)60035-5
Citation: TUO Jie, LI Shi-qing, XU Hao, GUAN Ye-jun, WU Peng. Research progress of structure design and acidity tuning of zeolites for the catalytic conversion of syngas[J]. Journal of Fuel Chemistry and Technology, 2023, 51(1): 1-18. doi: 10.1016/S1872-5813(22)60035-5

分子筛结构设计及酸性调控在合成气催化转化中的应用研究进展

doi: 10.1016/S1872-5813(22)60035-5
基金项目: 国家自然科学基金 (21872052, 21972044, 21773067)和科技部重点研发计划(2016YFA0202804)资助
详细信息
    通讯作者:

    Tel: 021-62232292, Fax: 021-62232292, E-mail: yjguan@chem.ecnu.edu.cn

    pwu@chem.ecnu.edu.cn

  • 中图分类号: O643.36; TQ519

Research progress of structure design and acidity tuning of zeolites for the catalytic conversion of syngas

Funds: The project was supported by National Natural Science Foundation of China (21872052, 21972044, 21773067) and the Ministry of Science and Technology of the People’s Republic of China (2016YFA0202804).
  • 摘要: 合成气催化转化是生物质或煤炭资源化清洁利用的重要路径,由此可获得烯烃和芳烃等多种高附加值碳氢化合物。分子筛由于具有独特的亚纳米孔道、可控活性位及分子择形性等优点,常被作为载体或直接作为活性组分用于催化合成气转化中C−C的形成和断裂等关键步骤。本综述总结了以分子筛负载金属、氧化物-分子筛(OX-ZEO)双功能以及核壳结构催化剂等直接催化转化合成气制备碳氢化合物的研究进展。重点介绍分子筛结构和酸性对反应路径和机理以及产物分布的影响,并展望分子筛催化合成气转化的未来发展方向。
  • 图  1  合成气转化制低烯烃和芳烃等烃类的典型途径

    Figure  1  Typical routes for syngas conversion to lower olefins, aromatics and various hydrocarbons

    图  2  费托合成产物分布ASF模型[2]

    Figure  2  ASF model of Fischer-Tropsch synthesis[2](with permission from RSC Publications)

    图  3  合成气通过Co/ASB直接合成异构烷烃的反应机理[19]

    Figure  3  Reaction mechanism of the direct synthesis of isoparaffins from syngas over Co/ASB[19](with permission from ACS Publications)

    图  4  Co/Ymeso催化剂合成气转化催化性能[28]

    Figure  4  Catalytic performance of Co/Ymeso in the transformation of syngas[28](a) FTS with conventional supports or Ymeso zeolites. Detailed product distribution over the Ymeso catalysts modified by different elements: (b) Co/Ymeso-Ce, (c) Co/Ymeso-La and (d) Co/Ymeso-K(with permission from Springer Nature)

    图  5  合成气转化OX-ZEO双功能催化剂

    Figure  5  Syngas conversion with the OX-ZEO bifunctional catalyst systems

    图  6  分子筛骨架结构示意图

    Figure  6  Framework structures of (a) Y, (b) MFI, and (c) CHA zeolites

    图  7  拓扑结构对双循环传播的影响[64]

    Figure  7  Impact of zeolite topology on the propagation of olefin- and aromatic-based cycles for the conversion of methanol to hydrocarbons (MTH) ((a), (b)): 8 MR zeolites, composed of large cavities with small window openings; ((c), (d)): 1D 10 MR zeolites; ((e), (f)): 3D 10 MR MFI zeolite; ((g), (h)): 1D 12 MR zeolite[64](with permission from Springer Nature)

    图  8  ZnAlOx/SAPO中SAPO分子筛的窗口尺寸对合成气转化反应的影响[65]

    Figure  8  Effect of window size of SAPO zeolites on the performance of related bifunctional ZnAlOx /SAPO catalysts in the syngas conversion[65](with permission from Elsevier)

    图  9  ZnAlOx/SAPO 催化合成气转化反应中,SAPO分子筛(8 MR)笼的大小对反应的影响[65]

    Figure  9  Effect of cage size of SAPO zeolites with 8 MR windows on the performance of related bifunctional ZnAlOx/SAPO catalysts in the syngas conversion[65](with permission from Elsevier)

    图  10  MOR分子筛不同酸位对合成气、乙烯酮、甲醇转化反应的影响[53]

    Figure  10  Hydrocarbon distributions in the conversion of syngas, ketene and methanol over different sites of MOR zeolites at 648 K (a)−(c): 8 MR acid sites; (d)−(f): 12 MR acid sites; (g)−(i): both the 8 MR and 12 MR acid sites; ((a), (d), (g)): syngas over ZnCrOx-MOR; ((b), (e), (h)); ketene conversion over MOR; ((c), (f), (i)): methanol conversion over MOR[53](with permission from Wiley)

    图  11  ZnCrOx-ZSM-5催化合成气制芳烃b/a取向长度比值对芳烃和C6+脂肪烃类分布的影响[51]

    Figure  11  Syngas to aromatics over ZnCrOx-ZSM-5 Distributions of aromatics and C6+ aliphatics in C6+ hydrocarbons as a function of the length ratio of the b/a axes[51](with permission from Elsevier)

    图  12  酸性对双循环传播过程的影响[64]

    Figure  12  Impact of acidity on the propagation of two cycles in MTH. dependence of selectivity to ${\rm{C}}_{3}^{{=}}$ (a) and aromatics (b) on the Si/Al ratio for the ZSM-5 zeolites summarized from literatures; the reaction process in the zeolite with low (c) and high (d) density of Brønsted acid site (BAS)[64](with permission from Springer Nature)

    图  13  ZnCrOx-SAPO-18双功能催化剂催化合成气转化的催化性能与硅铝比的关系[44]

    Figure  13  Performance of the bifunctional ZnCrOx -SAPO-18 catalyst in syngas conversion as a function of the Si/Al ratio[44] (a): CO conversion and selectivity; (b): ratio of C3/C2 and olefins to paraffins (O/P) (with permission from American Chemical Society)

    图  14  B酸位点密度对双功能Zn-ZrO2/SSZ-13催化剂催化行为的影响[34]

    Figure  14  Effect of density of Brønsted acid sites on the catalytic behaviors of the bifunctional Zn-ZrO2/SSZ-13 catalyst in syngas conversion[34](with permission from RSC Publications)

    图  15  Co/Al2O3/H-beta核壳催化剂[87]

    Figure  15  Core/shell catalyst of Co/Al2O3/H-beta[87](with permission from Wiley Publications)

    图  16  Na-Zn-Fe5C2@ H-ZSM-5催化剂合成气制备芳烃的机理示意图[93]

    Figure  16  Proposed scheme for direct production of aromatics from syngas on Na-Zn-Fe5C2@ H-ZSM-5 catalyst[93]

    表  1  FTS反应的代表性金属负载催化剂

    Table  1  Representative metal loaded catalysts of FTS reaction

    CatalystT/Kp/MPaGHSV
    /(mL·g−1·h−1)
    H2/COCO
    conv. /%
    CO2 sel. /%Main product /%Ref.
    mBulk Fe613215001973432a (0.57b)[8]
    Fe/α-Al2O3804053a (8.48b)
    Fe/CNF884252a (2.98b)
    Fe3O45931.530002974435a[9]
    Fe3O4@SiO2342330a
    Fe/PANI623190002794447a[11]
    Co/SiO25032240013760d (0.3c)[18]
    Co/Al2O33956d (0.5c)
    Co/H-Y3672d (3.2c)
    Co/H-meso-Y4079d (2.7c)
    Co/SiO2513122402200.07c[19]
    Co/Beta302.43c
    Co/ASB361.50c
    Ru/SiO25332240013225e (0.42c)[16]
    Ru/Al2O34022e (0.53c)
    Ru/TiO22026e (1.1c)
    Ru/H-Mordenite3152e (1.8c)
    Ru/H-Beta2458e (3.3c)
    Ru/H-MCM-222254e (4.1c)
    Ru/H-ZSM-52547e (2.7c)
    Co/H-meso-ZSM-5-0.5M5132240024270e (2.3b)[20]
    10%Fe/HZSM-5593240001815027 (60)[21]
    25%Fe/HZSM-5855031 (70)
    a: Selectivity to ${\rm{C} }_{ {\rm{2-4} } }^{\rm{=} } $; b: FTY; c: Molar ratio of isoparaffins to n-paraffins; d: Selectivity to C5−20; e: Selectivity to C5−11;
    f: Aromatics selectivity in C5+ hydrocarbons
    下载: 导出CSV

    表  2  合成气催化转化代表性OX-ZEO双功能催化剂

    Table  2  Representative OX-ZEO bifunctional catalysts of syngas catalytic conversion

    Zeolite
    topology
    ZeoliteOxideT/Kp/MPaGHSV/
    (mL·g−1·h−1)
    H2/COCO
    conv. /%
    CO2
    sel. /%
    Main product /%Ref.
    ${\boldsymbol{ {\rm{C} } } }_{2-4}^{\rm{=} }$C5+
    CHA
    (3D, 8 MR)
    SAPO-34 ZnCrOx 673 3.5 4800 2.5 17 41 80 [34]
    SAPO-34 ZnO-ZrO2 673 1 3600 2 7 43 69 2 [34]
    SAPO-34 ZnAlOx 663 4 12000 1 7 33 78 4 [32]
    SAPO-34 MnOx 673 2.5 4800 2.5 7 43 79 5 [38]
    SAPO-34 ZnCeZrO4 573 1 5400 2 6 6 83 9 [40]
    SAPO-34 ZrCeZnOx 673 1 3900 2 13 45 82 3 [35]
    SAPO-34 MnGaOx 673 2.5 4875 2 14 45 88 2 [41]
    SAPO-34 ZnO 673 4 1600 2.5 32 42 77 5 [37]
    SAPO-34 Zr-In2O3 673 2.5 3600 1 28 40 74 2 [42]
    SSZ-13 Zn-ZrO2 673 3 3000 2 29 42 77 3 [34]
    BAl-CHA ZnAlOx 623 1 2400 2 10 43 83 [43]
    AEI
    (3D, 8 MR)
    SAPO-18 ZnCrOx 673 4 5000 2.5 36 41 82 [44]
    AlPO-18 ZnCrOx 663 4 3600 1 25 48 87 9 [45]
    AEL
    (1D 10 MR)
    SAPO-11 Zn2Mn1Ox 633 4 1000 1 20 77a [46]
    TON
    (1D 10 MR)
    ZSM-22 Zn2Mn1Ox 633 4 1000 1 19 64a [46]
    MTW
    (1D 12 MR)
    ZSM-12 Zn2Mn1Ox 633 4 1000 1 21 70a [46]
    MFI
    (3D 10 MR)
    ZSM-5 Zn2Mn1Ox 633 4 1000 1 23 67a [46]
    ZSM-5 CeZrO2 653 2 600 1 8 32.9 83b [47]
    ZSM-5 Mo-ZrO2 673 4 3000 2 22 76b [48]
    ZSM-5 MnO 623 2 333 2 21 83b [49]
    ZSM-5 ZnCrOx 623 4 1500 1 16 74b [50]
    ZSM-5 ZnCrOx 623 4 1500 1 18 49 69b [51]
    ZSM-5 1Zn-3Cr 668 2 4000 1 11 72b [52]
    MEL
    (3D 10 MR)
    ZSM-11 Zn2Mn1Ox 633 4 1000 1 23 64a [46]
    MOR
    (3D, 8 MR &12 MR)
    MOR ZnCrOx 633 2 1600 1 26 48 91 5 [53]
    MOR ZnAl2O4 643 3 1500 1 10 44 77 6 [54]
    a: Selectivity of C5–11 b: Aromatics
    下载: 导出CSV
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  • 收稿日期:  2022-04-30
  • 修回日期:  2022-05-12
  • 录用日期:  2022-05-19
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