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合成气催化转化直接制备低碳烯烃研究进展

于飞 李正甲 安芸蕾 高鹏 钟良枢 孙予罕

于飞, 李正甲, 安芸蕾, 高鹏, 钟良枢, 孙予罕. 合成气催化转化直接制备低碳烯烃研究进展[J]. 燃料化学学报, 2016, 44(7): 801-814.
引用本文: 于飞, 李正甲, 安芸蕾, 高鹏, 钟良枢, 孙予罕. 合成气催化转化直接制备低碳烯烃研究进展[J]. 燃料化学学报, 2016, 44(7): 801-814.
YU Fei, LI Zheng-jia, AN Yun-lei, GAO Peng, ZHONG Liang-shu, SUN Yu-han. Research progress in the direct conversion of syngas to lower olefins[J]. Journal of Fuel Chemistry and Technology, 2016, 44(7): 801-814.
Citation: YU Fei, LI Zheng-jia, AN Yun-lei, GAO Peng, ZHONG Liang-shu, SUN Yu-han. Research progress in the direct conversion of syngas to lower olefins[J]. Journal of Fuel Chemistry and Technology, 2016, 44(7): 801-814.

合成气催化转化直接制备低碳烯烃研究进展

基金项目: 

国家自然科学基金 21403278

国家自然科学基金 21573271

国家自然科学基金 91545112

上海市科委项目 15DZ1170500

详细信息
    通讯作者:

    钟良枢, Tel: +86-021-20608002; Fax: +86-021-20325034; E-mail: zhongls@sari.ac.cn

    孙予罕, Tel: +86-021-20325009; Fax: +86-021-20325039; E-mail: sunyh@sari.ac.cn

  • 中图分类号: Q643;TQ519

Research progress in the direct conversion of syngas to lower olefins

Funds: 

The project was supported by the National Natural Science Foundation of China 21403278

The project was supported by the National Natural Science Foundation of China 21573271

The project was supported by the National Natural Science Foundation of China 91545112

Shanghai Municipal Science and Technology Commission, China 15DZ1170500

More Information
    Corresponding author: ZHONG Liang-shu, Tel: +86-021-20608002; Fax: +86-021-20325034; E-mail: zhongls@sari.ac.cnSUN Yu-han, Tel: +86-021-20325009; Fax: +86-021-20325039; E-mail: sunyh@sari.ac.cn
  • 摘要: 合成气直接催化转化制备低碳烯烃是C1化学与化工领域中一个极具挑战性的研究课题, 具有流程短、能耗低等优势, 已成为非石油路径生产烯烃的新途径。直接转化方式主要包括经由OX-ZEO双功能催化剂直接制低碳烯烃的双功能催化路线以及经由费托反应直接制备低碳烯烃的FTO路线。综述简述了近年来在合成气直接制备低碳烯烃方面的研究进展, 重点讨论了低碳烯烃的形成机理、新型催化剂的研发及助剂对其催化性能的影响, 并对合成气直接制烯烃的未来进行了展望。
  • 图  1  合成气转化制备低碳烯烃路径示意图

    Figure  1.  Various routes for the production of lower olefins via syngas

    图  2  Zr-Zn氧化物与SAPO-34分子筛不同结合方式对反应性的影响[14]

    Figure  2.  Effect of integration manner on the catalytic behaviors of the composite catalysts containing Zr-Zn (Zr/Zn=2:1) oxide and SAPO-34

    (a): dual-bed configuration; (b): stacking of granules with sizes of 250-600 mm; (c): simple mixing of the two components in an agate mortar; (d): ball-milling of two components together for 24 h the o/p ratio denotes the ratio of C2-4 olefin/paraffin[14]

    图  3  OX-ZEO双功能催化剂的催化性能[5]

    Figure  3.  Performance of the bifunctional OX-ZEO catalyst in the conversion of syngas to olefins[5] (a) CO conversion and product distribution at different H2/CO volume ratios over ZnCrOx/MSAPO; (b) hydrocarbon distribution over OX-ZEO in comparison with that reported for FTTO and that in FTS predicted by the ASF model at a chain growth probability of 0.46; (c) stability test of the ZnCrOx/MSAPO catalyst[5] FTTO or FTO, Fischer-Tropsch to olefin

    图  4  OX-ZEO双功能催化剂的反应过程示意图[15]

    Figure  4.  Reaction scheme for the syngas to olefins over the bifunctional OX-ZEO catalyst[15]

    图  5  ASF模型预测得到费托合成产物分布曲线

    Figure  5.  Product distribution predicted on the basis of Anderson-Schulz-Flory (ASF) model

    图  6  碳化物机理[22]

    Figure  6.  Carbide mechanism for FT synthesis[22]

    图  7  Fe基催化剂积炭测试[59]

    Figure  7.  Carbon lay-down measurements for the iron-based catalysts[59]

    the Fischer-Tropsch reaction was carried out at 350 ℃, 2.0×106 Pa, H2/CO (volume ratio)=1, and GHSV=180 000 h-1

    图  8  (a) Mn/Fe3O4结构模型;(b) Fe3O4微球的扫描电镜照片;(c) 还原后Mn/Fe3O4催化剂的TEM照片;(d) Mn/Fe3O4催化剂的STEM照片;(e) 相应的STEM-EDX元素分析[79]

    Figure  8.  (a) Structural model for the Mn/Fe3O4 catalyst; (b) SEM images of the Fe3O4 microspheres; (c) TEM images of theMn/Fe3O4 catalyst after reduction; (d) original STEM image of Mn/Fe3O4 catalyst as prepared; (e) corresponding STEM-EDX elemental mapping of Fe, O and Mn on the catalyst[79]

    图  9  高比表面积载体可提高Fe基纳米颗粒的稳定性[2]

    Figure  9.  Stabilization of iron-based nanoparticles by using catalyst support with high specific surface area[2]

    图  10  负载量为10%的Fe/NCNTs (a,b)、Fe/t-CNTs (c)、Fe/u-CNTs (d) 的TEM以及HRTEM照片,内嵌图为粒径分布柱状图[96]

    Figure  10.  TEM and HRTEM images of activated catalysts with an Fe loading of 10%[96]

    (a, b) Fe/NCNTs; (c) Fe/t-CNTs; (d) Fe/u-CNTs the insets in (a) and (c) are the corresponding particle size distributions

    表  1  S和Na对负载铁催化剂性能的影响[59]

    Table  1.   Effect of S and Na promoters on the catalytic performance of supported iorn catalysts in FT synthesis[59]

    Catalyst Fischer-Tropsch yield/(10-5 molCO·gFe-1·s-1) Product selectivity s/%
    CH4 C2-4 olefins C2-4 paraffins C5+
    Fe/Al2O3 0.14 54 42 3 2
    Fe/Al2O3 + 0.2% Na 0.08 50 43 5 3
    Fe/Al2O3 + 0.03% S 1.70 33 58 3 5
    Fe/Al2O3 + 0.2% Na + 0.03% S 0.57 15 64 2 19
    Fe/Al2O3 + 0.4% Na + 0.03% S 0.16 23 51 3 22
    Fe 0.02 78 13 2 7
    Fe + 0.4% Na + 0.4% S 0.30 21 60 3 16
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  • 收稿日期:  2016-03-28
  • 修回日期:  2016-04-13
  • 网络出版日期:  2021-01-23
  • 刊出日期:  2016-07-10

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