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钾掺杂对Fe/GO催化合成气制α-烯烃的影响

李玉峰 杨鹏举 姜枫 刘冰 胥月兵 刘小浩

李玉峰, 杨鹏举, 姜枫, 刘冰, 胥月兵, 刘小浩. 钾掺杂对Fe/GO催化合成气制α-烯烃的影响[J]. 燃料化学学报(中英文), 2021, 49(7): 933-944. doi: 10.1016/S1872-5813(21)60063-4
引用本文: 李玉峰, 杨鹏举, 姜枫, 刘冰, 胥月兵, 刘小浩. 钾掺杂对Fe/GO催化合成气制α-烯烃的影响[J]. 燃料化学学报(中英文), 2021, 49(7): 933-944. doi: 10.1016/S1872-5813(21)60063-4
LI Yu-feng, YANG Peng-ju, JIANG Feng, LIU Bing, XU Yue-bing, LIU Xiao-hao. Effect of potassium on GO-modified large Fe3O4 microspheres for the production of α-olefins[J]. Journal of Fuel Chemistry and Technology, 2021, 49(7): 933-944. doi: 10.1016/S1872-5813(21)60063-4
Citation: LI Yu-feng, YANG Peng-ju, JIANG Feng, LIU Bing, XU Yue-bing, LIU Xiao-hao. Effect of potassium on GO-modified large Fe3O4 microspheres for the production of α-olefins[J]. Journal of Fuel Chemistry and Technology, 2021, 49(7): 933-944. doi: 10.1016/S1872-5813(21)60063-4

钾掺杂对Fe/GO催化合成气制α-烯烃的影响

doi: 10.1016/S1872-5813(21)60063-4
详细信息
    作者简介:

    李玉峰:1154369775@qq.com

    通讯作者:

    E-mail: liuxh@jiangnan.edu.cn

  • 中图分类号: O643

Effect of potassium on GO-modified large Fe3O4 microspheres for the production of α-olefins

  • 摘要: 铁基催化剂在费托合成反应中对高附加值α-烯烃具有高选择性,然而,催化剂容易由于碳沉积而失活,并且高CO2选择性明显降低了合成气的碳利用效率。为此,本文开发了一种简单有效的铁基催化剂制备方法来解决这一问题。具体地说,采用水热法制备了平均粒径约580 nm Fe3O4微球,并将其与GO在溶液中超声混合,离心、干燥后即得到Fe/GO催化剂。GO引入能使大的Fe3O4微球在反应过程中逐渐演变成小尺寸碳化铁纳米粒子(约9.1 nm),有效地抑制了催化剂的烧结和积炭。催化剂显示了优异的活性、稳定性和高α-烯烃选择性。表征结果表明,K加入到Fe3O4微球中,催化剂在演变过程中形成了更高的ε′-Fe2.2C含量(约为58.9%),有利于显著降低CO2选择性。
  • FIG. 799.  FIG. 799.

    FIG. 799.  FIG. 799.

    图  1  催化剂的XRD谱图

    Figure  1  XRD patterns of the various fresh catalysts

    图  2  新鲜催化剂的N2吸附-脱附曲线(a)及相应的孔径分布(b)

    Figure  2  N2 adsorption-desorption isotherms (a) and corresponding pore size distribution curves (b)

    图  3  新鲜催化剂的SEM照片

    Figure  3  SEM images of the fresh catalysts

    图  4  新鲜催化剂拉曼光谱(a)和CO-TPD谱图(b)

    Figure  4  Raman spectra (a) and CO-TPD (b) of the fresh catalysts

    图  5  催化剂的H2-TPR谱图

    Figure  5  H2-TPR profiles of catalysts

    图  6  新鲜和反应后催化剂的TEM照片

    Figure  6  TEM images of the fresh and spent catalysts

    图  7  反应后催化剂的XRD谱图

    Figure  7  XRD patterns of the spent catalysts

    图  8  Fe3O4和Fe/GO的催化性能

    Figure  8  Catalytic performances of Fe3O4 and Fe/GO catalysts

    Reaction conditions: 0.1 g of catalyst, 1 MPa, H2/CO/N2 = 48.5∶48.5∶3, GHSV = 22.2 L/(gcat·h), 340 ℃

    图  9  反应的碳数分布

    Figure  9  Carbon number distribution (catalysts and reaction conditions are same as shown in Figure 8)

    图  10  H2/CO比对0.4KFe/GO催化FTS反应的影响

    Figure  10  Effects of the H2/CO ratio on FTS over 0.4KFe/GO catalyst

    Reaction conditions: 0.1 g of catalyst, 1 MPa, GHSV = 22.2 L/(gcat·h), 340 ℃

    图  11  反应的碳数分布(催化剂和反应条件同图10

    Figure  11  Carbon number distribution (catalysts and reaction conditions are same as shown in Figure 10)

    表  1  新鲜催化剂的H2-TPR表征

    Table  1  H2-TPR results of the fresh catalysts

    SampleTotal H2 consumption/
    (mmol·$ {\rm{g}}^{-1}_ {\rm{cat} } $)
    Reduction
    degree/%
    Fe3O421.984.1
    Fe/GO8.475.3
    0.4KFe/GO9.282.3
    0.8KFe/GO9.180.2
    下载: 导出CSV

    表  2  反应后催化剂的穆斯堡尔光谱

    Table  2  Mössbauer spectra of the spent catalysts

    CatalystH(KOe)IS/(mm·s−1)QS/(mm·s−1)Г/2/(mm·s−1)Phase ascriptionArea/%
    Fe3O42160.25−0.110.18χ-Fe5C2(Ⅰ)39.3
    1860.18−0.060.23χ-Fe5C2(Ⅱ)44.1
    1110.21−0.110.16χ-Fe5C2(Ⅲ)16.5
    Fe/GO0.501.070.68Fe(Ⅱ)/Fe(Ⅲ)16.1
    1690.38−0.110.15ε′-Fe2.2C44.8
    2190.40−0.060.20χ-Fe5C2(Ⅰ)15.0
    1820.380.060.22χ-Fe5C2(Ⅱ)19.8
    1030.11−0.070.12χ-Fe5C2(Ⅲ)4.3
    0.4KFe/GO0.371.120.50Fe(Ⅱ)/Fe(Ⅲ)21.7
    1660.25−0.100.16ε′-Fe2.2C58.9
    2160.31−0.050.21χ-Fe5C2(Ⅰ)9.5
    1790.300.090.18χ-Fe5C2(Ⅱ)9.9
    0.8KFe/GO0.371.140.48Fe(Ⅱ)/Fe(Ⅲ)23.1
    1670.24−0.110.16ε′-Fe2.2C53.4
    2150.29−0.060.19χ-Fe5C2(Ⅰ)11.4
    1820.280.120.21χ-Fe5C2(Ⅱ)12.1
    下载: 导出CSV

    表  3  不同催化剂的FTS反应结果。

    Table  3  Catalytic performance of the FTS reactions over various catalysts

    CatalystxCO/%$ s_{{\rm{CO}}_{2}} $/%Hydrocarbon selectivity/%$ {\rm{C}}^{=}_{2-4} $/C2−4 (%)$ {\rm{C}}^{=}_{2+} $/C2+ (%)$ {\rm{C}}^{=}_{2+} $/(C1+C2+) (%)
    CH4$ {\rm{C}}^{=}_{2}-{{\rm{C}}^{=}_{4}} $$ {\rm{C}}^{\circ}_{2}-{\rm{C}}^{\circ}_{4} $C5+
    Fe3O4a8.542.730.121.42.645.989.284.659.1
    Fe/GOa83.645.88.030.74.756.786.986.679.7
    0.4KFe/GOa77.038.34.618.51.975.090.687.683.5
    0.8KFe/GOa68.742.25.619.62.372.589.587.282.3
    0.4KFe/GOb83.535.67.724.33.065.189.187.380.5
    0.4KFe/GOc80.131.69.830.63.855.888.986.177.6
    aReaction conditions: 100 mg catalyst, 340 ℃, 1 MPa, H2/CO = 1, GHSV = 22.2 L/(gcat·h), 50 h, bH2/CO = 2, cH2/CO = 3
    下载: 导出CSV
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出版历程
  • 收稿日期:  2020-12-28
  • 修回日期:  2021-02-28
  • 网络出版日期:  2021-03-18
  • 刊出日期:  2021-07-15

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