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Effect of Zn on performance of Ni/SiO2 for hydrodeoxygenation of anisole

WANG Dan-dan GU Xiao-yu SHI Hao-nan CHEN Ji-xiang

王丹丹, 谷孝雨, 史浩楠, 陈吉祥. Zn对Ni/SiO2催化剂苯甲醚氢脱氧性能的影响[J]. 燃料化学学报. doi: 10.1016/S1872-5813(22)60029-X
引用本文: 王丹丹, 谷孝雨, 史浩楠, 陈吉祥. Zn对Ni/SiO2催化剂苯甲醚氢脱氧性能的影响[J]. 燃料化学学报. doi: 10.1016/S1872-5813(22)60029-X
WANG Dan-dan, GU Xiao-yu, SHI Hao-nan, CHEN Ji-xiang. Effect of Zn on performance of Ni/SiO2 for hydrodeoxygenation of anisole[J]. Journal of Fuel Chemistry and Technology. doi: 10.1016/S1872-5813(22)60029-X
Citation: WANG Dan-dan, GU Xiao-yu, SHI Hao-nan, CHEN Ji-xiang. Effect of Zn on performance of Ni/SiO2 for hydrodeoxygenation of anisole[J]. Journal of Fuel Chemistry and Technology. doi: 10.1016/S1872-5813(22)60029-X

Zn对Ni/SiO2催化剂苯甲醚氢脱氧性能的影响

doi: 10.1016/S1872-5813(22)60029-X

Effect of Zn on performance of Ni/SiO2 for hydrodeoxygenation of anisole

More Information
  • 摘要: 采用等体积浸渍法制备了Ni/SiO2及NixZn/SiO2(x代表Ni/Zn原子比)催化剂,在常压固定床反应器上考察了催化剂苯甲醚气相加氢脱氧性能。研究发现,经550 ℃还原后NixZn/SiO2中形成了Ni-Zn合金,当Ni/Zn原子比为30时可获得较小合金晶粒尺寸和较高H2化学吸附量。在苯甲醚加氢脱氧反应中, Ni-Zn合金的形成有利于苯甲醚直接脱氧形成苯,同时抑制了CO甲烷化及C−C键氢解,有利于降低耗氢量和提高目的产物收率,这是因为形成合金后亲氧性金属Zn对Ni的几何隔离作用有关。Ni30Zn/SiO2催化剂的活性和苯选择性均高于Ni/SiO2。结果表明,Ni30Zn/SiO2催化剂失活与产物水氧化Ni-Zn 合金表面及积炭有关。
  • Figure  1  XRD patterns of calcined Ni/SiO2, Ni30Zn/SiO2, and Ni10Zn/SiO2

    Figure  2  H2-TPR profiles of (a) reduced and (b) calcined Ni/SiO2 and NixZn/SiO2 catalysts

    Figure  3  XRD patterns of reduced Ni/SiO2 and NixZn/SiO2 catalysts

    Figure  4  TEM images and particle size distributions of (a) Ni/SiO2; (b) Ni30Zn/SiO2 and (c) Ni10Zn/SiO2

    Figure  5  H2-TPD profiles of reduced Ni/SiO2 and NixZn/SiO2 catalysts

    Figure  6  Proposed reaction pathway in HDO of anisole

    Figure  7  Performance of Ni/SiO2, Ni30Zn/SiO2 and Ni10Zn/SiO2 in HDO of anisole

    (a): anisole conversion and product selectivity; (b): $n_{{\rm{CH}}_4} $/nΔAnisole, nCO/nΔAnisole and $n_{{\rm{CH}}_3{\rm{OH}}} $/nΔAnisole molar ratios reaction conditions: 300 °C, 0.1 MPa, H2/anisole molar ratio of 25, anisole WHSV of 2 h−1.

    Figure  8  Possible reaction mechanism in HDO of anisole on NixZn/SiO2

    Figure  9  Performance of Ni30Zn/SiO2 in HDO of anisole as a function of WHSV

    (a): Anisole conversion and product selectivity; (b): $n_{{\rm{CH}}_4} $/nΔAnisole, nCO/nΔAnisole and $n_{{\rm{CH}}_3{\rm{OH}}} $/nΔAnisole molar ratios reaction conditions: 300 °C, 0.1 MPa, H2/anisole molar ratio of 25

    Figure  10  Effect of reaction temperature on Ni30Zn/SiO2 for HDO of anisole

    (a): Anisole conversion and product selectivity; (b): $n_{{\rm{CH}}_4} $/nΔAnisole, nCO/nΔAnisole and $n_{{\rm{CH}}_3{\rm{OH}}} $/nΔAnisole molar ratios reaction conditions: 0.1 MPa, H2/anisole molar ratio of 25, anisole WHSV of 2 h−1

    Figure  11  Anisole conversion and product selectivity on Ni30Zn/SiO2 with time on stream

    reaction conditions: 300 °C, 0.1 MPa, H2/anisole molar ratio of 25, anisole WHSV of 2 h−1

    Figure  12  XRD patterns of fresh and spent Ni30Zn/SiO2 catalysts

    Table  1  Properties of different catalysts

    CatalystSBET/(m2∙g−1)dp/nmvp/(cm3∙g−1)Crystallite
    size/nm
    Ni/SiO24095.70.7811.0
    Ni30Zn/SiO23055.70.6510.4
    Ni10Zn/SiO22445.70.5112.5
    Spent-Ni30Zn/SiO23396.60.568.5
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  • 收稿日期:  2022-01-27
  • 录用日期:  2022-04-17
  • 修回日期:  2022-04-17
  • 网络出版日期:  2022-05-12

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