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Catalytic hydrogenolysis of diphenyl ether over Ru supported on amorphous silicon-aluminum-TiO2

CHEN Bo LI Lei DIAO Zhi-ju CAO Rui-dong SONG Li-fei HUANG Liang-qiu WANG Xue

陈博, 李磊, 刁智俊, 曹瑞栋, 宋利飞, 黄粱秋, 王学. 无定形硅铝改性TiO2负载Ru催化加氢解聚二苯醚的研究[J]. 燃料化学学报(中英文), 2022, 50(5): 621-627. doi: 10.1016/S1872-5813(21)60191-3
引用本文: 陈博, 李磊, 刁智俊, 曹瑞栋, 宋利飞, 黄粱秋, 王学. 无定形硅铝改性TiO2负载Ru催化加氢解聚二苯醚的研究[J]. 燃料化学学报(中英文), 2022, 50(5): 621-627. doi: 10.1016/S1872-5813(21)60191-3
CHEN Bo, LI Lei, DIAO Zhi-ju, CAO Rui-dong, SONG Li-fei, HUANG Liang-qiu, WANG Xue. Catalytic hydrogenolysis of diphenyl ether over Ru supported on amorphous silicon-aluminum-TiO2[J]. Journal of Fuel Chemistry and Technology, 2022, 50(5): 621-627. doi: 10.1016/S1872-5813(21)60191-3
Citation: CHEN Bo, LI Lei, DIAO Zhi-ju, CAO Rui-dong, SONG Li-fei, HUANG Liang-qiu, WANG Xue. Catalytic hydrogenolysis of diphenyl ether over Ru supported on amorphous silicon-aluminum-TiO2[J]. Journal of Fuel Chemistry and Technology, 2022, 50(5): 621-627. doi: 10.1016/S1872-5813(21)60191-3

无定形硅铝改性TiO2负载Ru催化加氢解聚二苯醚的研究

doi: 10.1016/S1872-5813(21)60191-3
详细信息
  • 中图分类号: TQ536.1

Catalytic hydrogenolysis of diphenyl ether over Ru supported on amorphous silicon-aluminum-TiO2

Funds: The project was supported by the National Natural Science Foundation of China (21875186), Natural Science Basic Research Plan in Shaanxi Province of China (2019JM-259), Foundation of State Key Laboratory of High-efficiency Utilization of Coal and Green Chemical Engineering (2019-KF-17), China Postdoctoral Science Foundation (2017M623205) and Special Research Foundation of Education Bureau of Shaanxi Province (15JK1692).
More Information
  • 摘要: 采用蒸汽辅助法合成了无定形硅铝(ASA)-TiO2复合载体,并在此基础上制备了双功能催化剂Ru5/ASA-TiO2。利用X-射线衍射(XRD)、吡啶吸附红外(Py-FTIR)、氨-程序升温脱附(NH3-TPD)、扫描电子显微镜(SEM)、透射电子显微镜(TEM)和X射线光电子能谱(XPS)等手段对所制备催化剂的结构和酸性进行了详细表征。以二苯醚为褐煤模型化合物,在温和条件下考察了催化剂Ru5/ASA-TiO2加氢解聚4–O–5类型醚键的反应活性,二苯醚的转化率高于98%,苯收率为67.1%。弱Brønsted酸和/或Lewis酸而非强Brønsted酸是提高二苯醚的加氢解聚转化率和苯收率的主要因素,并且反应温度能够影响各类型酸的相对含量从而显著影响二苯醚加氢解聚产物的选择性。
  • FIG. 1530.  FIG. 1530.

    FIG. 1530. 

    Figure  1  XRD patterns of different supports

    Figure  2  Characterizations of the catalyst of Ru5/ASA-TiO2 with (a) SEM, (b)−(d), (f) TEM and (e) XPS Inset in (d) is the fast Fourier transformation of the selected area

    Figure  3  Py-FTIR spectra of the support after desorption at different temperatures

    Figure  4  Hydrogenolysis of diphenyl ether with different catalystsGeneral conditions: diphenyl ether (0.2 mmol), catalyst (0.02 g), water (5 mL), 250 °C, 1 h, 0.2 MPa H2 + 0.6 MPa N2

    Figure  5  Effect of temperature on the distribution of primary products General conditions: diphenyl ether (0.2 mmol), catalyst (0.02 g), water (5 mL), 1 h, 0.2 MPa H2+0.6 MPa N2

    Figure  6  Effect of reaction time on the distribution of primary products General conditions: diphenyl ether (0.2 mmol), catalyst (0.02 g), water (5 mL), 250 °C, 0.2 MPa H2 + 0.6 MPa N2

    Figure  7  Possible pathways for the hydrogenolysis of diphenyl ether over Ru5/ASA-TiO2

    Table  1  Number of BA and LA sites in different supports a

    SampleRelative amount /%cacid /(mmol·g−1)bLA1/LA2dBA/LAd
    LA1LA2
    ASA-TiO2 59.39 40.61 0.42 1.46 0.30
    HZSM-5 0 100 0.50 0 1.22
    HZSM-5c 0 100 1.58 0 4.89
    TiO2 100 0 0.25 0
    Ru5/ASA-TiO2 69.11 30.89 0.49 2.24 0.26
    a Py-FTIR characterization was performed at 150 °C; b NH3-TPD profiles were obtained in the temperature range of 50−550 °C; c commercial molecular sieve; d relative content of Lewis and Brønsted sites were calculated according to the areas of the absorption peaks and their corresponding extinction coefficients
    下载: 导出CSV

    Table  2  Validation tests for the production of benzene over Ru5/ASA-TiO2

    ReactantConv. /%Yield /%
    97.042.87.04.53.9
    88.330.07.04.89.7
    92.052.12.82.90.54.1
    > 99%1.86.21.467.4
    Reaction conditions: reactant (0.2 mmol), catalyst (0.02 g), water (5 mL), 250 °C, 0.2 MPa H2+0.6 MPa N2; a reaction was performed at 160 °C
    下载: 导出CSV
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出版历程
  • 收稿日期:  2021-08-18
  • 修回日期:  2021-09-04
  • 录用日期:  2021-09-07
  • 网络出版日期:  2022-01-28
  • 刊出日期:  2022-05-24

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