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NiPt/SBA-15纳米催化剂的制备及其催化水合肼分解产氢性能研究

梁雨 李贵 郑君宁 许立信 叶明富 万超

梁雨, 李贵, 郑君宁, 许立信, 叶明富, 万超. NiPt/SBA-15纳米催化剂的制备及其催化水合肼分解产氢性能研究[J]. 燃料化学学报(中英文), 2023, 51(5): 684-692. doi: 10.19906/j.cnki.JFCT.2022072
引用本文: 梁雨, 李贵, 郑君宁, 许立信, 叶明富, 万超. NiPt/SBA-15纳米催化剂的制备及其催化水合肼分解产氢性能研究[J]. 燃料化学学报(中英文), 2023, 51(5): 684-692. doi: 10.19906/j.cnki.JFCT.2022072
LIANG Yu, LI Gui, ZHENG Jun-ning, XU Li-xin, YE Ming-fu, WAN Chao. Preparation of NiPt/SBA-15 nanocatalyst and its catalytic performance for the dehydrogenation of hydrous hydrazine[J]. Journal of Fuel Chemistry and Technology, 2023, 51(5): 684-692. doi: 10.19906/j.cnki.JFCT.2022072
Citation: LIANG Yu, LI Gui, ZHENG Jun-ning, XU Li-xin, YE Ming-fu, WAN Chao. Preparation of NiPt/SBA-15 nanocatalyst and its catalytic performance for the dehydrogenation of hydrous hydrazine[J]. Journal of Fuel Chemistry and Technology, 2023, 51(5): 684-692. doi: 10.19906/j.cnki.JFCT.2022072

NiPt/SBA-15纳米催化剂的制备及其催化水合肼分解产氢性能研究

doi: 10.19906/j.cnki.JFCT.2022072
基金项目: 国家自然科学基金青年基金(22108238, U22A20408),安徽省自然科学基金青年基金(1908085QB68),安徽省科技重大专项(201903a05020055),中国博士后面上项目(2019M662060)和特别资助站中项目(2020T130580),博士后国际交流派出项目(PC2022046),安徽省光电磁性功能材料重点实验室开放研究基金(ZD2021007)和江西省生态化工工程研究中心开放研究基金(STKF2109)资助
详细信息
    通讯作者:

    E-mail: lxxu@hotmail.com

    wanchao@zju.edu.cn

  • 中图分类号: O643.36

Preparation of NiPt/SBA-15 nanocatalyst and its catalytic performance for the dehydrogenation of hydrous hydrazine

Funds: The project was supported by the National Natural Science Foundation of China (22108238, U22A20408), Anhui Provincial Natural Science Foundation (1908085QB68), Major Science and Technology Project of Anhui Province (201903a05020055), China Postdoctoral Science Foundation (2019M662060, 2020T130580), Postdoctoral International Exchange Program(PC2022046), Open Research Funds of Anhui Key Laboratory of Photoelectric-Magnetic Functional Materials (ZD2021007) and Open Research Funds of Jiangxi Province Engineering Research Center of Ecological Chemical Industry (STKF2109).
  • 摘要: 本研究采用浸渍还原法制备了不同金属比例的NiPt双金属负载SBA-15(介孔二氧化硅)催化剂,对其催化水合肼脱氢性能进行了研究。研究结果表明,在催化剂的制备过程中Pt和Ni形成了合金,两种金属的电子协同效应可以有效地促进催化剂的催化性能,SBA-15与金属活性组分之间的相互作用有助于改善催化剂的催化性能和循环稳定性。Pt6Ni4/SBA-15催化剂催化水合肼脱氢的反应活化能为45.6 kJ/mol,TOF值为2123.3 h−1,优于大部分已经报道的催化剂。
  • FIG. 2298.  FIG. 2298.

    FIG. 2298.  FIG. 2298.

    图  1  Pt6Ni4/SBA-15催化剂的TEM照片

    Figure  1  TEM images of Pt6Ni4/SBA-15

    图  2  (a) SBA-15和Pt6Ni4/SBA-15氮气吸附-脱附曲线和(b) SBA-15和Pt6Ni4/SBA-15孔径分布

    Figure  2  (a) Nitrogen adsorption-desorption curves of SBA-15 and Pt6Ni4/SBA-15, (b) pore size distribution of SBA-15 and Pt6Ni4/SBA-15

    图  3  (a) 不同催化剂的XRD谱图和 (b) 催化反应生成气体的质谱谱图

    Figure  3  (a) XRD patterns of different catalysts and (b) mass spectrum of gases produced by catalytic reactions

    图  4  SBA-15和Pt6Ni4/SBA-15催化剂在Pt 4f和Ni 2p的XPS光谱谱图对比

    Figure  4  Comparison of XPS spectra of SBA-15 and Pt6Ni4/SBA-15 catalysts in the Pt 4f and Ni 2p region

    图  5  (a) 不同Pt/Ni物质的量比PtNi/SBA-15催化水合肼脱氢产生的气体当量与反应时间曲线和(b) 对应催化剂的TOF值

    Figure  5  (a) PtNi/SBA-15 catalysts with different Pt/Ni molar ratios for the dehydrogenation of hydrous hydrazine catalyzed by gas equivalent versus reaction time and (b) TOF value map of the corresponding catalyst (323 K)

    图  6  (a) 不同温度下Pt6Ni4/SBA-15催化水合肼脱氢的速率,(b) 为(a)对应的阿伦尼乌斯曲线

    Figure  6  (a) Rate curves of Pt6Ni4/SBA-15 catalyzed dehydrogenation of hydrous hydrazine at different temperatures; (b) is the corresponding Arrhenius plot obtained from the Graph (a)

    图  7  (a) Pt6Ni4/SBA-15在不同浓度的碱溶液中催化水合肼脱氢产生的气体当量与反应时间曲线,(b) Pt6Ni4/SBA-15催化水合肼脱氢循环使用性能

    Figure  7  (a) Pt6Ni4/SBA-15 catalyzed dehydrogenation of hydrous hydrazine in alkaline solutions with different concentrations of gas equivalent versus reaction time under the condition of 323 K; (b) Pt6Ni4/SBA-15 in fives run for decomposition of hydrous hydrazine

    表  1  323 K下碱性溶液中水合肼分解制氢各种金属催化剂的催化活性

    Table  1  Catalytic performances of various metal catalysts for hydrogen generation from the decomposition of hydrous hydrazine in alkaline solution at 323 K

    Catalyst TOF/h−1 Ea/(kJ·mol−1) Ref.
    Pt6Ni4/SBA-15 2123.3 45.6 this work
    Ni3Pt7/BNG-1000 199.4 28.4 [27]
    G4-OH (Pt12Ni48) 240 [33]
    Ni84Pt16/graphene 415 40 [34]
    Ni60Pt40/NC-700 1602 48.3 [16]
    Ni87Pt13/MA 160 55.7 [14]
    Ni@Ni-Pt/La2O3 312 56.2 [32]
    Ni0.8Pt0.2/DT-Ti3C2Tx 1220 67.1 [35]
    Ni0.9Pt0.1/MIL-101/rGO 960 50.6 [36]
    Ni88Pt12@MIL‐101 375.1 51.29 [11]
    Ni3Pt7/graphene 416 49.36 [37]
    (Ni3Pt7)0.5-(MnOx)0.5/NPC-900 706 50.2 [38]
    Rh47Ni18P35@MOF-74 715.4 49.39 [39]
    Ni37Pt63/g-C3N4 570 36.6 [40]
    Ni0.4Pt0.6/CNTs 1725.3 36.3 [4]
    Pt0.6Ni0.4/PDA-rGO 2056 33.39 [23]
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  • 收稿日期:  2022-06-25
  • 修回日期:  2022-08-26
  • 录用日期:  2022-09-07
  • 网络出版日期:  2022-09-08
  • 刊出日期:  2023-05-15

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