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火焰喷雾热解制Pd-Pt/CeO2催化甲烷燃烧的性能研究

武琳渊 王乙 陈召英 田庆玲 王琳茹 付紫君 赵宁 王晓波 黄鑫

武琳渊, 王乙, 陈召英, 田庆玲, 王琳茹, 付紫君, 赵宁, 王晓波, 黄鑫. 火焰喷雾热解制Pd-Pt/CeO2催化甲烷燃烧的性能研究[J]. 燃料化学学报(中英文). doi: 10.19906/j.cnki.JFCT.2023083
引用本文: 武琳渊, 王乙, 陈召英, 田庆玲, 王琳茹, 付紫君, 赵宁, 王晓波, 黄鑫. 火焰喷雾热解制Pd-Pt/CeO2催化甲烷燃烧的性能研究[J]. 燃料化学学报(中英文). doi: 10.19906/j.cnki.JFCT.2023083
WU Linyuan, WANG Yi, CHEN Zhaoying, TIAN Qingling, WANG Linru, FU Zijun, ZHAO Ning, WANG Xiaobo, HUANG Xin. Methane catalytic combustion over flame spray pyrolysis-synthesized Pd-Pt/CeO2 catalyst[J]. Journal of Fuel Chemistry and Technology. doi: 10.19906/j.cnki.JFCT.2023083
Citation: WU Linyuan, WANG Yi, CHEN Zhaoying, TIAN Qingling, WANG Linru, FU Zijun, ZHAO Ning, WANG Xiaobo, HUANG Xin. Methane catalytic combustion over flame spray pyrolysis-synthesized Pd-Pt/CeO2 catalyst[J]. Journal of Fuel Chemistry and Technology. doi: 10.19906/j.cnki.JFCT.2023083

火焰喷雾热解制Pd-Pt/CeO2催化甲烷燃烧的性能研究

doi: 10.19906/j.cnki.JFCT.2023083
基金项目: 煤与煤层气共采国家重点实验室开放基金 (2022KF12),山西省科技成果转化引导专项 (202204021301010),山西省科技创新人才团队项目 (202204051002025)和国家自然科学基金 (52004177)资助
详细信息
    通讯作者:

    Tel: 15535198775, E-mail: wxbtyut@163.com

    huangxin11987@163.com

  • 中图分类号: O643

Methane catalytic combustion over flame spray pyrolysis-synthesized Pd-Pt/CeO2 catalyst

Funds: The project was supported by State Key Laboratory of Coal and CBM Co-mining (2022KF12), Shanxi Province Science and Technology Achievement Transformation Guidance Special Project (202204021301010), Shanxi Province Science and Technology Innovation Talent Team (202204051002025), National Natural Science Foundation of China (52004177).
  • 摘要: 火焰喷雾热解法(FSP)是一种简单、快速、可规模化制备纳米催化剂的技术。通过火焰喷雾热解法合成CeO2和Pt-CeO2载体、Pd-Pt-CeO2催化剂,采用浸渍法在CeO2和Pt-CeO2载体分别沉积Pd-Pt和Pd而制得Pd-Pt双金属催化剂,并考察其甲烷催化燃烧性能。利用ICP、XRD、TEM、BET、H2-TPR、XPS和Raman对催化剂的物化性质进行分析。TEM结果表明,Pd-Pt/CeO2催化剂中Pd和Pt物种高分散于CeO2载体。相比于一步法(one step)制得的Pd-Pt-CeO2(OS-FSP)催化剂,共浸渍法制得Pd-Pt/CeO2(0.25)-WI的催化活性更高,其t50降低了60 ℃,且稳定运行60 h而没有明显失活。这归因于Pd-Pt/CeO2(0.25)-WI催化剂表面上Pd0/Pd2+和Ce3+/Ce4+物质的量比更高、晶格氧更多,进而导致其具有良好的甲烷催化燃烧性能。
  • 图  1  FSP装置示意图(a)和实际照片(b)

    Figure  1  Schematic diagram and photograph of the FSP device

    图  2  四种催化剂的(a) CH4转化率随反应温度的变化、(b) 表观活化能比较和(c) Pd-Pt/CeO2(0.25)-WI和Pd-Pt-CeO2(OS-FSP)催化剂在710 ℃的稳定性比较

    Figure  2  (a) CH4 conversion as a function of reaction temperature, (b) corresponding Arrhenius plots over four catalysts and (c) stability test over Pd-Pt/CeO2(0.25)-WI and Pd-Pt-CeO2(OS-FSP) catalysts at 710 ℃ (0.1 g catalysts, CH4:O2:N2 = 0.5:10:89.5, GHSV = 15000 mL/(g·h))

    图  3  四种催化剂的XRD谱图

    Figure  3  XRD patterns of four catalysts

    图  4  (a)−(f) Pd-Pt/CeO2(0.25)-WI和(g)−(l) Pd-Pt-CeO2(OS-FSP)催化剂的HAADF-STEM图像及其EDX元素扫描

    Figure  4  HAADF-STEM and corresponding EDX elemental mapping of (a)-(f) Pd-Pt/CeO2(0.25)-WI and (g)-(l) Pd-Pt-CeO2(OS-FSP) catalysts

    图  5  Pd-Pt/CeO2(0.25)-WI和Pd-Pt-CeO2(OS-FSP)催化剂的(a) N2吸附-脱附曲线和(b) 孔径分布

    Figure  5  (a)N2 adsorption-desorption isotherm and (b) pore size distribution of Pd-Pt/CeO2(0.25)-WI and Pd-Pt-CeO2(OS-FSP) catalysts

    图  6  (a)、(b) Pd-Pt/CeO2(0.25)-WI和(c)、(d) Pd-Pt-CeO2(OS-FSP)催化剂的HR-TEM图像

    Figure  6  HR-TEM images of (a), (b) Pd-Pt/CeO2(0.25)-WI and (c), (d) Pd-Pt-CeO2(OS-FSP) catalysts

    图  7  四种催化剂的H2-TPR谱图

    Figure  7  H2-TPR profiles of four catalysts

    图  8  四种催化剂的Raman谱图

    Figure  8  Raman profiles of four catalysts

    图  9  Pd-Pt/CeO2(0.25)-WI和Pd-Pt-CeO2(OS-FSP)催化剂的(a) 全谱谱图、(b) Pd 3d、(c) O 1s、(d) Ce 3d XPS谱图

    Figure  9  XPS profiles of (a) wide, (b) Pd 3d, (c) O 1s, (d) Ce 3d for Pd-Pt/CeO2(0.25)-WI and Pd-Pt-CeO2(OS-FSP) catalysts

    表  1  四种催化剂的ICP-OES结果

    Table  1  ICP-OES results of four catalysts

    CatalystMetal loading w/%
    PdPt
    Pd-Pt-CeO2(OS-FSP)0.890.09
    Pd-Pt/CeO2(0.25)-WI0.910.11
    Pd-Pt/CeO2(0.5)-WI0.890.10
    Pd/Pt-CeO2(FSP)-WI0.880.12
    下载: 导出CSV

    表  2  四种催化剂的t10t50t90

    Table  2  t10, t50 and t90 results of four catalysts

    Catalystt10/℃t50/℃t90/℃
    Pd-Pt-CeO2(OS-FSP)540677785
    Pd-Pt/CeO2(0.25)-WI510617729
    Pd-Pt/CeO2(0.5)-WI540654761
    Pd/Pt-CeO2(FSP)-WI511622740
    下载: 导出CSV

    表  3  Pd-Pt/CeO2(0.25)-WI和Pd-Pt-CeO2(OS-FSP)催化剂上Pd、Pt、Ce和O的表面原子浓度和不同元素的价态分布

    Table  3  Surface atom concentration of Pd, Pt, Ce and O and valence distribution of different elements from XPS data on Pd-Pt/CeO2(0.25)-WI and Pd-Pt-CeO2(OS-FSP) catalysts

    CatalystSurface atom concentrationPd0/Pd2+Ce3+/Ce4+Oads/Olat
    PdPtCeO
    Pd-Pt/CeO2(0.25)-WI0.570.1017.3981.940.850.530.54
    Pd-Pt-CeO2(OS-FSP)0.470.0417.0482.450.270.470.50
    下载: 导出CSV
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  • 收稿日期:  2023-11-27
  • 修回日期:  2023-12-11
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