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原位同步辐射光电离质谱研究压力对3Mn10Fe/Ni催化剂上N2O形成途径的影响

许鸣皋 朱宝忠 文武 杨玖重 潘洋 孙运兰

许鸣皋, 朱宝忠, 文武, 杨玖重, 潘洋, 孙运兰. 原位同步辐射光电离质谱研究压力对3Mn10Fe/Ni催化剂上N2O形成途径的影响[J]. 燃料化学学报. doi: 10.19906/j.cnki.JFCT.2021042
引用本文: 许鸣皋, 朱宝忠, 文武, 杨玖重, 潘洋, 孙运兰. 原位同步辐射光电离质谱研究压力对3Mn10Fe/Ni催化剂上N2O形成途径的影响[J]. 燃料化学学报. doi: 10.19906/j.cnki.JFCT.2021042
XU Ming-gao, ZHU Bao-zhong, WEN Wu, YANG Jiu-zhong, PAN Yang, SUN Yun-nan. The study of effects of pressure on the formation pathways of N2O over 3Mn10Fe/Ni catalyst by in-situ synchrotron radiation photoionization mass spectrometry[J]. Journal of Fuel Chemistry and Technology. doi: 10.19906/j.cnki.JFCT.2021042
Citation: XU Ming-gao, ZHU Bao-zhong, WEN Wu, YANG Jiu-zhong, PAN Yang, SUN Yun-nan. The study of effects of pressure on the formation pathways of N2O over 3Mn10Fe/Ni catalyst by in-situ synchrotron radiation photoionization mass spectrometry[J]. Journal of Fuel Chemistry and Technology. doi: 10.19906/j.cnki.JFCT.2021042

原位同步辐射光电离质谱研究压力对3Mn10Fe/Ni催化剂上N2O形成途径的影响

doi: 10.19906/j.cnki.JFCT.2021042
基金项目: 国家自然科学基金(52076016)
详细信息

The study of effects of pressure on the formation pathways of N2O over 3Mn10Fe/Ni catalyst by in-situ synchrotron radiation photoionization mass spectrometry

Funds: The project was supported by the National Natural Science Foundation of China (52076016)
  • 摘要: 为了研究N2O在氨选择性催化还原脱硝(NH3-SCR)过程中的形成途径及其选择性受压力影响的变化规律,采用原位光电离质谱研究方法结合流动管反应器,对3Mn10Fe/Ni催化剂NH3-SCR反应体系中气相物种进行了原位检测并获得了各组分的质谱图,进一步分析了不同工况、温度和压力条件下N2O选择性以及NOx和NH3转化率的变化规律。研究结果表明:N2O形成主要来源于非选择性催化反应(NSCR)和吸附态NH3氧化(NSNO)反应,其中,100−250 ℃由NSCR占据生成N2O的主导地位,250−400 ℃两种形成途径贡献相当,400−500 ℃ NSNO成为主要来源。此外,低压降低了催化剂在低温区的脱硝活性,却促进了在高温区通过NSNO反应生成N2O的形成途径。
  • 图  1  原位光电离质谱示意图

    Figure  1.  Schematic diagram of in-situ synchrotron radiation photoionization mass spectrometry

    (Ⅰ: Atmospheric/high pressure reactor; Ⅱ: Low pressure reactor)

    图  2  光子能量为13 eV时fresh催化剂上SCR反应气相物种的光电离质谱图;插图为N2O的PIE图[36]

    Figure  2.  Mass spectrum of the gas phase species in SCR reaction on fresh catalyst at the photon energy of 13 eV

    Inset is the PIE spectrum of the m/z = 44 speciesreaction conditions:101.325 kPa; 400 ℃; NH3+NO+O2+fresh; GHSV: 30000 h−1

    图  3  不同压力下N2O选择性随温度的变化趋势图

    Figure  3.  Trend diagram of N2O selectivity with temperature under different pressures

    图  4  不同压力下NOx转换率随温度的变化趋势图

    Figure  4.  Trend diagram of NOx conversion rates with temperature under different pressures

    图  5  不同压力下NH3转换率随温度的变化趋势图

    Figure  5.  The trend diagram of NH3 conversion rates with temperature under different pressures

    表  1  不同工况下N2O生成途径分析

    Table  1.   Inlet gas composition for N2O formation pathway analysis

    gas composition (mole fraction)catalystpossible reaction
    400 × 10−6 NH3,400 × 10−6 NO,5% O2freshR1,R2,R3,R5,R5,R6
    400 × 10−6 NH3,400 × 10−6 NO,5% O2/R3
    400 × 10-6 NH3,400 × 10-6 NOfreshR4,R5,R6
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