Pt基催化剂的制备及12H-苄基甲苯脱氢催化性能研究
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    摘要:

    利用高温焙烧Al2O3载体、采用低酸性的羟基磷灰石载体、加入金属助剂的策略降低催化剂酸性,使用等体积饱和浸渍法制备了一系列不同的铂基负载型催化剂,,用于有机液相储氢载体(LOHC)的脱氢供氢;采用X-射线衍射(XRD)、高分辨透射电子显微镜(HRTEM)、氨气程序升温脱附(NH3-TPD)、低温N2吸附手段,对所制备的催化剂进行了表征。使用固定床反应器,以12H-苄基甲苯为原料,对所制备的催化剂进行脱氢反应性能评价。结果表明:利用上述三种方法所改性的催化剂表面酸性均低于未经过任何改性的0.5Pt/Al2O3-500-8催化剂,且Al2O3载体焙烧温度越高,所制备的催化剂表面酸量、酸强度越弱。筛选出了脱氢效果最优的催化剂0.5Pt-0.2Sn/Al2O3-700-8,在反应温度320℃下连续运行60小时表现出了85%以上12H-苄基甲苯脱氢率,94%以上的完全脱氢产物0H-苄基甲苯选择性。脱氢产物中轻组分杂质含量不高于0.24%,重组分杂质含量不高于0.54%。

    Abstract:

    A series of Al2O3 supported and Pt-based metal catalysts were prepared using an equal volume saturation co-impregnation method, applied for the dehydrogenation of 12H-benzyltoluene (12H-MBT)liquid Organic Hydrogen Carrier(LOHC). In order to reduce the surface acidity of as-prepared catalysts, low-acidity hydroxyapatite support, addition of a second metal active components, and high temperature calcination Al2O3 supports were applied for the design and preparation of catalysts. The physical and chemical properties of the catalyst were characterized using NH3-TPD, XRD, BET, and HRTEM, the characterization results indicate that the acidity of as-prepared catalysts modified by the above three methods is lower than that of the 0.5Pt/Al2O3-500-8 catalyst which has no modification, and the higher the calcination temperature of Al2O3 support, the lower the acidity of as-prepared catalysts.The optimized 0.5%Pt-0.2%Sn/Al2O3-700-8 catalyst shows high catalytic activity and selectivity for the 12H-monobenzyltoluene dehydrogenation. At the reaction temperature of 320°C, the 12H-monobenzyltoluene dehydrogenation rate exceeds 85% and the selectivity of the completely dehydrogenated product 0H-monobenzyltoluene is more than 94%. The light component by-product content in the dehydrogenation product is less than 0.24%, and the heavy component by-product content is less than 0.54%.

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  • 收稿日期:2025-01-25
  • 最后修改日期:2025-02-20
  • 录用日期:2025-02-21
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