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The origin of a large apparent tortuosity factor for the Knudsen diffusion inside monoliths of a samaria-alumina aerogel catalyst: a diffusion NMR study

机译:纳米氧化铝气凝胶催化剂整料内部Knudsen扩散的大表观曲折因子的起源:扩散NMR研究

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摘要

Pulsed field gradient (PFG) NMR was applied to measure tortuosity factors for carbon dioxide diffusion in the Knudsen and gas regimes inside monoliths of a samaria-alumina aerogel catalyst, a high porosity material containing micropores in addition to meso- and macropores. The apparent tortuosity factor obtained from PFG NMR measurements for the Knudsen diffusion in the meso- and macropores of the catalyst has an unexpectedly large value of approximately 6 if carbon dioxide adsorption in the micropores and other types of surface adsorption sites of the catalyst is ignored. At the same time, the corresponding apparent tortuosity factor in the gas regime was found to be around 2. Application of a proposed model which describes fast molecular exchange between the surface adsorption sites and the main pore volume of the catalyst yields corrected tortuosity factors which depend only on the pore system geometry. Using this model, the corrected tortuosity factors were found to be around 2 for both diffusion regimes, in agreement with the expectations based on a high porosity of the studied catalyst.
机译:脉冲场梯度(PFG)NMR用于测量曲折度因子,以测量在am骨-氧化铝气凝胶催化剂整体式内部的Knudsen和气体状态下二氧化碳扩散的曲折系数,这是一种高孔隙率材料,除了中孔和大孔外还包含微孔。如果忽略了催化剂在微孔中的二氧化碳吸附和其他类型的催化剂表面吸附位点,则从PFG NMR测量获得的Knudsen扩散在催化剂的中孔和大孔中的表观曲折因子具有意想不到的大值,约为6。同时,发现在气体状态下相应的表观曲折因子约为2。应用提议的模型描述了表面吸附位点和催化剂主要孔体积之间的快速分子交换,产生了校正的曲折因子,该曲折因子取决于仅关于孔隙系统的几何形状。使用该模型,发现两种扩散方案的校正曲折因子约为2,这与基于所研究催化剂的高孔隙率的预期相符。

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