化学
催化作用
解吸
路易斯酸
吸附
吡啶
纳米纤维
无机化学
化学工程
热脱附光谱法
布朗斯特德-洛瑞酸碱理论
氨
物理化学
有机化学
工程类
作者
M.A. Rodriguez-Olguin,Hanan Atia,Marta V. Bosco,Alicia Aguirre,Reinhard Eckelt,Edidiong D. Asuquo,Matthias Vandichel,Han Gardeniers,Arturo Susarrey-Arce
标识
DOI:10.1016/j.jcat.2021.11.019
摘要
Alumina (Al2O3) is a widely used material for catalysis in the chemical industry. Besides a high specific surface area, acid sites on Al2O3 play a crucial role in the chemical transformation of adsorbed molecules, which ultimately react and desorb from the catalyst. This study introduces a synthetic method based on electrospinning to produce Al2O3 nanofibers (ANFs) with acidity and porosity tuned using different aluminum precursor formulations. After electrospinning and heat treatment, the nanofibers form a non-woven network with macropores (∼4 μm). Nanofibers produced from aluminum di(sec-butoxide)acetoacetic ester chelate (ASB) show the highest total acidity of ca. 0.70 µmol/m2 determined with temperature-programmed desorption of ammonia (NH3-TPD) and BET. The nature of the acid site in ASB ANFs is studied in detail with infrared (IR) spectroscopy. Pyridine is used as a molecular probe for the identification of acid sites in ASB. Pyridine showed the presence of Lewis acid sites prominently. Density-functional theory (DFT) is conducted to understand the desorption kinetics of the adsorbed chemical species, such as ammonia (NH3) on crystalline γ-Al2O3. For our analysis, we focused on a mobile approach for chemisorbed and physisorbed NH3. The computational results are compared with NH3-TPD experiments, ultimately utilized to estimate the desorption energy and kinetic desorption parameters. The experiments are found to pair up with our simulation results. We predict that these non-woven structures will find application as a dispersion medium of metallic particles in catalysis.
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