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Kinetics and mechanism of catalytic ozonation of acetone in air over MnOx/Al2O3 catalyst
Reaction Kinetics, Mechanisms and Catalysis ( IF 1.7 ) Pub Date : 2021-07-16 , DOI: 10.1007/s11144-021-02024-6
M. Ghavami 1 , J. Soltan 1
Affiliation  

The catalytic ozonation of acetone using MnOx/Al2O3 catalysts prepared by polyol and impregnation methods was investigated. The synthesized catalysts exhibited excellent catalytic activity at room temperature with conversions of around 95%. Although many studies focus on catalytic processes to oxidize VOCs more efficiently, the mechanism behind this reaction is still unknown. The In-situ DRIFTS and activity results show that alumina not only acts as a support for MnOx, but it also involves in the reaction with acetone and creates surface carboxylate intermediates. MnOx sites are required for further oxidation of the generated intermediates to the final products. Therefore, Langmuir–Hinshelwood dual-site (LHd) mechanism was evaluated to demonstrate the reaction pathway. The kinetic data were expressed well by LHd model, indicating that both MnOx and Al2O3 sites are essential and involved in the reaction. The cooperation of these sites on the surface of the catalyst provides the adjacent attack and migration of intermediates and enables the dual-site mechanism. The reaction order, activation energy, and kinetic parameters were determined for both catalysts and confirmed that the model is physically meaningful. Other than LHd, common Langmuir–Hinshelwood single-site (LHs) and power law (PL) kinetic models were tested to describe the acetone ozonation process and kinetic mechanism. Although the models can describe the reaction kinetic adequately, the LHs did not properly fit the experimental data suggesting that more than a single site is involved in the reaction and PL model in unable to provide the mechanistic view for the reaction.



中文翻译:

MnOx/Al2O3催化剂上空气中丙酮催化臭氧化的动力学及机理

研究了以多元醇和浸渍法制备的MnO x /Al 2 O 3催化剂对丙酮的催化臭氧化反应。合成的催化剂在室温下表现出优异的催化活性,转化率约为 95%。尽管许多研究集中在更有效地氧化 VOC 的催化过程上,但该反应背后的机制仍然未知。所述原位DRIFTS和活性的结果表明,氧化铝不仅充当用于MNO A支持X,但它也涉及在用丙酮进行反应和产生表面羧化物中间体。MnO的X生成的中间体进一步氧化为最终产物需要位点。因此,评估了 Langmuir-Hinshelwood 双位点 (LHd) 机制以证明反应途径。LHd 模型很好地表达了动力学数据,表明 MnO x和 Al 2 O 3位点是必不可少的并参与反应。这些位点在催化剂表面的合作提供了中间体的相邻攻击和迁移,并实现了双位点机制。确定了两种催化剂的反应顺序、活化能和动力学参数,并证实该模型具有物理意义。除了 LHd 之外,还测试了常见的 Langmuir-Hinshelwood 单中心 (LHs) 和幂律 (PL) 动力学模型来描述丙酮臭氧化过程和动力学机制。尽管模型可以充分描述反应动力学,但 LH 没有正确拟合实验数据,表明反应中涉及多个位点,而 PL 模型无法提供反应的机理视图。

更新日期:2021-07-16
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