The key role of Brønsted acid sites in olefin metathesis over promoted MoO3/Al2O3 catalytic systems

IF 6.5 1区 化学 Q2 CHEMISTRY, PHYSICAL Journal of Catalysis Pub Date : 2024-05-29 DOI:10.1016/j.jcat.2024.115578
Alexander I. Nikiforov , Evgeny A. Chesnokov , Andrey G. Popov , Irina I. Ivanova
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Abstract

One important way to increase the production of higher-margin products from less valuable unsaturated hydrocarbons is the widely used process of catalytic metathesis. Progress in the development of more advanced metathesis catalysts is hampered by obvious gaps in scientific knowledge about this process. This work is aimed at establishing the influence of physicochemical properties of Mo-containing lower olefins metathesis catalysts and developing methods for increasing their activity through promotion. A classic support for Mo-oxide metathesis catalyst was promoted with NH4HF2, (NH4)2SiF6, H3BO3 additives. The synthesized systems were analyzed by a large set of methods. The catalytic properties of obtained systems were determined in the propylene metathesis reaction. It was shown that the proposed promotion leads to an increase in activity of the catalyst up to 8.5 times. It was shown that strong Brønsted acid sites play a decisive role in increasing activity. In addition, it has been experimentally proven that the formation of active centers occurs when the substrate interacts with Brønsted, but not Lewis acid sites on the surface of the catalyst. The discoveries obtained in this work can serve as the basis for the creation of a new generation highly active lower olefins metathesis catalysts.

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布氏酸位点在促进的氧化钼/氧化铝催化体系上的烯烃复分解反应中的关键作用
利用价值较低的不饱和碳氢化合物生产利润更高的产品的一个重要方法是广泛使用的催化偏析过程。由于对这一过程的科学认识存在明显差距,阻碍了在开发更先进的偏析催化剂方面取得进展。这项工作旨在确定含钼低级烯烃偏析催化剂理化性质的影响,并开发通过促进提高其活性的方法。研究人员使用 NH4HF2、(NH4)2SiF6 和 H3BO3 添加剂对氧化钼偏合成催化剂的经典载体进行了促进。通过大量方法对合成的体系进行了分析。测定了所获体系在丙烯偏析反应中的催化特性。结果表明,拟议的促进作用可使催化剂的活性提高 8.5 倍。结果表明,强勃氏酸位点在提高活性方面起着决定性作用。此外,实验还证明,当底物与催化剂表面的布氏酸位点而非路易斯酸位点相互作用时,活性中心就会形成。这项研究的发现可作为制造新一代高活性低级烯烃偏析催化剂的基础。
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来源期刊
Journal of Catalysis
Journal of Catalysis 工程技术-工程:化工
CiteScore
12.30
自引率
5.50%
发文量
447
审稿时长
31 days
期刊介绍: The Journal of Catalysis publishes scholarly articles on both heterogeneous and homogeneous catalysis, covering a wide range of chemical transformations. These include various types of catalysis, such as those mediated by photons, plasmons, and electrons. The focus of the studies is to understand the relationship between catalytic function and the underlying chemical properties of surfaces and metal complexes. The articles in the journal offer innovative concepts and explore the synthesis and kinetics of inorganic solids and homogeneous complexes. Furthermore, they discuss spectroscopic techniques for characterizing catalysts, investigate the interaction of probes and reacting species with catalysts, and employ theoretical methods. The research presented in the journal should have direct relevance to the field of catalytic processes, addressing either fundamental aspects or applications of catalysis.
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