Metal-Containing Granulated Yh Zeolites with Hierarchic Structure in Isophorone Aromatization

IF 1.3 4区工程技术 Q3 CHEMISTRY, ORGANIC Petroleum Chemistry Pub Date : 2024-05-14 DOI:10.1134/S0965544124020038

N. G. Grigor’eva, V. Yu. Kirsanov, L. F. Korzhova, S. G. Karchevskii, A. N. Khazipova, S. V. Bubennov, V. R. Bikbaeva, D. V. Serebrennikov, B. I. Kutepov

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Abstract

The physicochemical properties of a series of catalysts based on granulated Na-Yh zeolite with the hierarchic (micro–meso–macro) pore structure (Na-Yh, HNa-Yh, MgO/Na-Yh, La₂O₃/Na-Yh, TiO₂/Na-Yh) and the activity and selectivity of these catalysts in isophorone aromatization were studied. MgO/Na-Yh and La₂O₃/Na-Yh zeolites with high content of basic sites and low content of Brønsted acid sites are the most effective in the synthesis of 3,5-dimethylphenol: The 3,5-dimethylphenol formation selectivity reaches 63–69% at 87–94% isophorone conversion. In the presence of Na-Yh zeolite containing both acid and base sites, the prevalent reactions are isophorone isomerization and synthesis of trimethylbenzenes. The modification of Na-Yh with titanium oxide leads to an increase in the content of acid sites on the TiO₂/Na-Yh surface and to the prevalence of the aromatization to form trimethylbenzenes. In the presence of HNa-Yh containing a set of the strongest Brønsted and Lewis acid sites, isophorone transforms into a mixture of polymethylbenzenes.

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异佛尔酮芳香化过程中具有层次结构的含金属粒状 Yh 沸石

摘要研究了一系列基于具有分级（微-中-宏）孔结构的粒状 Na-Yh 沸石催化剂（Na-Yh、HNa-Yh、MgO/Na-Yh、La2O3/Na-Yh、TiO2/Na-Yh）的理化性质，以及这些催化剂在异佛尔酮芳香化中的活性和选择性。碱性位点含量高、布氏酸位点含量低的 MgO/Na-Yh 和 La2O3/Na-Yh 沸石在合成 3,5-二甲基苯酚中最为有效：在异佛尔酮转化率为 87-94% 时，3,5-二甲基苯酚的生成选择性达到 63-69%。在含有酸和碱位点的 Na-Yh 沸石存在下，主要反应是异佛尔酮异构化和合成三甲苯。用氧化钛修饰 Na-Yh 后，TiO2/Na-Yh 表面的酸性位点含量增加，芳香化形成三甲基苯的反应更为普遍。在含有一组最强的布氏和路易斯酸位点的 HNa-Yh 存在下，异佛尔酮会转化为多甲基苯的混合物。

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来源期刊

Petroleum Chemistry 工程技术-工程：化工

CiteScore

2.50

自引率

21.40%

发文量

102

审稿时长

6-12 weeks

期刊介绍： Petroleum Chemistry (Neftekhimiya), founded in 1961, offers original papers on and reviews of theoretical and experimental studies concerned with current problems of petroleum chemistry and processing such as chemical composition of crude oils and natural gas liquids; petroleum refining (cracking, hydrocracking, and catalytic reforming); catalysts for petrochemical processes (hydrogenation, isomerization, oxidation, hydroformylation, etc.); activation and catalytic transformation of hydrocarbons and other components of petroleum, natural gas, and other complex organic mixtures; new petrochemicals including lubricants and additives; environmental problems; and information on scientific meetings relevant to these areas. Petroleum Chemistry publishes articles on these topics from members of the scientific community of the former Soviet Union.