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Cu and Fe Catalysts Based on Porous Aromatic Frameworks for Oxidation of Alkylaromatics
Industrial & Engineering Chemistry Research ( IF 3.8 ) Pub Date : 2024-12-25 , DOI: 10.1021/acs.iecr.4c03159
Victoria A. Makhova, Leonid A. Kulikov, Kirill A. Cherednichenko, Anton L. Maximov, Eduard A. Karakhanov

In this paper, we present a new simple approach to synthesizing catalysts for the oxidation of alkylaromatics based on the immobilization of metal ions by conventional ion exchange. By sulfation of high-stable porous polymers, porous aromatic framework (PAFs), we prepared the PAF-30-SO3H carrier, which was used for immobilization of Cu(II) and Fe(III) ions. The resulting Cu/PAF-30-SO3H and Fe/PAF-30-SO3H catalysts were successfully applied for the oxidation of ethylbenzene, 3-ethyltoluene, n-propylbenzene, Indane, and tetralin to the corresponding α-ketones. The catalysts were stable against metal leaching and showed high activity in alkylaromatics oxidation: The conversion of substrates reached 80% in 24 h at 80 °C, and did not decrease during for at least 5 cycles. The performance of catalysts was also compared with Cu/PAF-30-MEA and Fe/PAF-30-MEA catalysts, synthesized from PAF-30-MEA carrier, which structure was modified with monoethanolamine-based chelating groups. The structure of the materials and catalysts was established using advanced analytical techniques: low temperature N2 adsorption, elemental analysis, FTIR spectroscopy, solid state NMR, XPS, TEM, and EDX mapping.

中文翻译:


基于多孔芳烃框架的 Cu 和 Fe 催化剂用于烷基芳烃的氧化



在本文中,我们提出了一种新的简单方法,该方法基于通过常规离子交换固定化金属离子来合成用于烷基芳烃氧化的催化剂。通过对高稳定性多孔聚合物、多孔芳烃骨架 (PAF) 进行硫酸化,制备了 PAF-30-SO3H 载体,用于固定 Cu(II) 和 Fe(III) 离子。所得的Cu/PAF-30-SO3H和Fe/PAF-30-SO3H催化剂成功地用于将乙苯、3-乙基甲苯、丙苯、茚和四醇氧化成相应的α酮。催化剂对金属浸出稳定,在烷基芳烃氧化中表现出高活性:在 80 °C 下,底物的转化率在 24 小时内达到 80%,并且在至少 5 个循环期间没有降低。还将催化剂的性能与由 PAF-30-MEA 载体合成的 Cu/PAF-30-MEA 和 Fe/PAF-30-MEA 催化剂进行了比较,其结构由基于单乙醇胺的螯合基团修饰。材料和催化剂的结构是使用先进的分析技术建立的:低温 N2 吸附、元素分析、FTIR 光谱、固态 NMR、XPS、TEM 和 EDX 映射。
更新日期:2024-12-26
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