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Fe-Doped Mesoporous Alumina: Facile One-Pot Synthesis, Modified Surface-Acidity and Its Enhanced Catalytic Performance in Phenol Hydroxylation
Catalysis Letters ( IF 2.3 ) Pub Date : 2020-02-23 , DOI: 10.1007/s10562-020-03153-8
Yongjuan Wang , Yuming Zhou , Man He , Qiang He , Yangyang Zhong

Abstract Fe-doped mesoporous alumina (MA) was successfully synthesized via a facile one-pot synthesis method. The resulting Fe-doped MA samples possess typical mesoporous structure, relatively high BET surface area, and narrowed pore size diameter. Besides, the iron species are well-dispersed in the alumina matrix, and more importantly, some small oligonuclear iron oxide clusters are linked on the surface of alumina, leading to the elimination of strong acid sites. The reaction of phenol hydroxylation was preceded at room temperature for 2 h. The introduction of mesoporous structure in alumina would be favorable for the adsorption and diffusion process of reactant and product molecules, and also the well-dispersed iron species in alumina matrix and large amount of acid sites stimulate more active hydroxyl radicals which are greatly beneficial for the catalytic process, especially the elimination of strong acid sites would inhibit the over-oxidation reaction. In this case, the sample of 5Fe–MA displays the best catalytic performance especially with the extremely high dihydroxybenzene selectivity of 93.2%, and the good catalytic stability is also evidenced by the five times recycling tests. Graphic Abstract In this work, the Fe-doped mesoporous alumina (MA) was successfully prepared. The iron species are well-dispersed in the alumina matrix, and some small oligonuclear iron oxide clusters are linked on the surface of alumina, leading to the elimination of strong acid sites. The advanced properties of mesoporous structure, well-dispersed metal active centers and lack of strong acid sites in Fe-doped MA are greatly beneficial for the catalytic process, especially for the dihydroxybenzene selectivity with extremely high value of 93.2%.

中文翻译:

Fe掺杂的介孔氧化铝:简便的一锅法合成,改性表面酸度及其在苯酚羟基化中增强的催化性能

摘要 通过简便的一锅法合成铁掺杂介孔氧化铝(MA)。所得的 Fe 掺杂 MA 样品具有典型的介孔结构、相对较高的 BET 表面积和较窄的孔径。此外,铁物质在氧化铝基体中分散良好,更重要的是,一些小的寡核氧化铁簇连接在氧化铝表面,导致强酸位点的消除。酚羟基化反应在室温下进行2小时。在氧化铝中引入介孔结构有利于反应物和产物分子的吸附和扩散过程,并且氧化铝基体中分散良好的铁物种和大量的酸性位点会激发更多的活性羟基自由基,这对催化过程非常有利,特别是强酸性位点的消除会抑制过氧化反应。在这种情况下,5Fe-MA 样品表现出最好的催化性能,特别是具有 93.2% 的极高的二羟基苯选择性,并且良好的催化稳定性也得到了五次回收试验的证明。图形摘要 在这项工作中,成功地制备了Fe 掺杂的介孔氧化铝(MA)。铁物种在氧化铝基体中分散良好,一些小的寡核氧化铁簇连接在氧化铝表面,导致强酸位点的消除。介孔结构的先进性能,
更新日期:2020-02-23
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