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Enhanced catalytic performance of spinel-type Cu-Mn oxides for benzene oxidation under microwave irradiation
Journal of Hazardous Materials ( IF 12.2 ) Pub Date : 2021-10-16 , DOI: 10.1016/j.jhazmat.2021.127523
Siyu Ding 1 , Chen Zhu 1 , Hajime Hojo 2 , Hisahiro Einaga 2
Affiliation  

Microwave-assisted heterogeneous catalytic oxidation of benzene was investigated over Cu-Mn spinel oxides. The spinel oxides were synthesized by a coprecipitation method from metal nitrate hydrolysis in a solution using tetramethylammonium hydroxide (TMAH) as a precipitation reagent. The catalysts were characterized by X-ray diffraction, X-ray photoelectron spectroscopy, X-ray absorption fine structure, scanning electron microscopy, transmission electron microscope and H2-temperature-programmed reduction studies. Microwave absorption by the Cu-Mn spinel oxide is mainly driven by dielectric losses (dielectric heating). Cu-Mn spinel oxide with a Cu/Mn ratio of 1 exhibited superior activity to single oxides under microwave heating, demonstrating lower apparent activation energy than that obtained under conventional heating. Microwave irradiation lowered the reaction temperature required for benzene oxidation compared with conventional heating. Transient tests were used to investigate the reactivity of oxygen species in the catalytic reaction, and the high reactivity of Cu-Mn spinel oxides was related to the high reactivity of lattice oxygen on the catalyst surface. The reactivity of the oxygen species was enhanced under microwave heating, leading to an enhanced benzene oxidation reaction. The combination of adsorption and catalytic oxidation processes using Cu-Mn spinel oxides and zeolites efficiently decomposed benzene at low concentrations.



中文翻译:

尖晶石型Cu-Mn氧化物在微波辐射下对苯氧化的增强催化性能

在 Cu-Mn 尖晶石氧化物上研究了苯的微波辅助多相催化氧化。尖晶石氧化物是通过共沉淀法从金属硝酸盐在溶液中水解合成的,使用四甲基氢氧化铵 (TMAH) 作为沉淀试剂。通过X射线衍射、X射线光电子能谱、X射线吸收精细结构、扫描电子显微镜、透射电子显微镜和H 2-程序升温还原研究。Cu-Mn 尖晶石氧化物的微波吸收主要由介电损耗(介电加热)驱动。Cu/Mn 比为 1 的 Cu-Mn 尖晶石氧化物在微波加热下表现出优于单一氧化物的活性,表现出比常规加热下获得的表观活化能更低。与传统加热相比,微波辐射降低了苯氧化所需的反应温度。瞬态试验用于研究氧物种在催化反应中的反应性,Cu-Mn 尖晶石氧化物的高反应性与催化剂表面晶格氧的高反应性有关。在微波加热下氧物种的反应性增强,导致苯氧化反应增强。

更新日期:2021-11-02
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