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微波辐射下尖晶石型铜锰氧化物对苯氧化的催化性能增强

Enhanced catalytic performance of spinel-type Cu-Mn oxides for benzene oxidation under microwave irradiation.

作者信息

Ding Siyu, Zhu Chen, Hojo Hajime, Einaga Hisahiro

机构信息

Department of Molecular and Material Sciences, Graduate School of Engineering Sciences, Kyushu University, 6-1, Kasugakoen, Kasuga, Fukuoka 816-8580, Japan.

Department of Material Sciences, Faculty of Engineering Sciences, Kyushu University, 6-1, Kasugakoen, Kasuga, Fukuoka 816-8580, Japan.

出版信息

J Hazard Mater. 2022 Feb 15;424(Pt C):127523. doi: 10.1016/j.jhazmat.2021.127523. Epub 2021 Oct 16.

Abstract

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 H-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.

摘要

研究了Cu-Mn尖晶石氧化物对苯的微波辅助多相催化氧化。尖晶石氧化物通过共沉淀法,以四甲基氢氧化铵(TMAH)为沉淀剂,由金属硝酸盐在溶液中水解合成。采用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程序升温还原研究对催化剂进行了表征。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。在微波加热下,Cu/Mn比为1的Cu-Mn尖晶石氧化物表现出比单一氧化物更高的活性,其表观活化能低于传统加热条件下的表观活化能。与传统加热相比,微波辐射降低了苯氧化所需的反应温度。采用瞬态试验研究了催化反应中氧物种的反应活性,Cu-Mn尖晶石氧化物的高反应活性与催化剂表面晶格氧的高反应活性有关。在微波加热下,氧物种的反应活性增强,导致苯氧化反应增强。使用Cu-Mn尖晶石氧化物和沸石的吸附与催化氧化过程相结合,能够在低浓度下有效分解苯。

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