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掺杂锰的尖晶石铁氧体在煅烧过程中阳离子微结构的变化及其对甲醛催化氧化的影响。

The variation of cationic microstructure in Mn-doped spinel ferrite during calcination and its effect on formaldehyde catalytic oxidation.

机构信息

CAS Key Laboratory of Mineralogy and Metallogeny, Guangzhou Institute of Geochemistry, Chinese Academy of Sciences, Guangzhou 510640, PR China; Guangdong Provincial Key Laboratory of Mineral Physics and Materials, Guangzhou 510640, PR China.

CAS Key Laboratory of Mineralogy and Metallogeny, Guangzhou Institute of Geochemistry, Chinese Academy of Sciences, Guangzhou 510640, PR China; University of Chinese Academy of Sciences, Beijing 100049, PR China; Guangdong Provincial Key Laboratory of Mineral Physics and Materials, Guangzhou 510640, PR China.

出版信息

J Hazard Mater. 2016 Apr 5;306:305-312. doi: 10.1016/j.jhazmat.2015.12.035. Epub 2015 Dec 24.

Abstract

In this study, a series of Mn substituted spinel ferrites calcinated at different temperatures were used as catalysts for the oxidation of formaldehyde (HCHO). X-ray diffraction, Raman spectroscopy, X-ray photoelectron spectroscopy and H2 temperature-programmed reduction were conducted to characterize the structure and physico-chemical properties of catalysts, which were affected by calcination in the range of 200-600°C. Results show that all the ferrites were with spinel structure, and those calcinated in the range of 300-600°C were in the phase of maghemite. The calcination changed the valence and distribution of Mn and Fe on the ferrite surface, and accordingly the reducibility of ferrites. The HCHO catalytic oxidation test showed that with the increase of calcination temperature, the activity was initially improved until 400°C, but then decreased. The variation of HCHO conversion performance was well positively correlated to the variation of reduction temperature of surface Mn(4+) species. The remarkable effect of calcination on the catalytic activity of Mn-doped spinel ferrites for HCHO oxidation was discussed in view of reaction mechanism and variations in cationic microstructure of Mn-doped ferrites.

摘要

在这项研究中,使用了一系列在不同温度下煅烧的 Mn 取代尖晶石铁氧体作为甲醛(HCHO)氧化的催化剂。通过 X 射线衍射、拉曼光谱、X 射线光电子能谱和 H2 程序升温还原对催化剂的结构和物理化学性质进行了表征,这些性质受到 200-600°C 煅烧范围的影响。结果表明,所有铁氧体都具有尖晶石结构,在 300-600°C 范围内煅烧的铁氧体处于磁赤铁矿相。煅烧改变了铁氧体表面 Mn 和 Fe 的价态和分布,从而改变了铁氧体的还原性。HCHO 催化氧化试验表明,随着煅烧温度的升高,活性最初在 400°C 之前提高,但随后降低。表面 Mn(4+)物种还原温度的变化与 HCHO 转化率性能的变化呈良好的正相关。从反应机理和 Mn 掺杂铁氧体的阳离子微结构变化的角度讨论了煅烧对 Mn 掺杂尖晶石铁氧体催化 HCHO 氧化活性的显著影响。

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