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Engineering Manganese Defects in Mn3O4 for Catalytic Oxidation of Carcinogenic Formaldehyde

机译:Mn3O4中的工程锰缺陷,用于致癌甲醛的催化氧化

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摘要

Formaldehyde (HCHO) is a priority pollutant in the indoor environment, which is irritative and carcinogenic to humans. The non-noble metal oxides have a wide application prospect in the decomposition of HCHO. Defects in metal oxides have been widely accepted as active sites in heterogeneous catalysis. Compared with the extensive study of oxygen defects, the effect of cation defects has not been clearly addressed. Herein, Mn defect-rich Mn_(3)O_(4) was synthesized by pyrolysis of Ce-doped MnCO_(3). It is found for the first time that the content of Mn defects in Mn_(3)O_(4) can be adjusted by introducing Ce. The introduction of Ce resulted in the higher contents of Mn defects, which significantly enhances the HCHO decomposition. Moreover, Mn defect can effectively narrow the half-metallic gap of Mn_(3)O_(4), regulate the electronic structure and coordination environment of surrounding oxygen, and further improve the activity and mobility of neighboring oxygen atoms. Importantly, Mn defects are not only beneficial to the generation of neighboring oxygen vacancy but also conducive to enhancing the activation ability of oxygen vacancy for O_(2). The advantages resulting from Mn defects significantly enhance the HCHO decomposition. This research proposes a strategy to adjust cation defects and deepens the comprehension of the function of cation defects.
机译:甲醛(HCHO)是室内环境中的首要污染物,对人体具有刺激性和致癌性。非贵金属氧化物在HCHO分解中具有广阔的应用前景。金属氧化物中的缺陷被广泛认为是多相催化中的活性中心。与对氧缺陷的广泛研究相比,阳离子缺陷的影响还没有得到明确的解决。在此,通过热解掺铈的MnCO_3合成了富含Mn缺陷的Mn_3)O_4。首次发现通过引入Ce可以调节Mn_3)O_4中Mn缺陷的含量。Ce的引入导致Mn缺陷的含量增加,从而显著促进了HCHO的分解。此外,Mn缺陷可以有效地缩小Mn_3)O_4的半金属间隙,调节周围氧的电子结构和配位环境,进一步提高相邻氧原子的活性和迁移率。重要的是,Mn缺陷不仅有利于相邻氧空位的生成,而且有利于提高氧空位对O_2(2)的活化能力。Mn缺陷带来的优势显著增强了HCHO分解。本研究提出了调整阳离子缺陷的策略,加深了对阳离子缺陷功能的理解。

著录项

  • 来源
    《ACS applied materials & interfaces》 |2021年第25期|共12页
  • 作者单位

    Jiangsu Key Laboratory of Chemical Pollution Control and Resources Reuse School of Environmental and Biological Engineering Nanjing University of Science and Technology;

    Jiangsu Key Laboratory of Chemical Pollution Control and Resources Reuse School of Environmental and Biological Engineering Nanjing University of Science and Technology;

    Jiangsu Key Laboratory of Chemical Pollution Control and Resources Reuse School of Environmental and Biological Engineering Nanjing University of Science and Technology;

    Jiangsu Key Laboratory of Chemical Pollution Control and Resources Reuse School of Environmental and Biological Engineering Nanjing University of Science and Technology;

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  • 原文格式 PDF
  • 正文语种 eng
  • 中图分类 化学工业;
  • 关键词

    formaldehyde; manganese defects; Mnlt; subgt; 3lt; /subgt; Olt; subgt; 4lt; /subgt; catalytic oxidation; DFT calculation;

    机译:甲醛;锰缺陷;Mn;sub;3/sub;O;sub;4/sub;催化氧化;DFT计算;

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