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不同形貌MnO催化剂上柴油烟灰的燃烧:阐明活性氧物种在烟灰燃烧中的作用

Diesel Soot Combustion over Mn O Catalysts with Different Morphologies: Elucidating the Role of Active Oxygen Species in Soot Combustion.

作者信息

Kuwahara Yasutaka, Kato Genki, Fujibayashi Akihiro, Mori Kohsuke, Yamashita Hiromi

机构信息

Division of Materials and Manufacturing Science Graduate School of Engineering, Osaka University, 2-1 Yamada-oka, Suita, Osaka, 565-0871, Japan.

Unit of Elements Strategy Initiative for Catalysts & Batteries (ESICB), Kyoto University Katsura, Kyoto, 615-8520, Japan.

出版信息

Chem Asian J. 2020 Jul 1;15(13):2005-2014. doi: 10.1002/asia.202000461. Epub 2020 Jun 5.

Abstract

Catalytic diesel soot combustion was examined using a series of Mn O catalysts with different morphologies, including plate, prism, hollow spheres and powders. The plate-shaped Mn O (Mn O -plate) exhibited superior carbon soot combustion activity compared to the prism-shaped, hollow-structured and powdery Mn O under both tight and loose contact modes at soot combustion temperatures (T ) of 327 °C and 457 °C, respectively. Comprehensive characterization studies using scanning electron microscopy, scanning transmission electron microscopy, X-ray diffraction, X-ray photoelectron spectroscopy, temperature-programmed reduction and oxygen release measurements, revealed that the improved activity of Mn O -plate was mainly attributed to the high oxygen release rate of surface-adsorbed active oxygen species, which originated from oxygen vacancy sites introduced during the catalyst preparation, rather than specific surface-exposed planes. The study provides new insights for the design and synthesis of efficient oxidation catalysts for carbon soot combustion as well as for other oxidation reactions of harmful hydrocarbon compounds.

摘要

使用一系列具有不同形态的MnO催化剂对催化柴油烟灰燃烧进行了研究,这些形态包括片状、棱柱状、空心球体和粉末状。在烟灰燃烧温度(T)分别为327°C和457°C的情况下,无论是紧密接触模式还是松散接触模式,片状MnO(MnO-片状)相较于棱柱状、空心结构和粉末状MnO都表现出卓越的碳烟灰燃烧活性。使用扫描电子显微镜、扫描透射电子显微镜、X射线衍射、X射线光电子能谱、程序升温还原和氧释放测量进行的综合表征研究表明,MnO-片状活性的提高主要归因于表面吸附活性氧物种的高氧释放速率,这源于催化剂制备过程中引入的氧空位,而非特定的表面暴露平面。该研究为设计和合成用于碳烟灰燃烧以及其他有害碳氢化合物氧化反应的高效氧化催化剂提供了新的见解。

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