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负载于三维有序大孔-介孔钛硅催化剂上的碱/碱土金属改性MnO:制备及其对碳烟燃烧的催化性能

Alkali/alkaline-earth metal-modified MnO supported on three-dimensionally ordered macroporous-mesoporous TiSiO catalysts: Preparation and catalytic performance for soot combustion.

作者信息

Peng Chao, Yu Di, Zhang Chunlei, Chen Maozhong, Wang Lanyi, Yu Xuehua, Fan Xiaoqiang, Zhao Zhen, Cheng Kai, Chen Yongsheng, Wei Yuechang, Liu Jian

机构信息

Institute of Catalysis for Energy and Environment, College of Chemistry and Chemical Engineering, Shenyang Normal University, Shenyang 110034, China.

State Key Laboratory of Heavy Oil Processing, China University of Petroleum, Beijing 102249, China.

出版信息

J Environ Sci (China). 2023 Mar;125:82-94. doi: 10.1016/j.jes.2021.10.029. Epub 2022 Feb 3.

Abstract

The performance of catalysts used in after-treatment systems is the key factor for the removal of diesel soot, which is an important component of atmospheric fine particle emissions. Herein, three-dimensionally ordered macroporous-mesoporous TiSiO (3DOM-m TiSiO) and its supported MnO catalysts doped with different alkali/alkaline-earth metals (AMnO/3DOM-m TiSiO (A: Li, Na, K, Ru, Cs, Mg, Ca, Sr, Ba)) were prepared by mesoporous template (P123)-assisted colloidal crystal template (CCT) and incipient wetness impregnation methods, respectively. Physicochemical characterizations of the catalysts were performed using scanning electron microscopy, X-ray diffraction, N adsorption-desorption, H temperature-programmed reduction, O temperature-programmed desorption, NO temperature-programmed oxidation, and Raman spectroscopy techniques; then, we evaluated their catalytic performances for the removal of diesel soot particles. The results show that the 3DOM-m TiSiO supports exhibited a well-defined 3DOM-m nanostructure, and AMnO nanoparticles with 10-50 nm were evenly dispersed on the inner walls of the uniform macropores. In addition, the as-prepared catalysts exhibited good catalytic performance for soot combustion. Among the prepared catalysts, CsMnO/3DOM-m TiSiO had the highest catalytic activity for soot combustion, with T, T, and T (the temperatures corresponding to soot conversion rates of 10%, 50%, and 90%) values of 285, 355, and 393°C, respectively. The high catalytic activity of the CsMnO/3DOM-m TiSiO catalysts was attributed to their excellent low-temperature reducibility and homogeneous macroporous-mesoporous structure, as well as to the synergistic effects between Cs and Mn species and between CsMnO and the TiSiO support.

摘要

后处理系统中使用的催化剂性能是去除柴油烟灰的关键因素,柴油烟灰是大气细颗粒物排放的重要组成部分。在此,分别通过介孔模板(P123)辅助胶体晶体模板(CCT)法和初湿浸渍法制备了三维有序大孔-介孔TiSiO(3DOM-m TiSiO)及其负载不同碱金属/碱土金属的MnO催化剂(AMnO/3DOM-m TiSiO(A:Li、Na、K、Ru、Cs、Mg、Ca、Sr、Ba))。采用扫描电子显微镜、X射线衍射、N吸附-脱附、H程序升温还原、O程序升温脱附、NO程序升温氧化和拉曼光谱技术对催化剂进行了物理化学表征;然后,评估了它们对柴油烟灰颗粒的催化去除性能。结果表明,3DOM-m TiSiO载体呈现出明确的3DOM-m纳米结构,10-50 nm的AMnO纳米颗粒均匀分散在均匀大孔的内壁上。此外,所制备的催化剂对烟灰燃烧表现出良好的催化性能。在所制备的催化剂中,CsMnO/3DOM-m TiSiO对烟灰燃烧具有最高的催化活性,其T10、T50和T90(烟灰转化率分别为10%、50%和90%时对应的温度)值分别为285、355和393°C。CsMnO/3DOM-m TiSiO催化剂的高催化活性归因于其优异的低温还原性和均匀的大孔-介孔结构,以及Cs和Mn物种之间以及CsMnO与TiSiO载体之间的协同效应。

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