Fabrication of Spinel-Type PdxCo3–xO4 Binary Active Sites on 3D Ordered Meso-macroporous Ce-Zr-O2 with Enhanced Activity for Catalytic Soot Oxidation

尖晶石 催化作用 烟灰 纳米材料基催化剂 材料科学 化学工程 共沉淀 纳米结构 X射线光电子能谱 纳米颗粒 无机化学 化学 纳米技术 物理化学 燃烧 有机化学 冶金 工程类
作者
Jing Xiong,Qiangqiang Wu,Xuelei Mei,Jian Liu,Yuechang Wei,Zhen Zhao,Dan Wu,Jianmei Li
出处
期刊:ACS Catalysis [American Chemical Society]
卷期号:8 (9): 7915-7930 被引量:183
标识
DOI:10.1021/acscatal.8b01924
摘要

3D ordered meso-macroporous (3DOMM) Ce0.2Zr0.8O2 (CZO) was successfully synthesized by a combined method of evaporation-induced interfacial self-assembly (EISA) and colloidal crystal templates (CCT). The multifunctional catalysts of spinel-type PdxCo3–xO4 nanoparticles (NPs) supported on 3DOMM CZO were fabricated by a gas bubbling assisted coprecipitation (GBCP) method. The relationship between nanostructure (hierarchical pore and spinel-type active phase) and activity during catalytic soot oxidation was studied by the techniques of SEM, TEM, XPS, H2-TPR, NO oxidation, soot-TPO, and so on. The 3DOMM structure with a larger surface area and total pore volume increases the amount of supported active sites and enhances the contact efficiency between reactants (soot, O2, and NO) and catalysts. Spinel-type PdxCo3–xO4 (AB2O4) binary active sites by substitution for Co2+ (A site) with Pd2+ cations are beneficial for improving activation efficiency for gaseous reactants (NO and O2). The novel nanocatalysts of 3DOMM CZO-supported spinel-type PdxCo3–xO4 NPs exhibited superb catalytic performance and strong nanostructure-dependent activity for soot oxidation under loose contact of soot with catalyst. For instance, the T10, T50, and T90 values of 3DOMM PdCo2O4/CZO catalyst with the highest catalytic activity (TOF = 2.56 h–1) are only 313, 367, and 404 °C, respectively. The NO2-assisted catalytic mechanism for soot oxidation is studied and proposed by in situ Raman spectra, and the role of spinel-type PdCo2O4 binary active sites is revealed. 3DOMM PdxCo3–xO4/CZO catalysts are decent systems for soot oxidation, and the easy preparation technology has the potential for application to catalysts with other element compositions.

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