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

被引:176
作者
Xiang, Jing [1 ]
Wu, Qiangqiang [1 ]
Mei, Xuelei [1 ]
Liu, Jian [1 ]
Wei, Yuechang [1 ]
Zhao, Zhen [1 ]
Wu, Dan [1 ]
Li, Jianmei [1 ]
机构
[1] China Univ Petr, Coll Sci, State Key Lab Heavy Oil Proc, Beijing 102249, Peoples R China
基金
中国国家自然科学基金; 北京市自然科学基金;
关键词
3DOMM materials; ceria-zirconia solid solution; spinel-type active site; PdxCa3-xO4; nanoparticles; soot oxidation; LOW-TEMPERATURE OXIDATION; CORE-SHELL NANOPARTICLES; GOLD NANOPARTICLES; IN-SITU; OXYGEN REDUCTION; FACILE SYNTHESIS; SOLID-SOLUTIONS; DIESEL SOOT; COMBUSTION; CERIA;
D O I
10.1021/acscatal.8b01924
中图分类号
O64 [物理化学(理论化学)、化学物理学];
学科分类号
070304 ; 081704 ;
摘要
3D ordered meso-macroporous (3DOMM) CeZ(0.2)Zr(0.8)O(2) (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, H-2-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, O-2, and NO) and catalysts. Spinel-type PdxCo3-xO4 (AB(2)O(4)) binary active sites by substitution for Co2+ (A site) with Pd2+ cations are beneficial for improving activation efficiency for gaseous reactants (NO and O-2). 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 T-10, T-50, and T-90 values of 3DOMM PdCo2O4/CZO catalyst with the highest catalytic activity (TOF = 2.56 h(-1)) are only 313, 367, and 404 degrees 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.
引用
收藏
页码:7915 / 7930
页数:31
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