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Issue 13, 2017
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Catalysts of self-assembled Pt@CeO2−δ-rich core–shell nanoparticles on 3D ordered macroporous Ce1−xZrxO2 for soot oxidation: nanostructure-dependent catalytic activity

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Abstract

The catalytic performance in heterogeneous catalytic reactions consisting of solid reactants is strongly dependent on the nanostructure of the catalysts. Metal-oxides core–shell (MOCS) nanostructures have potential to enhance the catalytic activity for soot oxidation reactions as a result of optimizing the density of active sites located at the metal–oxide interface. Here, we report a facile strategy for fabricating nanocatalysts with self-assembled Pt@CeO2−δ-rich core–shell nanoparticles (NPs) supported on three-dimensionally ordered macroporous (3DOM) Ce1−xZrxO2via the in situ colloidal crystal template (CCT) method. The nanostructure-dependent activity of the catalysts for soot oxidation were investigated by means of SEM, TEM, H2-TPR, XPS, O2-isothermal chemisorption, soot-TPO and so on. A CeO2−δ-rich shell on a Pt core is preferentially separated from Ce1−xZrxO2 precursors and could self-assemble to form MOCS nanostructures. 3DOM structures can enhance the contact efficiency between catalysts and solid reactants (soot). Pt@CeO2−δ-rich core–shell nanostructures can optimize the density of oxygen vacancies (Ov) as active sites located at the interface of Pt–Ce1−xZrxO2. Remarkably, 3DOM Pt@CeO2−δ-rich/Ce1−xZrxO2 catalysts show super catalytic performance and strongly nanostructure-dependent activity for soot oxidation in the absence of NO and NO2. For example, the T50 of the 3DOM Pt@CeO2−δ-rich/Ce0.8Zr0.2O2 catalyst is lowered down to 408 °C, and the reaction rate of the 3DOM Pt@CeO2−δ-rich/Ce0.2Zr0.8O2 catalyst (0.12 μmol g−1 s−1) at 300 °C is 4 times that of the 3DOM Pt/Ce0.2Zr0.8O2 catalyst (0.03 μmol g−1 s−1). The structures of 3DOM Ce1−xZrxO2-supported Pt@CeO2−δ-rich core–shell NPs are decent systems for deep oxidation of solid reactants or macromolecules, and this facile technique for synthesizing catalysts has potential to be applied to other element compositions.

Graphical abstract: Catalysts of self-assembled Pt@CeO2−δ-rich core–shell nanoparticles on 3D ordered macroporous Ce1−xZrxO2 for soot oxidation: nanostructure-dependent catalytic activity

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Publication details

The article was received on 14 Jan 2017, accepted on 04 Mar 2017 and first published on 09 Mar 2017


Article type: Paper
DOI: 10.1039/C7NR00326A
Citation: Nanoscale, 2017,9, 4558-4571
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    Catalysts of self-assembled Pt@CeO2−δ-rich core–shell nanoparticles on 3D ordered macroporous Ce1−xZrxO2 for soot oxidation: nanostructure-dependent catalytic activity

    Y. Wei, J. Jiao, X. Zhang, B. Jin, Z. Zhao, J. Xiong, Y. Li, J. Liu and J. Li, Nanoscale, 2017, 9, 4558
    DOI: 10.1039/C7NR00326A

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