Highlights on the key roles of interfaces between CeO2-based oxide and perovskite (LaMnO3/LaFeO3) in creating active oxygen species for soot oxidation

高分辨率透射电子显微镜 烟灰 氧气 X射线光电子能谱 钙钛矿(结构) 氧化物 催化作用 材料科学 化学工程 化学 无机化学 透射电子显微镜 纳米技术 结晶学 燃烧 物理化学 有机化学 工程类 冶金
作者
Linmei Wang,Nanrong Zhao,Xinyi Yin,Wei Wang,Yi Zhao,Zixuan Zheng,Shanshan Li,Jianli Wang,Yaoqiang Chen
出处
期刊:Fuel [Elsevier]
卷期号:356: 129444-129444 被引量:13
标识
DOI:10.1016/j.fuel.2023.129444
摘要

Design efficient catalyst which can activate oxygen molecules or supply active oxygen species is a key challenge for soot abatement under the much lower concentration of oxygen from gasoline vehicle exhaust. Herein, combining with the advantages of both CeO2-based oxide (CeO2–ZrO2–Y2O3–La2O3, CZ for short) and perovskite (LaMnO3 and LaFeO3) in oxygen storage/release, two hybrids catalysts, CZ-LaMnO3 (LM) and CZ-LaFeO3 (LF), with more oxygen vacancies and enhanced lattice oxygen transport at lower temperatures due to the heterointerface effects have been successfully synthesized for soot oxidation. Combining with X-ray diffraction (XRD), high-resolution transmission electron microscopy (HRTEM), X-ray photoelectron spectroscopy (XPS), oxygen temperature-programmed desorption (O2-TPD) and H2 temperature-programmed reduction (H2-TPR), it was found that electrons transfer from Ce3+ to Fe3+ and an interfacial La diffusion from LM to CZ may have been occurred in LF-CZ and LM-CZ, respectively, which leads to the increased unsaturated sites and oxygen vacancies. More importantly, the obvious enhancement of active surface lattice oxygen transport at low temperatures due to interfacial interaction has also been demonstrated in LM-CZ, which highly promotes the soot oxidation. And consequently, 5LM-CZ (with 5 wt% content of LM) showed the highest soot conversion activity, whose T50 (50 % soot conversion temperature) (379 °C) was lower than 5LF-CZ (395 °C) and CZ (401°C) at tight contact mode in 1 %O2/N2 atmosphere, indicating that the activation of lattice oxygen at the interface plays an important role in soot oxidation. Furthermore, when further varying the content of LM in xLM-CZ (x = 5 wt%, 10 wt%, 15 wt%, 20 wt%), it was found that 10LM-CZ, whose content of LM reached the monolayer dispersion capacity of CZ, exhibited the most abundant active surface lattice oxygen species due to the optimized interface area. As a result, 10LM-CZ displayed superior activity even than pure LM in both loose and tight contact with/without NO, indicating that the composite catalyst has a wide application environment. This work has a certain guiding significance for the utilization of heterointerface effect among different components to prepare effective soot oxidation catalyst with multi-components.
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