Abstract Ceria-zirconia based mixed oxides (CZs) have been applied in three-way catalysts (TWCs) for their high surface area and oxygen storage capacity (OSC). In this work, enhanced thermal stability of Ce0.33Zr0.55(LaNdY)0.12O2 mixed oxides was realized via a facile and scalable approach, namely, sulfate-aided coprecipitation method (CZ-S). Sulfate ion ( SO 4 2 − ) was added into raw solution in the form of sulfuric acid and acted as coordination agent. The control sample was prepared by conventional coprecipitation method without sulfuric acid added and labelled as CZ. The promotion effect of sulfate ion was analyzed systematically by X-ray diffraction (XRD), transmission electron microscopy (TEM), scanning electron microscopy (SEM), N2 adsorption-desorption, Fourier transform infrared spectroscopy (FT-IR), X-ray photoelectron spectroscopy (XPS), OSC and hydrogen temperature-programmed reduction (H2-TPR) analysis. XRD and high resolution TEM results reveal that CZ-S have homogeneous distributions of elements. TEM and SEM images show that fresh samples of CZ-S have narrower distributions of grain sizes and larger pore sizes than those of CZ. Through cross analysis of structure and morphology of CZ and CZ-S, we found that the introduction of sulfate ions results in uniform distributions of elements, narrow distributions of grain sizes, and enables the formation of secondary loose packing of sub-particles, which lead to enhanced thermal stability of the samples of CZ-S upon aging process at high temperature. After aging treatment at 1100 °C for 10 h, aged samples of CZ-S present larger specific surface areas and pore volumes than the aged sample prepared by conventional coprecipitation method without sulfate ions added. Furthermore, the aged sample of CZ-S2 ( SO 4 2 − /Zr = 1) possesses the highest specific surface area of 21.9 m2/g and the biggest pore volume of 0.035 mL/g among all aged samples.

中文翻译：

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硫酸盐辅助共沉淀法制备Ce0.33Zr0.55(LaNdY)0.12O2混合氧化物的热稳定性增强

摘要 氧化铈-氧化锆基混合氧化物（CZs）因其高表面积和储氧能力（OSC）而被应用于三元催化剂（TWCs）。在这项工作中，通过一种简便且可扩展的方法，即硫酸盐辅助共沉淀法 (CZ-S)，实现了 Ce0.33Zr0.55(LaNdY)0.12O2 混合氧化物的热稳定性增强。硫酸根离子（SO 4 2 - ）以硫酸的形式加入原液中作为配位剂。对照样品采用常规共沉淀法制备，不添加硫酸并标记为 CZ。通过X射线衍射（XRD）、透射电子显微镜（TEM）、扫描电子显微镜（SEM）、N2吸附-解吸、傅里叶变换红外光谱（FT-IR）等系统分析了硫酸根离子的促进作用，X 射线光电子能谱 (XPS)、OSC 和氢气程序升温还原 (H2-TPR) 分析。XRD 和高分辨率 TEM 结果表明 CZ-S 具有均匀的元素分布。TEM 和 SEM 图像显示，与 CZ 相比，CZ-S 的新鲜样品具有更窄的粒度分布和更大的孔径。通过对 CZ 和 CZ-S 结构和形貌的交叉分析，我们发现硫酸根离子的引入导致元素分布均匀，晶粒尺寸分布窄，并能够形成亚颗粒的二次松散堆积，导致提高 CZ-S 样品在高温老化过程中的热稳定性。1100℃时效处理10h后，与不添加硫酸根离子的常规共沉淀法制备的老化样品相比，CZ-S 老化样品具有更大的比表面积和孔体积。此外，CZ-S2（SO 4 2 - /Zr = 1）的老化样品在所有老化样品中具有最高的比表面积21.9 m2/g和最大的孔体积0.035 mL/g。