Promotional Effect of La in the Three-Way Catalysis of La-Loaded Al2O3-Supported Pd Catalysts (Pd/La/Al2O3)

催化作用 X射线光电子能谱 化学 氮氧化物 反应性(心理学) X射线吸收精细结构 多相催化 密度泛函理论 热稳定性 红外光谱学 物理化学 化学工程 光谱学 燃烧 计算化学 有机化学 物理 工程类 病理 医学 量子力学 替代医学
作者
Yuan Jing,Zhengxu Cai,Chong Liu,Takashi Toyao,Zen Maeno,Hiroyuki Asakura,Satoru Hiwasa,Shuhei Nagaoka,Hiroshi Kondoh,Ken‐ichi Shimizu
出处
期刊:ACS Catalysis [American Chemical Society]
卷期号:10 (2): 1010-1023 被引量:63
标识
DOI:10.1021/acscatal.9b03766
摘要

La-loaded Al2O3 (La/Al2O3) is a practical support for three-way catalysis (TWC) reactions. Although it has been reported that the addition of La to Al2O3 results in improved thermal stability to retain high specific surface areas, its effect on the catalytic reduction of NOx (DeNOx) has not been studied systematically. Herein, we describe the role of La in La/Al2O3-supported Pd catalysts (Pd/La/Al2O3) for TWC reactions. For that purpose, we employed various in situ spectroscopic studies, including infrared (IR), X-ray absorption fine structure (XAFS), and near-ambient-pressure X-ray photoelectron spectroscopy (NAP-XPS) in combination with density functional theory (DFT) calculations. The obtained results revealed that Pd0 species supported on La/Al2O3 are more electron-deficient compared to those on pristine Al2O3 without La(Pd/Al2O3). Kinetic studies using powdered catalysts revealed that the addition of La suppresses the poisoning effect by CO during the DeNOx reactions. In addition to the catalytic tests with powdered catalysts, monolithic honeycomb forms of the catalysts were prepared and employed for TWC reactions, which showed that Pd/La/Al2O3 exhibits higher DeNOx activity than Pd/Al2O3. In this study, we also reexamined the effective loading amount of La, which has traditionally been ∼3–5 wt % of La for TWC processes in order to retain the high specific surface area of the La/Al2O3 supports. Our investigations showed that an increased La loading (15 wt %) is even more effective for the DeNOx reactions tested in this study due to the higher reactivity toward NO and the greater suppression of the poisoning effect of CO. The developed catalyst Pd/La(15)/Al2O3 has also been tested in a commercial vehicle and has been evaluated on a practical driving mode test cycle (LA-4; city cycle of U.S. Federal and California), where it showed a better catalytic performance than the conventionally used Pd/La(3–5)/Al2O3 catalysts. Our study suggests that the loading amount of La in Pd/La/Al2O3 catalysts needs to be adjusted depending on the application systems, considering not only the support stability (surface areas) but also the promotional effect in the TWC process.
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