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Promoting effect of basic metal additives on DeNOx reactions over Pt-based three-way catalysts
Journal of Catalysis ( IF 6.5 ) Pub Date : 2022-11-04 , DOI: 10.1016/j.jcat.2022.10.018
Yuan Jing , Gang Wang , Shinya Mine , Jumpei Kawai , Ryo Toyoshima , Hiroshi Kondoh , Xiaorui Zhang , Shuhei Nagaoka , Ken-ichi Shimizu , Takashi Toyao

Pt has been economically favored over Rh and Pd. However, Pt-based three-way catalysts (TWCs) have been studied less than Pd- and Rh-based TWCs; therefore, their properties have not yet been sufficiently evaluated, especially under conditions relevant to modern three-way catalysis operation, wherein deviations from stoichiometric conditions are often encountered. In this study, we examined the promotional effect of basic metal additives in Pt/M/Al2O3 (M = Ba, La, Sr) on the efficiency of three-way catalytic reactions. The catalytic activities of the Pt/M/Al2O3 catalysts for NO, CO, and total hydrocarbons were superior to those of Pt/Al2O3; moreover, Ba enhanced the catalytic activity of Pt-based catalysts more efficiently than La and Sr. The best-performing catalyst, Pt/Ba/Al2O3, was subjected to kinetic studies and various in situ/operando spectroscopic experiments, namely, X-ray absorption spectroscopy, infrared spectroscopy, and ambient-pressure X-ray photoelectron spectroscopy (AP-XPS), to investigate the role of Ba in the NO reduction reaction. The Pt0 species loaded on Ba/Al2O3 were more electron-rich than those loaded on Al2O3, thereby promoting NO dissociation into N and O atoms, as revealed by the AP-XPS results. Moreover, the efficient formation of intermediate surface NOx species, including nitrites and nitrates, and their reactivities toward reductant gases, such as H2 or CO, were critical for promoting the effect of Ba on the NO reduction reaction.



中文翻译:

碱性金属添加剂对铂基三元催化剂上脱硝反应的促进作用

Pt 在经济上比 Rh 和 Pd 更受青睐。然而,Pt 基三元催化剂 (TWCs) 的研究少于 Pd 和 Rh 基 TWCs;因此,它们的性质尚未得到充分评估,特别是在与现代三元催化操作相关的条件下,其中经常遇到与化学计量条件的偏差。在本研究中,我们研究了 Pt/M/Al 2 O 3 (M = Ba, La, Sr) 中碱性金属添加剂对三元催化反应效率的促进作用。Pt/M/Al 2 O 3催化剂对NO、CO和总烃的催化活性优于Pt/Al 2 O 3; 此外,Ba 比 La 和 Sr 更有效地增强了 Pt 基催化剂的催化活性。性能最佳的催化剂 Pt/Ba/Al 2 O 3进行了动力学研究和各种原位/操作光谱实验,即, X 射线吸收光谱、红外光谱和环境压力 X 射线光电子能谱 (AP-XPS),以研究 Ba 在 NO 还原反应中的作用。负载在 Ba/Al 2 O 3上的 Pt 0比负载在 Al 2 O 3上的更富电子,从而促进 NO 解离为 N 和 O 原子,如 AP-XPS 结果所示。此外,中间表面NO x物质(包括亚硝酸盐和硝酸盐)的有效形成及其对还原剂气体(如H 2或CO)的反应性对于促进Ba对NO还原反应的影响至关重要。

更新日期:2022-11-04
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