Catalytic performance of Pt-Rh/CeZrYLa+LaAl with stoichiometric natural gas vehicles emissions

doi:10.1016/S1872-2067(14)60270-9

Chinese Journal of Catalysis ›› 2015, Vol. 36 ›› Issue (3): 290-298.DOI: 10.1016/S1872-2067(14)60270-9

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Catalytic performance of Pt-Rh/CeZrYLa+LaAl with stoichiometric natural gas vehicles emissions

Hongyan Shang^a, Yun Wang^b, Yajuan Cui^c, Ruimei Fang^a, Wei Hu^a, Maochu Gong^d, Yaoqiang Chen^a,c,d

a College of Chemical Engineering, Sichuan University, Chengdu 610065, Sichun, China;
b Sichuan Zhongzi Exhaust Gas Cleaning Co., Ltd., Chengdu 611731, Sichuan, China;
c College of Architecture and Environment, Sichuan University, Chengdu 610065, Sichuan, China;
d Key Laboratory of Green Chemistry & Technology of Ministry of Education, College of Chemistry, Sichuan University, Chengdu 610064, Sichun, China

Received:2014-10-19 Revised:2014-12-12 Online:2015-02-14 Published:2015-02-14
Supported by:
This work was supported by the National Natural Science Foundation of China (21173153) and the Science and Technology Department of Science and Technology Support Project of Sichuan Province, China (2011GZ0035).

Abstract

Abstract:

The composite support CeZrYLa+LaAl was prepared by a co-precipitation method, and Pt-Rh bimetallic catalysts were fabricated on this support using different preparation procedures. The catalytic activities of these materials were tested in a gas mixture simulating the exhaust from a stoichiometric natural gas vehicle. The as-prepared catalysts were also characterized by X-ray photoelectron spectroscopy, X-ray diffraction, N₂ adsorption-desorption and H₂-temperature-programmed reduction. It was found that the order of activities for CH₄, CO and NO conversion was Cat3 ≈ Cat2 > Cat1, where Cat3 had the lowest light-off temperature (T₅₀) for CO (114 ℃) and NO (149 ℃), the lowest complete conversion temperature (T₉₀) for CH₄ (398 ℃) and CO (179 ℃), and the lowest ΔT (T₉₀-T₅₀) for CH₄ (34 ℃) and CO (65 ℃). Cat2 showed the lowest T₅₀ for CH₄ (342 ℃), the lowest T₉₀ for NO (174 ℃), and the lowest ΔT for NO (17 ℃). Cat1 had the highest T₅₀ and T₉₀ and the largest ΔT out of all three catalysts. Indicating that Pt-Rh bimetallic catalysts (Cat2 and Cat3) prepared by physically mixing Pt and Rh powders exhibited much better catalytic activity than those (Cat1) prepared by co-impregnation, since homogeneous Pt and Rh sites made a significant contribution to CH₄/CO/NO conversions. In contrast, strong Pt-Rh interactions in the co-impregnation materials affected the oxidation states of Pt, and the Pt-enriched surface blocked active Rh sites. Moreover, Cat3 was prepared by adding additives (La³⁺, Zr⁴⁺ and Ba²⁺) into the physically mixed Pt-Rh catalysts. XRD results demonstrated that the additive cation (Zr⁴⁺) was incorporated into the CeO₂-ZrO₂ lattice, thus creating a higher concentration of defects and improving the O₂-mobility. XPS results showed that the Cat3 had the highest Ce³⁺/Ce ratio, suggesting the presence of a significant quantity of oxygen vacancies and cerium in the Ce³⁺ state. All of these further promoted the three-way catalytic activity and widened the air-to-fuel working-window.

Key words: Platium-rhodium, Nanocomposite CeZrYLa+LaAl, La-Zr-Ba additive, Stoichiometric natural gas vehicle, Exhaust purification

Hongyan Shang, Yun Wang, Yajuan Cui, Ruimei Fang, Wei Hu, Maochu Gong, Yaoqiang Chen. Catalytic performance of Pt-Rh/CeZrYLa+LaAl with stoichiometric natural gas vehicles emissions[J]. Chinese Journal of Catalysis, 2015, 36(3): 290-298.

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Catalytic performance of Pt-Rh/CeZrYLa+LaAl with stoichiometric natural gas vehicles emissions

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