Cooperative effect between copper species and oxygen vacancy in Ce0.7−xZrxCu0.3O2 catalysts for carbon monoxide oxidation

doi:10.1007/s11705-021-2106-2

Front. Chem. Sci. Eng.

2021, Vol. 15

Issue (6) : 1524-1536 https://doi.org/10.1007/s11705-021-2106-2

RESEARCH ARTICLE

Cooperative effect between copper species and oxygen vacancy in Ce_0.7−_xZr_xCu_0.3O₂ catalysts for carbon monoxide oxidation

Shan Wang^1,², Xuelian Xu², Ping Xiao², Junjiang Zhu²(

), Xinying Liu¹(

)

¹. Institute for the Development of Energy for African Sustainability, College of Science, Engineering and Technology, University of South Africa, Johannesburg 1710, South Africa
². Hubei Key Laboratory of Biomass Fibers and Eco-dyeing & Finishing, College of Chemistry and Chemical Engineering, Wuhan Textile University, Wuhan 430200, China

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Abstract

The effects of Zr doping on the existence of Cu and the catalytic performance of Ce_0.7−_xZr_xCu_0.3O₂ for CO oxidation were investigated. The characterization results showed that all samples have a cubic structure, and a small amount of Zr doping facilitates Cu²⁺ ions entering the CeO₂ lattice, but excessive Zr doping leads to the formation of surface CuO crystals again. Thus, the number of oxygen vacancies caused by the Cu²⁺ entering the lattice (e.g., Cu²⁺–□–Ce⁴⁺; □: oxygen vacancy), and the amount of reducible copper species caused by CuO crystals, varies with the Zr doping. Catalytic CO oxidation tests indicated that the oxygen vacancy and the reducible copper species were the adsorption and activation sites of O₂ and CO, respectively, and the cooperative effects between them accounted for the high CO oxidation activity. Thus, the samples x = 0.1 and 0.3, which possessed the most oxygen vacancy or reducible copper species, showed the best activity for CO oxidation, with full CO conversion obtained at 110 °C. The catalyst is also stable and has good resistance to water during the reaction.

Keywords Ce–Zr–Cu–O CO oxidation reducible copper species oxygen vacancy cooperative effect

Corresponding Author(s): Junjiang Zhu,Xinying Liu

Online First Date: 22 October 2021 Issue Date: 09 November 2021

Cite this article:

Shan Wang,Xuelian Xu,Ping Xiao, et al. Cooperative effect between copper species and oxygen vacancy in Ce_0.7−_xZr_xCu_0.3O₂ catalysts for carbon monoxide oxidation[J]. Front. Chem. Sci. Eng., 2021, 15(6): 1524-1536.

URL:

https://academic.hep.com.cn/fcse/EN/10.1007/s11705-021-2106-2
https://academic.hep.com.cn/fcse/EN/Y2021/V15/I6/1524

Fig.1 XRD patterns for: (a) individual CuO, CeO₂ and Ce_0.7Cu_0.3O₂ composites and (b) the Zr doped Ce_0.7−_xZr_xCu_0.3O₂ composites, together with a standard diffraction diagram of the cubic ZrO_2.

Fig.2 N₂ physisorption isotherms of the Ce_0.7−_xZr_xCu_0.3O₂, with BET surface area and pore size data inserted.

Fig.3 SEM images of the Ce_0.7−_xZr_xCu_0.3O₂ series samples.

Fig.4 Normal-(a–c) and high-(d–f) resolutionTEM images of: Ce_0.7Cu_0.3O₂ (a, d), Ce_0.4Zr_0.3Cu_0.3O₂ (b, e), and Ce_0.2Zr_0.5Cu_0.3O₂ (c, f).

Fig.5 H₂-TPR profiles of the Ce_0.7−_xZr_xCu_0.3O₂ series composites.

Tab.1 H₂-TPR and O₂-TPD data of the Ce_0.7−_xZr_xCu_0.3O₂ composite oxides

Fig.6 O₂-TPD profiles of the Ce_0.7−_xZr_xCu_0.3O₂ composite oxides.

Fig.7 Ce 3d, Zr 3d, Cu 2p and O 1s fine XPS spectra of the Ce_0.7−_xZr_xCu_0.3O₂ composites.

Tab.2 Surface atomic copper and oxygen molar ratios obtained from the XPS spectra

Fig.8 CO conversion obtained from the catalysts: (a) Ce_1–_xCu_xO₂ composites; (b) Ce_0.7–_xZr_xCu_0.3O₂ composites; (c) La substituted Ce_0.4Zr_0.3Cu_0.3–_yLa_yO₂; (d) CuO, CeO₂ and Ce_0.4Zr_0.3Cu_0.3O_2.

Fig.9 Comparison of the activity of Ce_0.4Zr_0.3Cu_0.3O₂ before and after etching, and of the impregnated CuO/CeO_2.

Fig.10 Scheme 1 Sketch of CO and O₂ activation and their reaction to form CO₂ over the Ce_0.7−_xZr_xCu_0.3O₂ composites.

Fig.11 (a) Long-term stability of Ce_0.4Zr_0.3Cu_0.3O₂ for CO oxidation at 95 °C, and (b) the water resistance of Ce_0.4Zr_0.3Cu_0.3O₂ for CO oxidation at 95 °C (Reaction conditions: using the 0.15 g Ce_0.4Zr_0.3Cu_0.3O₂ reacted as the catalyst. The reactant (0.8 vol-% CO+ 6.0 vol-% O₂ or 5% H₂O, balanced with Ar) was passed at 60 mL·min^–1 flow rate, during which the WHSV is equivalent to 31000 h^–1).

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