Effects of preparation methods on the activity of CuO/CeO<sub>2</sub> catalysts for CO oxidation

doi:10.1007/s11705-017-1661-z

Front. Chem. Sci. Eng.

2017, Vol. 11

Issue (4) : 603-612 https://doi.org/10.1007/s11705-017-1661-z

RESEARCH ARTICLE

Effects of preparation methods on the activity of CuO/CeO₂ catalysts for CO oxidation

Huanhuan Shang, Xiaoman Zhang, Jing Xu(

), Yifan Han

State Key Laboratory of Chemical Engineering, East China University of Science and Technology, Shanghai 200237, China

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Abstract

CO oxidation has been investigated on three CuO/CeO₂ catalysts prepared by impregnation, co-precipitation and mechanical mixing. The origin of active sites was explored by the multiple techniques. The catalyst prepared by impregnation has more highly dispersed CuO and stronger interactions between CuO and CeO₂ to promote the reduction of CuO to Cu⁺ species at the Cu-Ce interface, leading to its highest catalytic activity. For the catalyst prepared by co-precipitation, solid solution structures observed in Raman spectra suppress the formation of the Cu-Ce interface, where the adsorbed CO will react with active lattice oxygen to form CO₂, and thus it displays a lower catalytic performance. No Cu-Ce interface exists in the catalyst prepared by the mechanical mixing method due to the separate phases of CuO and CeO₂, resulting in its lowest activity among the three catalysts.

Keywords CuO/CeO₂ CO oxidation interfaces structure-performance relationship active sites

Corresponding Author(s): Jing Xu

Just Accepted Date: 10 May 2017 Online First Date: 08 November 2017 Issue Date: 06 November 2017

Cite this article:

Huanhuan Shang,Xiaoman Zhang,Jing Xu, et al. Effects of preparation methods on the activity of CuO/CeO₂ catalysts for CO oxidation[J]. Front. Chem. Sci. Eng., 2017, 11(4): 603-612.

URL:

https://academic.hep.com.cn/fcse/EN/10.1007/s11705-017-1661-z
https://academic.hep.com.cn/fcse/EN/Y2017/V11/I4/603

Tab.1 Physical properties of different 5Cu/CeO₂ catalysts

Fig.1 Temperature-dependent CO oxidation over different 5Cu/CeO₂ catalysts: (■) 5Cu/CeO₂(IM), (●) 5Cu/CeO₂(CP), (▲) 5Cu/CeO₂(MIX), (▾) CeO₂, and (♦) 5Cu/SiO₂(IM)

Fig.2 XRD patterns of different 5Cu/CeO₂ catalysts: (A) 5Cu/CeO₂(IM), (B) 5Cu/CeO₂(CP), (C) 5Cu/CeO₂(MIX), and (D) CeO₂

Fig.3 TEM mapping images of 5Cu/CeO₂(IM) catalyst (left): Ce (red) and Cu (green); EDX element analysis (right)

Fig.4 Raman spectra of different 5Cu/CeO₂ catalysts: (A) 5Cu/CeO₂(IM), (B) 5Cu/CeO₂(CP), (C) 5Cu/CeO₂(MIX), and (D) CeO₂

Tab.2 A_Ov/A_F2g ratio of different 5Cu/CeO₂ catalysts

Fig.5 H₂-TPR profiles of different 5Cu/CeO₂ catalysts: (A) 5Cu/CeO₂(IM), (B) 5Cu/CeO₂(CP), (C) 5Cu/CeO₂(MIX), (D) 5Cu/SiO₂, and (E) CeO₂

Fig.6 In situ DRIFTS under the reaction conditions over different 5Cu/CeO₂ catalysts: (a) 5Cu/CeO₂(IM), (b) 5Cu/CeO₂(CP), and (c) 5Cu/CeO₂(MIX)

Fig.7 Integral area of the Cu⁺-carbonyl as a function of the reaction temperature over different 5Cu/CeO₂ catalysts: (■) 5Cu/CeO₂(IM), (♦) 5Cu/CeO₂(CP), (▲) and 5Cu/CeO₂(MIX)

Fig.8 (a) Cu 2p and (b) Cu LMM core levels of XPS spectra of different 5Cu/CeO₂ catalysts: (A) 5Cu/CeO₂(IM), (B) 5Cu/CeO₂(CP), and (C) 5Cu/CeO₂(MIX)

Tab.3 XPS data of different 5Cu/CeO₂ catalysts

Fig.9 The structure-performance relationship over 5Cu/CeO₂ catalysts for CO oxidation

Fig.10 Scheme 1Proposed reaction mechanism for three catalysts: (a) 5Cu/CeO₂(IM), (b) 5Cu/CeO₂(CP), and (c) 5Cu/CeO₂(MIX)

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