Promotion of transition metal oxides on the NH3-SCR performance of ZrO2-CeO2 catalyst

doi:10.1007/s11783-017-0914-x

Front. Environ. Sci. Eng.

2017, Vol. 11

Issue (2) : 6 https://doi.org/10.1007/s11783-017-0914-x

RESEARCH ARTICLE

Promotion of transition metal oxides on the NH₃-SCR performance of ZrO₂-CeO₂ catalyst

Weiman Li^1,^2,³,Haidi Liu^1,³,Yunfa Chen^1,³(

)

¹. State Key Laboratory of Multi-phase Complex Systems, Institute of Process Engineering, Chinese Academy of Sciences, Beijing 100190, China
². University of Chinese Academy of Sciences, Beijing 100049, China
³. Center for Excellence in Urban Atmospheric Environment, Institute of Urban Environment, Chinese Academy of Sciences, Xiamen 361021, China

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Abstract

Manganese and chromium oxides promote the NH₃-SCR activity of Zr-Ce mixed oxide.

Cr-Zr-Ce mixed oxide exhibited>80% NO_x conversion at a wide temperature window.

More acid sites and higher reducibility may responsible for the high SCR ability.

Chromium oxide and manganese oxide promoted ZrO₂-CeO₂ catalysts were prepared by a homogeneous precipitation method for the selective catalytic reduction of NO_x with NH₃. A series of characterization including X-ray diffraction (XRD), high-resolution transmission electron microscope (HR-TEM), Brunauer–Emmett–Teller (BET) surface area analysis, H₂ temperature-programmed reduction (H₂-TPR), and X-ray photoelectron spectroscopy (XPS) were used to evaluate the influence of the physicochemical properties on NH₃-SCR activity. Cr-Zr-Ce and Mn-Zr-Ce catalysts are much more active than ZrO₂-CeO₂ binary oxide for the low temperature NH₃-SCR, mainly because of the high specific surface area, more surface oxygen species, improved reducibility derived from synergistic effect among different elements. Mn-Zr-Ce catalyst exhibited high tolerance to SO₂ and H₂O. Cr-Zr-Ce mixed oxide exhibited>80% NO_x conversion at a wide temperature window of 100°C–300°C. In situ DRIFT studies showed that the addition of Cr is beneficial to the formation of Bronsted acid sites and prevents the formation of stable nitrate species because of the presence of Cr⁶⁺. The present mixed oxide can be a candidate for the low temperature abatement of NO_x.

Keywords NH₃-selective catalytic reduction NO_x Low temperature Cr-Zr-Ce

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Corresponding Author(s): Yunfa Chen

Issue Date: 23 March 2017

Cite this article:

Weiman Li,Haidi Liu,Yunfa Chen. Promotion of transition metal oxides on the NH₃-SCR performance of ZrO₂-CeO₂ catalyst[J]. Front. Environ. Sci. Eng., 2017, 11(2): 6.

URL:

https://academic.hep.com.cn/fese/EN/10.1007/s11783-017-0914-x
https://academic.hep.com.cn/fese/EN/Y2017/V11/I2/6

Fig.1 SCR activity of different samples

Fig.2 XRD patterns of Zr-Ce, Mn-Zr-Ce, and Cr-Zr-Ce samples, respectively

Fig.3 TEM images of as-prepared (a) Zr-Ce, (b) Mn-Zr-Ce, and (c) Cr-Zr-Ce catalysts

Fig.4 N₂ adsorption–desorption isotherms curves and (inset) pore size distributions calculated from the desorption branch of as-synthesized catalysts

Tab.1 BET results and XPS surface atomic ratios of different samples

Fig.5 H₂-TPR analysis of three samples

Fig.6 (a) Cr 2p and Mn 2p XPS spectra of Cr-Zr-Ce and Mn-Zr-Ce sample, respectively; (b) Zr 3d XPS spectra of different samples; (c) O 1s XPS spectra of different samples; (d) Ce 3d XPS spectra of different samples

Fig.7 In situ DRIFT spectras of three catalysts in (a) NH₃ + air, (b) NO+ air, and (c) NH₃ + NO+ air flow, respectively

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