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Frontiers of Environmental Science & Engineering

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 Li1,2,3,Haidi Liu1,3,Yunfa Chen1,3()
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% NOx 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 NOx 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% NOx 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 NOx.

Keywords NH3-selective catalytic reduction      NOx      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.
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http://journal.hep.com.cn/fese/EN/10.1007/s11783-017-0914-x
http://journal.hep.com.cn/fese/EN/Y2017/V11/I2/6
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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
sample specific surface/(m2·g−1) average pore size/nm BJH pore volume /(mL·g−1) Ce3+/(Ce3+ + Ce4+)/% Oβ/(Oα + Oβ)/%
Zr-Ce 76.53 5.87 0.091 13.7 33.9
Mn-Zr-Ce 109.64 9.81 0.25 15.3 48.9
Cr-Zr-Ce 168.95 7.14 0.31 15.8 53.6
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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