A study of the mechanism of low-temperature SCR of NO with NH3 on MnOx/CeO2

Li Xu; Xiao Song Li; Mark Crocker; Zhao Shun Zhang; Ai Min Zhu; Chuan Shi

doi:10.1016/j.molcata.2013.05.021

A study of the mechanism of low-temperature SCR of NO with NH₃ on MnO_x/CeO₂

Li Xu, Xiao Song Li, Mark Crocker, Zhao Shun Zhang, Ai Min Zhu, Chuan Shi

Chemistry

Research output: Contribution to journal › Article › peer-review

124 Scopus citations

Abstract

A MnO_x/CeO₂ supported catalyst was prepared using the deposition-precipitation (DP) method for low-temperature selective catalytic reduction (SCR) of NO with NH₃. At short reaction time, nearly 100% NO conversion was obtained across the whole evaluated temperature range of 80-150 C at a space velocity of 50,000 h^-1. The catalyst rapidly lost its activity at 80 C, while stable activity was achieved at 120 C at a space velocity of 120,000 h^-1 in a 36 h test. A possible reaction pathway is proposed based on the results of an in situ diffuse reflectance infrared Fourier transform spectroscopy (DRIFTS) study coupled with mass spectrometric (MS) data. It is suggested that the NH₃-SCR reaction on the MnO _x/CeO₂ catalyst involves a [NH₃â̄ NO^-] complex as an intermediate, the decomposition of which into N₂ and H₂O is the rate-limiting step. The role of oxygen in the SCR reaction is to reoxidize the reduced catalyst surface, thereby completing the catalytic cycle.

Original language	English
Pages (from-to)	82-90
Number of pages	9
Journal	Journal of Molecular Catalysis A: Chemical
Volume	378
DOIs	https://doi.org/10.1016/j.molcata.2013.05.021
State	Published - 2013

Bibliographical note

Funding Information:
This work was supported by the National Natural Science Foundation of China (Nos. 20573014 and 21073024 ), Natural Science Foundation of Liaoning Province ( 201102034 ), as well as by the Fundamental Research Funds for the Central Universities (No. DUT12LK23 ).

Keywords

Deposition-precipitation
Low temperature
Mechanism
MnO/CeO
NH-SCR

ASJC Scopus subject areas

Catalysis
Process Chemistry and Technology
Physical and Theoretical Chemistry

Access to Document

10.1016/j.molcata.2013.05.021

Cite this

@article{68b98e2a022c4f5081c51338e721e113,

title = "A study of the mechanism of low-temperature SCR of NO with NH3 on MnOx/CeO2",

abstract = "A MnOx/CeO2 supported catalyst was prepared using the deposition-precipitation (DP) method for low-temperature selective catalytic reduction (SCR) of NO with NH3. At short reaction time, nearly 100% NO conversion was obtained across the whole evaluated temperature range of 80-150 C at a space velocity of 50,000 h-1. The catalyst rapidly lost its activity at 80 C, while stable activity was achieved at 120 C at a space velocity of 120,000 h-1 in a 36 h test. A possible reaction pathway is proposed based on the results of an in situ diffuse reflectance infrared Fourier transform spectroscopy (DRIFTS) study coupled with mass spectrometric (MS) data. It is suggested that the NH3-SCR reaction on the MnO x/CeO2 catalyst involves a [NH3{\^a}̄ NO-] complex as an intermediate, the decomposition of which into N2 and H2O is the rate-limiting step. The role of oxygen in the SCR reaction is to reoxidize the reduced catalyst surface, thereby completing the catalytic cycle.",

keywords = "Deposition-precipitation, Low temperature, Mechanism, MnO/CeO, NH-SCR",

author = "Li Xu and Li, {Xiao Song} and Mark Crocker and Zhang, {Zhao Shun} and Zhu, {Ai Min} and Chuan Shi",

note = "Funding Information: This work was supported by the National Natural Science Foundation of China (Nos. 20573014 and 21073024 ), Natural Science Foundation of Liaoning Province ( 201102034 ), as well as by the Fundamental Research Funds for the Central Universities (No. DUT12LK23 ). ",

year = "2013",

doi = "10.1016/j.molcata.2013.05.021",

language = "English",

volume = "378",

pages = "82--90",

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T1 - A study of the mechanism of low-temperature SCR of NO with NH3 on MnOx/CeO2

AU - Xu, Li

AU - Li, Xiao Song

AU - Crocker, Mark

AU - Zhang, Zhao Shun

AU - Zhu, Ai Min

AU - Shi, Chuan

N1 - Funding Information: This work was supported by the National Natural Science Foundation of China (Nos. 20573014 and 21073024 ), Natural Science Foundation of Liaoning Province ( 201102034 ), as well as by the Fundamental Research Funds for the Central Universities (No. DUT12LK23 ).

PY - 2013

Y1 - 2013

N2 - A MnOx/CeO2 supported catalyst was prepared using the deposition-precipitation (DP) method for low-temperature selective catalytic reduction (SCR) of NO with NH3. At short reaction time, nearly 100% NO conversion was obtained across the whole evaluated temperature range of 80-150 C at a space velocity of 50,000 h-1. The catalyst rapidly lost its activity at 80 C, while stable activity was achieved at 120 C at a space velocity of 120,000 h-1 in a 36 h test. A possible reaction pathway is proposed based on the results of an in situ diffuse reflectance infrared Fourier transform spectroscopy (DRIFTS) study coupled with mass spectrometric (MS) data. It is suggested that the NH3-SCR reaction on the MnO x/CeO2 catalyst involves a [NH3â̄ NO-] complex as an intermediate, the decomposition of which into N2 and H2O is the rate-limiting step. The role of oxygen in the SCR reaction is to reoxidize the reduced catalyst surface, thereby completing the catalytic cycle.

AB - A MnOx/CeO2 supported catalyst was prepared using the deposition-precipitation (DP) method for low-temperature selective catalytic reduction (SCR) of NO with NH3. At short reaction time, nearly 100% NO conversion was obtained across the whole evaluated temperature range of 80-150 C at a space velocity of 50,000 h-1. The catalyst rapidly lost its activity at 80 C, while stable activity was achieved at 120 C at a space velocity of 120,000 h-1 in a 36 h test. A possible reaction pathway is proposed based on the results of an in situ diffuse reflectance infrared Fourier transform spectroscopy (DRIFTS) study coupled with mass spectrometric (MS) data. It is suggested that the NH3-SCR reaction on the MnO x/CeO2 catalyst involves a [NH3â̄ NO-] complex as an intermediate, the decomposition of which into N2 and H2O is the rate-limiting step. The role of oxygen in the SCR reaction is to reoxidize the reduced catalyst surface, thereby completing the catalytic cycle.

KW - Deposition-precipitation

KW - Low temperature

KW - Mechanism

KW - MnO/CeO

KW - NH-SCR

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