Surface insights into MnOx-based catalysts containing metal oxides for the selective catalytic reduction of NOX with NH3

Dong Ho Kim; Yeon Jae Park; Kwan Young Lee; Heon Phil Ha; Dong Wook Kwon

doi:10.1016/j.apcata.2022.118770

Surface insights into MnOx-based catalysts containing metal oxides for the selective catalytic reduction of NO_X with NH₃

Dong Ho Kim, Yeon Jae Park, Kwan Young Lee, Heon Phil Ha, Dong Wook Kwon

Department of Chemical and Biological Engineering

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

3 Citations (Scopus)

Abstract

The MnOx/TiO₂-based NO_X reduction catalyst showed moderate performance at low temperature and had the disadvantage of low N₂ selectivity. Herein, the effect of Sm and Ce interactions on MnOx-based catalysts in selective catalytic reduction was investigated. Sm increased the redox properties of the MnOx catalyst and the ratio of Mn⁴⁺. Meanwhile, Ce enhanced the additional redox trait of the Sm-modified catalyst. When exposed to SO₂/O₂, Sm and Ce-modified MnOx not only suppressed performance degradation, but also increased N₂ selectivity. Sm and Ce suppress the formation of N₂O by inhibiting the formation of N₂O₄ intermediate species. Additionally, regardless of exposure to SO₂/O₂, Sm/Ce modified MnOx is an LH-ER mechanism (Langmuir-Hinshelwood and Eley-Rideal mechanism), but in the case of MnOx, it is suggested to be mainly an ER mechanism when exposed to SO₂/O₂. From these results, a strategy for improving the N₂ selectivity/SCR performance of MnOx/TiO₂-based catalysts with SO₂ resistance was provided.

Original language	English
Article number	118770
Journal	Applied Catalysis A: General
Volume	643
DOIs	https://doi.org/10.1016/j.apcata.2022.118770
Publication status	Published - 2022 Aug 5

Keywords

Mechanism
MnOx
N selectivity
NH-SCR
NO reduction

ASJC Scopus subject areas

Catalysis
Process Chemistry and Technology

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10.1016/j.apcata.2022.118770

Cite this

@article{c2625016dd3c4d26ace9c62907a0583e,

title = "Surface insights into MnOx-based catalysts containing metal oxides for the selective catalytic reduction of NOX with NH3",

abstract = "The MnOx/TiO2-based NOX reduction catalyst showed moderate performance at low temperature and had the disadvantage of low N2 selectivity. Herein, the effect of Sm and Ce interactions on MnOx-based catalysts in selective catalytic reduction was investigated. Sm increased the redox properties of the MnOx catalyst and the ratio of Mn4+. Meanwhile, Ce enhanced the additional redox trait of the Sm-modified catalyst. When exposed to SO2/O2, Sm and Ce-modified MnOx not only suppressed performance degradation, but also increased N2 selectivity. Sm and Ce suppress the formation of N2O by inhibiting the formation of N2O4 intermediate species. Additionally, regardless of exposure to SO2/O2, Sm/Ce modified MnOx is an LH-ER mechanism (Langmuir-Hinshelwood and Eley-Rideal mechanism), but in the case of MnOx, it is suggested to be mainly an ER mechanism when exposed to SO2/O2. From these results, a strategy for improving the N2 selectivity/SCR performance of MnOx/TiO2-based catalysts with SO2 resistance was provided.",

keywords = "Mechanism, MnOx, N selectivity, NH-SCR, NO reduction",

author = "Kim, {Dong Ho} and Park, {Yeon Jae} and Lee, {Kwan Young} and Ha, {Heon Phil} and Kwon, {Dong Wook}",

note = "Funding Information: We are grateful to the Korea Institute of Science and Technology (KIST) for supporting this project through the Future R&D program ( #2E31751 ) and Interfacial Engineering for Catalytic Solids (K-Lab) ( #2E31804 ). This work was partly supported by a Korea Institute of Energy Technology Evaluation and Planning (KETEP) grant funded by the Korea government (MOTIE) ( 20217010100110 ). Publisher Copyright: {\textcopyright} 2022 Elsevier B.V.",

year = "2022",

month = aug,

day = "5",

doi = "10.1016/j.apcata.2022.118770",

language = "English",

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T1 - Surface insights into MnOx-based catalysts containing metal oxides for the selective catalytic reduction of NOX with NH3

AU - Kim, Dong Ho

AU - Park, Yeon Jae

AU - Lee, Kwan Young

AU - Ha, Heon Phil

AU - Kwon, Dong Wook

N1 - Funding Information: We are grateful to the Korea Institute of Science and Technology (KIST) for supporting this project through the Future R&D program ( #2E31751 ) and Interfacial Engineering for Catalytic Solids (K-Lab) ( #2E31804 ). This work was partly supported by a Korea Institute of Energy Technology Evaluation and Planning (KETEP) grant funded by the Korea government (MOTIE) ( 20217010100110 ). Publisher Copyright: © 2022 Elsevier B.V.

PY - 2022/8/5

Y1 - 2022/8/5

N2 - The MnOx/TiO2-based NOX reduction catalyst showed moderate performance at low temperature and had the disadvantage of low N2 selectivity. Herein, the effect of Sm and Ce interactions on MnOx-based catalysts in selective catalytic reduction was investigated. Sm increased the redox properties of the MnOx catalyst and the ratio of Mn4+. Meanwhile, Ce enhanced the additional redox trait of the Sm-modified catalyst. When exposed to SO2/O2, Sm and Ce-modified MnOx not only suppressed performance degradation, but also increased N2 selectivity. Sm and Ce suppress the formation of N2O by inhibiting the formation of N2O4 intermediate species. Additionally, regardless of exposure to SO2/O2, Sm/Ce modified MnOx is an LH-ER mechanism (Langmuir-Hinshelwood and Eley-Rideal mechanism), but in the case of MnOx, it is suggested to be mainly an ER mechanism when exposed to SO2/O2. From these results, a strategy for improving the N2 selectivity/SCR performance of MnOx/TiO2-based catalysts with SO2 resistance was provided.

AB - The MnOx/TiO2-based NOX reduction catalyst showed moderate performance at low temperature and had the disadvantage of low N2 selectivity. Herein, the effect of Sm and Ce interactions on MnOx-based catalysts in selective catalytic reduction was investigated. Sm increased the redox properties of the MnOx catalyst and the ratio of Mn4+. Meanwhile, Ce enhanced the additional redox trait of the Sm-modified catalyst. When exposed to SO2/O2, Sm and Ce-modified MnOx not only suppressed performance degradation, but also increased N2 selectivity. Sm and Ce suppress the formation of N2O by inhibiting the formation of N2O4 intermediate species. Additionally, regardless of exposure to SO2/O2, Sm/Ce modified MnOx is an LH-ER mechanism (Langmuir-Hinshelwood and Eley-Rideal mechanism), but in the case of MnOx, it is suggested to be mainly an ER mechanism when exposed to SO2/O2. From these results, a strategy for improving the N2 selectivity/SCR performance of MnOx/TiO2-based catalysts with SO2 resistance was provided.

KW - Mechanism

KW - MnOx

KW - N selectivity

KW - NH-SCR

KW - NO reduction

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