Molecular-Level Insight into Selective Catalytic Reduction of NO x with NH 3 to N 2 over a Highly Efficient Bifunctional V a -MnO x Catalyst at Low Temperature

Ying Xin, Hao Li, Nana Zhang, Qian Li, Zhaoliang Zhang*, Xiaoming Cao, P. Hu, Lirong Zheng, James A. Anderson

*Corresponding author for this work

Research output: Contribution to journalArticle

11 Citations (Scopus)

Abstract

Selective catalytic reduction of NO x with ammonia (SCR) is not only an important model catalytic reaction but is also significant in terms of improving environmental air quality and human health. However, SCR catalysts suffer from low activity and selectivity to N 2 at low temperature, which in part may be attributed to our limited understanding of the reaction mechanism. Here, an unambiguous molecular-level mechanism is presented for an improved low-temperature SCR activity using bifunctional catalysts composed of highly active oxides (Mn 2 O 3 ) for NH 3 activation and highly selective vanadates (Mn 2 V 2 O 7 ) that promote N 2 formation. NH 3 is initially activated by Mn 2 O 3 to form an NH 2 intermediate. Transfer of NH 2 to Mn 2 V 2 O 7 then takes place, which facilitates the capture of gaseous NO leading to the formation of NH 2 NO over Mn 2 V 2 O 7 , whereafter NH 2 NO is efficiently converted to the preferred N 2 rather than the undesired byproduct, N 2 O. The proximity of the two components achieved via sol-gel preparation plays a crucial role in the transfer of active intermediates.

Original languageEnglish
Pages (from-to)4937-4949
Number of pages13
JournalACS Catalysis
Volume8
Issue number6
Early online date23 Apr 2018
DOIs
Publication statusPublished - 01 Jun 2018

Fingerprint

Selective catalytic reduction
Thyristors
Catalysts
Vanadates
Catalyst selectivity
Ammonia
Air quality
Temperature
Oxides
Sol-gels
Byproducts
Catalyst activity
Chemical activation
Health

Keywords

  • bifunctional catalyst
  • density functional theory
  • mechanism
  • nitrogen oxides
  • selective catalytic reduction

Cite this

Xin, Ying ; Li, Hao ; Zhang, Nana ; Li, Qian ; Zhang, Zhaoliang ; Cao, Xiaoming ; Hu, P. ; Zheng, Lirong ; Anderson, James A. / Molecular-Level Insight into Selective Catalytic Reduction of NO x with NH 3 to N 2 over a Highly Efficient Bifunctional V a -MnO x Catalyst at Low Temperature. In: ACS Catalysis. 2018 ; Vol. 8, No. 6. pp. 4937-4949.
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abstract = "Selective catalytic reduction of NO x with ammonia (SCR) is not only an important model catalytic reaction but is also significant in terms of improving environmental air quality and human health. However, SCR catalysts suffer from low activity and selectivity to N 2 at low temperature, which in part may be attributed to our limited understanding of the reaction mechanism. Here, an unambiguous molecular-level mechanism is presented for an improved low-temperature SCR activity using bifunctional catalysts composed of highly active oxides (Mn 2 O 3 ) for NH 3 activation and highly selective vanadates (Mn 2 V 2 O 7 ) that promote N 2 formation. NH 3 is initially activated by Mn 2 O 3 to form an NH 2 intermediate. Transfer of NH 2 to Mn 2 V 2 O 7 then takes place, which facilitates the capture of gaseous NO leading to the formation of NH 2 NO over Mn 2 V 2 O 7 , whereafter NH 2 NO is efficiently converted to the preferred N 2 rather than the undesired byproduct, N 2 O. The proximity of the two components achieved via sol-gel preparation plays a crucial role in the transfer of active intermediates.",
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Molecular-Level Insight into Selective Catalytic Reduction of NO x with NH 3 to N 2 over a Highly Efficient Bifunctional V a -MnO x Catalyst at Low Temperature. / Xin, Ying; Li, Hao; Zhang, Nana; Li, Qian; Zhang, Zhaoliang; Cao, Xiaoming; Hu, P.; Zheng, Lirong; Anderson, James A.

In: ACS Catalysis, Vol. 8, No. 6, 01.06.2018, p. 4937-4949.

Research output: Contribution to journalArticle

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T1 - Molecular-Level Insight into Selective Catalytic Reduction of NO x with NH 3 to N 2 over a Highly Efficient Bifunctional V a -MnO x Catalyst at Low Temperature

AU - Xin, Ying

AU - Li, Hao

AU - Zhang, Nana

AU - Li, Qian

AU - Zhang, Zhaoliang

AU - Cao, Xiaoming

AU - Hu, P.

AU - Zheng, Lirong

AU - Anderson, James A.

PY - 2018/6/1

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N2 - Selective catalytic reduction of NO x with ammonia (SCR) is not only an important model catalytic reaction but is also significant in terms of improving environmental air quality and human health. However, SCR catalysts suffer from low activity and selectivity to N 2 at low temperature, which in part may be attributed to our limited understanding of the reaction mechanism. Here, an unambiguous molecular-level mechanism is presented for an improved low-temperature SCR activity using bifunctional catalysts composed of highly active oxides (Mn 2 O 3 ) for NH 3 activation and highly selective vanadates (Mn 2 V 2 O 7 ) that promote N 2 formation. NH 3 is initially activated by Mn 2 O 3 to form an NH 2 intermediate. Transfer of NH 2 to Mn 2 V 2 O 7 then takes place, which facilitates the capture of gaseous NO leading to the formation of NH 2 NO over Mn 2 V 2 O 7 , whereafter NH 2 NO is efficiently converted to the preferred N 2 rather than the undesired byproduct, N 2 O. The proximity of the two components achieved via sol-gel preparation plays a crucial role in the transfer of active intermediates.

AB - Selective catalytic reduction of NO x with ammonia (SCR) is not only an important model catalytic reaction but is also significant in terms of improving environmental air quality and human health. However, SCR catalysts suffer from low activity and selectivity to N 2 at low temperature, which in part may be attributed to our limited understanding of the reaction mechanism. Here, an unambiguous molecular-level mechanism is presented for an improved low-temperature SCR activity using bifunctional catalysts composed of highly active oxides (Mn 2 O 3 ) for NH 3 activation and highly selective vanadates (Mn 2 V 2 O 7 ) that promote N 2 formation. NH 3 is initially activated by Mn 2 O 3 to form an NH 2 intermediate. Transfer of NH 2 to Mn 2 V 2 O 7 then takes place, which facilitates the capture of gaseous NO leading to the formation of NH 2 NO over Mn 2 V 2 O 7 , whereafter NH 2 NO is efficiently converted to the preferred N 2 rather than the undesired byproduct, N 2 O. The proximity of the two components achieved via sol-gel preparation plays a crucial role in the transfer of active intermediates.

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