Insight into the mechanism of selective catalytic reduction of NO x by propene over the Cu/Ti0.7Zr0.3O 2 catalyst by fourier transform infrared spectroscopy and density functional theory calculations

The mechanism of selective catalytic reduction of NOx by propene (C3H6-SCR) over the Cu/Ti0.7Zr 0.3O2 catalyst was studied by in situ Fourier transform infrared (FTIR) spectroscopy and density functional theory (DFT) calculations. Especially, the formation and transformation of cyanide (-CN species)...

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Main Authors: Liu, J., Li, Xin Yong, Zhao, Q., Hao, C., Zhang, D.
Format: Journal Article
Published: 2013
Online Access:http://hdl.handle.net/20.500.11937/8625
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author Liu, J.
Li, Xin Yong
Zhao, Q.
Hao, C.
Zhang, D.
author_facet Liu, J.
Li, Xin Yong
Zhao, Q.
Hao, C.
Zhang, D.
author_sort Liu, J.
building Curtin Institutional Repository
collection Online Access
description The mechanism of selective catalytic reduction of NOx by propene (C3H6-SCR) over the Cu/Ti0.7Zr 0.3O2 catalyst was studied by in situ Fourier transform infrared (FTIR) spectroscopy and density functional theory (DFT) calculations. Especially, the formation and transformation of cyanide (-CN species) during the reaction was discussed. According to FTIR results, the excellent performance of the Cu/Ti0.7Zr0.3O2 catalyst in C 3H6-SCR was attributed to the coexistence of two parallel pathways to produce N2 by the isocyanate (-NCO species) and -CN species intermediates. Besides the hydrolysis of the -NCO species, the reaction between the -CN species and nitrates and/or NO2 was also a crucial pathway for the NO reduction. On the basis of the DFT calculations on the energy of possible intermediates and transition states at the B3LYP/6-311 G (d, p) level of theory, the reaction channel of -CN species in the SCR reaction was identified and the role of -CN species as a crucial intermediate to generate N2 was also confirmed from the thermodynamics view. In combination of the FTIR and DFT results, a modified mechanism with two parallel pathways to produce N2 by the reaction of -NCO and -CN species over the Cu/Ti0.7Zr0.3O2 catalyst was proposed. © 2013 American Chemical Society.
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spelling curtin-20.500.11937-86252017-09-13T14:51:29Z Insight into the mechanism of selective catalytic reduction of NO x by propene over the Cu/Ti0.7Zr0.3O 2 catalyst by fourier transform infrared spectroscopy and density functional theory calculations Liu, J. Li, Xin Yong Zhao, Q. Hao, C. Zhang, D. The mechanism of selective catalytic reduction of NOx by propene (C3H6-SCR) over the Cu/Ti0.7Zr 0.3O2 catalyst was studied by in situ Fourier transform infrared (FTIR) spectroscopy and density functional theory (DFT) calculations. Especially, the formation and transformation of cyanide (-CN species) during the reaction was discussed. According to FTIR results, the excellent performance of the Cu/Ti0.7Zr0.3O2 catalyst in C 3H6-SCR was attributed to the coexistence of two parallel pathways to produce N2 by the isocyanate (-NCO species) and -CN species intermediates. Besides the hydrolysis of the -NCO species, the reaction between the -CN species and nitrates and/or NO2 was also a crucial pathway for the NO reduction. On the basis of the DFT calculations on the energy of possible intermediates and transition states at the B3LYP/6-311 G (d, p) level of theory, the reaction channel of -CN species in the SCR reaction was identified and the role of -CN species as a crucial intermediate to generate N2 was also confirmed from the thermodynamics view. In combination of the FTIR and DFT results, a modified mechanism with two parallel pathways to produce N2 by the reaction of -NCO and -CN species over the Cu/Ti0.7Zr0.3O2 catalyst was proposed. © 2013 American Chemical Society. 2013 Journal Article http://hdl.handle.net/20.500.11937/8625 10.1021/es3049898 restricted
spellingShingle Liu, J.
Li, Xin Yong
Zhao, Q.
Hao, C.
Zhang, D.
Insight into the mechanism of selective catalytic reduction of NO x by propene over the Cu/Ti0.7Zr0.3O 2 catalyst by fourier transform infrared spectroscopy and density functional theory calculations
title Insight into the mechanism of selective catalytic reduction of NO x by propene over the Cu/Ti0.7Zr0.3O 2 catalyst by fourier transform infrared spectroscopy and density functional theory calculations
title_full Insight into the mechanism of selective catalytic reduction of NO x by propene over the Cu/Ti0.7Zr0.3O 2 catalyst by fourier transform infrared spectroscopy and density functional theory calculations
title_fullStr Insight into the mechanism of selective catalytic reduction of NO x by propene over the Cu/Ti0.7Zr0.3O 2 catalyst by fourier transform infrared spectroscopy and density functional theory calculations
title_full_unstemmed Insight into the mechanism of selective catalytic reduction of NO x by propene over the Cu/Ti0.7Zr0.3O 2 catalyst by fourier transform infrared spectroscopy and density functional theory calculations
title_short Insight into the mechanism of selective catalytic reduction of NO x by propene over the Cu/Ti0.7Zr0.3O 2 catalyst by fourier transform infrared spectroscopy and density functional theory calculations
title_sort insight into the mechanism of selective catalytic reduction of no x by propene over the cu/ti0.7zr0.3o 2 catalyst by fourier transform infrared spectroscopy and density functional theory calculations
url http://hdl.handle.net/20.500.11937/8625