An investigation of the NO/H2/O2 (Lean De-NOx) reaction on a highly active and selective Pt/La0.7Sr0.2Ce0.1FeO3 catalyst at low temperatures

C. N. Costa; P. G. Savva; C. Andronikou; P. S. Lambrou; K. Polychronopoulou; V. C. Belessi; V. N. Stathopoulos; P. J. Pomonis; A. M. Efstathiou

doi:10.1006/jcat.2002.3645

An investigation of the NO/H₂/O₂ (Lean De-NO_x) reaction on a highly active and selective Pt/La_0.7Sr_0.2Ce_0.1FeO₃ catalyst at low temperatures

C. N. Costa, P. G. Savva, C. Andronikou, P. S. Lambrou, K. Polychronopoulou, V. C. Belessi, V. N. Stathopoulos, P. J. Pomonis, A. M. Efstathiou

Mechanical & Nuclear Engineering

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Abstract

A 0.1 wt% Pt supported on La_0.7Sr_0.2Ce_0.1FeO₃ solid (mixed oxide containing LaFeO₃, SrFeO_3-x, CeO₂, and Fe₂O₃ phases) has been studied for the NO/H₂/O₂ reaction in the 100-400°C range. For a critical comparison, 0.1 wt% Pt was supported on SiO₂, CeO₂, and Fe₂O₃ and tested under the same reaction conditions. For the Pt/La_0.7Sr_0.2Ce_0.1FeO₃ catalyst a maximum in the NO conversion (83%) has been observed at 150°C with a N₂ selectivity value of 93%, while for the Pt/SiO₂ catalyst at 120°C (82% conversion) with a N₂ selectivity value of 65% using a GHSV of 80, 000 h⁻¹ Low N₂ selectivity values, less than 45%, were obtained with the Pt/CeO₂ and Pt/Fe₂O₃ catalysts in the 100-400°C range. For the Pt/La_0.7Sr_0.2Ce_0.1FeO₃ catalyst, addition of 5% H₂O in the feed stream at 140°C resulted in a widening of the operating temperature window with appreciable NO conversion and no negative effect on the stability of the catalyst during 20 h on stream. In addition, a remarkable N₂ yield (93%) after 20 h on 0.25% NO/1% H₂/5% O₂/5% H₂O/He gas stream at 140°C has been observed. Remarkable N₂ selectivity values in the range of 80-90% have also been observed in the 100-200°C low-temperature range either in the absence or in the presence of water in the feed stream. A maximum specific integral reaction rate of 443.5 μmol N₂/s·g of Pt metal was measured at 160°C during reaction with a 0.25% NO/1% H₂/5% O₂/5% H₂O/He gas mixture. This value is higher by 90% than the corresponding one observed on the 0.1 wt% Pt/SiO₂ catalyst at 120°C and it is the highest value ever reported for the reaction at hand in the 100-200°C low-temperature range on Pt-based catalysts. A TOF value of 13.4 × 10⁻² s⁻¹ for N₂ formation was calculated at 110°C for the Pt/La_0.7Sr_0.2Ce_0.1FeO₃ catalyst. Temperature-programmed desorption (TPD) of NO and transient titration experiments of the catalyst surface following NO/H₂/O₂ reaction have revealed important information concerning the amount and chemical composition of active and inactive (spectator) adsorbed N-containing species present under reaction conditions.

Original language	British English
Pages (from-to)	456-471
Number of pages	16
Journal	Journal of Catalysis
Volume	209
Issue number	2
DOIs	https://doi.org/10.1006/jcat.2002.3645
State	Published - 2002

Keywords

Lean de-NO
NO reduction
NO TPD
Perovskites

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10.1006/jcat.2002.3645

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Costa, C. N., Savva, P. G., Andronikou, C., Lambrou, P. S., Polychronopoulou, K., Belessi, V. C., Stathopoulos, V. N., Pomonis, P. J., & Efstathiou, A. M. (2002). An investigation of the NO/H₂/O₂ (Lean De-NO_x) reaction on a highly active and selective Pt/La_0.7Sr_0.2Ce_0.1FeO₃ catalyst at low temperatures. Journal of Catalysis, 209(2), 456-471. https://doi.org/10.1006/jcat.2002.3645

@article{0100ff0210784b5ab06486af79494405,

title = "An investigation of the NO/H2/O2 (Lean De-NOx) reaction on a highly active and selective Pt/La0.7Sr0.2Ce0.1FeO3 catalyst at low temperatures",

abstract = "A 0.1 wt% Pt supported on La0.7Sr0.2Ce0.1FeO3 solid (mixed oxide containing LaFeO3, SrFeO3-x, CeO2, and Fe2O3 phases) has been studied for the NO/H2/O2 reaction in the 100-400°C range. For a critical comparison, 0.1 wt% Pt was supported on SiO2, CeO2, and Fe2O3 and tested under the same reaction conditions. For the Pt/La0.7Sr0.2Ce0.1FeO3 catalyst a maximum in the NO conversion (83%) has been observed at 150°C with a N2 selectivity value of 93%, while for the Pt/SiO2 catalyst at 120°C (82% conversion) with a N2 selectivity value of 65% using a GHSV of 80, 000 h−1 Low N2 selectivity values, less than 45%, were obtained with the Pt/CeO2 and Pt/Fe2O3 catalysts in the 100-400°C range. For the Pt/La0.7Sr0.2Ce0.1FeO3 catalyst, addition of 5% H2O in the feed stream at 140°C resulted in a widening of the operating temperature window with appreciable NO conversion and no negative effect on the stability of the catalyst during 20 h on stream. In addition, a remarkable N2 yield (93%) after 20 h on 0.25% NO/1% H2/5% O2/5% H2O/He gas stream at 140°C has been observed. Remarkable N2 selectivity values in the range of 80-90% have also been observed in the 100-200°C low-temperature range either in the absence or in the presence of water in the feed stream. A maximum specific integral reaction rate of 443.5 μmol N2/s·g of Pt metal was measured at 160°C during reaction with a 0.25% NO/1% H2/5% O2/5% H2O/He gas mixture. This value is higher by 90% than the corresponding one observed on the 0.1 wt% Pt/SiO2 catalyst at 120°C and it is the highest value ever reported for the reaction at hand in the 100-200°C low-temperature range on Pt-based catalysts. A TOF value of 13.4 × 10−2 s−1 for N2 formation was calculated at 110°C for the Pt/La0.7Sr0.2Ce0.1FeO3 catalyst. Temperature-programmed desorption (TPD) of NO and transient titration experiments of the catalyst surface following NO/H2/O2 reaction have revealed important information concerning the amount and chemical composition of active and inactive (spectator) adsorbed N-containing species present under reaction conditions.",

keywords = "Lean de-NO, NO reduction, NO TPD, Perovskites",

author = "Costa, {C. N.} and Savva, {P. G.} and C. Andronikou and Lambrou, {P. S.} and K. Polychronopoulou and Belessi, {V. C.} and Stathopoulos, {V. N.} and Pomonis, {P. J.} and Efstathiou, {A. M.}",

note = "Funding Information: Financial support by the Research Committee of the University of Cyprus and the European Union (GROWTH-GRDI-2000-25043) is gratefully acknowledged. The experimental assistance of Christos Christofides and Niovi Michael (final-year-project students of this university) is also acknowledged.",

year = "2002",

doi = "10.1006/jcat.2002.3645",

language = "British English",

volume = "209",

pages = "456--471",

journal = "Journal of Catalysis",

issn = "0021-9517",

publisher = "Academic Press Inc.",

number = "2",

}

Costa, CN, Savva, PG, Andronikou, C, Lambrou, PS, Polychronopoulou, K, Belessi, VC, Stathopoulos, VN, Pomonis, PJ & Efstathiou, AM 2002, 'An investigation of the NO/H₂/O₂ (Lean De-NO_x) reaction on a highly active and selective Pt/La_0.7Sr_0.2Ce_0.1FeO₃ catalyst at low temperatures', Journal of Catalysis, vol. 209, no. 2, pp. 456-471. https://doi.org/10.1006/jcat.2002.3645

TY - JOUR

T1 - An investigation of the NO/H2/O2 (Lean De-NOx) reaction on a highly active and selective Pt/La0.7Sr0.2Ce0.1FeO3 catalyst at low temperatures

AU - Costa, C. N.

AU - Savva, P. G.

AU - Andronikou, C.

AU - Lambrou, P. S.

AU - Polychronopoulou, K.

AU - Belessi, V. C.

AU - Stathopoulos, V. N.

AU - Pomonis, P. J.

AU - Efstathiou, A. M.

N1 - Funding Information: Financial support by the Research Committee of the University of Cyprus and the European Union (GROWTH-GRDI-2000-25043) is gratefully acknowledged. The experimental assistance of Christos Christofides and Niovi Michael (final-year-project students of this university) is also acknowledged.

PY - 2002

Y1 - 2002

N2 - A 0.1 wt% Pt supported on La0.7Sr0.2Ce0.1FeO3 solid (mixed oxide containing LaFeO3, SrFeO3-x, CeO2, and Fe2O3 phases) has been studied for the NO/H2/O2 reaction in the 100-400°C range. For a critical comparison, 0.1 wt% Pt was supported on SiO2, CeO2, and Fe2O3 and tested under the same reaction conditions. For the Pt/La0.7Sr0.2Ce0.1FeO3 catalyst a maximum in the NO conversion (83%) has been observed at 150°C with a N2 selectivity value of 93%, while for the Pt/SiO2 catalyst at 120°C (82% conversion) with a N2 selectivity value of 65% using a GHSV of 80, 000 h−1 Low N2 selectivity values, less than 45%, were obtained with the Pt/CeO2 and Pt/Fe2O3 catalysts in the 100-400°C range. For the Pt/La0.7Sr0.2Ce0.1FeO3 catalyst, addition of 5% H2O in the feed stream at 140°C resulted in a widening of the operating temperature window with appreciable NO conversion and no negative effect on the stability of the catalyst during 20 h on stream. In addition, a remarkable N2 yield (93%) after 20 h on 0.25% NO/1% H2/5% O2/5% H2O/He gas stream at 140°C has been observed. Remarkable N2 selectivity values in the range of 80-90% have also been observed in the 100-200°C low-temperature range either in the absence or in the presence of water in the feed stream. A maximum specific integral reaction rate of 443.5 μmol N2/s·g of Pt metal was measured at 160°C during reaction with a 0.25% NO/1% H2/5% O2/5% H2O/He gas mixture. This value is higher by 90% than the corresponding one observed on the 0.1 wt% Pt/SiO2 catalyst at 120°C and it is the highest value ever reported for the reaction at hand in the 100-200°C low-temperature range on Pt-based catalysts. A TOF value of 13.4 × 10−2 s−1 for N2 formation was calculated at 110°C for the Pt/La0.7Sr0.2Ce0.1FeO3 catalyst. Temperature-programmed desorption (TPD) of NO and transient titration experiments of the catalyst surface following NO/H2/O2 reaction have revealed important information concerning the amount and chemical composition of active and inactive (spectator) adsorbed N-containing species present under reaction conditions.

AB - A 0.1 wt% Pt supported on La0.7Sr0.2Ce0.1FeO3 solid (mixed oxide containing LaFeO3, SrFeO3-x, CeO2, and Fe2O3 phases) has been studied for the NO/H2/O2 reaction in the 100-400°C range. For a critical comparison, 0.1 wt% Pt was supported on SiO2, CeO2, and Fe2O3 and tested under the same reaction conditions. For the Pt/La0.7Sr0.2Ce0.1FeO3 catalyst a maximum in the NO conversion (83%) has been observed at 150°C with a N2 selectivity value of 93%, while for the Pt/SiO2 catalyst at 120°C (82% conversion) with a N2 selectivity value of 65% using a GHSV of 80, 000 h−1 Low N2 selectivity values, less than 45%, were obtained with the Pt/CeO2 and Pt/Fe2O3 catalysts in the 100-400°C range. For the Pt/La0.7Sr0.2Ce0.1FeO3 catalyst, addition of 5% H2O in the feed stream at 140°C resulted in a widening of the operating temperature window with appreciable NO conversion and no negative effect on the stability of the catalyst during 20 h on stream. In addition, a remarkable N2 yield (93%) after 20 h on 0.25% NO/1% H2/5% O2/5% H2O/He gas stream at 140°C has been observed. Remarkable N2 selectivity values in the range of 80-90% have also been observed in the 100-200°C low-temperature range either in the absence or in the presence of water in the feed stream. A maximum specific integral reaction rate of 443.5 μmol N2/s·g of Pt metal was measured at 160°C during reaction with a 0.25% NO/1% H2/5% O2/5% H2O/He gas mixture. This value is higher by 90% than the corresponding one observed on the 0.1 wt% Pt/SiO2 catalyst at 120°C and it is the highest value ever reported for the reaction at hand in the 100-200°C low-temperature range on Pt-based catalysts. A TOF value of 13.4 × 10−2 s−1 for N2 formation was calculated at 110°C for the Pt/La0.7Sr0.2Ce0.1FeO3 catalyst. Temperature-programmed desorption (TPD) of NO and transient titration experiments of the catalyst surface following NO/H2/O2 reaction have revealed important information concerning the amount and chemical composition of active and inactive (spectator) adsorbed N-containing species present under reaction conditions.

KW - Lean de-NO

KW - NO reduction

KW - NO TPD

KW - Perovskites

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U2 - 10.1006/jcat.2002.3645

DO - 10.1006/jcat.2002.3645

M3 - Article

AN - SCOPUS:0037173403

SN - 0021-9517

VL - 209

SP - 456

EP - 471

JO - Journal of Catalysis

JF - Journal of Catalysis

IS - 2

ER -

An investigation of the NO/H₂/O₂ (Lean De-NO_x) reaction on a highly active and selective Pt/La_0.7Sr_0.2Ce_0.1FeO₃ catalyst at low temperatures

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Keywords

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