Impact of Copper Loading on NH3-Selective Catalytic Reduction, Oxidation Reactions and N2O Formation over Cu/SAPO-34

We developed a procedure for aqueous ion exchange to obtain different Cu loadings of Cu/SAPO-34 (between 0 and 2.6 wt %.) The catalysts were washcoated on monoliths and characterised with respect to their activity and selectivity under standard selective catalytic reduction (SCR), fast SCR, NH3 oxid...

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Main Authors: Kirsten Leistner, Florian Brüsewitz, Kurnia Wijayanti, Ashok Kumar, Krishna Kamasamudram, Louise Olsson
Format: Article
Language:English
Published: MDPI AG 2017-04-01
Series:Energies
Subjects:
Online Access:http://www.mdpi.com/1996-1073/10/4/489
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author Kirsten Leistner
Florian Brüsewitz
Kurnia Wijayanti
Ashok Kumar
Krishna Kamasamudram
Louise Olsson
author_facet Kirsten Leistner
Florian Brüsewitz
Kurnia Wijayanti
Ashok Kumar
Krishna Kamasamudram
Louise Olsson
author_sort Kirsten Leistner
collection DOAJ
description We developed a procedure for aqueous ion exchange to obtain different Cu loadings of Cu/SAPO-34 (between 0 and 2.6 wt %.) The catalysts were washcoated on monoliths and characterised with respect to their activity and selectivity under standard selective catalytic reduction (SCR), fast SCR, NH3 oxidation and NO oxidation reactions. They were further characterised using X-ray diffraction (XRD), Brunauer–Emmett–Teller (BET), H2-temperature programmed reduction (H2-TPR), ultraviolet (UV)-vis spectroscopy and NH3 adsorption. As expected, activity of all reactions increased with copper loading, due to increased number of active sites. However, the N2O formation during standard and fast SCR yielded interesting mechanistic information. We observed that N2O formation at low temperature increased with copper loading for the standard SCR reaction, while it decreased for fast SCR. The low-temperature N2O formation during fast SCR thus occurs predominantly over Brønsted sites. Species responsible for N2O formation during standard SCR, on the other hand, are formed on the copper sites. We further found that the fast SCR reaction occurs to a significant extent even over the H/SAPO-34 form. The Brønsted sites in SAPO-34 are thus active for the fast SCR reaction.
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spelling doaj.art-3bed7d61b4db4ba19cac06a8a7f690442022-12-22T01:58:21ZengMDPI AGEnergies1996-10732017-04-0110448910.3390/en10040489en10040489Impact of Copper Loading on NH3-Selective Catalytic Reduction, Oxidation Reactions and N2O Formation over Cu/SAPO-34Kirsten Leistner0Florian Brüsewitz1Kurnia Wijayanti2Ashok Kumar3Krishna Kamasamudram4Louise Olsson5Competence Centre for Catalysis, Chemical Engineering, Chalmers University of Technology, SE-412 96 Gothenburg, SwedenCompetence Centre for Catalysis, Chemical Engineering, Chalmers University of Technology, SE-412 96 Gothenburg, SwedenCompetence Centre for Catalysis, Chemical Engineering, Chalmers University of Technology, SE-412 96 Gothenburg, SwedenCummins Inc., 1900 McKinley Ave, MC 50183, Columbus, IN 47201, USACummins Inc., 1900 McKinley Ave, MC 50183, Columbus, IN 47201, USACompetence Centre for Catalysis, Chemical Engineering, Chalmers University of Technology, SE-412 96 Gothenburg, SwedenWe developed a procedure for aqueous ion exchange to obtain different Cu loadings of Cu/SAPO-34 (between 0 and 2.6 wt %.) The catalysts were washcoated on monoliths and characterised with respect to their activity and selectivity under standard selective catalytic reduction (SCR), fast SCR, NH3 oxidation and NO oxidation reactions. They were further characterised using X-ray diffraction (XRD), Brunauer–Emmett–Teller (BET), H2-temperature programmed reduction (H2-TPR), ultraviolet (UV)-vis spectroscopy and NH3 adsorption. As expected, activity of all reactions increased with copper loading, due to increased number of active sites. However, the N2O formation during standard and fast SCR yielded interesting mechanistic information. We observed that N2O formation at low temperature increased with copper loading for the standard SCR reaction, while it decreased for fast SCR. The low-temperature N2O formation during fast SCR thus occurs predominantly over Brønsted sites. Species responsible for N2O formation during standard SCR, on the other hand, are formed on the copper sites. We further found that the fast SCR reaction occurs to a significant extent even over the H/SAPO-34 form. The Brønsted sites in SAPO-34 are thus active for the fast SCR reaction.http://www.mdpi.com/1996-1073/10/4/489selective catalytic reduction (SCR)Cu/SAPO-34copper loadingchabazitefast SCRammonia oxidationN2O
spellingShingle Kirsten Leistner
Florian Brüsewitz
Kurnia Wijayanti
Ashok Kumar
Krishna Kamasamudram
Louise Olsson
Impact of Copper Loading on NH3-Selective Catalytic Reduction, Oxidation Reactions and N2O Formation over Cu/SAPO-34
Energies
selective catalytic reduction (SCR)
Cu/SAPO-34
copper loading
chabazite
fast SCR
ammonia oxidation
N2O
title Impact of Copper Loading on NH3-Selective Catalytic Reduction, Oxidation Reactions and N2O Formation over Cu/SAPO-34
title_full Impact of Copper Loading on NH3-Selective Catalytic Reduction, Oxidation Reactions and N2O Formation over Cu/SAPO-34
title_fullStr Impact of Copper Loading on NH3-Selective Catalytic Reduction, Oxidation Reactions and N2O Formation over Cu/SAPO-34
title_full_unstemmed Impact of Copper Loading on NH3-Selective Catalytic Reduction, Oxidation Reactions and N2O Formation over Cu/SAPO-34
title_short Impact of Copper Loading on NH3-Selective Catalytic Reduction, Oxidation Reactions and N2O Formation over Cu/SAPO-34
title_sort impact of copper loading on nh3 selective catalytic reduction oxidation reactions and n2o formation over cu sapo 34
topic selective catalytic reduction (SCR)
Cu/SAPO-34
copper loading
chabazite
fast SCR
ammonia oxidation
N2O
url http://www.mdpi.com/1996-1073/10/4/489
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