Influence of iron aggregation on the catalytic performance of desilicated MFI in the DeNO(x) process

[EN] In the present study, an influence of the iron aggregation in conventional and micro-mesoporous MFI on their catalytic activity in the NO reduction with ammonia (DeNO(x) process) was studied. Modification of MFI zeolite properties was done by the desilication in the presence of NaOH and TPAOH (...

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Published in:Microporous and Mesoporous Materials
Main Authors: Rutkowska, M., Borcuch, A., Marzec, A., Kowalczyk, A., Samojeden, B., Moreno, J.M., DÍAZ MORALES, URBANO MANUEL, Chmielarz, L.
Other Authors: Universitat Politècnica de València. Instituto Universitario Mixto de Tecnología Química - Institut Universitari Mixt de Tecnologia Química, National Science Centre, Polonia, Agencia Estatal de Investigación, Ministerstwo Edukacji i Nauki, Polonia
Format: Article in Journal/Newspaper
Language:English
Published: Elsevier 2020
Subjects:
Online Access:http://hdl.handle.net/10251/176437
https://doi.org/10.1016/j.micromeso.2018.09.015
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collection Politechnical University of Valencia: RiuNet
op_collection_id ftunivpvalencia
language English
topic Iron aggregation
Oligocations
Mesoporous MFI
DeNO(x) process
spellingShingle Iron aggregation
Oligocations
Mesoporous MFI
DeNO(x) process
Rutkowska, M.
Borcuch, A.
Marzec, A.
Kowalczyk, A.
Samojeden, B.
Moreno, J.M.
DÍAZ MORALES, URBANO MANUEL
Chmielarz, L.
Influence of iron aggregation on the catalytic performance of desilicated MFI in the DeNO(x) process
topic_facet Iron aggregation
Oligocations
Mesoporous MFI
DeNO(x) process
description [EN] In the present study, an influence of the iron aggregation in conventional and micro-mesoporous MFI on their catalytic activity in the NO reduction with ammonia (DeNO(x) process) was studied. Modification of MFI zeolite properties was done by the desilication in the presence of NaOH and TPAOH (tertapropylammonium hydroxide). In the next step, the samples were modified with iron by ion-exchange with the use of a conventional solution of Fe cations (FeSO4) and a solution of iron triple-metallic aggregates (oligocations) ([Fe-3(OAc)(6)O(H2O)(3)](+)). Both of the applied modification techniques (desilication and modification with Fe-3 oligocations) increased the catalytic activity of the MFI zeolite in the DeNO(x) process. This increased catalytic activity was connected with changes in sample porosity, Si/Al ratio, topology, as well as aggregation and dispersion of iron species on the catalyst surface, which was investigated by N-2-sorption, XRD, ICP, NMR, HRTEM and UV-vis-DRS techniques. This work was carried out in the frame of project No. 0670/IP3/2016/74 from the Polish Ministry of Science and Higher Education in the years 2016-2019 and in the frame of project No. 2012/05/B/ST5/00269 from the National Science Centre (Poland). U. D. acknowledges to the Spanish Government by the funding (MAT2017-82288-C2-1-P). Rutkowska, M.; Borcuch, A.; Marzec, A.; Kowalczyk, A.; Samojeden, B.; Moreno, J.; Díaz Morales, UM. (2020). Influence of iron aggregation on the catalytic performance of desilicated MFI in the DeNO(x) process. Microporous and Mesoporous Materials. 304:1-8. https://doi.org/10.1016/j.micromeso.2018.09.015 1 8 304
author2 Universitat Politècnica de València. Instituto Universitario Mixto de Tecnología Química - Institut Universitari Mixt de Tecnologia Química
National Science Centre, Polonia
Agencia Estatal de Investigación
Ministerstwo Edukacji i Nauki, Polonia
format Article in Journal/Newspaper
author Rutkowska, M.
Borcuch, A.
Marzec, A.
Kowalczyk, A.
Samojeden, B.
Moreno, J.M.
DÍAZ MORALES, URBANO MANUEL
Chmielarz, L.
author_facet Rutkowska, M.
Borcuch, A.
Marzec, A.
Kowalczyk, A.
Samojeden, B.
Moreno, J.M.
DÍAZ MORALES, URBANO MANUEL
Chmielarz, L.
author_sort Rutkowska, M.
title Influence of iron aggregation on the catalytic performance of desilicated MFI in the DeNO(x) process
title_short Influence of iron aggregation on the catalytic performance of desilicated MFI in the DeNO(x) process
title_full Influence of iron aggregation on the catalytic performance of desilicated MFI in the DeNO(x) process
title_fullStr Influence of iron aggregation on the catalytic performance of desilicated MFI in the DeNO(x) process
title_full_unstemmed Influence of iron aggregation on the catalytic performance of desilicated MFI in the DeNO(x) process
title_sort influence of iron aggregation on the catalytic performance of desilicated mfi in the deno(x) process
publisher Elsevier
publishDate 2020
url http://hdl.handle.net/10251/176437
https://doi.org/10.1016/j.micromeso.2018.09.015
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spelling ftunivpvalencia:oai:riunet.upv.es:10251/176437 2024-01-28T10:08:59+01:00 Influence of iron aggregation on the catalytic performance of desilicated MFI in the DeNO(x) process Rutkowska, M. Borcuch, A. Marzec, A. Kowalczyk, A. Samojeden, B. Moreno, J.M. DÍAZ MORALES, URBANO MANUEL Chmielarz, L. Universitat Politècnica de València. Instituto Universitario Mixto de Tecnología Química - Institut Universitari Mixt de Tecnologia Química National Science Centre, Polonia Agencia Estatal de Investigación Ministerstwo Edukacji i Nauki, Polonia 2020-09 http://hdl.handle.net/10251/176437 https://doi.org/10.1016/j.micromeso.2018.09.015 eng eng Elsevier Microporous and Mesoporous Materials info:eu-repo/grantAgreement/NCN//2012%2F05%2FB%2FST5%2F00269/ info:eu-repo/grantAgreement/Ministerstwo Edukacji i Nauki, Polonia//0670%2FIP3%2F2016%2F74/ info:eu-repo/grantAgreement/AEI//MAT2017-82288-C2-1-P//MATERIALES HIBRIDOS MULTIFUNCIONALES BASADOS EN NANO-UNIDADES ESTRUCTURALES ACTIVAS/ https://doi.org/10.1016/j.micromeso.2018.09.015 10.1021/cr00035a006 10.1002/chem.200401329 10.1039/C2CS35330J 10.1080/01614940701583240 10.1039/B517510K 10.1016/j.apcatb.2007.06.006 10.1016/j.micromeso.2017.03.017 10.1016/j.crci.2017.05.001 10.1016/j.apcatb.2013.05.005 10.1016/j.micromeso.2014.10.011 10.1039/C6CY00040A 10.1016/j.apcatb.2015.01.016 10.1016/j.colsurfa.2004.04.012 10.1016/j.micromeso.2004.01.002 10.1021/ie061146v 10.1021/jp047194f 10.1002/adfm.200901394 10.1016/j.pnsc.2013.08.005 10.1016/j.apcatb.2015.05.053 10.1016/j.jcat.2004.08.003 10.1016/j.jcat.2005.01.031 10.1016/j.materresbull.2016.02.026 10.1016/j.matchemphys.2016.11.047 10.1016/0927-6513(94)00080-F 10.1016/S0926-860X(01)00832-8 10.1016/S0926-3373(98)00040-X 10.1006/jcat.1993.1232 10.1016/j.apcatb.2013.03.022 10.1016/j.micromeso.2014.10.023 10.1016/0926-860X(95)00154-9 10.1016/j.apcatb.2006.03.012 10.1016/j.apcatb.2010.01.013 10.1023/A:1016689822033 10.1016/j.cattod.2014.12.017 10.1016/S0167-2991(07)80008-5 10.1515/pac-2014-1117 10.1007/s10934-013-9751-x 10.1016/j.apcatb.2015.03.006 10.1016/j.micromeso.2012.03.045 10.1016/j.cattod.2010.01.059 10.1016/j.micromeso.2011.02.013 10.1016/j.cattod.2014.03.018 10.1016/j.jcat.2017.12.011 10.1016/S1872-2067(16)62534-2 urn:issn:1387-1811 http://creativecommons.org/licenses/by-nc-nd/4.0/ info:eu-repo/semantics/openAccess Iron aggregation Oligocations Mesoporous MFI DeNO(x) process info:eu-repo/semantics/article info:eu-repo/semantics/publishedVersion 2020 ftunivpvalencia https://doi.org/10.1016/j.micromeso.2018.09.015 2024-01-03T00:05:56Z [EN] In the present study, an influence of the iron aggregation in conventional and micro-mesoporous MFI on their catalytic activity in the NO reduction with ammonia (DeNO(x) process) was studied. Modification of MFI zeolite properties was done by the desilication in the presence of NaOH and TPAOH (tertapropylammonium hydroxide). In the next step, the samples were modified with iron by ion-exchange with the use of a conventional solution of Fe cations (FeSO4) and a solution of iron triple-metallic aggregates (oligocations) ([Fe-3(OAc)(6)O(H2O)(3)](+)). Both of the applied modification techniques (desilication and modification with Fe-3 oligocations) increased the catalytic activity of the MFI zeolite in the DeNO(x) process. This increased catalytic activity was connected with changes in sample porosity, Si/Al ratio, topology, as well as aggregation and dispersion of iron species on the catalyst surface, which was investigated by N-2-sorption, XRD, ICP, NMR, HRTEM and UV-vis-DRS techniques. This work was carried out in the frame of project No. 0670/IP3/2016/74 from the Polish Ministry of Science and Higher Education in the years 2016-2019 and in the frame of project No. 2012/05/B/ST5/00269 from the National Science Centre (Poland). U. D. acknowledges to the Spanish Government by the funding (MAT2017-82288-C2-1-P). Rutkowska, M.; Borcuch, A.; Marzec, A.; Kowalczyk, A.; Samojeden, B.; Moreno, J.; Díaz Morales, UM. (2020). Influence of iron aggregation on the catalytic performance of desilicated MFI in the DeNO(x) process. Microporous and Mesoporous Materials. 304:1-8. https://doi.org/10.1016/j.micromeso.2018.09.015 1 8 304 Article in Journal/Newspaper samojed* samojed* Politechnical University of Valencia: RiuNet Kowalczyk ENVELOPE(163.783,163.783,-77.933,-77.933) Morales ENVELOPE(-55.833,-55.833,-63.000,-63.000) Moreno ENVELOPE(-62.300,-62.300,-64.083,-64.083) Microporous and Mesoporous Materials 304 109114