Effect of hydrocarbons on the ammonia selective catalytic reduction of nitrogen oxides under typical diesel engine exhausts conditions over copper-based zeolites

ABSTRACT: The use of diesel engines is growing due to their advantages over the gasoline engines, but they increase nitrogen oxides (NOX) emissions. The ammonia selective catalytic reduction (NH3-SCR) with Cu-based zeolites is the most promising and studied technique for the abatement of NOX. Howeve...

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Autores:
Álvarez Montoya, Andrés Camilo
Tipo de recurso:
Doctoral thesis
Fecha de publicación:
2020
Institución:
Universidad de Antioquia
Repositorio:
Repositorio UdeA
Idioma:
eng
OAI Identifier:
oai:bibliotecadigital.udea.edu.co:10495/17180
Acceso en línea:
http://hdl.handle.net/10495/17180
Palabra clave:
Hydrocarbons
Hidrocarburo
Nitrogen
Nitrógeno
X-rays
Rayos X
Temperature
Temperatura
Nitrogen oxides
Óxidos de nitrógeno
Cu-zeolite
Hidrocarbons
Kinetics
NH3-SCR of NO
NH3-TPD
http://aims.fao.org/aos/agrovoc/c_16002
http://vocabularies.unesco.org/thesaurus/concept11253
http://vocabularies.unesco.org/thesaurus/concept3491
http://vocabularies.unesco.org/thesaurus/concept9535
http://vocabularies.unesco.org/thesaurus/concept4155
Rights
openAccess
License
Atribución-NoComercial-SinDerivadas 2.5 Colombia (CC BY-NC-ND 2.5 CO)
id UDEA2_9d48c7e68117657b13ae71faa8534f6f
oai_identifier_str oai:bibliotecadigital.udea.edu.co:10495/17180
network_acronym_str UDEA2
network_name_str Repositorio UdeA
repository_id_str
dc.title.spa.fl_str_mv Effect of hydrocarbons on the ammonia selective catalytic reduction of nitrogen oxides under typical diesel engine exhausts conditions over copper-based zeolites
dc.title.alternative.spa.fl_str_mv Efecto de hidrocarburos en la reducción catalítica selectiva de óxidos de nitrógeno bajo condiciones típicas de motores diésel en zeolitas basadas en cobre
title Effect of hydrocarbons on the ammonia selective catalytic reduction of nitrogen oxides under typical diesel engine exhausts conditions over copper-based zeolites
spellingShingle Effect of hydrocarbons on the ammonia selective catalytic reduction of nitrogen oxides under typical diesel engine exhausts conditions over copper-based zeolites
Hydrocarbons
Hidrocarburo
Nitrogen
Nitrógeno
X-rays
Rayos X
Temperature
Temperatura
Nitrogen oxides
Óxidos de nitrógeno
Cu-zeolite
Hidrocarbons
Kinetics
NH3-SCR of NO
NH3-TPD
http://aims.fao.org/aos/agrovoc/c_16002
http://vocabularies.unesco.org/thesaurus/concept11253
http://vocabularies.unesco.org/thesaurus/concept3491
http://vocabularies.unesco.org/thesaurus/concept9535
http://vocabularies.unesco.org/thesaurus/concept4155
title_short Effect of hydrocarbons on the ammonia selective catalytic reduction of nitrogen oxides under typical diesel engine exhausts conditions over copper-based zeolites
title_full Effect of hydrocarbons on the ammonia selective catalytic reduction of nitrogen oxides under typical diesel engine exhausts conditions over copper-based zeolites
title_fullStr Effect of hydrocarbons on the ammonia selective catalytic reduction of nitrogen oxides under typical diesel engine exhausts conditions over copper-based zeolites
title_full_unstemmed Effect of hydrocarbons on the ammonia selective catalytic reduction of nitrogen oxides under typical diesel engine exhausts conditions over copper-based zeolites
title_sort Effect of hydrocarbons on the ammonia selective catalytic reduction of nitrogen oxides under typical diesel engine exhausts conditions over copper-based zeolites
dc.creator.fl_str_mv Álvarez Montoya, Andrés Camilo
dc.contributor.advisor.none.fl_str_mv González Rodríguez, Lina María
dc.contributor.author.none.fl_str_mv Álvarez Montoya, Andrés Camilo
dc.subject.unesco.none.fl_str_mv Hydrocarbons
Hidrocarburo
Nitrogen
Nitrógeno
X-rays
Rayos X
Temperature
Temperatura
topic Hydrocarbons
Hidrocarburo
Nitrogen
Nitrógeno
X-rays
Rayos X
Temperature
Temperatura
Nitrogen oxides
Óxidos de nitrógeno
Cu-zeolite
Hidrocarbons
Kinetics
NH3-SCR of NO
NH3-TPD
http://aims.fao.org/aos/agrovoc/c_16002
http://vocabularies.unesco.org/thesaurus/concept11253
http://vocabularies.unesco.org/thesaurus/concept3491
http://vocabularies.unesco.org/thesaurus/concept9535
http://vocabularies.unesco.org/thesaurus/concept4155
dc.subject.agrovoc.none.fl_str_mv Nitrogen oxides
Óxidos de nitrógeno
dc.subject.proposal.spa.fl_str_mv Cu-zeolite
Hidrocarbons
Kinetics
NH3-SCR of NO
NH3-TPD
dc.subject.agrovocuri.none.fl_str_mv http://aims.fao.org/aos/agrovoc/c_16002
dc.subject.unescouri.none.fl_str_mv http://vocabularies.unesco.org/thesaurus/concept11253
http://vocabularies.unesco.org/thesaurus/concept3491
http://vocabularies.unesco.org/thesaurus/concept9535
http://vocabularies.unesco.org/thesaurus/concept4155
description ABSTRACT: The use of diesel engines is growing due to their advantages over the gasoline engines, but they increase nitrogen oxides (NOX) emissions. The ammonia selective catalytic reduction (NH3-SCR) with Cu-based zeolites is the most promising and studied technique for the abatement of NOX. However, research under more realistic conditions, such as including hydrocarbons on the simulated gas, needs to be studied deeply. We selected Cu-ZSM-5, Cu-SSZ-13, and Cu-SAPO-34 (three of the most successful and investigated catalysts in the NH3-SCR of NOX) to perform a series of experiments regarding the effect of propylene and dodecane (two hydrocarbons that can be present in diesel exhausts) on the NH3-SCR of NO and adsorption of NH3. We synthesized the catalysts by ion exchange and confirmed their structure by X-ray diffraction. We found that both propylene and dodecane reduced the amount NH3 adsorbed on the catalysts. Also, we determined that experiments of temperature-programmed desorption of NH3 of Cu-ZSM-5 and Cu-SAPO-34 saturated with propylene changed the parameters of the desorption kinetic of the catalysts, and mainly affected the acid sites that not concern copper. We confirmed that dodecane (a long-chain hydrocarbon) affected the performance of Cu-SSZ-13 (a small-pore zeolite) on the NH3-SCR and NH3oxidation. Finally, we found that the hydrocarbons decreased the activation energy and changed the parameters of a power-law kinetic of Cu-ZSM-5 and Cu-SSZ-13 in the NH3-SCR of NO.
publishDate 2020
dc.date.accessioned.none.fl_str_mv 2020-11-05T16:37:59Z
dc.date.available.none.fl_str_mv 2020-11-05T16:37:59Z
dc.date.issued.none.fl_str_mv 2020
dc.type.spa.fl_str_mv info:eu-repo/semantics/doctoralThesis
dc.type.coarversion.fl_str_mv http://purl.org/coar/version/c_b1a7d7d4d402bcce
dc.type.hasversion.spa.fl_str_mv info:eu-repo/semantics/draft
dc.type.coar.spa.fl_str_mv http://purl.org/coar/resource_type/c_db06
dc.type.redcol.spa.fl_str_mv https://purl.org/redcol/resource_type/TD
dc.type.local.spa.fl_str_mv Tesis/Trabajo de grado - Monografía - Doctorado
format http://purl.org/coar/resource_type/c_db06
status_str draft
dc.identifier.uri.none.fl_str_mv http://hdl.handle.net/10495/17180
url http://hdl.handle.net/10495/17180
dc.language.iso.spa.fl_str_mv eng
language eng
dc.rights.*.fl_str_mv Atribución-NoComercial-SinDerivadas 2.5 Colombia (CC BY-NC-ND 2.5 CO)
dc.rights.spa.fl_str_mv info:eu-repo/semantics/openAccess
dc.rights.uri.*.fl_str_mv http://creativecommons.org/licenses/by-nc-nd/2.5/co/
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dc.rights.creativecommons.spa.fl_str_mv https://creativecommons.org/licenses/by-nc-nd/4.0/
rights_invalid_str_mv Atribución-NoComercial-SinDerivadas 2.5 Colombia (CC BY-NC-ND 2.5 CO)
http://creativecommons.org/licenses/by-nc-nd/2.5/co/
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eu_rights_str_mv openAccess
dc.format.extent.spa.fl_str_mv 141
dc.format.mimetype.spa.fl_str_mv application/pdf
dc.publisher.group.spa.fl_str_mv Catálisis Ambiental
dc.publisher.place.spa.fl_str_mv Medellín, Colombia
institution Universidad de Antioquia
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spelling González Rodríguez, Lina MaríaÁlvarez Montoya, Andrés Camilo2020-11-05T16:37:59Z2020-11-05T16:37:59Z2020http://hdl.handle.net/10495/17180ABSTRACT: The use of diesel engines is growing due to their advantages over the gasoline engines, but they increase nitrogen oxides (NOX) emissions. The ammonia selective catalytic reduction (NH3-SCR) with Cu-based zeolites is the most promising and studied technique for the abatement of NOX. However, research under more realistic conditions, such as including hydrocarbons on the simulated gas, needs to be studied deeply. We selected Cu-ZSM-5, Cu-SSZ-13, and Cu-SAPO-34 (three of the most successful and investigated catalysts in the NH3-SCR of NOX) to perform a series of experiments regarding the effect of propylene and dodecane (two hydrocarbons that can be present in diesel exhausts) on the NH3-SCR of NO and adsorption of NH3. We synthesized the catalysts by ion exchange and confirmed their structure by X-ray diffraction. We found that both propylene and dodecane reduced the amount NH3 adsorbed on the catalysts. Also, we determined that experiments of temperature-programmed desorption of NH3 of Cu-ZSM-5 and Cu-SAPO-34 saturated with propylene changed the parameters of the desorption kinetic of the catalysts, and mainly affected the acid sites that not concern copper. We confirmed that dodecane (a long-chain hydrocarbon) affected the performance of Cu-SSZ-13 (a small-pore zeolite) on the NH3-SCR and NH3oxidation. Finally, we found that the hydrocarbons decreased the activation energy and changed the parameters of a power-law kinetic of Cu-ZSM-5 and Cu-SSZ-13 in the NH3-SCR of NO.RESUMEN: El uso de motores diésel está creciendo debido a sus ventajas sobre los motores a gasolina, pero aumentan las emisiones de óxidos de nitrógeno (NOX). La reducción catalítica selectiva con amoniaco (NH3-RCS) utilizando zeolitas basadas en cobre es la técnica más prometedora y estudiada para la reducción de NOX. Sin embargo, su investigación bajo condiciones más reales, como la inclusión de hidrocarburos en el gas simulado, necesitan ser estudiadas profundamente. Se seleccionaron Cu-ZSM-5, Cu-SSZ-13 y Cu-SAPO-34 (tres de los catalizadores más exitosos e investigados en la NH3-RCS deNOX) para desarrollar una serie de experimentos concernientes al efecto del propileno y el dodecano (dos hidrocarburos que pueden estar presentes en exhostos de motores diésel) en procesos relacionados con la NH3-RCS de NOX. Los catalizadores se sintetizaron por intercambio iónico y su estructura fue corroborada por difracción de rayos X. Se encontró que tanto el propileno como el dodecano redujeron la cantidad de amoniaco desorbida en los catalizadores, la cual es una etapa muy importante para que la reacción de NH3-RCS ocurra. Además, se determinó que experimentos de desorción a temperatura programada de amoniaco de Cu-ZSM-5 y Cu-SAPO-34 saturados con propileno cambia los parámetros de la cinética de desorción de ambos catalizadores y principalmente afecta los sitios ácidos no relacionados con cobre. Se encontró que el dodecano (un hidrocarburo de cadena larga) afecta el desempeño la Cu-SSZ-13 (una zeolita de poro pequeño) en la NH3-RCS de NO y en la oxidación de NH3. Finalmente, se encontró que los hidrocarburos disminuyeron la energía de activación y cambiaron los parámetros de una cinética de ley de potencias de la Cu-ZSM-5 y la Cu-SSZ-13 en la reacción de NH3-RCS de NO.141application/pdfenginfo:eu-repo/semantics/draftinfo:eu-repo/semantics/doctoralThesishttp://purl.org/coar/resource_type/c_db06https://purl.org/redcol/resource_type/TDTesis/Trabajo de grado - Monografía - Doctoradohttp://purl.org/coar/version/c_b1a7d7d4d402bcceAtribución-NoComercial-SinDerivadas 2.5 Colombia (CC BY-NC-ND 2.5 CO)info:eu-repo/semantics/openAccesshttp://creativecommons.org/licenses/by-nc-nd/2.5/co/http://purl.org/coar/access_right/c_abf2https://creativecommons.org/licenses/by-nc-nd/4.0/Effect of hydrocarbons on the ammonia selective catalytic reduction of nitrogen oxides under typical diesel engine exhausts conditions over copper-based zeolitesEfecto de hidrocarburos en la reducción catalítica selectiva de óxidos de nitrógeno bajo condiciones típicas de motores diésel en zeolitas basadas en cobreCatálisis AmbientalMedellín, ColombiaHydrocarbonsHidrocarburoNitrogenNitrógenoX-raysRayos XTemperatureTemperaturaNitrogen oxidesÓxidos de nitrógenoCu-zeoliteHidrocarbonsKineticsNH3-SCR of NONH3-TPDhttp://aims.fao.org/aos/agrovoc/c_16002http://vocabularies.unesco.org/thesaurus/concept11253http://vocabularies.unesco.org/thesaurus/concept3491http://vocabularies.unesco.org/thesaurus/concept9535http://vocabularies.unesco.org/thesaurus/concept4155Doctor en Ingeniería QuímicaDoctoradoFacultad de Ingeniería. Doctorado en Ingeniería QuímicaUniversidad de AntioquiaCC-LICENSElicense_rdflicense_rdfapplication/rdf+xml; charset=utf-8712http://bibliotecadigital.udea.edu.co/bitstream/10495/17180/3/license_rdffd0548b8694973befb689f3e7a707f1dMD53LICENSElicense.txtlicense.txttext/plain; charset=utf-81748http://bibliotecadigital.udea.edu.co/bitstream/10495/17180/4/license.txt8a4605be74aa9ea9d79846c1fba20a33MD54ORIGINALAlvarezAndres_2020_EffectHydrocarbonsSCR.pdfAlvarezAndres_2020_EffectHydrocarbonsSCR.pdfTesis doctoralapplication/pdf17629885http://bibliotecadigital.udea.edu.co/bitstream/10495/17180/2/AlvarezAndres_2020_EffectHydrocarbonsSCR.pdfcec79888718c849ee2fc97a65259fc0cMD5210495/17180oai:bibliotecadigital.udea.edu.co:10495/171802021-05-21 11:44:41.612Repositorio Institucional Universidad de Antioquiaandres.perez@udea.edu.coTk9URTogUExBQ0UgWU9VUiBPV04gTElDRU5TRSBIRVJFClRoaXMgc2FtcGxlIGxpY2Vuc2UgaXMgcHJvdmlkZWQgZm9yIGluZm9ybWF0aW9uYWwgcHVycG9zZXMgb25seS4KCk5PTi1FWENMVVNJVkUgRElTVFJJQlVUSU9OIExJQ0VOU0UKCkJ5IHNpZ25pbmcgYW5kIHN1Ym1pdHRpbmcgdGhpcyBsaWNlbnNlLCB5b3UgKHRoZSBhdXRob3Iocykgb3IgY29weXJpZ2h0Cm93bmVyKSBncmFudHMgdG8gRFNwYWNlIFVuaXZlcnNpdHkgKERTVSkgdGhlIG5vbi1leGNsdXNpdmUgcmlnaHQgdG8gcmVwcm9kdWNlLAp0cmFuc2xhdGUgKGFzIGRlZmluZWQgYmVsb3cpLCBhbmQvb3IgZGlzdHJpYnV0ZSB5b3VyIHN1Ym1pc3Npb24gKGluY2x1ZGluZwp0aGUgYWJzdHJhY3QpIHdvcmxkd2lkZSBpbiBwcmludCBhbmQgZWxlY3Ryb25pYyBmb3JtYXQgYW5kIGluIGFueSBtZWRpdW0sCmluY2x1ZGluZyBidXQgbm90IGxpbWl0ZWQgdG8gYXVkaW8gb3IgdmlkZW8uCgpZb3UgYWdyZWUgdGhhdCBEU1UgbWF5LCB3aXRob3V0IGNoYW5naW5nIHRoZSBjb250ZW50LCB0cmFuc2xhdGUgdGhlCnN1Ym1pc3Npb24gdG8gYW55IG1lZGl1bSBvciBmb3JtYXQgZm9yIHRoZSBwdXJwb3NlIG9mIHByZXNlcnZhdGlvbi4KCllvdSBhbHNvIGFncmVlIHRoYXQgRFNVIG1heSBrZWVwIG1vcmUgdGhhbiBvbmUgY29weSBvZiB0aGlzIHN1Ym1pc3Npb24gZm9yCnB1cnBvc2VzIG9mIHNlY3VyaXR5LCBiYWNrLXVwIGFuZCBwcmVzZXJ2YXRpb24uCgpZb3UgcmVwcmVzZW50IHRoYXQgdGhlIHN1Ym1pc3Npb24gaXMgeW91ciBvcmlnaW5hbCB3b3JrLCBhbmQgdGhhdCB5b3UgaGF2ZQp0aGUgcmlnaHQgdG8gZ3JhbnQgdGhlIHJpZ2h0cyBjb250YWluZWQgaW4gdGhpcyBsaWNlbnNlLiBZb3UgYWxzbyByZXByZXNlbnQKdGhhdCB5b3VyIHN1Ym1pc3Npb24gZG9lcyBub3QsIHRvIHRoZSBiZXN0IG9mIHlvdXIga25vd2xlZGdlLCBpbmZyaW5nZSB1cG9uCmFueW9uZSdzIGNvcHlyaWdodC4KCklmIHRoZSBzdWJtaXNzaW9uIGNvbnRhaW5zIG1hdGVyaWFsIGZvciB3aGljaCB5b3UgZG8gbm90IGhvbGQgY29weXJpZ2h0LAp5b3UgcmVwcmVzZW50IHRoYXQgeW91IGhhdmUgb2J0YWluZWQgdGhlIHVucmVzdHJpY3RlZCBwZXJtaXNzaW9uIG9mIHRoZQpjb3B5cmlnaHQgb3duZXIgdG8gZ3JhbnQgRFNVIHRoZSByaWdodHMgcmVxdWlyZWQgYnkgdGhpcyBsaWNlbnNlLCBhbmQgdGhhdApzdWNoIHRoaXJkLXBhcnR5IG93bmVkIG1hdGVyaWFsIGlzIGNsZWFybHkgaWRlbnRpZmllZCBhbmQgYWNrbm93bGVkZ2VkCndpdGhpbiB0aGUgdGV4dCBvciBjb250ZW50IG9mIHRoZSBzdWJtaXNzaW9uLgoKSUYgVEhFIFNVQk1JU1NJT04gSVMgQkFTRUQgVVBPTiBXT1JLIFRIQVQgSEFTIEJFRU4gU1BPTlNPUkVEIE9SIFNVUFBPUlRFRApCWSBBTiBBR0VOQ1kgT1IgT1JHQU5JWkFUSU9OIE9USEVSIFRIQU4gRFNVLCBZT1UgUkVQUkVTRU5UIFRIQVQgWU9VIEhBVkUKRlVMRklMTEVEIEFOWSBSSUdIVCBPRiBSRVZJRVcgT1IgT1RIRVIgT0JMSUdBVElPTlMgUkVRVUlSRUQgQlkgU1VDSApDT05UUkFDVCBPUiBBR1JFRU1FTlQuCgpEU1Ugd2lsbCBjbGVhcmx5IGlkZW50aWZ5IHlvdXIgbmFtZShzKSBhcyB0aGUgYXV0aG9yKHMpIG9yIG93bmVyKHMpIG9mIHRoZQpzdWJtaXNzaW9uLCBhbmQgd2lsbCBub3QgbWFrZSBhbnkgYWx0ZXJhdGlvbiwgb3RoZXIgdGhhbiBhcyBhbGxvd2VkIGJ5IHRoaXMKbGljZW5zZSwgdG8geW91ciBzdWJtaXNzaW9uLgo=