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...
- 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/ |
dc.rights.accessrights.spa.fl_str_mv |
http://purl.org/coar/access_right/c_abf2 |
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/ http://purl.org/coar/access_right/c_abf2 https://creativecommons.org/licenses/by-nc-nd/4.0/ |
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 |
bitstream.url.fl_str_mv |
http://bibliotecadigital.udea.edu.co/bitstream/10495/17180/3/license_rdf http://bibliotecadigital.udea.edu.co/bitstream/10495/17180/4/license.txt http://bibliotecadigital.udea.edu.co/bitstream/10495/17180/2/AlvarezAndres_2020_EffectHydrocarbonsSCR.pdf |
bitstream.checksum.fl_str_mv |
fd0548b8694973befb689f3e7a707f1d 8a4605be74aa9ea9d79846c1fba20a33 cec79888718c849ee2fc97a65259fc0c |
bitstream.checksumAlgorithm.fl_str_mv |
MD5 MD5 MD5 |
repository.name.fl_str_mv |
Repositorio Institucional Universidad de Antioquia |
repository.mail.fl_str_mv |
andres.perez@udea.edu.co |
_version_ |
1812173171735920640 |
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.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 |