Prediction of catalytic activity of Pt3Re1 alloy for C-C bond cleavage in the ethanol oxidation reaction
Design of catalysts able to cleave C-C bond in ethanol oxidation reaction at low temperatures is primordial for improving the direct ethanol proton exchange membrane fuel cells. Pt-Re alloy seems to be an appropriate material for C-C bond cleavage in ethanol decomposition, but yet, it has not been s...
- Autores:
-
Pérez Mendoza, Alejandro Esteban
- Tipo de recurso:
- Fecha de publicación:
- 2016
- Institución:
- Universidad Nacional de Colombia
- Repositorio:
- Universidad Nacional de Colombia
- Idioma:
- spa
- OAI Identifier:
- oai:repositorio.unal.edu.co:unal/58352
- Acceso en línea:
- https://repositorio.unal.edu.co/handle/unal/58352
http://bdigital.unal.edu.co/55117/
- Palabra clave:
- 54 Química y ciencias afines / Chemistry
66 Ingeniería química y Tecnologías relacionadas/ Chemical engineering
PtRe alloy
C-C bond cleavage
Ethanol Oxidation Reaction
Fuel cell
Density Functional Theory
Aleación Pt-Re
Rompimiento enlace C-C
Reacción de oxidación de etanol
Celdas de combustible
Teroría del funcional de densidad
- Rights
- openAccess
- License
- Atribución-NoComercial 4.0 Internacional
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Universidad Nacional de Colombia |
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|
dc.title.spa.fl_str_mv |
Prediction of catalytic activity of Pt3Re1 alloy for C-C bond cleavage in the ethanol oxidation reaction |
title |
Prediction of catalytic activity of Pt3Re1 alloy for C-C bond cleavage in the ethanol oxidation reaction |
spellingShingle |
Prediction of catalytic activity of Pt3Re1 alloy for C-C bond cleavage in the ethanol oxidation reaction 54 Química y ciencias afines / Chemistry 66 Ingeniería química y Tecnologías relacionadas/ Chemical engineering PtRe alloy C-C bond cleavage Ethanol Oxidation Reaction Fuel cell Density Functional Theory Aleación Pt-Re Rompimiento enlace C-C Reacción de oxidación de etanol Celdas de combustible Teroría del funcional de densidad |
title_short |
Prediction of catalytic activity of Pt3Re1 alloy for C-C bond cleavage in the ethanol oxidation reaction |
title_full |
Prediction of catalytic activity of Pt3Re1 alloy for C-C bond cleavage in the ethanol oxidation reaction |
title_fullStr |
Prediction of catalytic activity of Pt3Re1 alloy for C-C bond cleavage in the ethanol oxidation reaction |
title_full_unstemmed |
Prediction of catalytic activity of Pt3Re1 alloy for C-C bond cleavage in the ethanol oxidation reaction |
title_sort |
Prediction of catalytic activity of Pt3Re1 alloy for C-C bond cleavage in the ethanol oxidation reaction |
dc.creator.fl_str_mv |
Pérez Mendoza, Alejandro Esteban |
dc.contributor.author.spa.fl_str_mv |
Pérez Mendoza, Alejandro Esteban |
dc.contributor.spa.fl_str_mv |
Ribadeneira Paz, Rafael Esteban |
dc.subject.ddc.spa.fl_str_mv |
54 Química y ciencias afines / Chemistry 66 Ingeniería química y Tecnologías relacionadas/ Chemical engineering |
topic |
54 Química y ciencias afines / Chemistry 66 Ingeniería química y Tecnologías relacionadas/ Chemical engineering PtRe alloy C-C bond cleavage Ethanol Oxidation Reaction Fuel cell Density Functional Theory Aleación Pt-Re Rompimiento enlace C-C Reacción de oxidación de etanol Celdas de combustible Teroría del funcional de densidad |
dc.subject.proposal.spa.fl_str_mv |
PtRe alloy C-C bond cleavage Ethanol Oxidation Reaction Fuel cell Density Functional Theory Aleación Pt-Re Rompimiento enlace C-C Reacción de oxidación de etanol Celdas de combustible Teroría del funcional de densidad |
description |
Design of catalysts able to cleave C-C bond in ethanol oxidation reaction at low temperatures is primordial for improving the direct ethanol proton exchange membrane fuel cells. Pt-Re alloy seems to be an appropriate material for C-C bond cleavage in ethanol decomposition, but yet, it has not been studied in-depth the reactivity of this alloy for this step. Then, in this work, the reactivity of Pt$_3$Re$_1$ surface for the C-C bond cleavage is studied and compared with reactivity of pure metal surfaces Pt(111) and Re(0001), using Density Functional Theory (DFT) and the descriptor based approach for catalyst design. Adsorption energy of CH, CO and CHCO are proposed as descriptors since they are the molecules involved in C-C bond cleavage of CHCO, which is considered the most likely reaction step for C-C bond cleavage in ethanol oxidation reaction. Consequently, the energetic and geometrical properties of the adsorption of these molecules on Pt, Re and Pt3Re1 are studied and analyzed respect to the electronic structure of the surface in order to understand the reactivity for C-C bond cleavage of the studied surfaces. It was found that the addition of Re to Pt leads to form active sites with Re atoms, which are more reactive for the C-C bond cleavage in CHCO, but the sites without Re are less reactive for this step. These findings suggest that despite higher ability to interact with carbon atoms of Re, the Re addition to Pt does not enhance significantly the C-C cleavage in ethanol oxidation reaction, since the higher reactivity of sites with Re atom in Pt3Re1 should not compensate the lower reactivity of the sites without Re. |
publishDate |
2016 |
dc.date.issued.spa.fl_str_mv |
2016-05-30 |
dc.date.accessioned.spa.fl_str_mv |
2019-07-02T14:03:01Z |
dc.date.available.spa.fl_str_mv |
2019-07-02T14:03:01Z |
dc.type.spa.fl_str_mv |
Trabajo de grado - Maestría |
dc.type.driver.spa.fl_str_mv |
info:eu-repo/semantics/masterThesis |
dc.type.version.spa.fl_str_mv |
info:eu-repo/semantics/acceptedVersion |
dc.type.content.spa.fl_str_mv |
Text |
dc.type.redcol.spa.fl_str_mv |
http://purl.org/redcol/resource_type/TM |
status_str |
acceptedVersion |
dc.identifier.uri.none.fl_str_mv |
https://repositorio.unal.edu.co/handle/unal/58352 |
dc.identifier.eprints.spa.fl_str_mv |
http://bdigital.unal.edu.co/55117/ |
url |
https://repositorio.unal.edu.co/handle/unal/58352 http://bdigital.unal.edu.co/55117/ |
dc.language.iso.spa.fl_str_mv |
spa |
language |
spa |
dc.relation.ispartof.spa.fl_str_mv |
Universidad Nacional de Colombia Sede Medellín Facultad de Minas Escuela de Química y Petróleos Escuela de Química y Petróleos |
dc.relation.references.spa.fl_str_mv |
Pérez Mendoza, Alejandro Esteban (2016) Prediction of catalytic activity of Pt3Re1 alloy for C-C bond cleavage in the ethanol oxidation reaction. Maestría thesis, Universidad Nacional de Colombia - Sede Medellín. |
dc.rights.spa.fl_str_mv |
Derechos reservados - Universidad Nacional de Colombia |
dc.rights.coar.fl_str_mv |
http://purl.org/coar/access_right/c_abf2 |
dc.rights.license.spa.fl_str_mv |
Atribución-NoComercial 4.0 Internacional |
dc.rights.uri.spa.fl_str_mv |
http://creativecommons.org/licenses/by-nc/4.0/ |
dc.rights.accessrights.spa.fl_str_mv |
info:eu-repo/semantics/openAccess |
rights_invalid_str_mv |
Atribución-NoComercial 4.0 Internacional Derechos reservados - Universidad Nacional de Colombia http://creativecommons.org/licenses/by-nc/4.0/ http://purl.org/coar/access_right/c_abf2 |
eu_rights_str_mv |
openAccess |
dc.format.mimetype.spa.fl_str_mv |
application/pdf |
institution |
Universidad Nacional de Colombia |
bitstream.url.fl_str_mv |
https://repositorio.unal.edu.co/bitstream/unal/58352/1/1152685721-2016.pdf https://repositorio.unal.edu.co/bitstream/unal/58352/2/1152685721-2016.pdf.jpg |
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Repositorio Institucional Universidad Nacional de Colombia |
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repositorio_nal@unal.edu.co |
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1814089881483214848 |
spelling |
Atribución-NoComercial 4.0 InternacionalDerechos reservados - Universidad Nacional de Colombiahttp://creativecommons.org/licenses/by-nc/4.0/info:eu-repo/semantics/openAccesshttp://purl.org/coar/access_right/c_abf2Ribadeneira Paz, Rafael EstebanPérez Mendoza, Alejandro Estebanb3a5beba-9007-4201-a571-7df5b69801ee3002019-07-02T14:03:01Z2019-07-02T14:03:01Z2016-05-30https://repositorio.unal.edu.co/handle/unal/58352http://bdigital.unal.edu.co/55117/Design of catalysts able to cleave C-C bond in ethanol oxidation reaction at low temperatures is primordial for improving the direct ethanol proton exchange membrane fuel cells. Pt-Re alloy seems to be an appropriate material for C-C bond cleavage in ethanol decomposition, but yet, it has not been studied in-depth the reactivity of this alloy for this step. Then, in this work, the reactivity of Pt$_3$Re$_1$ surface for the C-C bond cleavage is studied and compared with reactivity of pure metal surfaces Pt(111) and Re(0001), using Density Functional Theory (DFT) and the descriptor based approach for catalyst design. Adsorption energy of CH, CO and CHCO are proposed as descriptors since they are the molecules involved in C-C bond cleavage of CHCO, which is considered the most likely reaction step for C-C bond cleavage in ethanol oxidation reaction. Consequently, the energetic and geometrical properties of the adsorption of these molecules on Pt, Re and Pt3Re1 are studied and analyzed respect to the electronic structure of the surface in order to understand the reactivity for C-C bond cleavage of the studied surfaces. It was found that the addition of Re to Pt leads to form active sites with Re atoms, which are more reactive for the C-C bond cleavage in CHCO, but the sites without Re are less reactive for this step. These findings suggest that despite higher ability to interact with carbon atoms of Re, the Re addition to Pt does not enhance significantly the C-C cleavage in ethanol oxidation reaction, since the higher reactivity of sites with Re atom in Pt3Re1 should not compensate the lower reactivity of the sites without Re.Resumen: El diseño de catalizadores capaces de romper el enlace C-C durante la reacción de oxidación de etanol a bajas temperaturas es primordial para la mejora de las celdas de combustible de membrana de intercambio protónico alimentadas directamente con etanol. La aleación Pt-Re parece un material apropiado para la desestabilazación del enlace C-C en la descomposición de etanol, sin embargo no se ha estudiado en profundidad la reactividad de esta aleación para el paso mencionado. Por tanto, este trabajo estudia la reactividad de Pt3Re1 para la desestabilización del enlace C-C y la compara con la de los metales puros Pt y Re utilizando la Teoría del Funcional de la Densidad (DFT) y el enfoque basado en descriptores de la actividad. Las adsorciones de CH, CO y CHCO se proponen como descriptores ya que son las moléculas implicadas en la desestabilizaciión del enlace C-C en el CHCO, considerada la etapa más probable para el paso de interés. En consecuencia, en este trabajo se calculan las propiedades energéticas y geométricas de la adsorción de estas moléculas sobre Pt, Re y Pt3Re1 y se analizan respecto a la estructura electrónica de las superficies consideradas con el fin de comprender la reactividad de las mismas. Se encontró que la adición de Re a Pt deriva en la formación de un sitio activo con un átomo de Re que es más reactivo para la romper el enlace C-C, pero los sitios sin Re son menos reactivos para este paso. Este hallazgo sugiere que aunque el renio presenta una fuerte interacción con los átomos de carbono en las moléculas estudiadas, la aleación de Pt con Re no tiene un efecto significativo en la promoción del rompimiento del enlace C-C, ya que la mayor reactividad de los sitios con átomos de Re no compensa la menor reactividad de los sitios sin Re.Maestríaapplication/pdfspaUniversidad Nacional de Colombia Sede Medellín Facultad de Minas Escuela de Química y PetróleosEscuela de Química y PetróleosPérez Mendoza, Alejandro Esteban (2016) Prediction of catalytic activity of Pt3Re1 alloy for C-C bond cleavage in the ethanol oxidation reaction. Maestría thesis, Universidad Nacional de Colombia - Sede Medellín.54 Química y ciencias afines / Chemistry66 Ingeniería química y Tecnologías relacionadas/ Chemical engineeringPtRe alloyC-C bond cleavageEthanol Oxidation ReactionFuel cellDensity Functional TheoryAleación Pt-ReRompimiento enlace C-CReacción de oxidación de etanolCeldas de combustibleTeroría del funcional de densidadPrediction of catalytic activity of Pt3Re1 alloy for C-C bond cleavage in the ethanol oxidation reactionTrabajo de grado - Maestríainfo:eu-repo/semantics/masterThesisinfo:eu-repo/semantics/acceptedVersionTexthttp://purl.org/redcol/resource_type/TMORIGINAL1152685721-2016.pdfTesis de Maestría en Ingeniería - Ingeniería Químicaapplication/pdf1903881https://repositorio.unal.edu.co/bitstream/unal/58352/1/1152685721-2016.pdfbd958c4f096503d9adf524fc68b8ef98MD51THUMBNAIL1152685721-2016.pdf.jpg1152685721-2016.pdf.jpgGenerated Thumbnailimage/jpeg4660https://repositorio.unal.edu.co/bitstream/unal/58352/2/1152685721-2016.pdf.jpg71606c99466068a4ade09b030533b9ebMD52unal/58352oai:repositorio.unal.edu.co:unal/583522023-10-10 23:16:11.339Repositorio Institucional Universidad Nacional de Colombiarepositorio_nal@unal.edu.co |