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...

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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
id UNACIONAL2_fc4bf2db6c8f0d8be0a8ea00e177382c
oai_identifier_str oai:repositorio.unal.edu.co:unal/58352
network_acronym_str UNACIONAL2
network_name_str Universidad Nacional de Colombia
repository_id_str
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
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repository.name.fl_str_mv Repositorio Institucional Universidad Nacional de Colombia
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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