Production of Solar Fuels by Photoelectrochemical Conversion of Carbon Dioxide

[eng] Growing global emission of carbon dioxide gas (CO2) reflects the world’s energy dependence on fossil fuels. The conversion of CO2 emission into value-added products, like fuels completes a circular CO2 economy which requires a renewable energy conversion and storage system. Amongst a few, phot...

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Autor: Irtem, Ibrahim Erdem
Tipo de recurso: tesis doctoral
Estado:Versión publicada
Fecha de publicación:2017
País:España
Institución:Universidad de Barcelona
Repositorio:Dipòsit Digital de la UB
OAI Identifier:oai:diposit.ub.edu:2445/112608
Acceso en línea:https://hdl.handle.net/2445/112608
http://hdl.handle.net/10803/404018
Access Level:acceso abierto
Palabra clave:Electroquímica
Diòxid de carboni
Catàlisi
Fotoelectroquímica
Galvanoplàstia
Electrochemistry
Carbon dioxide
Catalysis
Photoelectrochemistry
Electroplating
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oai_identifier_str oai:diposit.ub.edu:2445/112608
network_acronym_str ES
network_name_str España
repository_id_str
dc.title.none.fl_str_mv Production of Solar Fuels by Photoelectrochemical Conversion of Carbon Dioxide
title Production of Solar Fuels by Photoelectrochemical Conversion of Carbon Dioxide
spellingShingle Production of Solar Fuels by Photoelectrochemical Conversion of Carbon Dioxide
Irtem, Ibrahim Erdem
Electroquímica
Diòxid de carboni
Catàlisi
Fotoelectroquímica
Galvanoplàstia
Electrochemistry
Carbon dioxide
Catalysis
Photoelectrochemistry
Electroplating
title_short Production of Solar Fuels by Photoelectrochemical Conversion of Carbon Dioxide
title_full Production of Solar Fuels by Photoelectrochemical Conversion of Carbon Dioxide
title_fullStr Production of Solar Fuels by Photoelectrochemical Conversion of Carbon Dioxide
title_full_unstemmed Production of Solar Fuels by Photoelectrochemical Conversion of Carbon Dioxide
title_sort Production of Solar Fuels by Photoelectrochemical Conversion of Carbon Dioxide
dc.creator.none.fl_str_mv Irtem, Ibrahim Erdem
author Irtem, Ibrahim Erdem
author_facet Irtem, Ibrahim Erdem
author_role author
dc.contributor.none.fl_str_mv Morante i Lleonart, Joan Ramon
Andreu Arbella, Teresa
Universitat de Barcelona. Departament d'Enginyeries: Secció d'Electrònica
dc.subject.none.fl_str_mv Electroquímica
Diòxid de carboni
Catàlisi
Fotoelectroquímica
Galvanoplàstia
Electrochemistry
Carbon dioxide
Catalysis
Photoelectrochemistry
Electroplating
topic Electroquímica
Diòxid de carboni
Catàlisi
Fotoelectroquímica
Galvanoplàstia
Electrochemistry
Carbon dioxide
Catalysis
Photoelectrochemistry
Electroplating
description [eng] Growing global emission of carbon dioxide gas (CO2) reflects the world’s energy dependence on fossil fuels. The conversion of CO2 emission into value-added products, like fuels completes a circular CO2 economy which requires a renewable energy conversion and storage system. Amongst a few, photo/electrochemistry has been particularly appealing thanks to its energy efficiency and enormous potential for industrial applications. Formic acid (HCOOH) production from CO2 reduction appears as an alternative energy storage option based on the commercialization of this process. Herein, stable and selective catalysts working at low overpotential are needed to reduce CO2. Likewise, cell design is critical to have improved CO2 mass transport for obtaining high conversion efficiencies and to achieve feasible production yields. The initial work was conducted on the design and understanding of operational parameters of an electrochemical flow cell (ECf-cell) such as flow rates and electrode potentials. For CO2 reduction at the cathode site, two different gas diffusion electrodes were produced by electrodeposition: Sn-GDE and Cu-GDE. An optimum potential range was established to control HCOOH selectivity. The complementing reaction at the anode site, oxygen evolution reaction (OER), was studied using Mn-Co oxide nanoparticles to replace expensive DSA: Ir-Ta oxide catalyst. Subsequent efforts were devoted on the assembly of a photoelectrochemical flow cell (PECf-cell) which enabled coupling of Sn-GDE as cathode vs. TiO2 nanorods as photoanode. This led to nearly 1/3 reduction in overall cell voltage reaching an energy efficiency up to 70 %. The solar-to-fuel (STF) conversion efficiency was 0.25% which was one of the highest efficiencies reported amongst the data obtained from a cell in device level. The results proved that optimized system efficiency could be achieved with a large bandgap photoanode having superior stability and a GDE cathode with improved CO2 mass transfer. The deployment of renewable energy sources will require new technologies to emerge. The photoelectrochemical flow cell developed in this work can store energy from intermittent electricity sources (i.e. wind and solar) in a sustainable manner. This may pave the way for commercialization of this process and moving towards a circular CO2 economy.
publishDate 2017
dc.date.none.fl_str_mv 2017
dc.type.none.fl_str_mv info:eu-repo/semantics/doctoralThesis
info:eu-repo/semantics/publishedVersion
format doctoralThesis
status_str publishedVersion
dc.identifier.none.fl_str_mv https://hdl.handle.net/2445/112608
http://hdl.handle.net/10803/404018
url https://hdl.handle.net/2445/112608
http://hdl.handle.net/10803/404018
dc.language.none.fl_str_mv Inglés
language_invalid_str_mv Inglés
dc.rights.none.fl_str_mv (c) Irtem,, 2017
info:eu-repo/semantics/openAccess
rights_invalid_str_mv (c) Irtem,, 2017
eu_rights_str_mv openAccess
dc.format.none.fl_str_mv application/pdf
dc.publisher.none.fl_str_mv Universitat de Barcelona
publisher.none.fl_str_mv Universitat de Barcelona
dc.source.none.fl_str_mv Tesis Doctorals - Departament - Enginyeria Electrònica i Biomèdica
reponame:Dipòsit Digital de la UB
instname:Universidad de Barcelona
instname_str Universidad de Barcelona
reponame_str Dipòsit Digital de la UB
collection Dipòsit Digital de la UB
repository.name.fl_str_mv
repository.mail.fl_str_mv
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spelling Production of Solar Fuels by Photoelectrochemical Conversion of Carbon DioxideIrtem, Ibrahim ErdemElectroquímicaDiòxid de carboniCatàlisiFotoelectroquímicaGalvanoplàstiaElectrochemistryCarbon dioxideCatalysisPhotoelectrochemistryElectroplating[eng] Growing global emission of carbon dioxide gas (CO2) reflects the world’s energy dependence on fossil fuels. The conversion of CO2 emission into value-added products, like fuels completes a circular CO2 economy which requires a renewable energy conversion and storage system. Amongst a few, photo/electrochemistry has been particularly appealing thanks to its energy efficiency and enormous potential for industrial applications. Formic acid (HCOOH) production from CO2 reduction appears as an alternative energy storage option based on the commercialization of this process. Herein, stable and selective catalysts working at low overpotential are needed to reduce CO2. Likewise, cell design is critical to have improved CO2 mass transport for obtaining high conversion efficiencies and to achieve feasible production yields. The initial work was conducted on the design and understanding of operational parameters of an electrochemical flow cell (ECf-cell) such as flow rates and electrode potentials. For CO2 reduction at the cathode site, two different gas diffusion electrodes were produced by electrodeposition: Sn-GDE and Cu-GDE. An optimum potential range was established to control HCOOH selectivity. The complementing reaction at the anode site, oxygen evolution reaction (OER), was studied using Mn-Co oxide nanoparticles to replace expensive DSA: Ir-Ta oxide catalyst. Subsequent efforts were devoted on the assembly of a photoelectrochemical flow cell (PECf-cell) which enabled coupling of Sn-GDE as cathode vs. TiO2 nanorods as photoanode. This led to nearly 1/3 reduction in overall cell voltage reaching an energy efficiency up to 70 %. The solar-to-fuel (STF) conversion efficiency was 0.25% which was one of the highest efficiencies reported amongst the data obtained from a cell in device level. The results proved that optimized system efficiency could be achieved with a large bandgap photoanode having superior stability and a GDE cathode with improved CO2 mass transfer. The deployment of renewable energy sources will require new technologies to emerge. The photoelectrochemical flow cell developed in this work can store energy from intermittent electricity sources (i.e. wind and solar) in a sustainable manner. This may pave the way for commercialization of this process and moving towards a circular CO2 economy.[spa] La conversión de CO2 en productos de valor añadido con energías renovables resulta interesante para mitigar las emisiones de este. La conversión foto/electroquímica es atractiva por su eficiencia energética y su enorme potencial para aplicaciones industriales. La producción de ácido fórmico (HCOOH) a partir de la reducción de CO2 aparece como una vía alternativa para su comercialización. Sin embargo, se requieren catalizadores estables y selectivos que trabajen a bajo sobre potencial. Además, el diseño de la celda es crítico para mejorar el transporte de masa de CO2 y obtener elevadas eficiencias de conversión. En este trabajo se estudió en un primer lugar el diseño y la comprensión de los parámetros operativos de una celda de flujo electroquímica: caudales y potenciales de electrodo. Para la reducción de CO2 sobre el cátodo, se emplearon dos electrodos diferentes de difusión de gas preparados por electrodeposición: Sn-GDE y Cu-GDE. Se estableció un valor de operación óptimo para controlar la selectividad a HCOOH. Se estudió también la reacción complementaria en el ánodo (evolución de O2), empleando nanopartículas de óxido de Mn-Co para reemplazar el elevado coste del catalizador de óxido de Ir-Ta. Finalmente, se montó una celda fotoelectroquímica de flujo que permitió la inclusión de TiO2 nanorods como fotoánodo. El voltaje total de la celda se redujo alrededor 1/3 alcanzando una eficiencia energética del 70 %. El rendimiento de conversión de energía solar a combustible (STF) fue de 0,25%. Los resultados demuestran que se puede lograr una eficiencia optimizada del sistema con un fotoánodo que tiene una buena estabilidad y un cátodo que favorece la transferencia de masa de CO2. La celda de flujo fotoelectroquímica desarrollada en este trabajo permite almacenar energía de fuentes de electricidad intermitentes (eólica y/o solar) de una manera sostenible, con el consiguiente avance en una economía circular de CO2.Universitat de BarcelonaMorante i Lleonart, Joan RamonAndreu Arbella, TeresaUniversitat de Barcelona. Departament d'Enginyeries: Secció d'Electrònica2017info:eu-repo/semantics/doctoralThesisinfo:eu-repo/semantics/publishedVersionapplication/pdfhttps://hdl.handle.net/2445/112608http://hdl.handle.net/10803/404018Tesis Doctorals - Departament - Enginyeria Electrònica i Biomèdicareponame:Dipòsit Digital de la UBinstname:Universidad de BarcelonaInglés(c) Irtem,, 2017info:eu-repo/semantics/openAccessoai:diposit.ub.edu:2445/1126082026-05-27T06:46:51Z
score 15,300724

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