Catalyst and reactor design for carbon dioxide methanation

Programa de Doctorat en Nanociències / Tesi realitzada a l'Institut de Recerca de l'Energia de Catalunya (IREC)

Detalles Bibliográficos
Autor: Alarcón Avellán, Andreina
Tipo de recurso: tesis doctoral
Estado:Versión publicada
Fecha de publicación:2021
País:España
Institución:CBUC, CESCA
Repositorio:TDR. Tesis Doctorales en Red
OAI Identifier:oai:www.tdx.cat:10803/671781
Acceso en línea:http://hdl.handle.net/10803/671781
Access Level:acceso abierto
Palabra clave:Catàlisi
Catálisis
Catalysis
Cinemàtica
Cinemática
Kinematics
Reactors químics
Reactores químicos
Chemical reactors
Diòxid de carboni
Dióxido de carbono
Carbon dioxide
Metà
Metano
Methane
Ciències Experimentals i Matemàtiques
53
id ES_7fddd12e8d296940653978aeffb91e77
oai_identifier_str oai:www.tdx.cat:10803/671781
network_acronym_str ES
network_name_str España
repository_id_str
dc.title.none.fl_str_mv Catalyst and reactor design for carbon dioxide methanation
title Catalyst and reactor design for carbon dioxide methanation
spellingShingle Catalyst and reactor design for carbon dioxide methanation
Alarcón Avellán, Andreina
Catàlisi
Catálisis
Catalysis
Cinemàtica
Cinemática
Kinematics
Reactors químics
Reactores químicos
Chemical reactors
Diòxid de carboni
Dióxido de carbono
Carbon dioxide
Metà
Metano
Methane
Ciències Experimentals i Matemàtiques
53
title_short Catalyst and reactor design for carbon dioxide methanation
title_full Catalyst and reactor design for carbon dioxide methanation
title_fullStr Catalyst and reactor design for carbon dioxide methanation
title_full_unstemmed Catalyst and reactor design for carbon dioxide methanation
title_sort Catalyst and reactor design for carbon dioxide methanation
dc.creator.none.fl_str_mv Alarcón Avellán, Andreina
author Alarcón Avellán, Andreina
author_facet Alarcón Avellán, Andreina
author_role author
dc.contributor.none.fl_str_mv Andreu Arbella, Teresa
Guilera Sala, Jordi
Morante i Lleonart, Joan Ramon
Universitat de Barcelona. Facultat de Física
dc.subject.none.fl_str_mv Catàlisi
Catálisis
Catalysis
Cinemàtica
Cinemática
Kinematics
Reactors químics
Reactores químicos
Chemical reactors
Diòxid de carboni
Dióxido de carbono
Carbon dioxide
Metà
Metano
Methane
Ciències Experimentals i Matemàtiques
53
topic Catàlisi
Catálisis
Catalysis
Cinemàtica
Cinemática
Kinematics
Reactors químics
Reactores químicos
Chemical reactors
Diòxid de carboni
Dióxido de carbono
Carbon dioxide
Metà
Metano
Methane
Ciències Experimentals i Matemàtiques
53
description Programa de Doctorat en Nanociències / Tesi realitzada a l'Institut de Recerca de l'Energia de Catalunya (IREC)
publishDate 2021
dc.date.none.fl_str_mv 2021
2021
2021
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 http://hdl.handle.net/10803/671781
url http://hdl.handle.net/10803/671781
dc.language.none.fl_str_mv Inglés
language_invalid_str_mv Inglés
dc.rights.none.fl_str_mv http://creativecommons.org/licenses/by-nc/4.0/
info:eu-repo/semantics/openAccess
rights_invalid_str_mv http://creativecommons.org/licenses/by-nc/4.0/
eu_rights_str_mv openAccess
dc.format.none.fl_str_mv 236 p.
application/pdf
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 TDX (Tesis Doctorals en Xarxa)
reponame:TDR. Tesis Doctorales en Red
instname:CBUC, CESCA
instname_str CBUC, CESCA
reponame_str TDR. Tesis Doctorales en Red
collection TDR. Tesis Doctorales en Red
repository.name.fl_str_mv
repository.mail.fl_str_mv
_version_ 1869411856040329216
spelling Catalyst and reactor design for carbon dioxide methanationAlarcón Avellán, AndreinaCatàlisiCatálisisCatalysisCinemàticaCinemáticaKinematicsReactors químicsReactores químicosChemical reactorsDiòxid de carboniDióxido de carbonoCarbon dioxideMetàMetanoMethaneCiències Experimentals i Matemàtiques53Programa de Doctorat en Nanociències / Tesi realitzada a l'Institut de Recerca de l'Energia de Catalunya (IREC)The transformation of the current energy model towards a more sustainable mix, independent of fossil fuels, requires the exploration of new technologies that are capable of taking advantage of excess electricity derived from renewable energy sources and to use new alternative sources of carbon for the generation of clean fuels. An alternative that combines both is the Power-to-Gas (P2G) technology, whose concept is based on a two-stage process. In the first stage, excess electricity from renewable energies is converted to hydrogen by electrolysis. Then, in a second stage, the H2 produced is transformed to CH4 through methanation with CO2. The CH4 produced is referred to as synthetic natural gas (SNG) and allows large amounts of renewable energy to be distributed from the energy sector to the end-use sectors. The thermo-chemical CO2 methanation process is considered the most efficient route for large-scale SNG production. However, developing a cost-effective CO2 methanation technology is one of the biggest challenges facing the P2G concept. In this context, this thesis focused on the catalyst and reactor design for CO2 methanation. The thesis objectives were addressed in three main aspects, which are: i) design a high-performance catalyst based on metal oxide-promoted Ni/γ-Al2O3 and determine its reaction mechanism; ii) evaluate the stability of the catalyst and the tolerance to sulfur for its implementation in a relevant industrial environment (CoSin project); and finally, iii) develop a CFD model based on experimental kinetic data to understand the role of operating conditions and propose a new reactor configuration. In the first Chapter of this thesis it is presented a general introduction of the SNG production through CO2 methanation process. In the second Chapter, the addition of a promoter (X) on a system composed by Ni and γ-Al2O3 microspheres was studied as the design strategy to develop a micro-sized Ni-X/γ-Al2O3 catalyst. The catalysts based on Ni-CeO2/γ-Al2O3 was proposed as the most feasible due to its high catalytic performance in relation to its economic competitiveness. The optimal composition of each component of the Ni-CeO2/γ-Al2O3 was found through a systematic experimental design. The catalyst composed by 25wt.%Ni, 20wt.%CeO2 and 55wt.%γ-Al2O3 proved to be the most active and stable thanks to its enhanced Ni dispersion and reduction, its high metallic area, and the formation of moderate base sites. In Chapter three, the thermal stability and tolerance to sulfur impurities on the Ni-CeO2/γ-Al2O3 catalyst was further studied using high temperatures and the presence of H2S on the reactants. The strong metal-promoter interaction and the favourable formation of Ce2O2S were revealed as the main causes of its high stability and tolerance to H2S, respectively. Additionally, the implementation of Ni-CeO2/γ-Al2O3 in a two-stage industrial methanation process was performed to evaluate its technical feasibility. The desired gas composition (≥92.5%CH4) was successful obtained using a decreasing temperature profile (T=450-275°C) and P=5bar·g. The high stability recorded during the 2000h of experimentation demonstrated that Ni-CeO2/γ-Al2O3 can be a competitive catalyst for CO2 methanation. Regarding to reactor design, in Chapter four, the design of a fixed-bed multitubular reactor on a Ni-CeO2-Al2O3 catalyst was evaluated for mid-scale SNG production. A CFD mathematical model based on experimental kinetic data was developed. A reactor tube with a diameter of 9.25mm and a length of 250mm was proposed, which should be operated at Tinlet=473K, Twall=373K, GHSV=14,400h-1 and P=5atm to achieve XCO2=99% with Tmax of 673K. On the other hand, a reactor tube (di=4.6mm and L=250mm) with a heat management approach based on free convection was proposed for small-scale SNG production. The optimal conditions were found at GHSV=11,520h-1, Tinlet=503K, P=5atm, and Tair=298K. The feasibility of the simulated reactor proposal was experimentally validated over the micro-sized Ni-CeO2/γ-Al2O3 (XCO2=93% and T=830-495K).Power-to-Gas (P2G) es una tecnología prometedora para el almacenamiento de combustibles bajos en carbono. El concepto P2G implica la conversión de energía renovable en hidrógeno mediante electrólisis con la posibilidad de combinarlo con CO2 para producir metano (gas natural sintético, SNG). La producción de SNG mediante el proceso termoquímico de metanación de CO2 es particularmente interesante porque ofrece un combustible fácilmente transportable con un amplio mercado probado para aplicaciones de uso final de energía, calor y movilidad. Sin embargo, el desarrollo de una tecnología de metanación de CO2 rentable es uno de los mayores desafíos que enfrenta el concepto P2G. En este contexto, esta tesis se centró en el desarrollo de un catalizador y un reactor para la metanación de CO2. Los objetivos de la tesis se abordaron en tres aspectos principales, que son: i) diseñar un catalizador de alto rendimiento basado en Ni/The transformation of the current energy model towards a more sustainable mix, independent of fossil fuels, requires the exploration of new technologies that are capable of taking advantage of excess electricity derived from renewable energy sources and to use new alternative sources of carbon for the generation of clean fuels. An alternative that combines both is the Power-to-Gas (P2G) technology, whose concept is based on a two-stage process. In the first stage, excess electricity from renewable energies is converted to hydrogen by electrolysis. Then, in a second stage, the H2 produced is transformed to CH4 through methanation with CO2. The CH4 produced is referred to as synthetic natural gas (SNG) and allows large amounts of renewable energy to be distributed from the energy sector to the end-use sectors. The thermo-chemical CO2 methanation process is considered the most efficient route for large-scale SNG production. However, developing a cost-effective CO2 methanation technology is one of the biggest challenges facing the P2G concept. In this context, this thesis focused on the catalyst and reactor design for CO2 methanation. The thesis objectives were addressed in three main aspects, which are: i) design a high-performance catalyst based on metal oxide-promoted Ni/γ-Al2O3 and determine its reaction mechanism; ii) evaluate the stability of the catalyst and the tolerance to sulfur for its implementation in a relevant industrial environment (CoSin project); and finally, iii) develop a CFD model based on experimental kinetic data to understand the role of operating conditions and propose a new reactor configuration. In the first Chapter of this thesis it is presented a general introduction of the SNG production through CO2 methanation process. In the second Chapter, the addition of a promoter (X) on a system composed by Ni and γ-Al2O3 microspheres was studied as the design strategy to develop a micro-sized Ni-X/γ-Al2O3 catalyst. The catalysts based on Ni-CeO2/γ-Al2O3 was proposed as the most feasible due to its high catalytic performance in relation to its economic competitiveness. The optimal composition of each component of the Ni-CeO2/γ-Al2O3 was found through a systematic experimental design. The catalyst composed by 25wt.%Ni, 20wt.%CeO2 and 55wt.%γ-Al2O3 proved to be the most active and stable thanks to its enhanced Ni dispersion and reduction, its high metallic area, and the formation of moderate base sites. In Chapter three, the thermal stability and tolerance to sulfur impurities on the Ni-CeO2/γ-Al2O3 catalyst was further studied using high temperatures and the presence of H2S on the reactants. The strong metal-promoter interaction and the favourable formation of Ce2O2S were revealed as the main causes of its high stability and tolerance to H2S, respectively. Additionally, the implementation of Ni-CeO2/γ-Al2O3 in a two-stage industrial methanation process was performed to evaluate its technical feasibility. The desired gas composition (≥92.5%CH4) was successful obtained using a decreasing temperature profile (T=450-275°C) and P=5bar·g. The high stability recorded during the 2000h of experimentation demonstrated that Ni-CeO2/γ-Al2O3 can be a competitive catalyst for CO2 methanation. Regarding to reactor design, in Chapter four, the design of a fixed-bed multitubular reactor on a Ni-CeO2-Al2O3 catalyst was evaluated for mid-scale SNG production. A CFD mathematical model based on experimental kinetic data was developed. A reactor tube with a diameter of 9.25mm and a length of 250mm was proposed, which should be operated at Tinlet=473K, Twall=373K, GHSV=14,400h-1 and P=5atm to achieve XCO2=99% with Tmax of 673K. On the other hand, a reactor tube (di=4.6mm and L=250mm) with a heat management approach based on free convection was proposed for small-scale SNG production. The optimal conditions were found at GHSV=11,520h-1, Tinlet=503K, P=5atm, and Tair=298K. The feasibility of the simulated reactor proposal was experimentally validated over the micro-sized Ni-CeO2/γ-Al2O3 (XCO2=93% and T=830-495K).-Al2O3 promovido por óxido metálico y determinar su mecanismo, ii) evaluar la estabilidad del catalizador y la tolerancia al azufre para su implementación en un entorno industrial relevante (proyecto CoSin), and iii) desarrollar un modelo CFD basado en datos cinéticos experimentales para comprender el papel de las condiciones de operación y proponer una nueva configuración de reactor. En línea con estos objetivos, un catalizador ternario basado en 25wt.%Ni-20wt.%CeO2-55wt.%The transformation of the current energy model towards a more sustainable mix, independent of fossil fuels, requires the exploration of new technologies that are capable of taking advantage of excess electricity derived from renewable energy sources and to use new alternative sources of carbon for the generation of clean fuels. An alternative that combines both is the Power-to-Gas (P2G) technology, whose concept is based on a two-stage process. In the first stage, excess electricity from renewable energies is converted to hydrogen by electrolysis. Then, in a second stage, the H2 produced is transformed to CH4 through methanation with CO2. The CH4 produced is referred to as synthetic natural gas (SNG) and allows large amounts of renewable energy to be distributed from the energy sector to the end-use sectors. The thermo-chemical CO2 methanation process is considered the most efficient route for large-scale SNG production. However, developing a cost-effective CO2 methanation technology is one of the biggest challenges facing the P2G concept. In this context, this thesis focused on the catalyst and reactor design for CO2 methanation. The thesis objectives were addressed in three main aspects, which are: i) design a high-performance catalyst based on metal oxide-promoted Ni/γ-Al2O3 and determine its reaction mechanism; ii) evaluate the stability of the catalyst and the tolerance to sulfur for its implementation in a relevant industrial environment (CoSin project); and finally, iii) develop a CFD model based on experimental kinetic data to understand the role of operating conditions and propose a new reactor configuration. In the first Chapter of this thesis it is presented a general introduction of the SNG production through CO2 methanation process. In the second Chapter, the addition of a promoter (X) on a system composed by Ni and γ-Al2O3 microspheres was studied as the design strategy to develop a micro-sized Ni-X/γ-Al2O3 catalyst. The catalysts based on Ni-CeO2/γ-Al2O3 was proposed as the most feasible due to its high catalytic performance in relation to its economic competitiveness. The optimal composition of each component of the Ni-CeO2/γ-Al2O3 was found through a systematic experimental design. The catalyst composed by 25wt.%Ni, 20wt.%CeO2 and 55wt.%γ-Al2O3 proved to be the most active and stable thanks to its enhanced Ni dispersion and reduction, its high metallic area, and the formation of moderate base sites. In Chapter three, the thermal stability and tolerance to sulfur impurities on the Ni-CeO2/γ-Al2O3 catalyst was further studied using high temperatures and the presence of H2S on the reactants. The strong metal-promoter interaction and the favourable formation of Ce2O2S were revealed as the main causes of its high stability and tolerance to H2S, respectively. Additionally, the implementation of Ni-CeO2/γ-Al2O3 in a two-stage industrial methanation process was performed to evaluate its technical feasibility. The desired gas composition (≥92.5%CH4) was successful obtained using a decreasing temperature profile (T=450-275°C) and P=5bar·g. The high stability recorded during the 2000h of experimentation demonstrated that Ni-CeO2/γ-Al2O3 can be a competitive catalyst for CO2 methanation. Regarding to reactor design, in Chapter four, the design of a fixed-bed multitubular reactor on a Ni-CeO2-Al2O3 catalyst was evaluated for mid-scale SNG production. A CFD mathematical model based on experimental kinetic data was developed. A reactor tube with a diameter of 9.25mm and a length of 250mm was proposed, which should be operated at Tinlet=473K, Twall=373K, GHSV=14,400h-1 and P=5atm to achieve XCO2=99% with Tmax of 673K. On the other hand, a reactor tube (di=4.6mm and L=250mm) with a heat management approach based on free convection was proposed for small-scale SNG production. The optimal conditions were found at GHSV=11,520h-1, Tinlet=503K, P=5atm, and Tair=298K. The feasibility of the simulated reactor proposal was experimentally validated over the micro-sized Ni-CeO2/γ-Al2O3 (XCO2=93% and T=830-495K).-Al2O3 se propone como el más factible debido a su alto rendimiento catalítico en relación a su competitividad económica. La fuerte interacción metal-promotor y la formación favorable de Ce2O2S se revelaron como las principales causas de su alta estabilidad y tolerancia al H2S, respectivamente. Adicionalmente, su exitosa implementación en un proceso de metanación industrial de dos etapas demostró su viabilidad técnica. Finalmente, se propone un reactor multitubular para la producción de SNG a mediana escala. Por otro lado, para la producción de SNG a pequeña escala, se propone un nuevo diseño de reactor con un enfoque de gestión del calor basado en la libre convención.Universitat de BarcelonaAndreu Arbella, TeresaGuilera Sala, JordiMorante i Lleonart, Joan RamonUniversitat de Barcelona. Facultat de Física202120212021info:eu-repo/semantics/doctoralThesisinfo:eu-repo/semantics/publishedVersion236 p.application/pdfapplication/pdfhttp://hdl.handle.net/10803/671781TDX (Tesis Doctorals en Xarxa)reponame:TDR. Tesis Doctorales en Redinstname:CBUC, CESCAInglésL'accés als continguts d'aquesta tesi queda condicionat a l'acceptació de les condicions d'ús establertes per la següent llicència Creative Commons: http://creativecommons.org/licenses/by-nc/4.0/http://creativecommons.org/licenses/by-nc/4.0/info:eu-repo/semantics/openAccessoai:www.tdx.cat:10803/6717812026-06-14T12:46:07Z
score 15,300724

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