Structure-sensitivity in CO2 methanation over CeO2 supported metal catalysts

Tushar Ramesh Sakpal

Research output: ThesisPhD Thesis - Research UT, graduation UTAcademic

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Abstract

The CO2 methanation reaction often attracts attention in the energy sector, since combined water electrolysis and methanation can store the surplus renewable electrical energy into chemical energy. This reaction was first introduced in 1902 and has been studied extensively since then. A catalyst is required to obtain a better efficiency of CO2 methanation reaction. It has been established that Ni and Ru are the best performing metals in terms of activity, selectivity, and stability. Highly dispersed nanoparticles of these
metals on support (usually, thermally stable metal oxide) are generally used during the reaction. There are two types of supports, namely reducible supports, and non-reducible supports. Reducible supports (e.g. CeO2, TiO2) are more active than non-reducible supports (e.g. Al2O3, SiO2) since they provide additional sites for CO2 activation.

CeO2 can easily switch between 4+ and 3+ oxidation without phase change, which results in the formation of abundant oxygen vacancies. As a result of this unique property, CeO2 supported catalysts show excellent activity for CO2 methanation reaction compared to other supported catalysts. In the last decade, significant research was done in studying the CeO2 nano-shapes, with wellcontrolled crystal planes, such as rods, cubes, and octahedra. Variation in the shape of CeO2 results in variation in properties and
activities of these materials. Previous publications reporting on the effect of CeO2 morphology on the activity for CO2 methanation, as well as other reactions, often neglected the effect of metal particle size.

Therefore, this study reports the effect of metal (Ni and Ru) particle size on the activity of catalysts. Moreover, we also studied the morphology effect of CeO2 nano-shapes by keeping identical metal particle size on all three supports. The thesis is mainly divided into two parts, studying the morphology and particle size effects using Ru/CeO2 (chapter 2 and 3) and Ni/CeO2 (chapter 4) catalysts.
Original languageEnglish
QualificationDoctor of Philosophy
Awarding Institution
  • University of Twente
Supervisors/Advisors
  • Lefferts, Leon, Supervisor
Award date7 Jun 2019
Place of PublicationEnschede
Publisher
Print ISBNs978-90-365-4781-9
DOIs
Publication statusPublished - 7 Jun 2019

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Methanation
Metals
Catalysts
Particle size
Catalyst supports
Oxygen vacancies
Electrolysis
Oxides
Catalyst activity
Chemical activation
Switches
Nanoparticles
Oxidation
Crystals
Water

Cite this

Sakpal, Tushar Ramesh. / Structure-sensitivity in CO2 methanation over CeO2 supported metal catalysts. Enschede : University of Twente, 2019. 153 p.
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Structure-sensitivity in CO2 methanation over CeO2 supported metal catalysts. / Sakpal, Tushar Ramesh.

Enschede : University of Twente, 2019. 153 p.

Research output: ThesisPhD Thesis - Research UT, graduation UTAcademic

TY - THES

T1 - Structure-sensitivity in CO2 methanation over CeO2 supported metal catalysts

AU - Sakpal, Tushar Ramesh

PY - 2019/6/7

Y1 - 2019/6/7

N2 - The CO2 methanation reaction often attracts attention in the energy sector, since combined water electrolysis and methanation can store the surplus renewable electrical energy into chemical energy. This reaction was first introduced in 1902 and has been studied extensively since then. A catalyst is required to obtain a better efficiency of CO2 methanation reaction. It has been established that Ni and Ru are the best performing metals in terms of activity, selectivity, and stability. Highly dispersed nanoparticles of thesemetals on support (usually, thermally stable metal oxide) are generally used during the reaction. There are two types of supports, namely reducible supports, and non-reducible supports. Reducible supports (e.g. CeO2, TiO2) are more active than non-reducible supports (e.g. Al2O3, SiO2) since they provide additional sites for CO2 activation.CeO2 can easily switch between 4+ and 3+ oxidation without phase change, which results in the formation of abundant oxygen vacancies. As a result of this unique property, CeO2 supported catalysts show excellent activity for CO2 methanation reaction compared to other supported catalysts. In the last decade, significant research was done in studying the CeO2 nano-shapes, with wellcontrolled crystal planes, such as rods, cubes, and octahedra. Variation in the shape of CeO2 results in variation in properties andactivities of these materials. Previous publications reporting on the effect of CeO2 morphology on the activity for CO2 methanation, as well as other reactions, often neglected the effect of metal particle size.Therefore, this study reports the effect of metal (Ni and Ru) particle size on the activity of catalysts. Moreover, we also studied the morphology effect of CeO2 nano-shapes by keeping identical metal particle size on all three supports. The thesis is mainly divided into two parts, studying the morphology and particle size effects using Ru/CeO2 (chapter 2 and 3) and Ni/CeO2 (chapter 4) catalysts.

AB - The CO2 methanation reaction often attracts attention in the energy sector, since combined water electrolysis and methanation can store the surplus renewable electrical energy into chemical energy. This reaction was first introduced in 1902 and has been studied extensively since then. A catalyst is required to obtain a better efficiency of CO2 methanation reaction. It has been established that Ni and Ru are the best performing metals in terms of activity, selectivity, and stability. Highly dispersed nanoparticles of thesemetals on support (usually, thermally stable metal oxide) are generally used during the reaction. There are two types of supports, namely reducible supports, and non-reducible supports. Reducible supports (e.g. CeO2, TiO2) are more active than non-reducible supports (e.g. Al2O3, SiO2) since they provide additional sites for CO2 activation.CeO2 can easily switch between 4+ and 3+ oxidation without phase change, which results in the formation of abundant oxygen vacancies. As a result of this unique property, CeO2 supported catalysts show excellent activity for CO2 methanation reaction compared to other supported catalysts. In the last decade, significant research was done in studying the CeO2 nano-shapes, with wellcontrolled crystal planes, such as rods, cubes, and octahedra. Variation in the shape of CeO2 results in variation in properties andactivities of these materials. Previous publications reporting on the effect of CeO2 morphology on the activity for CO2 methanation, as well as other reactions, often neglected the effect of metal particle size.Therefore, this study reports the effect of metal (Ni and Ru) particle size on the activity of catalysts. Moreover, we also studied the morphology effect of CeO2 nano-shapes by keeping identical metal particle size on all three supports. The thesis is mainly divided into two parts, studying the morphology and particle size effects using Ru/CeO2 (chapter 2 and 3) and Ni/CeO2 (chapter 4) catalysts.

U2 - 10.3990/1.9789036547819

DO - 10.3990/1.9789036547819

M3 - PhD Thesis - Research UT, graduation UT

SN - 978-90-365-4781-9

PB - University of Twente

CY - Enschede

ER -