Designing Advanced Nanocatalysts: Synthesis of complex CeO2-based Nanostructures
[eng] The main objective of this dissertation has been to stablish a bridge between materials science and its fields of application. The scope of this thesis work, under this premise, is aimed towards understanding the catalytical properties of CeO2 nanocrystals and the applications arising from the...
| Autor: | |
|---|---|
| Tipo de recurso: | tesis doctoral |
| Estado: | Versión publicada |
| Fecha de publicación: | 2023 |
| País: | España |
| Institución: | Universidad de Barcelona |
| Repositorio: | Dipòsit Digital de la UB |
| OAI Identifier: | oai:diposit.ub.edu:2445/198921 |
| Acceso en línea: | https://hdl.handle.net/2445/198921 http://hdl.handle.net/10803/688442 |
| Access Level: | acceso abierto |
| Palabra clave: | Catàlisi Materials nanoestructurats Síntesi asimètrica Col·loides Antioxidants Ceri (Element químic) Catalysis Nanostructured materials Asymmetric synthesis Colloids Cerium |
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España |
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| dc.title.none.fl_str_mv |
Designing Advanced Nanocatalysts: Synthesis of complex CeO2-based Nanostructures |
| title |
Designing Advanced Nanocatalysts: Synthesis of complex CeO2-based Nanostructures |
| spellingShingle |
Designing Advanced Nanocatalysts: Synthesis of complex CeO2-based Nanostructures Hervés Carrete, Carmen Catàlisi Materials nanoestructurats Síntesi asimètrica Col·loides Antioxidants Ceri (Element químic) Catalysis Nanostructured materials Asymmetric synthesis Colloids Cerium |
| title_short |
Designing Advanced Nanocatalysts: Synthesis of complex CeO2-based Nanostructures |
| title_full |
Designing Advanced Nanocatalysts: Synthesis of complex CeO2-based Nanostructures |
| title_fullStr |
Designing Advanced Nanocatalysts: Synthesis of complex CeO2-based Nanostructures |
| title_full_unstemmed |
Designing Advanced Nanocatalysts: Synthesis of complex CeO2-based Nanostructures |
| title_sort |
Designing Advanced Nanocatalysts: Synthesis of complex CeO2-based Nanostructures |
| dc.creator.none.fl_str_mv |
Hervés Carrete, Carmen |
| author |
Hervés Carrete, Carmen |
| author_facet |
Hervés Carrete, Carmen |
| author_role |
author |
| dc.contributor.none.fl_str_mv |
Puntes, Víctor Gómez i Bastús, Neus Universitat de Barcelona. Facultat de Química |
| dc.subject.none.fl_str_mv |
Catàlisi Materials nanoestructurats Síntesi asimètrica Col·loides Antioxidants Ceri (Element químic) Catalysis Nanostructured materials Asymmetric synthesis Colloids Cerium |
| topic |
Catàlisi Materials nanoestructurats Síntesi asimètrica Col·loides Antioxidants Ceri (Element químic) Catalysis Nanostructured materials Asymmetric synthesis Colloids Cerium |
| description |
[eng] The main objective of this dissertation has been to stablish a bridge between materials science and its fields of application. The scope of this thesis work, under this premise, is aimed towards understanding the catalytical properties of CeO2 nanocrystals and the applications arising from them. In order to tackle it, the chemist labour consists in providing a cutting-edge nanosynthesis technology able to improve efficiencies of the chemical processes, reducing energy consumption and minimizing the environmental impact of both activity and waste products. At the same time, research on nanomaterial synthesis involves the design and formulation of nanomaterials under total control of their physicochemical, morphological, and colloidal properties. Coupled with the appropriate description of the structure-activity relations, the current aim of nanomaterial synthesis is an application-oriented design strategy towards programmable properties of the products. Within this framework, this thesis work is divided into two parts. The first part revolves around nanomaterial synthesis. It pursues the optimised formulation of nanostructured CeO2, a semiconductor material that holds a broad set of intrinsic catalytic properties, describing the synthesis of the minimal stable size for colloidal monocrystalline particles of the material and its complete physicochemical characterization (size, composition, morphology, crystal structure, optical and colloidal properties). It is followed by the extension of the material’s functionality through different derivation strategies, such as doping with different trivalent lanthanide ions and coupling to plasmonic metal domains (Au and Ag) via different synthetic approaches to produce several types of hybrid architectures (core-shell, heterodimers, hollow structures, and other anisotropic shapes) of controlled size. The second part of this work involves the characterization of structure-activity relations of the CeO2-based nanomaterials synthesised in the first part. These are evaluated first through the catalytic performance of each nanomaterial. It has been carried out for two different processes. As a heterogeneous catalyst for methanol production and as ROS scavenger for biomedical applications, coupled with the correspondent assessment of the nanomaterials’ toxicity through in vitro assays. To complete the description of the structure-activity relations, the characterization of the singular electronic structure of CeO2, that confers its characteristic catalytical properties, has been also carried out. Employing core-level spectroscopic techniques, the differences between bulk and nanosized CeO2 have been evaluated through the Ce 3d and O 1s spectra in XPS and Ce L3 edge in XANES. |
| publishDate |
2023 |
| dc.date.none.fl_str_mv |
2023 |
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info:eu-repo/semantics/doctoralThesis info:eu-repo/semantics/publishedVersion |
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doctoralThesis |
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publishedVersion |
| dc.identifier.none.fl_str_mv |
https://hdl.handle.net/2445/198921 http://hdl.handle.net/10803/688442 |
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https://hdl.handle.net/2445/198921 http://hdl.handle.net/10803/688442 |
| dc.language.none.fl_str_mv |
Inglés |
| language_invalid_str_mv |
Inglés |
| dc.rights.none.fl_str_mv |
cc by (c) Hervés Carrete, Carmen, 2023 http://creativecommons.org/licenses/by/3.0/es/ info:eu-repo/semantics/openAccess |
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cc by (c) Hervés Carrete, Carmen, 2023 http://creativecommons.org/licenses/by/3.0/es/ |
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openAccess |
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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 - Facultat - Química reponame:Dipòsit Digital de la UB instname:Universidad de Barcelona |
| instname_str |
Universidad de Barcelona |
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Dipòsit Digital de la UB |
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Dipòsit Digital de la UB |
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1869423830196289536 |
| spelling |
Designing Advanced Nanocatalysts: Synthesis of complex CeO2-based NanostructuresHervés Carrete, CarmenCatàlisiMaterials nanoestructuratsSíntesi asimètricaCol·loidesAntioxidantsCeri (Element químic)CatalysisNanostructured materialsAsymmetric synthesisColloidsCerium[eng] The main objective of this dissertation has been to stablish a bridge between materials science and its fields of application. The scope of this thesis work, under this premise, is aimed towards understanding the catalytical properties of CeO2 nanocrystals and the applications arising from them. In order to tackle it, the chemist labour consists in providing a cutting-edge nanosynthesis technology able to improve efficiencies of the chemical processes, reducing energy consumption and minimizing the environmental impact of both activity and waste products. At the same time, research on nanomaterial synthesis involves the design and formulation of nanomaterials under total control of their physicochemical, morphological, and colloidal properties. Coupled with the appropriate description of the structure-activity relations, the current aim of nanomaterial synthesis is an application-oriented design strategy towards programmable properties of the products. Within this framework, this thesis work is divided into two parts. The first part revolves around nanomaterial synthesis. It pursues the optimised formulation of nanostructured CeO2, a semiconductor material that holds a broad set of intrinsic catalytic properties, describing the synthesis of the minimal stable size for colloidal monocrystalline particles of the material and its complete physicochemical characterization (size, composition, morphology, crystal structure, optical and colloidal properties). It is followed by the extension of the material’s functionality through different derivation strategies, such as doping with different trivalent lanthanide ions and coupling to plasmonic metal domains (Au and Ag) via different synthetic approaches to produce several types of hybrid architectures (core-shell, heterodimers, hollow structures, and other anisotropic shapes) of controlled size. The second part of this work involves the characterization of structure-activity relations of the CeO2-based nanomaterials synthesised in the first part. These are evaluated first through the catalytic performance of each nanomaterial. It has been carried out for two different processes. As a heterogeneous catalyst for methanol production and as ROS scavenger for biomedical applications, coupled with the correspondent assessment of the nanomaterials’ toxicity through in vitro assays. To complete the description of the structure-activity relations, the characterization of the singular electronic structure of CeO2, that confers its characteristic catalytical properties, has been also carried out. Employing core-level spectroscopic techniques, the differences between bulk and nanosized CeO2 have been evaluated through the Ce 3d and O 1s spectra in XPS and Ce L3 edge in XANES.[cat] L'objectiu principal d'aquesta tesi doctoral és fomentar ponts entre la ciència de materials i els seus diferents camps d'aplicació. Partint d'aquesta premissa, la finalitat concreta del treball és assolir uns millor coneixement de les propietats catalítiques del CeO2 nanoestructurat i les aplicacions que en poden emergir. Per abordar aquesta qüestió, des de l'àmbit de la química s'ha de proveir d’una tecnologia capdavantera de síntesi de nanomaterials, capaç de millorar les eficiències dels processos químics reduint el consum d'energia i la producció de residus per minimitzar-ne l'impacte ambiental. Alhora, la investigació actual en síntesi de nanomaterials es fonamenta en el disseny i formulació dels mateixos sota el control total de les seves propietats fisicoquímiques, morfològiques i col·loidals. En conjunt amb la descripció adequada de les relacions activitat-estructura dels materials formulats, l'objectiu actual de la síntesi de nanomaterials és el disseny orientat a la aplicació final mitjançant la programació de les propietats del producte. Dins d'aquest marc, aquesta tesi compta amb dues parts. La primera gira al voltant de la síntesi de nanomaterials. Es busca la formulació optimitzada de nanocristalls de CeO2, un material semiconductor que posseeix un ampli ventall de propietats catalítiques, a través de la descripció de la síntesi de partícules col·loidals monocristal·lines de menor mida possible dins de la seva estabilitat termodinàmica. Aquesta part es completa amb l'extensió de la funcionalitat del material mitjançant diferents estratègies d'hibridació d'aquest, com ara bé el dopatge amb cations trivalents lantànids o l'acoblament de dominis de metalls plasmònics (Au i Ag) seguint diferents estratègies de síntesi. La segona part d'aquest treball tracta la caracterització de les relacions estructura-activitat dels materials ja sintetitzats en la primera. Aquestes són avaluades, en primer lloc, a través de la activitat catalítica de cada nanomaterial per a un procés de catàlisi heterogènia (producció de metanol) i com a neutralitzador de radicals lliures per aplicacions biomèdiques. En segon lloc, l'origen de les propietats catalítiques del material es descriu a través de la caracterització de la singular estructura electrònica del CeO2 nanostructurat, emprant tècniques d'espectroscòpia com XPS i XANES.Universitat de BarcelonaPuntes, VíctorGómez i Bastús, NeusUniversitat de Barcelona. Facultat de Química2023info:eu-repo/semantics/doctoralThesisinfo:eu-repo/semantics/publishedVersionapplication/pdfhttps://hdl.handle.net/2445/198921http://hdl.handle.net/10803/688442Tesis Doctorals - Facultat - Químicareponame:Dipòsit Digital de la UBinstname:Universidad de BarcelonaIngléscc by (c) Hervés Carrete, Carmen, 2023http://creativecommons.org/licenses/by/3.0/es/info:eu-repo/semantics/openAccessoai:diposit.ub.edu:2445/1989212026-05-27T06:46:51Z |
| score |
15.300719 |