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Ceria Nanoparticle Hybrid Materials: Interfacial Design and Structure Control
KTH, School of Chemical Science and Engineering (CHE), Fibre and Polymer Technology, Coating Technology.
2015 (English)Doctoral thesis, comprehensive summary (Other academic)
Abstract [en]

This doctoral thesis addresses the challenge of bringing two very different materials into intimate chemical contact: inorganic metal oxide nanoparticles and acrylic polymers. In order to achieve this ambitious goal, the work has been divided into a series of more accessible tasks. Pedagogically designed, these tasks build upon one another to finally develop the knowledge and skills necessary to successfully formulate novel nanocomposites.

A fundamental study on the bulk and surface bonding of ceria was carried out to show that, due to the ceria content in small and highly charged ions, which are difficult to polarize, the preferred chemical interactions are ionic. Among the different capping agents, the carboxylate ligands —through the rich and localized electron density of their oxygen atoms— formed an ionic bond with cerium oxides. This provided stability to the ceria nanoparticles and opened up a vast robust and versatile library of carboxylates to us. This is exemplified by the development of synthetic routes for understanding and modifying ceria nanoparticles with carboxylic acids carrying reactive moieties, which were used to extend the stability of the nanoparticle dispersions. This allowed us to perform in situ polymerization, which resulted in homogeneous ceria–polymer hybrid nanocomposites. This interfacial design offers not only structure control but also strong bonding between the covalent polymer network and the ionic nanocrystals.

The focus of the present work, however, is not on characterization of the polymeric materials used but rather on how the embedded nanoparticles interact with the polymeric matrix with respect to chemical interfacial aspects. The following cases were studied: i) unreactive nanoceria dispersed in a polymer matrix; ii) dispersed nanoceria endowed with the ability to initiate polymerizations; and iii) dispersed nanoceria capable of copolymerizing with the propagating chains of the polymer.

These processes led to the development of novel hybrid nanocomposites that preserved the optical properties of ceria (e.g. UV absorption) while enhancing mechanical properties such as stiffness and glass transition temperature.

Place, publisher, year, edition, pages
Stockholm: KTH Royal Institute of Technology, 2015. , xviii, 124 p.
Series
TRITA-CHE-Report, ISSN 1654-1081 ; 2015:46
National Category
Polymer Chemistry
Identifiers
URN: urn:nbn:se:kth:diva-173367ISBN: 978-91-7595-674-9 (print)OAI: oai:DiVA.org:kth-173367DiVA: diva2:852883
Public defence
2015-09-18, Kollegiesalen, Brinellvägen 8, KTH, Stockholm, 10:00 (English)
Opponent
Supervisors
Note

QC 20150910

Available from: 2015-09-10 Created: 2015-09-10 Last updated: 2015-09-10Bibliographically approved
List of papers
1. Aminopolycarboxylic acids as a versatile tool to stabilize ceria nanoparticles-a fundamental model experimentally demonstrated
Open this publication in new window or tab >>Aminopolycarboxylic acids as a versatile tool to stabilize ceria nanoparticles-a fundamental model experimentally demonstrated
2014 (English)In: RSC Advances, ISSN 2046-2069, E-ISSN 2046-2069, Vol. 4, no 18, 9048-9055 p.Article in journal (Refereed) Published
Abstract [en]

An extremely stable water dispersion of cerium oxide nanoparticles was prepared by colloidal synthesis, using nitrilotriacetic acid (NTA) as a stabilizer. Based on FT-IR measurements, the surface characteristics of NTA-stabilized ceria nanoparticles are clarified and a fundamental stabilization mechanism is proposed. The mechanism is based on the combination of the ionic nature of cerium oxide surface and the inner-sphere complexation model. From an application perspective it is remarkable that ceria nanoparticle dispersions stabilized by NTA are stable at neutral pH, which makes them a potential successful additive in UV screening applications.

Keyword
Nuclear-Magnetic-Resonance, Outer-Sphere, Aminocarboxylate Ligands, Lanthanide Complexation, Trivalent Lanthanide, Oxide Nanoparticles, Actinide Ions, Fuel-Cell, CEO2, Thermodynamics
National Category
Chemical Sciences
Identifiers
urn:nbn:se:kth:diva-142785 (URN)10.1039/c3ra45875j (DOI)000330800700016 ()2-s2.0-84893943174 (Scopus ID)
Funder
EU, FP7, Seventh Framework Programme, 246434
Note

QC 20140312

Available from: 2014-03-12 Created: 2014-03-12 Last updated: 2017-12-05Bibliographically approved
2. Radical initiator modified cerium oxide nanoparticles for polymer encapsulation via grafting from the surface
Open this publication in new window or tab >>Radical initiator modified cerium oxide nanoparticles for polymer encapsulation via grafting from the surface
Show others...
2014 (English)In: RSC Advances, ISSN 2046-2069, E-ISSN 2046-2069, Vol. 4, no 106, 61863-61868 p.Article in journal (Refereed) Published
Abstract [en]

The present paper describes a versatile route to modify and stabilize ceria nanoparticles with a radical initiator, 4,4'-azobis(4-cyanovaleric acid) (ACVA), allowing a strong interface to be formed via grafting of polymers from the surface. This leads to the successful encapsulation of cerium oxide nanoparticles in a poly(methyl methacrylate) matrix. The interaction between the radical initiator and the surface of ceria is studied by FTIR spectroscopy where a consistent shift of the carboxylate band unequivocally demonstrates that the carboxylate groups of this acidic initiator complex the cerium ions on the ceria surface by means of strong and stable ionic bonding.

Keyword
Hybrid Latexes, Corrosion, Agents
National Category
Chemical Sciences
Identifiers
urn:nbn:se:kth:diva-158313 (URN)10.1039/c4ra09044f (DOI)000345656600084 ()2-s2.0-84912055127 (Scopus ID)
Funder
EU, FP7, Seventh Framework Programme, 246434
Note

QC 20150107

Available from: 2015-01-07 Created: 2015-01-07 Last updated: 2017-12-05Bibliographically approved
3. Hybrid acrylic/CeO2 nanocomposites using hydrophilic, spherical and high aspect ratio CeO2 nanoparticles
Open this publication in new window or tab >>Hybrid acrylic/CeO2 nanocomposites using hydrophilic, spherical and high aspect ratio CeO2 nanoparticles
Show others...
2014 (English)In: Journal of Materials Chemistry A, ISSN 2050-7488, Vol. 2, no 47, 20280-20287 p.Article in journal (Refereed) Published
Abstract [en]

A dispersion of CeO2 nanoparticles and nanorods stabilized with nitrilotriacetic acid (NTA) and a 4,4'-azobis(4-cyanovaleric acid) (V-501) initiator has been used to initiate the emulsion polymerization of acrylic monomers, yielding stable hybrid CeO2 nanoparticle-nanorod/polyacrylate latexes for the first time. Films cast from these hybrid latexes are transparent due to the very homogenous distribution of the polymer compatibilized CeO2. Furthermore, it has been proven that the UV-Vis absorption capacity of the hybrid latexes is enhanced with the incorporation of the nanorods.

National Category
Chemical Sciences
Identifiers
urn:nbn:se:kth:diva-158853 (URN)10.1039/c4ta03620d (DOI)000345066900044 ()2-s2.0-84910136292 (Scopus ID)
Note

QC 20150120

Available from: 2015-01-20 Created: 2015-01-12 Last updated: 2017-12-05Bibliographically approved
4. A versatile synthesis route to prepare Ceria nanoparticles with polymerizable capping ligands
Open this publication in new window or tab >>A versatile synthesis route to prepare Ceria nanoparticles with polymerizable capping ligands
Show others...
(English)Manuscript (preprint) (Other academic)
National Category
Nano Technology
Research subject
Chemistry
Identifiers
urn:nbn:se:kth:diva-173351 (URN)
Note

QS 2015

Available from: 2015-09-10 Created: 2015-09-10 Last updated: 2015-09-10Bibliographically approved
5. Thermodynamically driven ligand exchange on ceria nanoparticle surfaces – an efficient route to tailor ceria nanostructure properties
Open this publication in new window or tab >>Thermodynamically driven ligand exchange on ceria nanoparticle surfaces – an efficient route to tailor ceria nanostructure properties
(English)Manuscript (preprint) (Other academic)
National Category
Nano Technology
Identifiers
urn:nbn:se:kth:diva-173366 (URN)
Note

QS 2015

Available from: 2015-09-10 Created: 2015-09-10 Last updated: 2015-09-10Bibliographically approved

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