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Polymer-grafted Al2O3-nanoparticles for controlled dispersion in poly(ethylene-co-butyl acrylate) nanocomposites
KTH, School of Chemical Science and Engineering (CHE), Fibre and Polymer Technology, Coating Technology.ORCID iD: 0000-0002-3310-9964
KTH, School of Chemical Science and Engineering (CHE), Fibre and Polymer Technology, Polymeric Materials.
KTH, School of Chemical Science and Engineering (CHE), Fibre and Polymer Technology, Coating Technology.
KTH, School of Chemical Science and Engineering (CHE), Fibre and Polymer Technology.
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2014 (English)In: Polymer, ISSN 0032-3861, E-ISSN 1873-2291, Vol. 55, no 9, 2125-2138 p.Article in journal (Refereed) Published
Abstract [en]

We report a model system to control the dispersion and inter-particle distance of polymer-grafted Al2O3-nanoparticles in high molecular weight poly(ethylene-co-butyl acrylate). The proposed methods make it possible to extend the use of surface initiated atom transfer radical polymerization (SI-ATRP) in combination with more commercial grades of silanes and particles, showing the versatility of this polymerization process. The nanoparticles were surface-modified by an amine-terminated silane, forming multilayered silane coatings to which moieties capable of initiating ATRP were attached. Subsequently, "short" (DP: 117) and "long" (DP: 265) chains of poly(n-butyl acrylate) were grafted from the particles via SI-ATRP. The graft density was found to be in accordance with the density of the accessible amine groups and could therefore be assessed directly after the initial silanization step using UV-Vis spectrometry. From AFM micrographs, the grafted nanoparticles were found to be well-dispersed in the matrix. This observation was corroborated by a novel simulation method capable of transforming the inter-particle distances from 2D to 3D, for the closest and more distant neighbors. Further, we calculated the deviation ratios and concluded that the dispersions were homogeneous and that the inter-particle distances were related to the graft length. The homogeneous dispersions were explained by dominating enthalpic contributions of the polymer grafts to the nanocomposites in combination with shielding of the nanoparticle core-core attraction by the silane multilayer (similar to bimodal systems).

Place, publisher, year, edition, pages
2014. Vol. 55, no 9, 2125-2138 p.
Keyword [en]
Surface-initiated atom transfer radical, polymerization (SI-ATRP) of aluminum, oxide nanoparticles, Nanocomposites of poly(ethylene-co-butyl acrylate), Simulation of particle dispersion
National Category
Polymer Chemistry
Identifiers
URN: urn:nbn:se:kth:diva-145825DOI: 10.1016/j.polymer.2014.03.005ISI: 000335205200001Scopus ID: 2-s2.0-84898859798OAI: oai:DiVA.org:kth-145825DiVA: diva2:721399
Funder
Swedish Research Council, IFA 2007-5095
Note

QC 20140604

Available from: 2014-06-04 Created: 2014-06-02 Last updated: 2017-12-05Bibliographically approved
In thesis
1. Controlled Polymer Grafting from Nanoparticles for the Design of Dielectric Nanocomposites
Open this publication in new window or tab >>Controlled Polymer Grafting from Nanoparticles for the Design of Dielectric Nanocomposites
2017 (English)Doctoral thesis, comprehensive summary (Other academic)
Abstract [en]

The interest for polymeric nanocomposites has rapidly grown during the last decades, fuelled by the great potential and superior properties of nanoparticles (NPs). The production volumes of commercial NPs have increased exponentially during the last ten years, and the quality has been significantly improved. The aim of this study was to design polymer grafted commercially available metal-oxide NPs, and graphene oxide (GO), to develop isotropic (homogeneous) and anisotropic (heterogeneous) polymer nanocomposites for dielectric applications. The motivation was to formulate functional insulation materials for compact components in future power-grid systems using high-voltage direct-current (HVDC) or high-voltage alternating-current (HVAC), and to fabricate responsive sensor materials for monitoring e.g. temperature and voltage fluctuations in so called “Smart Grids”.

Aluminium oxide (Al2O3), zinc oxide (ZnO) and reduced GO (rGO) NPs were modified with sparse polymer grafts via a controlled “covalent route” and were mixed with silicone (PDMS) or polyethylene matrices (EBA and LDPE) commonly used in HV-cable systems. The graft length and the graft-to-matrix compatibility were tailored to obtain nanocomposites with various self-assembled NP-morphologies, including well-dispersed, connected and phase-separated structures. The graft length was used to adjust the inter-particle distance of nanocomposites with continuous morphologies or connected (percolated) NPs. It was found that nanocomposites with percolated NPs and short inter-particle distances exhibited 10-100 times higher conductivity than the unfilled (neat) polymer, or displayed a rapid non-linear increase in conductivity (~1 million times) with increasingelectric field, while well-dispersed NPs with long inter-particle distances exhibited 10-100 times lower conductivity (i.e. higher resistivity) as an effect of their trapping of charge carriers. These tunable and functional properties are desirable for HV-insulation, field-grading applications, and flexible electronics.

In addition it was shown that GO modified with dense polymer grafts via a “physisorption route” formed suspensions with liquid crystals, or matrix-free GO-composites with well-dispersed GO in isotropic or nematic states. These materials were reinforced by the GO, and exhibited elevated glass transition temperatures and a rapid thermo-responsive shape-memory effect, and are thus proposed to have a great potential as sensor materials and responsive separation membranes.

Abstract [sv]

Intresset för polymera nanokompositer har snabbt ökat under de senaste decennierna, drivet av den stora potentialen och de överlägsna egenskaperna hos nanopartiklar (NPs). Produktionsvolymerna för kommersiella NP har ökat exponentiellt under de senaste tio åren, och kvaliteten har förbättrats avsevärt. Syftet med denna studie var att polymer-ympa kommersiellt tillgängliga metalloxid-NPs, och grafenoxid (GO), för att designa isotropa (homogena) och anisotropa (heterogena) polymera nanokompositer för dielektriska tillämpningar. Motiveringen var att formulera funktionella isoleringsmaterial för kompakta komponenter i framtida kraftnätssystem som använder högspänd likström (HVDC) eller högspänd växelström (HVAC), samt att tillverka responsiva sensormaterial för övervakning av t.ex. temperatur- and spänningsvariationer i så kallade "Smart Grids".

Aluminiumoxid (Al2O3), zinkoxid (ZnO) och reducerad GO (rGO) NPs modifierades med glesa polymerympar via en kontrollerad "kovalent väg" och blandades med silikon (PDMS) eller polyeten matriser (EBA och LDPE) som är vanliga i HV-kabelsystem. Ymplängden och ymp-till-matrix kompatibiliteten skräddarsyddes för att erhålla nanokompositer med olika självordnande NP-morfologier, inklusive väldispergerade, länkade och fasseparerade strukturer. Ymplängden användes för att justera partikelavståndet i nanokompositer med förbundna morfologier eller länkade NPs. Man fann att nanokompositer med länkade NPs och korta interpartikelavstånd uppvisade 10-100 gånger högre konduktivitet än den ofyllda (rena) polymeren, eller erhöll en snabb icke-linjär ökning i konduktivitet (~1 miljon gånger) med ökande elektriskt fält, medan väldispergerade NPs med långa interpartikelavstånd uppvisade 10-100 gånger lägre ledningsförmåga (dvs. högre resistivitet) som en effekt av deras infångande av laddningsbärare. Dessa inställbara och funktionella egenskaper är önskvärda för HV-isolering, fältstyrande applikationer och flexibel elektronik.

Dessutom visades att GO, som modifierats med täta polymerympar via en "fysisorptionsväg", bildade suspensioner med flytande kristaller, eller matrisfria GO-kompositer med väldispergerad GO i isotropa eller nematiska tillstånd. Dessa material armerades av GO och uppvisade förhöjda glastransitionstemperaturer och en snabb värmeresponsiv form-minneseffekt, och föreslås därigenom ha en stor potential som sensor-material och responsiva separationsmembran.

Place, publisher, year, edition, pages
Stockholm: KTH Royal Institute of Technology, 2017. 96 p.
Series
TRITA-CHE-Report, ISSN 1654-1081 ; 2017:16
National Category
Polymer Chemistry
Research subject
Fibre and Polymer Science
Identifiers
urn:nbn:se:kth:diva-204036 (URN)
Public defence
2017-04-28, Kollegiesalen, Brinellvägen 8, KTH-huset, KTH Campus, Stockholm, 10:00 (English)
Opponent
Supervisors
Funder
SweGRIDS - Swedish Centre for Smart Grids and Energy Storage
Note

QC 20170323

Available from: 2017-03-23 Created: 2017-03-23 Last updated: 2017-08-10Bibliographically approved

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