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Simulations of Semi-Crystalline Polymers and Polymer Composites in order to predict Electrical, Thermal, Mechanical and Diffusion Properties
KTH, School of Chemical Science and Engineering (CHE), Fibre and Polymer Technology, Polymeric Materials.
2012 (English)Doctoral thesis, comprehensive summary (Other academic)
Abstract [en]

Several novel computer simulation models were developed for predicting electrical, mechanical, thermal and diffusion properties of materials with complex microstructures, such as composites, semi-crystalline polymers and foams.

A Monte Carlo model for simulating solvent diffusion through spherulitic semicrystalline polyethylene was developed. The spherulite model, based on findings by electron microscopy, could mimic polyethylenes with crystallinities up to 64 wt%. Due to the dendritic structure of the spherulites, the diffusion was surprisingly independent of the aspect ratio of the individual crystals. A correlation was found between the geometrical impedance factor (τ) and the average free path length of the penetrant molecules in the amorphous phase. A new relationship was found between volume crystallinity and τ. The equation was confirmed with experimental diffusivity data for Ar, CH4, N2 and n-hexane in polyethylene.

For electrostatics, a novel analytical mixing model was formulated to predict the effective dielectric permittivity of 2- and 3-component composites. Results obtained with the model showed a clearly better agreement with corresponding finite element data than previous models. The analytical 3-component equation was in accordance with experimental data for nanocomposites based on mica/polyimide and epoxy/ hollow glass sphere composites. Two finite element models for composite electrostatics were developed.

It is generally recognized that the fracture toughness and the slow crack growth of semicrystalline polymers depend on the concentrations of tie chains and trapped entanglements bridging adjacent crystal layers in the polymer. A Monte Carlo simulation method for calculating these properties was developed. The simulations revealed that the concentration of trapped entanglements is substantial and probably has a major impact on the stress transfer between crystals. The simulations were in accordance with experimental rubber modulus data.

A finite element model (FEM) including diffusion and heat transfer was developed for determining the concentration of gases/solutes in polymers. As part of the FEM model, two accurate pressure-volume-temperature (PVT) relations were developed. To predict solubility, the current "state of the art" model NELF was improved by including the PVT models and by including chemical interactions using the Hansen solubility parameters. To predict diffusivity, a novel free-volume diffusion model was derived based on group contribution methods. All the models were used without adjustable parameters and gave results in agreement with experimental data, including recent data obtained for polycarbonate and poly(ether-etherketone) pressurized with nitrogen at 67 MPa.

Place, publisher, year, edition, pages
Stockholm: KTH Royal Institute of Technology, 2012. , 59 p.
Series
Trita-CHE-Report, ISSN 1654-1081 ; 2012:15
National Category
Polymer Chemistry
Identifiers
URN: urn:nbn:se:kth:diva-93519ISBN: 978-91-7501-290-2 (print)OAI: oai:DiVA.org:kth-93519DiVA: diva2:516855
Public defence
2012-04-20, F2,, Lindstedtsvägen 28, entréplan, KTH, Stockholm, 10:00 (English)
Opponent
Supervisors
Note
QC 20120420Available from: 2012-04-20 Created: 2012-04-20 Last updated: 2012-04-23Bibliographically approved
List of papers
1. Penetrant diffusion in polyethylene spherulites assessed by a novel off-lattice Monte-Carlo technique
Open this publication in new window or tab >>Penetrant diffusion in polyethylene spherulites assessed by a novel off-lattice Monte-Carlo technique
2009 (English)In: European Polymer Journal, ISSN 0014-3057, E-ISSN 1873-1945, Vol. 45, no 12, 3409-3417 p.Article in journal (Refereed) Published
Abstract [en]

Semi-crystalline polymers have a complex hierarchical structure. The purpose of this study was to mimic the real structure of polyethylene spherulites by computer simulation using an off-lattice method in order to predict their diffusion properties. The principles used to build the spherulites were based on established findings obtained by electron microscopy. Spherulites in the crystallinity range of 0-55 vol% were built. Diffusion of small-molecule penetrants assuming no interfacial trapping at the amorphous-crystal boundary was studied using a Monte-Carlo technique. The main findings were: (i) diffusion was isotropic; (ii) diffusion was independent of the aspect ratio of the crystal building bricks, clearly in disagreement with the Fricke model: (iii) the geometrical impedance factor showed a dependence on the average free path length of the penetrant molecules in the amorphous phase: and (iv) data for the geometrical impedance factor obtained by simulation compared favourably with experimental data obtained for several penetrants showing limited interfacial trapping.

Keyword
Polyethylene spherulite, Off-lattice mesoscale simulation, Diffusion, Monte-Carlo model, molecular-dynamics simulation, melt-crystallized polyethylene, lamellar, morphology, isotactic polypropylene, transport-properties, free-volume, n-alkanes, organization, polymers, gases
National Category
Polymer Chemistry
Identifiers
urn:nbn:se:kth:diva-19054 (URN)10.1016/j.eurpolymj.2009.09.018 (DOI)000272871400011 ()2-s2.0-70449481086 (Scopus ID)
Note
QC 20100525Available from: 2010-08-05 Created: 2010-08-05 Last updated: 2017-12-12Bibliographically approved
2. Modelling the Relative Permittivity of Anisotropic Insulating Composites
Open this publication in new window or tab >>Modelling the Relative Permittivity of Anisotropic Insulating Composites
2011 (English)In: Composites Science And Technology, ISSN 0266-3538, E-ISSN 1879-1050, Vol. 71, no 2, 216-221 p.Article in journal (Refereed) Published
Abstract [en]

Three models have been developed for predicting the dielectric permittivity of insulating composites with inclusions of different lengths (from nm and larger) and different shapes. Firstly, for approximately periodic materials, a finite element model based on a smallest repeating box method was used in order to mimic frameworks with fibres, crystals, clay platelets, foams and lamellar layers. The introduction of parameters for relative aspect ratio, overlap, rotation and packing density made the model very flexible while maintaining its simplicity. Secondly, a finite element composite model with oriented, randomly positioned particles of different shapes was constructed. Thirdly, an analytical relationship to approximate the effective permittivity of two- or three-phase insulators with brick-shaped inclusions was derived. For a wide range of volume fractions, permittivity ratios and packing conditions, this model gave solutions very close to corresponding finite element simulation data for lamellae, much closer than all the other analytical relationships found in the literature. Results obtained by simulation were in agreement with experimental data from the literature for composites of micrometre-sized hollow glass spheres in epoxy and nanocomposites of mica platelets in polyimide, provided that a third (interfacial) component was introduced.

Keyword
Polymer-matrix composites (PMCs), Electrical properties, Modelling
National Category
Materials Engineering
Identifiers
urn:nbn:se:kth:diva-25417 (URN)10.1016/j.compscitech.2010.11.016 (DOI)000286909100020 ()2-s2.0-78650877405 (Scopus ID)
Funder
Swedish Research Council, VR-05-6138
Note
QC 20110317 Ändrad från submitted till published 20110317Available from: 2010-10-21 Created: 2010-10-21 Last updated: 2017-12-12Bibliographically approved
3. Small-Molecule Diffusion in Semicrystalline Polymers as Revealed by Experimental and Simulation Studies
Open this publication in new window or tab >>Small-Molecule Diffusion in Semicrystalline Polymers as Revealed by Experimental and Simulation Studies
2010 (English)In: POLYCHAR-18 WORLD FORUM ON ADVANCED MATERIALS / [ed] Mormann, W., Weinheim: WILEY-V C H VERLAG , 2010, Vol. 298, 108-115 p.Conference paper, Published paper (Refereed)
Abstract [en]

Diffusion of n-hexane in poly(ethylene-co-1-hexene)s with 15-75 wt.% crystallinity was studied by desorption experiments analyzing data using the Fickian equations with a concentration dependent diffusivity. The effect of the impenetrable crystalline phase on the penetrant diffusivity (D) is described by D = D-a/(tau beta), where D-a is the diffusivity of the amorphous polymer, tau is the geometrical impedance factor and beta is a factor describing the constraining effect of the crystals on the non-crystalline phase. For a polymer with 75 wt.% crystallinity, tau beta varied markedly with penetrant concentration (V-1a) in the penetrable phase: 1000 (V-1a = 0) and 10 (V-1a = 0.15). This penetrant-uptake had no effect on the gross crystal morphology, i.e. beta must be strongly dependent on V-1a. Samples saturated in n-hexane exhibited a penetrant-induced loosening of the interfacial structure, as revealed by an increase in crystal density that require an increased mobility in the interfacial component and by a decrease in the intensity of the asymmetric X-ray scattering associated with the interfacial component. The geometrical impedance factor has been modelled by mimicking spherulite growth and tau was obtained as the ratio of the diffusivities of the fully amorphous and semicrystalline systems. The maximum tau obtained from these simulations is ca. ten, which suggests that beta in the systems with V-1a = 0.15 takes values close to unity. The simulations showed that the geometrical impedance factor is insensitive to the ratio of the crystal width and the crystal thickness. A free path length scaling parameter characteristic of the amorphous phase correlated with tau.

Place, publisher, year, edition, pages
Weinheim: WILEY-V C H VERLAG, 2010
Series
MACROMOLECULAR SYMPOSIA, ISSN 1022-1360
Keyword
diffusion, morphology, polyethylene, simulation
National Category
Other Basic Medicine
Identifiers
urn:nbn:se:kth:diva-31639 (URN)10.1002/masy.201000027 (DOI)000288040500015 ()2-s2.0-78651303047 (Scopus ID)
Conference
18th World Forum on Advanced Polymeric Materials Siegen, GERMANY, APR 07-10, 2010
Note
QC 20110322Available from: 2011-03-22 Created: 2011-03-21 Last updated: 2012-04-23Bibliographically approved
4. Mass transport and high barrier properties of foodpackaging polymers
Open this publication in new window or tab >>Mass transport and high barrier properties of foodpackaging polymers
2011 (English)In: Multi-functional and nano-reinforcedpolymers for food packaging / [ed] J M Lagarón, Cambridge: Woodhead publishing , 2011, 129-149 p.Chapter in book (Other academic)
Place, publisher, year, edition, pages
Cambridge: Woodhead publishing, 2011
Keyword
transport properties, diffusivity, solubility, barrier, prediction
National Category
Polymer Chemistry
Identifiers
urn:nbn:se:kth:diva-93510 (URN)2-s2.0-84882850605 (Scopus ID)978 1 84569 738 9 (ISBN)
Note
QC 20120420Available from: 2012-04-20 Created: 2012-04-20 Last updated: 2012-04-23Bibliographically approved
5. Predicting Solubility and Diffusivity of Gases in Polymers under High Pressure: N-2 in Polycarbonate and Poly(ether-ether-ketone)
Open this publication in new window or tab >>Predicting Solubility and Diffusivity of Gases in Polymers under High Pressure: N-2 in Polycarbonate and Poly(ether-ether-ketone)
Show others...
2013 (English)In: Industrial & Engineering Chemistry Research, ISSN 0888-5885, E-ISSN 1520-5045, Vol. 52, no 26, 8655-8663 p.Article in journal (Refereed) Published
Abstract [en]

The aim of this study was to develop a model that predicts the gas solubility and the sorption and desorption kinetics in polymer granulates over large temperature and pressure intervals. Besides the part predicting the solubility and diffusivity, the model involves the simultaneous solution of the diffusion equation and the heat equation in three dimensions using a finite element method (FEM). When the temperature- and pressure-dependent solubility of a specific polymer/gas combination is not known, an improved version of the non-equilibrium lattice fluid model (NELF) is used to predict the solubility. The improvement of the NELF model includes the use of Hansen's solubility parameters, and it uses pressure-volume-temperature (PVT) data from two new empirical models, which accurately estimate polymer densities over a wide range of temperatures and pressures. The new solubility model predicted the solubility-pressure data of N-2 in poly(ethyl methacrylate) and N-2 and CH4 in polycarbonate (PC) at pressures below 4.5 MPa, without using any adjustable interaction parameters. The model was used to predict the solubility of N-2 in poly(ether-ether-ketone) (PEEK) and PC at a very high pressure (67 MPa). Experimental N-2 solubility data were obtained with a specially built reactor yielding high pressure and temperature. For PEEK, it was possible to predict the very high pressure solubility using a gas-polymer interaction parameter obtained from data taken at low pressures In addition, a new free-volume-based diffusivity model requiring no adjustable interaction parameters was developed, and it successfully predicted the desorption kinetics of N-2 from PEEK and PC.

Place, publisher, year, edition, pages
American Chemical Society (ACS), 2013
Keyword
Desorption, Diffusion, Ethers, Forecasting, Ketones, Partial differential equations, Polycarbonates, Polymers
National Category
Polymer Chemistry
Identifiers
urn:nbn:se:kth:diva-93549 (URN)10.1021/ie300975h (DOI)000321541600005 ()2-s2.0-84879862466 (Scopus ID)
Funder
EU, European Research Council, 218346Swedish Research Council, VR-05-6138
Note

Previous title: Predicting Solubility and Diffusivity of Gases in Polymers under High Pressure: N2 in Polycarbonate and Poly(ether-ether-ketone)

QC 20130205

Available from: 2013-02-05 Created: 2012-04-20 Last updated: 2017-12-07Bibliographically approved
6. Modelling tie-chains and trapped entanglements in polyethylene
Open this publication in new window or tab >>Modelling tie-chains and trapped entanglements in polyethylene
Show others...
2012 (English)In: Polymer, ISSN 0032-3861, E-ISSN 1873-2291, Vol. 53, no 16, 3594-3601 p.Article in journal (Refereed) Published
Abstract [en]

A Monte Carlo random walk model was developed to simulate the chain structure of amorphous layers in polyethylene. The chains emerging from the orthorhombic crystal lamellae were either folding back tightly (adjacent re-entry) or performing a random walk (obeying phantom chain statistics) forming statistical loops or tie chains. A correct amorphous density (ca. 85% of the crystalline density) was obtained by controlling the probability of tight folding. Important properties like fracture toughness depend on the number of chains covalently linking together the crystalline regions. The model structure was analysed with a novel numerical topology algorithm for calculating the concentration of tie chains and trapped entanglements. The numerical efficiency of the algorithm allowed molecular cubic systems with a side length of 100 nm to be readily analysed on a modern personal computer. Simulations showed that the concentration of trapped entanglements was larger than the concentration of tie chains and that the thickness of the amorphous layer (L a) had a greater impact than the crystal thickness (L c) on the tie-chain concentration. In several other commonly used models, such as the Huang-Brown model, the influence of trapped entanglements and the effect of the L a/L c ratio are neglected. Simulations using as input the morphology data from Patel generated results in agreement with experimental rubber modulus data.

Place, publisher, year, edition, pages
Elsevier, 2012
Keyword
Polyethylene, Tie chains, Trapped entanglements
National Category
Polymer Chemistry
Identifiers
urn:nbn:se:kth:diva-93552 (URN)10.1016/j.polymer.2012.05.045 (DOI)000306825400022 ()2-s2.0-84863726742 (Scopus ID)
Funder
Swedish Research Council, 621-2005-6138
Note

Updated from submitted to published.

QC 20130205

Available from: 2012-04-20 Created: 2012-04-20 Last updated: 2017-12-07Bibliographically approved
7. Validation of a 3D CT method for measurement of linear wear of acetabular cups: A hip simulator study
Open this publication in new window or tab >>Validation of a 3D CT method for measurement of linear wear of acetabular cups: A hip simulator study
Show others...
2011 (English)In: Acta Orthopaedica, ISSN 1745-3674, E-ISSN 1745-3682, Vol. 82, no 1, 35-41 p.Article in journal (Refereed) Published
Abstract [en]

Material and methods Ultra-high molecular weight polyethylene cups with a titanium mesh molded on the outside were subjected to wear using a hip simulator. Before and after wear, they were (1) imaged with a CT scanner using a phantom model device, (2) measured using a coordinate measurement machine (CMM), and (3) weighed. CMM was used as the reference method for measurement of femoral head penetration into the cup and for comparison with CT, and gravimetric measurements were used as a reference for both CT and CMM. Femoral head penetration and wear vector angle were studied. The head diameters were also measured with both CMM and CT. The repeatability of the method proposed was evaluated with two repeated measurements using different positions of the phantom in the CT scanner. Results The accuracy of the 3D CT method for evaluation of linear wear was 0.51 mm and the repeatability was 0.39 mm. Repeatability for wear vector angle was 17 degrees A degrees. Interpretation This study of metal-meshed hip-simulated acetabular cups shows that CT has the capacity for reliable measurement of linear wear of acetabular cups at a clinically relevant level of accuracy.

Keyword
Total Hip-Arthroplasty, Semiautomated Program, Component Migration, Computed-Tomography, Fusion, Repeatability, Penetration, Time
National Category
Surgery
Research subject
SRA - ICT
Identifiers
urn:nbn:se:kth:diva-31654 (URN)10.3109/17453674.2011.552777 (DOI)000287025400006 ()21281259 (PubMedID)2-s2.0-79751483254 (Scopus ID)
Note

QC 20110321

Available from: 2011-03-21 Created: 2011-03-21 Last updated: 2017-12-11Bibliographically approved
8. Water transport in aluminium oxide-poly(ethylene-co-butylacrylate) nanocomposites
Open this publication in new window or tab >>Water transport in aluminium oxide-poly(ethylene-co-butylacrylate) nanocomposites
Show others...
2011 (English)In: European Polymer Journal, ISSN 0014-3057, E-ISSN 1873-1945, Vol. 47, no 12, 2208-2215 p.Article in journal (Refereed) Published
Abstract [en]

Polymer composites with metal oxide nanoparticles are emerging materials to be used as insulations in electrical applications. However, the extensive interfacial surfaces and the presence of polar groups on the particle surfaces make these composites susceptible to water sorption. Water sorption kinetics data were taken at 23 °C and different relative humidities (18 to 90 %) for composites based on poly(ethylene-co-butyl acrylate) and aluminium oxide; the latter were in three different forms: uncoated and coated with either octyltriethoxy silane or aminopropyl triethoxy silane). The equilibrium water uptake increased in a linear fashion with increasing concentration of polar groups present on the nanoparticle surfaces. Composites with well-dispersed nanoparticles showed a Fickian sorption process with a diffusivity that decreased with increasing filler content. This effect was most pronounced for composites with accessible polar groups on the particle surfaces suggesting that water saturation of the composites is retarded by dual water sorption. Composites that contained a sizeable fraction of large nanoparticle agglomerates showed a two stage sorption process: a fast process associated the saturation of the matrix phase and slow diffusion process due to water sorption of the large nanoparticle agglomerates.

 

Keyword
Poly(ethylene-co-butyl acrylate), aluminium oxide, nanocomposites, water, sorption kinetics
National Category
Polymer Chemistry
Identifiers
urn:nbn:se:kth:diva-28779 (URN)10.1016/j.eurpolymj.2011.09.013 (DOI)000298204500004 ()2-s2.0-81155154434 (Scopus ID)
Note
QC 20110121. Updated from submitted to published 20120125Available from: 2011-01-21 Created: 2011-01-21 Last updated: 2017-12-11Bibliographically approved
9. Thermal Conductivity and Combustion Properties of Wheat Gluten Foams
Open this publication in new window or tab >>Thermal Conductivity and Combustion Properties of Wheat Gluten Foams
Show others...
2012 (English)In: ACS Applied Materials and Interfaces, ISSN 1944-8244, E-ISSN 1944-8252, Vol. 4, no 3, 1629-1635 p.Article in journal (Refereed) Published
Abstract [en]

Freeze-dried wheat gluten foams were evaluated with respect to their thermal and fire-retardant properties, which are important for insulation applications. The thermal properties were assessed by differential scanning calorimetry, the laser flash method and a hot plate method. The unplasticised foam showed a similar specific heat capacity, a lower thermal diffusivity and a slightly higher thermal conductivity than conventional rigid polystyrene and polyurethane insulation foams. Interestingly, the thermal conductivity was similar to that of closed cell polyethylene and glass-wool insulation materials. Cone calorimetry showed that, compared to a polyurethane foam, both unplasticised and glycerol-plasticised foams had a significantly longer time to ignition, a lower effective heat of combustion and a higher char content. Overall, the unplasticised foam showed better fire-proof properties than the plasticized foam. The UL 94 test revealed that the unplasticised foam did not drip (form droplets of low viscous material) and, although the burning times varied, self-extinguished after flame removal. To conclude both the insulation and fire-retardant properties were very promising for the wheat gluten foam.

Keyword
combustion, foam, freeze-drying; glycerol, thermal conductivity, wheat gluten
National Category
Polymer Chemistry
Identifiers
urn:nbn:se:kth:diva-52889 (URN)10.1021/am2017877 (DOI)000301968400066 ()22332837 (PubMedID)2-s2.0-84859149208 (Scopus ID)
Note
QC 20120420. Updated from manuscript to article in journalAvailable from: 2011-12-20 Created: 2011-12-20 Last updated: 2017-12-08Bibliographically approved
10. Dye release behavior from polyvinyl alcohol films in a hydro-alcoholic medium: Influence of physicochemical heterogeneity
Open this publication in new window or tab >>Dye release behavior from polyvinyl alcohol films in a hydro-alcoholic medium: Influence of physicochemical heterogeneity
Show others...
2012 (English)In: Colloids and Surfaces A: Physicochemical and Engineering Aspects, ISSN 0927-7757, E-ISSN 1873-4359, Vol. 403, 45-53 p.Article in journal (Refereed) Published
Abstract [en]

In this paper we investigated the release kinetics of a model drug-like compound (Coomassie brilliant blue) from polyvinyl alcohol (PVOH) films into a hydro-alcoholic solution as a function of the physicochemical properties of the polymer matrix. After 33 days of monitoring, the total amount released ranged from 10% for the high hydrolysis degree/low molecular weight PVOH films to 60% for the low hydrolysis degree/low molecular weight films. Mathematical modeling allowed for an estimation of the two diffusion coefficients (D 1 and D 2) that characterized the release profile of the dye from the films. The degree of hydrolysis dramatically affected both the morphology and the physical structure of the polymer network. A high hydroxyl group content was also associated with the shifting of second order and first order transitions toward higher temperatures, with a concurrent increase in crystallinity. Moreover, the higher the degree of hydrolysis, the higher the affinity of the polymer to the negatively charged molecule dye. Selection of the polymer matrix based on physicochemical criteria may help in achieving different release patterns, thereby representing the first step for the production of polymer systems with modulated release properties.

Keyword
Controlled release, Diffusion, Modeling, Morphology, Polyvinyl alcohol
National Category
Polymer Chemistry
Identifiers
urn:nbn:se:kth:diva-93674 (URN)10.1016/j.colsurfa.2012.03.054 (DOI)000304840700008 ()2-s2.0-84860916013 (Scopus ID)
Note
QC 20120529. Updated from submitted to published.Available from: 2012-04-23 Created: 2012-04-23 Last updated: 2017-12-07Bibliographically approved
11. The role of depolymerization in simultaneous gasification and melt flow of polystyrene.
Open this publication in new window or tab >>The role of depolymerization in simultaneous gasification and melt flow of polystyrene.
(English)Manuscript (preprint) (Other academic)
National Category
Polymer Chemistry
Identifiers
urn:nbn:se:kth:diva-14215 (URN)
Note
QC 20100726Available from: 2010-07-26 Created: 2010-07-26 Last updated: 2012-04-23Bibliographically approved

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