Nanopartículas de Pd suportadas em compósitos óxido-carbono: influência das interações metal-suporte na oxidação de etanol em meio básico

Fuel cells powered directly with ethanol (Direct Ethanol Fuel Cell-DEFC) are very attractive for the possibility of using a renewable fuel in the generation of clean energy. However, it is still necessary to deepen the understanding of catalytic processes and their dependence on the catalytic properties. This work proposes to study the catalytic activity of ethanol oxidation in an alkaline medium of Pd nanoparticles supported in carbon oxide hybrids using various transition metal oxides (MoO3, TiO2, WO3 and ZrO2). The materials prepared were characterized by techniques such as X-ray diffraction, transmission electron microscopy (TEM) and X-ray dispersive spectroscopy (EDX) to verify the structure, the distribution of particles in the supports and the presence of Pd on particles oxide. Experiments of X-rays absorption spectroscopy were carried out using soft X-rays (SXS) to evaluate the changes in the electronic properties of the Pd particles caused by interactions with different oxides. Measurements of cyclic voltammetry and potential sweeps of adsorbed CO oxidation allowed evaluating general aspects of the catalysts' electrochemical behavior and determining the electrochemically active area thereof. The catalytic performances of ethanol oxidation in alkaline medium were evaluated by electrochemical techniques (potential scan and chronoamperometry), and showed an improvement in activity with the addition of oxides in material containing only carbon, which was most pronounced for the catalyst containing TiO2. This improvement was predominantly associated with the electronic effects caused by the interaction of Pd on the support, causing a vacancy in the 4d band of Pd which, in turn, produces variations in adsorption energies of the species...

Effects of catalyst load in Pt and Pb-based catalysts using formic acid oxidation as a model

In this paper, we discuss the effects of catalyst load with respect to carbon powder for several Pt and Pb-based catalysts, using formic acid as a model molecule. The discussion is based on electrochemical tests, a complete morphological investigation and theoretical calculations. We show that the Pt and Pb-based catalysts presented activity in formic acid oxidation at very low catalyst loads (e.g., 0.5% in respect to the carbon content). Physical characterisations demonstrate that the electrodes are composed of separated phases of Pt and lead distributed in Pt nanometric-sized islands that are heterogeneously dispersed on the carbon support and Pb ultra-small particles homogeneously distributed throughout the entire carbon surface, as demonstrated by the microscopy studies. At high catalyst loads, very large clusters of Pb(x)O(y) could be observed. Electrochemical tests indicated an increase in the apparent resistance of the system (by a factor of 19.7 Omega) when the catalyst load was increased. The effect of lead in the materials was also studied by theoretical calculations (OFT). The main conclusion is that the presence of Pb atoms in the catalyst can improve the adsorption of formic acid in the catalytic system compared with a pure Pt-based catalyst. (C) 2011 Elsevier B.V. All rights reserved.

The influence of different co-catalysts in Pt-based ternary and quaternary electro-catalysts on the electro-oxidation of methanol and ethanol in acid media

One of the key objectives in fuel cell technology is to reduce Pt loading by the improvement of its catalytic activity towards alcohol oxidation. Here, a sol-gel based method was used to prepare ternary and quaternary carbon supported nanoparticles by combining Pt-Ru with Mo, Ta, Pb, Rh or Ir, which were used as electro-catalysts for the methanol and ethanol oxidation reactions in acid medium. Structural characterization performed by XRD measurements revealed that crystalline structures with crystallites ranging from 2.8 to 4.1 nm in size and with different alloy degrees were produced. Tantalum and lead deposited as a heterogeneous mixture of oxides with different valences resulting in materials with complex structures. The catalysts activities were evaluated by cyclic voltammetry and by Tafel plots and the results showed that the activity towards methanol oxidation was highly dependent of the alloy degree, while for ethanol the presence of a metal capable to promote the break of C-C bond, such as Rh, was necessary for a good performance. Additionally, the catalysts containing of TaOx or PbOx resulted in the best materials due to different effects: the hi-functional mechanism promoted by TaOx and a better dispersion of the catalysts constituents promoted by PbOx. (C) 2012 Elsevier B.V. All rights reserved.

Electrodeposition of PVA-protected PtCo electrocatalysts for the oxygen reduction reaction in H2SO4

In this paper we report the electrosynthesis of PVA-protected PtCo films (PVA = poly(vinylalcohol)) and their activities towards the oxygen reduction reaction (ORR). PtCo electrodeposits were potentiostatically obtained in the presence and absence of PVA at distinct potentials. The film morphology and composition were characterized by scanning electron microscopy (SEM) and energy-dispersive X-ray spectroscopy (EDX), which revealed that the use of PVA in the electrodeposition of PtCo films was decisive to achieve better film composition control. Cyclic voltammetry for PVA-protected PtCo films showed that the electrochemical surface area is dependent on the electrodeposition potentials and suggested different adsorption strengths of oxygen-containing species. Films produced in the presence of PVA presented the following activity order towards ORR as a function of the electrodeposition potential (vs. Ag/AgCl): -0.9 V> -0.8 V> -1.0 V> -0.7 V. In contrast, PtCo films electrodeposited in the absence of PVA displayed very similar activities regardless of the electrodeposition potential. The simplicity of the electrodeposition method combined with its effectiveness enabled the production of "model electrodes" for investigating the fundamental aspects of the reactions taking place in the fuel cell cathodes. (C) 2011 Elsevier B.V. All rights reserved.

Influence of Modifications to the Pechini Method on the Electroactivity and Stability of Pt-RuOx/C Catalysts

Since electrode electroactivity and stability depend directly on the nature, morphology, and structure of the material, we have investigated how modifications to the Pechini method during the synthesis of Pt-RuOx/C electrocatalysts affected catalyst activity. The structure and stability of the resulting materials were investigated after their submission to a large number of potential scans and to constant potential for a prolonged time period in sulfuric acid 0.5 mol L-1 and methanol 0.1 mol L-1 solution. DMFC tests were accomplished using membrane electrode assemblies (MEAs) prepared by hot-pressing a pretreated Nafion 117 membrane together with the prepared Pt-RuOx anodes and a Pt cathode (from E-TEK), in order to compare the catalytic activity of the materials prepared by different methods. The stability studies demonstrated that the catalyst whose resin/carbon support mixture was agitated in a balls mill before undergoing heat-treatment was more stable than the other prepared catalysts. The catalysts synthesized with the single resin consisting of Pt and Ru and subjected to ultrasound before heat-treatment furnished the highest power density in the single fuel cell. (C) 2012 The Electrochemical Society. [DOI: 10.1149/2.011208jes]

Performance and selectivity of PtxSn/C electro-catalysts for ethanol oxidation prepared by reduction with different formic acid concentrations

Carbon supported Pt-Sn catalysts were prepared by reduction of Pt and Sn precursors with formic acid and characterized in terms of structure, morphology and surface properties. The electrocatalytic activity for ethanol oxidation was studied in a direct ethanol fuel cell (DEFC) at 70 degrees C and 90 degrees C. Electrochemical and physico-chemical data indicated that a proper balance of Pt and Sn species in the near surface region was necessary to maximize the reaction rate. The best atomic surface composition, in terms of electrochemical performance, was Pt:Sn 65:35 corresponding to a bulk composition 75:25 namely Pt3Sn1/C. The reaction products of ethanol electro-oxidation in single cell and their distribution as a function of the nature of catalyst were determined. Essentially, acetaldehyde and acetic acid were detected as the main reaction products; whereas, a lower content of CO2 was formed. The selectivity toward acetic acid vs. acetaldehyde increased with the increase of the Sn content and decreased by decreasing the concentration of the reducing agent used in the catalyst preparation. According to the recent literature, these results have been interpreted on the basis of ethanol adsorption characteristics and ligand effects occurring for Sn-rich electrocatalysts. (C) 2012 Elsevier Ltd. All rights reserved.

Borohydride electrooxidation on Au and Pt electrodes

Direct borohydride fuel cells (DBFCs) are attractive energy generators for powering portable electronic devices, mainly due to their high energy density and number of electrons per borohydride ion. However, the lack of a highly efficient electrocatalyst for the borohydride oxidation reaction limits the performance of these devices. The most commonly studied electrocatalysts for this reaction are composed of gold and platinum. Nevertheless, for these metals, the borohydride electrooxidation reaction mechanism (BOR) is not completely understood, and the total oxidation reaction, involving eight electrons per BH4- species, competes with parallel reactions, with a lower number of exchanged electrons and/or with heterogeneous chemical hydrolysis. Considering the above-mentioned issues, this work presents recent advances in the knowledge of the BOR pathways on polycrystalline (bulk) Au and Pt electrocatalysts. It presents the studies of the BOR reaction on Au and Pt electrodes using in situ Fourier Transform Infrared Spectroscopy (FUR), and on-line Differential Electrochemical Mass Spectrometry (DEMS). The spectroscopic and spectrometric data provided physical evidence of intermediate species and the formation of H-2 in the course of the BOR as a function of the electrode potential. These results enabled to advance in the knowledge about the BOR pathways on Au and Pt electrocatalysts. (C) 2012 Elsevier Ltd. All rights reserved.

Self-potential signals from an analog biogeobattery mode

A tank experiment was conducted to check if self-potential (SP) signals can be generated when buried organic matter is wire-connected to a near-surface, oxygen-rich, sediment layer. This experiment demonstrated that once wired, there was a flux of electrons (hence an electric current) between the lower and upper layers of the sandbox with the system responding as a large-scale microbial fuel cell (a type of bioelectrochemical system). An electric current was generated by this process in the wire and the SP method was used to monitor the associated electric potential distribution at the top of the tank.. The electric field was controlled by the flux of electrons through the wire, the oxidation of the organic matter, the reduction of oxygen used as a terminal electron acceptor, and the distribution of the DC resistivity in the tank. The current density through the wire was limited by the availability of oxygen and not by the oxidation of the organic matter. This laboratory experiment incorporated key elements of the biogeobattery observed in some organic-rich contaminant plumes. This analogy includes the generation of SP signals associated with a flux of electrons, the capacity of buried organic matter in sustaining anodic reactions, network resistance connecting terminal redox reactions spatially separated in space, and the existence of anodic secondary coupled reactions. A resistivity tomogram of the tank, after almost a year in operation, suggests that oxidative processes triggered by this geobattery can be imaged with this method to determine the radius of influence of the bioelectrochemical system.

Ottimizzazione dei processi depurativi di reflui ad elevato carico organico a fini di recupero energetico

L’attuale condizione che caratterizza il settore energetico richiede un necessario processo di riconversione che, oltre a favorire il risparmio energetico, riduca la dipendenza dai combustibili fossili ed accresca l’impiego di fonti energetiche rinnovabili, dando un contributo fondamentale alla riduzione delle emissioni di gas serra come diversi accordi internazionali richiedono. Si rende pertanto necessario accelerare i processi che da alcuni anni stanno favorendo l’utilizzo di energia da fonti rinnovabili. Tra queste, le fonti legate ai processi di trattamento biologico dei reflui stanno avendo un interessante sviluppo. Esistono numerosi processi biologici che consentono la produzione di energia in maniera indiretta, quali ad esempio i processi di digestione anaerobica finalizzati alla produzione di biogas e/o produzione biologica di idrogeno. In tale contesto si inserisce la tecnologia delle Microbial Fuel Cell, che consente la produzione diretta di energia elettrica, finalizzata al recupero energetico inteso al miglioramento dell’efficienza energetica e alla riduzione dei costi d’esercizio di impianti di trattamento biologico dei reflui. Il presente lavoro di Tesi di Dottorato sperimentale, svoltosi in collaborazione al laboratorio PROT.-IDR. della sede ENEA di Bologna, riporta i risultati dell’attività di ricerca condotta su una MFC (Microbial Fuel Cell) a doppio stadio biologico per il trattamento di reflui ad elevato carico organico e produzione continua di energia elettrica. E’ stata provata l’applicabilità della MFC con entrambi i comparti biotici utilizzando elettrodi di grafite non trattata ottenendo, con un carico organico in ingresso di circa 9 gd-1, valori di potenza massima prodotta che si attestano su 74 mWm-2, corrente elettrica massima generata di 175 mAm-2 ad una tensione di 421 mV, ed una conversione di COD in elettricità pari a 1,2 gCODm-2d-1. I risultati sono stati molto positivi per quanto riguarda le prestazioni depurative ottenute dalla MFC. L’efficienza di depurazione misurata ha raggiunto un valore massimo del 98% di rimozione del COD in ingresso, mentre e la concentrazione di azoto ammoniacale nell’effluente raccolto all’uscita del sedimentatore è sempre stata inferiore a 1 mgN-NH4+l-1. Tra gli obiettivi posti all’inizio della sperimentazione si è rivelata di notevole interesse la valutazione del possibile utilizzo della MFC come sistema per il monitoraggio on-line del COD e degli acidi grassi volatili (VFA) prodotti all’interno di un digestore anaerobico, attraverso la definizione di una correlazione tra i dati elettrici registrati in continuo e le concentrazioni di CODanaer e VFA misurate in diversi periodi della sperimentazione. L’analisi DGGE della biomassa catodica ha fornito uno strumento analitico utile allo studio della diversità della comunità microbica sospesa ed adesa al catodo e ha confermato la forte similarità delle specie batteriche riconosciute nei campioni analizzati. In particolare, le bande di sequenziamento ottenute sono affiliate ai gruppi batterici Firmicutes, -Proteobacteria,  -Proteobacteria, -Proteobacteria e Bacteroidetes. Da quanto emerso dalla sperimentazione condotta si può pertanto concludere che ad oggi le MFC sono in fase di evoluzione rispetto ai primi prototipi utilizzati per lo studio delle comunità microbiali e per la comprensione dei meccanismi di trasferimento elettronico. Sfruttarne la potenza prodotta in maniera commerciale diviene una grande sfida per il futuro, ed è opinione comune che le prime applicazioni pratiche delle MFC saranno come fonte di recupero energetico per i dispositivi utilizzati per il monitoraggio dell’ambiente e per il trattamento delle acque reflue.

Wasserfreie, polymere Protonenleiter für Brennstoffzellen durch Immobilisierung von Imidazol

Es werden neuartige, polymere Protonenleiter vorgestellt die nach dem 'Konzept des polymergebunden Protonensolvens' realisiert wurden. Sie zeigen protonische Leitfähigkeit als intrinsische Eigenschaft, sodass keine zweite, flüssige Phase zur Protonenleitung nötig ist. Verwirklicht wurde das Konzept anhand von kammartigen Siloxanoligomeren und -polymeren, wobei Imidazol als Protonensolvens durch flexible Spacer kovalent an das Rückgrat gebunden ist. Durch Pfropfung mit imidazoltragenden Spacereinheiten wurden ferner Kieselgelnanopartikel oberflächenmodifiziert. Um die Auswirkungen der Immobilisierung von Imidazol auf die Leitfähigkeit zu untersuchen, wurden neben unterschiedlichen Molekulargewichten, die Verbindungen auch jeweils mit verschiedenen Spacerlängen synthetisiert. Die Materialien wurden umfassend charakterisiert und auf ihr thermisches Verhalten, Stabilität, Leitfähigkeit, Diffusion und dielektrisches Verhalten sowie auch nach Dotierung mit Säure untersucht. Thermisch stabil sind die Materialien bis ca. 200°C. Die Leitfähigkeiten betragen bis zu 1,5E-3 S/cm bei 160°C, welche aufgrund der Immobilisierung des Imidazols ausschließlich auf Strukturdiffusion zurückzuführen sind. Die Strukturdiffusion ist vergleichbar mit dem Grotthus-Mechanismus in Wasser und wird durch die lokale Mobilität der Imidazolmoleküle, d.h. durch die Glasübergangstemperatur des Systems bestimmt. Entsprechend wird das für Glasbildner typische Vogel-Tamman-Fulcher-Verhalten für alle untersuchten Transportprozesse gefunden. Die mit abnehmender Glasübergangstemperatur abnehmende mechanische Stabilität der Materialien kann, wie gezeigt ist, durch Compoundierung mit Kieselgelnanopartikeln entscheidend verbessert werden, was eine kostengünstige und aussichtsreiche Möglichkeit zur Herstellung von Membranen für Brennstoffzellen darstellt.

Ionenleitfähigkeit in polymeren Matrizes – Synthese, Charakterisierung und Untersuchung dynamischer Prozesse von neuen Lithium- und Protonenleitern

Die vorliegende Dissertation befasst sich mit der Synthese, physikochemischen und polymerspezifischen Charakterisierung und insbesondere der impedanzspektroskopischen Untersuchung von sowohl neuartigen, solvensfreien lithiumionen- als auch protonenleitfähigen Polymermaterialien für potentielle Anwendungen in sekundären Lithiumionenbatterien bzw. in Hochtemperatur-Protonenaustauschmembran-Brennstoffzellen (engl.: proton exchange membrane fuel cell, auch: polymer electrolyte membrane fuel cell, PEMFC). Beiden Typen von ionenleitfähigen Membranen liegt das gängige Prinzip der chemischen Anbindung einer für den Ionentransport verantwortlichen Seitengruppe an eine geeignete Polymerhauptkette zugrunde („Entkopplung“; auch Immobilisierung), welcher hinsichtlich Glasübergangstemperatur (Tg), elektrochemischer und thermischer Stabilität (Td) eine dynamisch entkoppelte, aber nicht minder bedeutsame Rolle zukommt. Die Transportaktivierung erfolgt in beiden Fällen thermisch. Im Falle der Protonenleiter liegt die zusätzliche Intention darin, eine Alternative aufzuzeigen, in der die Polymerhauptkette gekoppelt direkt am Protonentransportmechanismus beteiligt ist, d.h., dass der translatorisch diffusive Ionentransport entlang der Hauptkette stattfindet und nicht zwischen benachbarten Seitenketten. Ein Hauptaugenmerk der Untersuchungen liegt sowohl bei den lithiumionen- als auch den protonenleitfähigen Polymermembranen auf temperaturabhängigen dynamischen Prozessen der jeweiligen Ionenspezies in der polymeren Matrix, was die Ionenleitfähigkeit selbst, Relaxationsphänomene, die translatorische Ionendiffusion und im Falle der Protonenleiter etwaige mesomere Grenzstrukturübergänge umfasst. Lithiumionenleiter: Poly(meth)acrylate mit (2-Oxo-1,3-dioxolan)resten (Cyclocarbonat-) in der Seitenkette unterschiedlicher Spacerlänge wurden synthetisiert und charakterisiert. Die Leitfähigkeit s(,T) erreicht bei Poly(2-oxo-[1,3]dioxolan-4-yl)methylacrylat (PDOA): Lithium-bis-trifluormethansulfonimid (LiTFSI) (10:3) ca. 10^-3,5 S cm^-1 bei 150 °C. Weichmachen (Dotieren) mit äquimolaren Mengen an Propylencarbonat (PC) bewirkt in allen Fällen einen enormen Anstieg der Leitfähigkeit. Die höchsten Leitfähigkeiten von Mischungen dieser Polymere mit LiTFSI (und LiBOB) werden nicht beim System mit der niedrigsten Tg gefunden. Auch dient Tg nicht als Referenztemperatur (Tref) nach Williams-Landel-Ferry (WLF), so dass eine WLF-Anpassung der Leitfähigkeitsdaten nur über einen modifizierten WLF-Algorithmus gelingt. Die ermittelten Tref liegen deutlich unterhalb von Tg bei Temperaturen, die charakteristisch für die Seitenkettenrelaxation sind („Einfrieren“). Dies legt nahe, dass der Relaxation der Seitenketten eine entscheidende Rolle im Li^+-Leitfähigkeitsmechanismus zukommt. Die Li^+-Überführungszahlen tLi^+ in diesen Systemen schwanken zwischen 0,13 (40 °C) und 0,55 (160 °C). Protonenleiter: Polymere mit Barbitursäure- bzw. Hypoxanthinresten in der Seitenkette und Polyalkylenbiguanide unterschiedlicher Spacerlänge wurden synthetisiert und charakterisiert. Die Leitfähigkeit s(,T) erreicht bei Poly(2,4,6(1H,3H,5H)-trioxopyrimidin-5-yl)methacrylat (PTPMA) maximal ca. 10^-4,4 S cm^-1 bei 140 °C. Höhere Leitfähigkeiten sind nur durch Mischen mit aprotischen Lösungsmitteln erreichbar. Die höchste Leitfähigkeit wird im Falle der Polyalkylenbiguanide bei Polyethylenbiguanid (PEB) erzielt. Sie erreicht 10^-2,4 S cm^-1 bei 190 °C. Die Aktivierungsenergien EA der Polyalkylenbiguanide liegen (jeweils unterhalb von Tg) zwischen ca. 3 – 6 kJ mol^-1. In allen beobachteten Fällen dient Tg als Tref, so dass eine konventionelle WLF-Behandlung möglich ist und davon auszugehen ist, dass die Leitfähigkeit mit dem freien Volumen Vf korreliert.

Studio preliminare di una rete microcogenerativa con sistema ORC

Studio preliminare di una futura installazione di un banco prova con sistema ORC in parallelo ad una fuel cell. Analisi e scelta dell'impianto ORC, scelta della fonte di calore e del sistema di condensazione in base alle esigenze dell'impianto ORC scelto. Scrittura di un codice di calcolo per simulare l'intero sistema installato.

Theoretical and Experimental Analysis of micro-CHP Energy Systems

In the framework of the micro-CHP (Combined Heat and Power) energy systems and the Distributed Generation (GD) concept, an Integrated Energy System (IES) able to meet the energy and thermal requirements of specific users, using different types of fuel to feed several micro-CHP energy sources, with the integration of electric generators of renewable energy sources (RES), electrical and thermal storage systems and the control system was conceived and built. A 5 kWel Polymer Electrolyte Membrane Fuel Cell (PEMFC) has been studied. Using experimental data obtained from various measurement campaign, the electrical and CHP PEMFC system performance have been determinate. The analysis of the effect of the water management of the anodic exhaust at variable FC loads has been carried out, and the purge process programming logic was optimized, leading also to the determination of the optimal flooding times by varying the AC FC power delivered by the cell. Furthermore, the degradation mechanisms of the PEMFC system, in particular due to the flooding of the anodic side, have been assessed using an algorithm that considers the FC like a black box, and it is able to determine the amount of not-reacted H2 and, therefore, the causes which produce that. Using experimental data that cover a two-year time span, the ageing suffered by the FC system has been tested and analyzed.

The Effect of Various Electrode Microstructure Parameters on the Effective Conductivity and Three-Phase Boundary Density of Infiltrated SOFC Electrodes

Solid oxide fuel cell (SOFC) technology has the potential to be a significant player in our future energy technology repertoire based on its ability to convert chemical energy into electrical energy. Infiltrated SOFCs, in particular, have demonstrated improved performance and at lower cost than traditional SOFCs. An infiltrated electrode comprises porous ceramic scaffolding (typically constructed from the oxygen ion conducting material) that is infiltrated with electron conducting and catalytic particles. Two important SOFC electrode properties are effective conductivity and three phase boundary density (TPB). Researchers study these electrode properties separately, and fail to recognize them as competing properties. This thesis aims to (1) develop a method to model the TPB density and use it to determine the effect of porosity, scaffolding particle size, and pore former size on TPB density as well as to (2) compare the effect of porosity, scaffolding particle size, and pore former size on TPB density and effective conductivity to determine a desired set of parameters for infiltrated SOFC electrode performance. A computational model was used to study the effect of microstructure parameters on the effective conductivity and TPB density of the infiltrated SOFC electrode. From this study, effective conductivity and TPB density are determined to be competing properties of SOFC electrodes. Increased porosity, scaffolding particle size, and pore former particle size increase the effective conductivity for a given infiltrate loading above percolation threshold. Increased scaffolding particle size and pore former size ratio, however, decreases the TPB density. The maximum TPB density is achievable between porosities of 45% and 60%. The effect of microstructure parameters are more prominent at low loading with scaffolding particle size being the most significant factor and pore former size ratio being the least significant factor.

In-plane thermal conductivity modeling of carbon filled liquid crystal polymer based resins

Adding conductive carbon fillers to insulating thermoplastic resins increases composite electrical and thermal conductivity. Often, as much of a single type of carbon filler is added to achieve the desired conductivity, while still allowing the material to be molded into a bipolar plate for a fuel cell. In this study, varying amounts of three different carbons (carbon black, synthetic graphite particles, and carbon fiber) were added to Vectra A950RX Liquid Crystal Polymer. The in-plane thermal conductivity of the resulting single filler composites were tested. The results showed that adding synthetic graphite particles caused the largest increase in the in-plane thermal conductivity of the composite. The composites were modeled using ellipsoidal inclusion problems to predict the effective in-plane thermal conductivities at varying volume fractions with only physical property data of constituents. The synthetic graphite and carbon black were modeled using the average field approximation with ellipsoidal inclusions and the model showed good agreement with the experimental data. The carbon fiber polymer composite was modeled using an assemblage of coated ellipsoids and the model showed good agreement with the experimental data.