Publications of Rudi Cloots
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See detailCombining mesoporosity and Ti-doping in hematite films for water splitting
Toussaint, Caroline ULiege; Tran, Hoang Son ULiege; Colson, Pierre ULiege et al

in Journal of Physical Chemistry C (2015), 119(4), 1642-1650

(Graph Presented). In this study, we report the synthesis of Ti-doped mesoporous hematite films by soft-templating for application as photoanodes in the photoelectrolysis of water (water splitting ... [more ▼]

(Graph Presented). In this study, we report the synthesis of Ti-doped mesoporous hematite films by soft-templating for application as photoanodes in the photoelectrolysis of water (water splitting). Because the activation of the dopant requires a heat treatment at high temperature (≥800°C), it usually results in the collapse of the mesostructure. We have overcome this obstacle by using a temporary SiO2 scaffold to hinder crystallite growth and thereby maintain the mesoporosity. The beneficial effect of the activated dopant has been confirmed by comparing the photocurrent of doped and undoped films treated at different temperatures. The role of the mesostructure was investigated by comparing dense, collapsed, and mesoporous films heated at different temperatures and characterized under front and back illumination. It turns out that the preservation of the mesotructure enables a better penetration of the electrolyte into the film and therefore reduces the distance that the photogenerated holes have to travel to reach the electrolyte. As a result, we found that mesoporous films with dopant activation at 850°C perform better than comparable dense and collapsed films. [less ▲]

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See detailElucidating the opto-electrical properties of solid and hollow titania scattering layers for improvement of dye-sensitized solar cells
Thalluri, Venkata Visveswara Gopala Kris; Henrist, Catherine ULiege; Spronck, Gilles ULiege et al

in Thin Solid Films (2015)

The light scattering method has been adapted in dye-sensitized solar cells (DSCs) for optical absorption enhancement. In DSC's, particle-size of TiO2 should be inline with the scattering wavelength range ... [more ▼]

The light scattering method has been adapted in dye-sensitized solar cells (DSCs) for optical absorption enhancement. In DSC's, particle-size of TiO2 should be inline with the scattering wavelength range. Scattering particles can be used either by forming a bilayer structure with TiO2 nanocrystalline film or into the bulk of TiO2 nanocrystalline film. For improving the DSCs performances these scattering layers aim to refract/reflect the incident light by extending the traveling distance of UV-Visible/near-IR light within the dye-sensitized TiO2 nanocrystalline film. In this work, the scattering layers with two different particle-sizes (~200 nm-solid and ~400 nm-hollow) were deposited as an additional layer on the top of dye-sensitized TiO2 nanocrystalline film and the morphological properties were studied. By using various opto-electrical characterization techniques, the influence of these scattering layers for two different classes of DSCs prepared from N3 (UV-Vis) and SQ2 (near-IR) dyes were investigated. [less ▲]

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See detailAtmospheric Pressure Plasma as an Activation Step for Improving Protein Adsorption on Hydroxyapatite Powder
Ozhukil Kollath, Vinayaraj ULiege; Put, Sofie; Mullens, Steven et al

in Plasma Processes and Polymers (2015)

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See detailMicrowave sintering of Ge-doped In2O3 thermoelectric ceramics prepared by slip casting process
Combe, Emmanuel ULiege; Guilmeau, Emmanuel; Savary, E et al

in Journal of the European Ceramic Society (2015), 35

Ge doped In2O3 bulks were prepared by dry uniaxial compaction or slip casting shaping methods followed by a conventional or microwave sintering. Density of slip casted Ge doped In2O3 samples after ... [more ▼]

Ge doped In2O3 bulks were prepared by dry uniaxial compaction or slip casting shaping methods followed by a conventional or microwave sintering. Density of slip casted Ge doped In2O3 samples after conventional sintering reaches bulk density close to the theoretical one thanks to an optimized particles arrangement in the slip casted green bulks. Combined with a fast microwave sintering, slip casted bulks possess submicrometer grain size due to limited grain growth. A significant decrease of the electrical resistivity has been measured in slip casted samples sintered by conventional heat treatment. In bulk specimens sintered by microwave heating, a simultaneous increase of electrical resistivity and decrease of the thermal conductivity is observed. From room temperature to 1000 K in air, slip casted samples sintered by conventional or microwave sintering exhibit similar thermoelectric figure of merit (ZT) values. [less ▲]

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See detailEffects of Starch as Carbon precursor on hydrothermal synthesis and Electrochemical performance of Sodium manganese iron phosphate /carbon
Karegeya, Claude ULiege; Vertruyen, Bénédicte ULiege; Cloots, Rudi ULiege et al

Poster (2014, November 05)

Currently Sodium based electrode materials for Li and Na-ion batteries are getting more attention as the most promising potential alternatives of their lithiated counterparts due to their cost effective ... [more ▼]

Currently Sodium based electrode materials for Li and Na-ion batteries are getting more attention as the most promising potential alternatives of their lithiated counterparts due to their cost effective, environmental friendly characteristics and availability of sodium. Nevertheless, it remains a practical challenge to find an electrode material of LIBs and SIBs showing ideal performance. We report here a composite material of Sodium manganese iron phosphate/carbon, successfully synthesized by hydrothermal method. We have characterized our material by using a combination of Powder X-ray diffraction (XRD), scanning electron Microscopy (SEM) and thermal gravimetric analysis (TGA). Sodium manganese iron phosphate (NMFP) particles are electrochemically activated by starch and acetylene black to form NMFP/C cathode material for LIBs. NMFP/C composite in which starch is used as carbon precursor exhibits good discharge capacity due to the presence of pyran rings which increase NMFP/C conductivity. [less ▲]

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See detailInnovative materials improving energy efficiency of buildings
Dewalque, Jennifer ULiege; Denayer, Jessica ULiege; Schrijnemakers, Audrey ULiege et al

Conference (2014, July 01)

Detailed reference viewed: 41 (17 ULiège)
See detailElectrografting of polythiophenes on zinc oxide nanorods for photovoltaic cells
Demarteau, Jérémy ULiege; Ouhib, Farid ULiege; Henrist, Catherine ULiege et al

Poster (2014, May 20)

As the rarefaction of fossil energies, photovoltaic cells are certainly amongst the most important energy sources for the future. Our work concentrated on hybrid photovoltaic cells that are based on ... [more ▼]

As the rarefaction of fossil energies, photovoltaic cells are certainly amongst the most important energy sources for the future. Our work concentrated on hybrid photovoltaic cells that are based on organic (polythiophene) and inorganic components (ZnO nanorods). The technology that maximizes the contact area between the two semi-conductor n and p while maintaining two separate components is the interdigital configuration. As the inorganic part, perfectly well aligned zinc oxide (ZnO) 1D nanostructures have been synthesized by hydrothermal growth on ZnO-seeded FTO substrates. SEM, AFM and XRD characterizations evidence patterned well- aligned nanorods with high c-axis, their roughness of surface and the length of their nanostructure. Concerning the organic component, we synthetize polythiophenes based diblock copolymer with high degree of regioregularity and predetermined molecular weight using Grignard Methatis (GRIM) process. Diblock polythiophene based copolymers are of interest because of the possibility of generating multifunctional materials (by associating the specific properties of each block), including their ability for self-assembly into well-defined nanostructures (fibrils or micelles) with controllable dimensions. Poly(3-hexylthiophene) (P3HT) composes the first block and the second block is either a polythiophene bearing an acrylate group on each monomer unit (PAcET), or a polythiophene bearing both acrylate and poly(ethylene glycol) side chains (P(AcET-co-PEGET)). Typically, the acrylates are used to fixe in a covalent way the copolymer to ZnO nanorods, while the PEG grafts are necessary for the solubilisation of the copolymer in the electrografting medium. 1H NMR and DLS characterizations allow us to find the backbone and the micellar structure of the copolymer. Cathodic polarization (electrografting) of ZnO nanorods induces electropolymerization of acrylate groups, leading to an adherent organized film of poly(thiophene)-based micelles. During the illumination tests, we obtained a typical response of a photovoltaic despite the low yields. This promising synthetic route opens exciting perspectives for the production and the electrochemical functionalization of different lengths of ZnO nanowires, which seems to be promising candidate for hybrids photovoltaic cells. [less ▲]

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See detailEffect of the RE (RE = Eu, Er) doping on the structural and textural properties of mesoporous TiO2 thin films obtained by evaporation induced self-assembly method
Borlaf, Mario; Caes, Sébastien ULiege; Dewalque, Jennifer ULiege et al

in Thin Solid Films (2014), 558

Polymeric sol–gel route has been used for the preparation of TiO2 and RE2O3–TiO2 (RE = Eu, Er) mesoporous thin films by evaporation induced self-assembly method using Si (100) as a substrate. The ... [more ▼]

Polymeric sol–gel route has been used for the preparation of TiO2 and RE2O3–TiO2 (RE = Eu, Er) mesoporous thin films by evaporation induced self-assembly method using Si (100) as a substrate. The influence of the relative humidity (RH) on the preparation of the film has been studied being necessary to work under 40% RH in order to obtain homogeneous and transparent thin films. The films were annealed at different temperatures until 900 °C/1 h and the anatase crystallization and its crystal size evolution were followed by low angle X-ray diffraction. Neither the anatase–rutile transition nor the formation of other compounds was observed in the studied temperature range. Ellipsoporosimetry studies demonstrated that the thickness of the thin films did not change after calcination at 500 °C, the porosity was constant until 700 °C, the pore size increased and the specific surface area decreased with temperature. Moreover, the effect of the doping with Er3 + and Eu3 + was studied and a clear inhibition of the crystal growth and the sintering process was detected (by transmission electron and atomic force microscopy) when the doped films are compared with the undoped ones. Finally, Eu3 + and Er3 + f–f transitions were detected by PL measurements. [less ▲]

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See detailInfluence of mesoporosity in hematite films on water splitting efficiency
Toussaint, Caroline ULiege; Cloots, Rudi ULiege; Henrist, Catherine ULiege

Poster (2014)

Solar energy is inexhaustible but variable during the day and the seasons. Photoelectrolysis of water (water splitting) convert this energy into hydrogen to obtain an energy that can be stored and ... [more ▼]

Solar energy is inexhaustible but variable during the day and the seasons. Photoelectrolysis of water (water splitting) convert this energy into hydrogen to obtain an energy that can be stored and transported on demand. Hematite is a promising material for the photoanode in water splitting because of its high stability in water, cheapness, abundance and its band gap that enables the absorption of visible light (Eg: 2,1eV). Nevertheless, hematite has also some drawbacks including a short diffusion length of holes and a bad electronic conductivity. We have implemented spin coating and templating to produce doped mesoporous hematite films. The nanostructuration can improve the performances in water splitting by reducing the diffusion length of holes and increasing the specific surface between the film and the electrolyte. To suppress the collapse of the mesoporosity at high temperature (requested for dopant activation), we have used a temporary silica confinement scaffold that reduces the crystallite growth. To show the impact of the nanostructure, we have compared three films (mesoporous, collapsed and dense) in terms of hematite content (elemental analysis), nanostructure (electron microscopy), crystallinity (X-ray diffraction) and water splitting efficiency. We have also test two thermal treatments. This study highlights the effect of the effective interface with the electrolyte, through the preservation or not of open porosity and the different evolutions of the nanostructures as a function of the heat treatment. [less ▲]

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See detailLow temperature crystallization of yttrium orthoferrite by organic acid-assisted sol-gel synthesis
Stevens, Frédéric ULiege; Cloots, Rudi ULiege; Poelman, D. et al

in Materials Letters (2014), 114

Yttrium orthoferrite (YFeO3) is a promising material for visible light photocatalytic applications due to its band gap of 2.2-2.6 eV. However, during the synthesis of YFeO3, unwanted composition can be ... [more ▼]

Yttrium orthoferrite (YFeO3) is a promising material for visible light photocatalytic applications due to its band gap of 2.2-2.6 eV. However, during the synthesis of YFeO3, unwanted composition can be obtained and the crystallization requires temperatures as high as 850 C. Powders of YFeO3 were prepared using a sol-gel method with and without organic acids (citric acid, tartaric acid, malonic acid and oxalic acid) used as organic modifiers. The band gap of these powders was measured by diffuse reflection spectroscopy, and the crystallinity and crystalline phase content were characterized by X-ray diffraction. Organic acids allow a higher purity and facilitate crystallization. This work aims to produce YFeO3 powders at the lowest possible temperature. Citric acid was found to be the best additive: it reduces the crystallization temperature below 450 C. This opens new perspectives such as the deposition of crystalline YFeO3 thin films onto conductive glass for water-splitting applications. © 2013 Elsevier B.V. [less ▲]

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See detailStability of templated and nanoparticles dye-sensitized solar cells : photovoltaic and electrochemical investigation of degradation mechanisms at the photoelectrode interface
Dewalque, Jennifer ULiege; Nguyen, Ngoc Duy ULiege; Colson, Pierre ULiege et al

in Electrochimica Acta (2014), 115(1), 478-486

A key issue in the commercialization of dye-sensitized solar cells is to maintain high efficiency and long lifetime. As reported in the literature, dye-sensitized solar cells are stable under visible ... [more ▼]

A key issue in the commercialization of dye-sensitized solar cells is to maintain high efficiency and long lifetime. As reported in the literature, dye-sensitized solar cells are stable under visible light soaking but thermal stress and UV exposure lead to efficiency degradation. However, all the stability studies published so far have been performed on cells whose TiO2 electrodes were prepared by tape casting or screen printing of nanoparticle pastes/inks. The present study concerns cells based on highly porous templated TiO2 electrodes, whose larger surface area could enhance the negative effects of thermal stress, light soaking and UV exposure. The long-term stability of these cells is compared with a classical nanoparticle-based cell using current-voltage measurements (I-V curves) and electrochemical impedance spectroscopy. Due to their higher active interface, templated cells are more sensitive than nanoparticle cells to UV illumination, although this can be easily solved in both cases by the use of a UV filter. The templated cells are as stable as the nanoparticle cells under visible light soaking (UV filtered). However, we showed that templated cells are more stable under thermal stress. Moreover, as evidenced by electrochemical impedance spectroscopy, templated cells show lower transfer resistance, as well as lower recombination resistance compared to nanoparticle cells. The crystallite connectivity promoted by the templating route seems to favor the electron transfers inside the porous layer. Using templated films in dye-sensitized solar cells is therefore really promising because higher conversion efficiencies are reached without promoting cell degradation. [less ▲]

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See detailPore-filling of Spiro-OMeTAD determined by Rutherford backscattering spectrometry in templated TiO2 photoelectrodes
Dewalque, Jennifer ULiege; Colson, Pierre ULiege; Thalluri, Venkata Visveswara Gopala Kris ULiege et al

in Organic Electronics (2014), 15

Liquid-state dye-sensitized solar cells can suffer from electrolyte evaporation and leakage. Therefore solid-state hole transporting materials are investigated as alternative electrolyte materials ... [more ▼]

Liquid-state dye-sensitized solar cells can suffer from electrolyte evaporation and leakage. Therefore solid-state hole transporting materials are investigated as alternative electrolyte materials. However, in solid-state dye-sensitized solar cells, optimal TiO2 films thickness is limited to a few microns allowing the adsorption of only a low quantity of photoactive dye and thus leading to poor light harvesting and low conversion efficiency. In order to overcome this limitation, high surface area templated films are investigated as alternative to nanocrystalline films prepared by doctor-blade or screen-printing. Moreover, templating is expected to improve the pore accessibility what would promote the solid electrolyte penetration inside the porous network, making possible efficient charge transfers. In this study, films prepared from different structuring agents are discussed in terms of microstructural properties (porosity, crystallinity) as well as impact on the dye loading and Spiro-OMeTAD (2,2',7,7'-tetrakis-(N,N-di-p-methoxyphenylamine)9,9'-spirobifluorene) solid electrolyte filling. We first report Rutherford backscattering spectrometry as an innovative non-destructive tool to characterize the hole transporting materials infiltration. Templated films show dye loading more than two times higher than nanocrystalline films prepared by doctor-blade or screen-printing and solid electrolyte infiltration up to 88%. [less ▲]

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See detailSpray-drying synthesis of Na2FePO4F/carbon powders for lithium-ion batteries
Brisbois, Magali ULiege; Krins, Natacha ULiege; Hermann, Raphael et al

in Materials Letters (2014), 130

Sodium iron fluorophosphate Na2FePO4F is a candidate positive electrode material for both lithium-ion batteries and sodium-ion batteries. We report the synthesis of Na2FePO4F/carbon powders by the simple ... [more ▼]

Sodium iron fluorophosphate Na2FePO4F is a candidate positive electrode material for both lithium-ion batteries and sodium-ion batteries. We report the synthesis of Na2FePO4F/carbon powders by the simple and easily up-scalable technique of spray-drying. An aqueous solution containing citric acid as a carbon source was sprayed in a pilot-scale spray-dryer. Heat treatment at 600°C in argon for 12 hours was found appropriate to obtain single-phase Na2FePO4F; only 1.8% of Fe (III) were detected by iron-57 Mössbauer spectroscopy. When cycled against lithium, the discharge capacity reached 110 mAh g-1 at C/15 rate. (C) 2014 Elsevier B.V. All rights reserved. [less ▲]

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See detailYBa2Cu3O7-δ thick films for magnetic shielding: Electrophoretic deposition from butanol-based suspension
Closset, Raphaël ULiege; Kumar, Devendra; Wera, Laurent ULiege et al

in Materials Letters (2014), 119

Multilayered YBa2Cu3O7-δ (YBCO) thick films were coated on silver substrates by electrophoretic deposition (EPD) followed by heat treatment. A butanol-based YBCO suspension is used instead of the common ... [more ▼]

Multilayered YBa2Cu3O7-δ (YBCO) thick films were coated on silver substrates by electrophoretic deposition (EPD) followed by heat treatment. A butanol-based YBCO suspension is used instead of the common acetone-iodine combination. Tests with several dispersing agents reveal that a branched polyethyleneimine (PEI) dispersant develops large positive surface charge on suspended YBCO particles. As a demonstration of the performance of this new suspension formulation, a 12-layer 100 μm-thick YBCO coating was deposited on an Ag tube. The superconducting transition is sharp with onset critical temperature at 92 K. The sample can shield a magnetic field of ~1.3 mT at 77 K, i.e., the best value so far for an YBCO coating on a metallic substrate. © 2013 Elsevier B.V. [less ▲]

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See detailMesoporous amorphous tungsten oxide electrochromic films: a Raman analysis of their good switching behavior
Chatzikyriakou, Dafni ULiege; Krins, Natacha ULiege; Gilbert, Bernard ULiege et al

in Electrochimica Acta (2014), 137

The intercalation and de-intercalation of lithium cations in electrochromic tungsten oxide thin films are significantly influenced by their structural and surface characteristics. In this study, we ... [more ▼]

The intercalation and de-intercalation of lithium cations in electrochromic tungsten oxide thin films are significantly influenced by their structural and surface characteristics. In this study, we prepared two types of amorphous films via the sol-gel technique: one dense and one mesoporous in order to compare their response upon lithium intercalation and de-intercalation. According to chronoamperometric measurements, Li+ intercalates/de-intercalates faster in the mesoporous film (24s/6s) than in the dense film (48s/10s). The electrochemical measurements (cyclic voltammetry and chronoamperometry) also showed worse reversibility for the dense film compared to the mesoporous film, giving rise to important Li+ trapping and remaining coloration of the film. Raman analysis showed that the mesoporous film provides more accessible and various W-O surface bonds for Li+ intercalation. On the contrary, in the first electrochemical insertion and de-insertion in the dense film, Li+ selectively reacts with a few surface W-O bonds and preferentially intercalates into pre-existing crystallites to form stable irreversible LixWO3 bronze. [less ▲]

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See detailSurfactant-assisted ultrasonic spray pyrolysis of nickel oxide and lithium-doped nickel oxide thin films, towards electrochromic applications
Denayer, Jessica ULiege; Bister, Geoffroy; Simonis, Priscilla et al

in Applied Surface Science (2014), 321

Lithium-doped nickel oxide and undoped nickel oxide thin films have been deposited on FTO/glass substrates by a surfactant-assisted ultrasonic spray pyrolysis. The addition of polyethylene glycol in the ... [more ▼]

Lithium-doped nickel oxide and undoped nickel oxide thin films have been deposited on FTO/glass substrates by a surfactant-assisted ultrasonic spray pyrolysis. The addition of polyethylene glycol in the sprayed solution has led to improved uniformity and reduced light scattering compared to films made without surfactant. Furthermore, the presence of lithium ions in NiO films has resulted in improved electrochromic performances (coloration contrast and efficiency), but with a slight decrease of the electrochromic switching kinetics. [less ▲]

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See detailUltrasonic Spray Pyrolysis: an innovative fabrication method for electrochromic glazing
Maho, Anthony ULiege; Domercq, Benoit; Denayer, Jessica et al

Conference (2014)

Detailed reference viewed: 51 (9 ULiège)