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See detailDevelopment of new catalysts for proton exchange membrane fuel cells (PEMFCs)
Zubiaur, Anthony ULiege

Doctoral thesis (2017)

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See detailSynthesis, characterization, and durability study of Pt-Co hollow nanoparticles deposited on carbon xerogel electrocatalysts for Proton Exchange Membrane Fuel Cells (PEMFC)
Zubiaur, Anthony ULiege; Asset, Tristan ULiege; Olu, Pierre-Yves et al

Poster (2017, September)

Proton exchange membrane fuel cell (PEMFC) catalysts are generally made of carbon black (CB)supported platinum-based nanoparticles. However, the properties of CBs, as described by RodríguezReinoso [1 ... [more ▼]

Proton exchange membrane fuel cell (PEMFC) catalysts are generally made of carbon black (CB)supported platinum-based nanoparticles. However, the properties of CBs, as described by RodríguezReinoso [1], are not optimal for electrocatalysis. A possible solution to the drawbacks of CBs is the use of synthetic nanostructured materials with a controllable and reproducible texture and with a pure, known and constant chemical composition; carbon xerogels (CX) exhibit such properties [2]. Recently, various highly dispersed CX-supported Pt nanoparticles catalysts (Pt/CX) have been synthesized via several methods, such as the strong electrostatic adsorption (SEA) [3] or the charge-enhanced dry impregnation (CEDI) [4]. However, the decrease of the Pt mass contained in the PEMFC electrodes, in particular at the cathode where the oxygen reduction reaction (ORR) is processed, remains a major challenge. Improving the ORR mass activity is currently best achieved by alloying Pt with 3d-transition metal atoms such as cobalt (Co). These alloys perform better than the ORR because the substitution of some Pt atoms by 3d-metal atoms with smaller radius leads to a modified Pt electronic structure [5]. The synthesis and durability of Pt-Co hollow particles/CX (Fig. 1) is currently being studied in our groups. The results indicate that the specific and mass activity of the bimetallic hollow particles dispersed on CX is ca. 10 times higher than that of pure Pt/CB. The first durability results show good stability of the hollow particles structure. Performances and accelerated stress tests (ASTs) in PEMFCs were finally performed. [less ▲]

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See detailHighly efficient doped nanocristalline TiO2 for water Treatment
Mahy, Julien ULiege; Léonard, Géraldine ULiege; Zubiaur, Anthony ULiege et al

Conference (2017, July 13)

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See detailTowards a large scale aqueous sol-gel synthesis of doped TiO2: Study of various metallic dopings for the photocatalytic degradation of p-nitrophenol
Mahy, Julien ULiege; Lambert, Stéphanie ULiege; Léonard, Géraldine ULiege et al

in Journal of Photochemistry and Photobiology A : Chemistry (2016), 329

In this paper, an easy aqueous sol-gel synthesis developed previously by Mahy et al. [J. Sol-Gel Sci. Technol. (2016)] is adapted to produce highly active TiO2 catalysts doped with Fe3+, Ag+, Cu2+, Zn2 ... [more ▼]

In this paper, an easy aqueous sol-gel synthesis developed previously by Mahy et al. [J. Sol-Gel Sci. Technol. (2016)] is adapted to produce highly active TiO2 catalysts doped with Fe3+, Ag+, Cu2+, Zn2+, Cr3+, Al3+, Mn2+, and Co2+ ions and Pt metallic nanoparticles. Samples are characterized by inductively coupled plasma–atomic emission spectroscopy (ICP-AES), X-ray diffraction (XRD), Mössbauer spectroscopy, transmission electron microscopy (TEM), nitrogen adsorption–desorption measurements and diffuse reflectance spectroscopy measurements. Results show that the samples are composed of anatase-brookite TiO2 nanoparticles with a spherical shape and mean diameter of around 5-8 nm and a surface area of between about 150 - 250 m2 g-1. In each doped sample, the dopant is present in the form added during the synthesis, given that the sample has not undergone any particular treatment. Photoactivity tests show improvement in catalyst activity for Fe3+, Ag+, Cu2+, Zn2+, and Al3+ ion and Pt metallic nanoparticle dopants, while a decrease of activity is obtained for Cr3+, Mn2+ and Co2+ ion dopants. For some dopants, the activity of TiO2 doped with metallic ions and synthesized from the aqueous sol-gel process is equal or superior to the activity of the commercial photocatalyst Degussa P25. Some mechanisms are proposed to explain these modifications of activity with doping. Furthermore, cost comparison at laboratory scale showed that Zn and Cu nitrate salt dopings are clearly less expensive for a halogen light (UV/visible) or low energy light enhanced catalyst and may be considered for industrial applications. Using this method, a large scale Zn-doped TiO2 photocatalyst is synthesized with properties homologous to the lab-scale product. Results show that the aqueous sol-gel synthesis developed previously can be easily adapted for doping in order to produce an up-scalable synthesis. [less ▲]

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See detailDevelopment of a large scale aqueous sol-gel synthesis of doped TiO2
Mahy, Julien ULiege; Lambert, Stéphanie ULiege; Léonard, Géraldine ULiege et al

Conference (2016, July 20)

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See detailPt-Ni Hollow Nanoparticles for Oxygen Reduction Reaction: Controlling the Nanoparticles Morpholo-gy
Asset, Tristan ULiege; Chattot, Raphaël; Zubiaur, Anthony ULiege et al

Poster (2015, October 15)

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See detailPt-Ni Hollow Nanoparticles for Oxygen Reduction Reaction : Controlling the Nanoparticle Morphology
Asset, Tristan ULiege; Zubiaur, Anthony ULiege; Chattot, Raphael et al

Poster (2015, September 13)

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See detailDesign of Pt/carbon xerogel catalysts for PEM fuel cells
Job, Nathalie ULiege; Lambert, Stéphanie ULiege; Zubiaur, Anthony ULiege et al

in Catalysts (2015), 5

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See detailHighly dispersed iron xerogel catalysts for p-nitrophenol degradation by photo-Fenton effects
Mahy, Julien ULiege; Tasseroul, Ludivine ULiege; Zubiaur, Anthony ULiege et al

in Microporous and Mesoporous Materials (2014), 197

Several iron xerogel catalysts were synthesized by hydrolysis and condensation of tetraethoxysilane (TEOS) and 3-(2-aminoethylamino)propyltrimethoxysilane (EDAS) which is able to form a chelate with iron ... [more ▼]

Several iron xerogel catalysts were synthesized by hydrolysis and condensation of tetraethoxysilane (TEOS) and 3-(2-aminoethylamino)propyltrimethoxysilane (EDAS) which is able to form a chelate with iron ions. The EDAS/TEOS ratio strongly influences the texture of xerogel catalysts. The specific surface area and the micro- and mesoporous volume increase with this ratio. It seems that EDAS plays a nucleating agent role for silica particles and allows to anchor Fe-based moieties inside the silica network. Iron oxide nanoparticles of diameter 1-1.5 nm and Fe3+ ions result, encapsulated in silica particles with sizes of about 10-30 nm in diameter. The iron species was determined by Mössbauer spectroscopy and magnetometry measurements and only Fe3+ species were observed in xerogel catalysts. The Fenton and photo-Fenton effect of these catalysts were evaluated on the degradation of p-nitrophenol in aqueous media under different conditions. Results show that in the presence of H2O2, iron xerogel catalysts present a photo-Fenton effect, reaching 99 % of degradation after 24 h. [less ▲]

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See detailSynthesis of Pt/Carbon Xerogel Electrocatalysts for PEM Fuel Cells by the Multiple SEA Method
Zubiaur, Anthony ULiege; Chatenet, Marian; Maillard, Frédéric et al

Poster (2014, July)

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See detailHighly dispersed iron xerogel catalysts for p-nitrophenol degradation by photo-Fenton effects
Mahy, Julien ULiege; Tasseroul, Ludivine ULiege; Zubiaur, Anthony ULiege et al

Poster (2014, July)

Since the beginning of the industrial era, the various human activities have increased steadily, leading to a rapid technological development and a high population growth. Thus, the expansion of the ... [more ▼]

Since the beginning of the industrial era, the various human activities have increased steadily, leading to a rapid technological development and a high population growth. Thus, the expansion of the industry has heavily polluted the atmosphere, soil and water with negative consequences for humans and environment [1]. To decrease this pollution, it exists various treatment methods: chemical, physical and biological [2,3]. Among all these methods, a recent way of treatment is the degradation of pollutants in soils or waters by Fenton and photo-Fenton reactions [3] which use H2O2, iron-based compounds and UV light. In this way, several Fe2O3/SiO2 xerogel catalysts were synthesized by cogelation method by hydrolysis and condensation of tetraethoxysilane (TEOS) and 3-(2-aminoethylamino)propyltrimethoxysilane (EDAS) which is able to form a chelate with iron ions [4]. Five samples were synthesized: four samples with different percentage of iron (0.5, 1, 1.5 and 2.5 theoretical wt% confirmed by ICP-AES measurements), and a sample of pure silica. TEM pictures, nitrogen adsorption-desorption and mercury porosimetry measurements have established that EDAS plays a role of nucleating agent of silica particles [5,6] and allows to anchor iron particles inside silica network [4]. Indeed, it results iron nanoparticles of diameter 1-1.5 nm encapsulated in silica particles with sizes of about 10-30 nm in diameter. The species of iron was determined by Mössbauer spectroscopy and only Fe3+ ions were observed in xerogel catalysts. Then, the Fenton and photo-Fenton effect of these catalysts were evaluated on the degradation of p-nitrophenol (PNP) in aqueous medium in different conditions. Results show that Fe2O3/SiO2 xerogels present a photo-Fenton effect with H2O2, reaching with a sample 99 % of degradation after 24 h. [1] M. A. Khan, A. M. Ghouri, Environmental pollution: its effects on life and its remedies, Journal of Arts, Science & Commerce (Vol. 2), 2011, pg 276-285. [2] M. S. Kuyukina , I. B. Ivshina, Biology of rhodococcus: chapter 9, Springer, 2010, pg 232-256. [3] J. J. Pignatello, E. Oliveros, A. MacKay, Advanced Oxidation Processes for Organic Contaminant Destruction Based on the Fenton Reaction and Related Chemistry, Critical Reviews in Environmental Science and Technology (Vol. 36), 2006, pg 1-84. [4] B. Heinrichs, L. Rebbouh, J.W. Geus, S. Lambert, H.C.L. Abbenhuis, F. Grandjean, G.J. Long, J.-P. Pirard, R.A. van Santen, Iron (III) species dispersed in porous silica through sol-gel chemistry, Journal of Non-Crystalline Solids (Vol. 354), 2008, pg 665-672. [5] S. Lambert, C. Alié, J.-P. Pirard, B. Heinrichs, Study of textural properties and nucleation phenomenon in Pd/SiO2 , Ag/SiO2 and Cu/SiO2 cogelled xerogel catalysts, Journal of Non-Crystalline Solids (Vol. 342), 2004, pg 70-81. [6] B. Heinrichs, S. Lambert , N. Job , J.-P. Pirard, in "Catalyst Preparation: Science and Engineering, J. R. Regalbuto (Ed.)", CRC Press, Taylor & Francis Group, Boca Raton, 2007, p. 163-208. [less ▲]

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See detailSynthesis of Pt/Carbon Xerogel Electrocatalysts for Proton Exchange Membrane Fuel Cells (PEMFC): Effect of the Reduction Procedure
Zubiaur, Anthony ULiege; Chatenet, Marian; Maillard, Frédéric et al

Conference (2014, July)

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See detailDesign of Pt/carbon xerogel catalysts for PEM fuel cells
Job, Nathalie ULiege; Lambert, Stéphanie ULiege; Zubiaur, Anthony ULiege et al

Conference (2014, July)

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See detailUsing the Multiple SEA Method to Synthesize Pt/Carbon Xerogel Electrocatalysts for PEMFC Applications
Zubiaur, Anthony ULiege; Chatenet, Marian; Maillard, Frédéric et al

in Fuel Cells - From Fundamentals to Systems (2014), 14(3), 343-349

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See detailSynthesis of Pt/Carbon Xerogel Electrocatalysts for PEM Fuel Cells by the Multiple SEA Method
Zubiaur, Anthony ULiege; Chatenet, Marian; Maillard, Frédéric et al

Poster (2013, November 15)

1. Introduction Proton exchange membrane fuel cell (PEMFC) catalysts are generally made of carbon black-supported Pt-based nanoparticles. However, carbon blacks do not display optimal properties for ... [more ▼]

1. Introduction Proton exchange membrane fuel cell (PEMFC) catalysts are generally made of carbon black-supported Pt-based nanoparticles. However, carbon blacks do not display optimal properties for electrocatalysis: they may contain high amount of chemical impurities, are essentially microporous, and the final structure of the electrodes is hardly tunable, which may cause diffusional limitations within the catalytic layer [1]. A possible solution to these drawbacks is the use of synthetic nanostructured materials with a controllable and reproducible texture and with a pure, known and constant chemical composition; carbon xerogels (CX) exhibit such properties [2]. In addition, high Pt weight percentages are necessary to achieve high electrical performance with thin electrodes. Highly dispersed CX-supported Pt nanoparticles catalysts (Pt/CX) can be prepared by the strong electrostatic adsorption (SEA) method [3,4]. This method consists in impregnating the CX support by a solution of metal precursor at an optimum pH measured beforehand (2.4-2.5 for the impregnation of CX with H2PtCl6 [5]). If the conditions of synthesis are well controlled, the coulombic interactions between the support and the metal precursor are maximized. Metal nanoparticles are obtained after filtration, drying and reduction under hydrogen. However, achieving high Pt weight percentages requires multiple “impregnation-drying-reduction” cycles [4]. The use of large volumes of fresh 1 gPt L-1 solution for each impregnation step induces inacceptable Pt losses. In order to improve the synthesis efficiency, efforts were targeted so as to re-use the same, highly loaded Pt solution for several impregnation steps. The present study is focused on the synthesis and the characterization of Pt/CX nanoparticles by the “multiple SEA method” in view of testing and using them as PEMFC electrocatalysts. 2. Experimental The support used in this work was a CX prepared by drying and pyrolysis of a resorcinol-formaldehyde aqueous gel [6]. The pore size distribution of this CX was centred at 80 nm. After pyrolysis, the CX was crushed and sieved between 75 and 250 μm. To synthesize Pt/CX catalysts, 1 g of CX powder was first mixed with 567 mL of an H2PtCl6 solution at 8.97 mmol L-1 (i.e. 1.75 gPt L-1) with an initial pH of 2.5. The surface loading (SL), i.e. the total area of CX surface in solution, was equal to 1000 m² L-1 and the concentration of H2PtCl6 was chosen high enough to re-use the solution five times. After 1 h of stirring, the mixture was filtered and the filtrate was kept for re-use in another impregnation step. The solid was dried in an oven at 333 K during 12 h. Then, the dried material was reduced at 473 K under H2 flow (0.04 mmol s-1) during 1 h to obtain carbon-supported Pt nanoparticles. In order to synthesize several catalysts with various Pt weight percentages, the complete procedure was repeated one to five times on the same support. After the last impregnation, each catalyst was reduced at 723 K under H2 (0.04 mmol s-1) during 5 h to clean the surface of the Pt particles from chlorine residues [4]. The five catalysts are labelled according to the number of “impregnation-drying-reduction” cycles (e.g. Pt-2 for the catalyst obtained after two cycles). The Pt weight percentage of the catalysts was measured by inductively coupled plasma-atomic emission spectrometry (ICP-AES). The Pt particles were observed by transmission electron microscopy (TEM) and analysed by X-ray diffraction (XRD). The electro-active surface area of the Pt nanoparticles was measured by CO stripping voltammetry performed in 1 M sulphuric acid aqueous solution [7-9]. The specific activity of Pt particles for the Oxygen Reduction Reaction (ORR) was measured on a rotating disk electrode (RDE) in the same liquid electrolyte. 3. Results and discussion Table 1 summarizes some characteristics of the synthesized catalysts. The multiple SEA method leads to the synthesis of well dispersed Pt/CX catalysts with high Pt weight percentage, PtICP, which can be adjusted via the number of “impregnation-drying-reduction” cycles, and reaches 25 wt.% after five cycles. It is worth noting that the quantity of Pt deposited on the CX in one cycle, mPt, decreases after the first two cycles. This might be due to the successive impregnations in the acidic solution, the pH of which equals 2.4 - 2.5, and to the successive reduction steps: both procedures probably modify the surface chemistry of the CX, and leads to a shift of the optimal adsorption pH. This pH shift would induce a decrease in the amount of Pt deposited during the next cycles. This hypothesis remains under investigation. The analysis of TEM micrographs indicates that the five catalysts display the same mean Pt particle size, dTEM. This is corroborated by the comparison between the surface-averaged mean particle size, dS, and the CO equivalent diameter, dCO, or between the volume-averaged mean particle size, dV, and the average crystallite size calculated from XRD, dXRD. The values of the electroactive specific surface area of the Pt particles calculated from CO Journée scientifique GEPROC 2013 Procédés et Matériaux durables Université de Liège 15 novembre 2013 stripping, SCO, are the same for all the catalysts (ca. 95 m² gPt -1). The specific activity, SA, of the catalysts for the ORR is derived from the value of the Tafel plots and intercept. Fig. 1 shows that the Tafel plots are superimposed; as a result, the values of the specific activity at a given electrode potential are nearly identical for the five catalysts, and the Tafel slope, which is characteristic of the reaction mechanism, is almost constant as well (ca. -74 mV dec- 1). Since the specific activity depends on the average size of the Pt nanoparticles (the ORR is a structure-sensitive reaction), this result indicates that the number of impregnation sequences has no impact on the Pt nanoparticle size, and degree of agglomeration. 4. Conclusions The multiple SEA method allows obtaining well dispersed Pt/CX catalysts with high weight percentage up to 25 wt.%, and particle size close to ca. 2.5 nm. Studies are in progress to determine the maximum weight percentage that can be achieved without alteration of the metal dispersion. The multiple SEA method requires the use of less Pt than the SEA method from which it is inspired. Considering the synthesis of a 25 wt.% Pt/CX, the two methods require five “impregnation-drying-reduction” cycles but, for the SEA method, five solutions of 1gPt L-1 are used instead of only one solution of 1.75 gPt L-1, the latter being re-used in the case of multiple SEA. This difference leads to a nearly threefold decrease in the consumption of Pt. Further analyses will be performed so as to determine the optimal Pt weight percentage and the optimal thickness of the catalytic layer by modifying these two variables in a series of membrane-electrodes assemblies. [less ▲]

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See detailThe multiple SEA method: a method to synthesize Pt/carbon xerogel catalysts for Proton Exchange Membrane Fuel Cells (PEMFC)
Zubiaur, Anthony ULiege; Chatenet, Marian; Maillard, Frédéric et al

Poster (2013, April)

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