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2016

Articles:

Turgis, R., Arrachart, G., Dubois, V., Dourdain, S., Virieux, D., Michel, S., Legeai, S., Lejeune, M., Draye, M. and Pellet-Rostaing, S.
Dalton Transactions, 45(Copyright (C) 2016 American Chemical Society (ACS). All Rights Reserved.):1259-1268
2016

Resume: The extn. of rare earth elements (REEs) from nitric acid soln. with a triphosphine trioxide (TPO) is presented. Performances of such a ligand in ionic liqs. vs. a classical solvent (benzyl ether) are compared. TPO seems to be 10 to 100 times more efficient when it is dissolved in ionic media whatever the concn. of nitric acid involved. Mechanistic investigations reveal that cation exchange classically obsd. in ionic liqs. is not consistent with the exptl. data. Moreover, clear differences in the TPO/Ln complexes between classical and ionic media are highlighted. A stable complex of 1 lanthanide for 3 TPO is formed in an ionic liq. whereas a complex of 1 lanthanide for 6 to 9 TPO is formed in benzyl ether. Back extn. is also studied and good recovery of REEs could be obtained. The TPO/ionic liq. system shows remarkable performances i.e. efficiency and selectivity towards lanthanides in a simulated leaching soln. of a Nd/Fe/B/Dy magnet. [on SciFinder(R)]

Equipe: Département CP2S : Chimie et électrochimie des matériaux

2015

Articles:

Braghiroli, F. L., Fierro, V., Szczurek, A., Stein, N., Parmentier, J. and Celzard, A.
Ind. Crops Prod., 70:332-340
2015

Resume: Six porous carbon materials, produced by hydrothermal treatment of flavonoid tannin and subsequent carbonization at 1173 K, were tested as electrodes of supercapacitors. Four of these carbons were doped with nitrogen by putting tannin in contact with ammonia before or during the hydrothermal treatment. The pyrolyzed hydrothermal carbons had moderate surface areas, within the range 442-684 m2 g-1, and nitrogen contents ranging from 0.7 to 8.0 wt.%. Specific capacitances as high as 320 F g-1 and normalized capacitances as high as 58 ?F cm-2 were measured at 2 mV s-1. These performances are comparable with those obtained with high surface area-activated carbons, whereas, normalized capacitances values are among the highest ever reported. Mesostructuration, within the range 3-13 nm, of these materials appears to be a good strategy to improve their electrochem. performances at higher scan rates. We confirmed the beneficial role of oxygen up to 18 wt.%, while an optimum in nitrogen content exists from 3 to 6 wt.%. [on SciFinder(R)]

Equipe: Département CP2S : Chimie et électrochimie des matériaux

Braghiroli, F. L., Fierro, V., Szczurek, A., Stein, N., Parmentier, J. and Celzard, A.
Carbon, 90(0):63-74
2015

Resume: Abstract Aminated tannin submitted to hydrothermal treatment led to nitrogen-doped gels in the absence of any cross-linker. Such gels were subcritically dried, freeze-dried or supercritically dried to obtain organic xerogels, cryogels and aerogels, respectively, having nitrogen contents between 3.0 and 3.7 wt.%. After pyrolysis at 900 °C, the materials presented nitrogen contents ranging from 1.9 to 3.0 wt.%, and surface areas as high as 860, 754 and 585 m2 g?1 for carbon aerogels, cryogels and xerogels, respectively. All of them displayed micropores associated with different mesopore volumes, depending on both the drying method and initial dilution of the precursor. When tested as supercapacitor electrodes, these carbon gels presented outstanding specific and normalised capacitances, up to 387.6 F g?1 and 69.5 ?F cm?2, respectively, at a scan rate of 2 mV s?1 in 4 mol L?1 H2SO4 aqueous solution. These performances are higher than those obtained with high apparent surface area-activated carbons, as the measured capacitances are indeed among the highest ever reported. The influence of nitrogen- and oxygen-based moieties was investigated, and optimal N and O contents of 2–3 and 17–18 wt.%, respectively, were observed.

Equipe: Département CP2S : Chimie et électrochimie des matériaux

Escande, Vincent, Petit, Eddy, Garoux, Laetitia, Boulanger, Clotilde and Grison, Claude
ACS Sustainable Chemistry & Engineering,
2015

Resume: A novel Mn-derived catalyst was prepared starting from biomass of Mn-hyperaccumulating plants growing on metal-rich soils. Recovery of this biomass as value-added ?ecocatalysts? provides incentives for the development of phytoextraction programs on soils degraded by mining activities. Characterization of the resulting plant-based ?Eco-Mn?? catalyst by inductively coupled plasma mass spectrometry (ICP-MS), X-ray diffraction (XRD), X-ray fluorescence spectrometry (XRF) and X-ray photoelectron spectroscopy (XPS) demonstrated the presence of unusual polymetallic complexes of Mn(II) in the catalyst, along with Fe(III). Incorporation of these species into montmorillonite K10 as solid support provided a supported Eco-Mn? catalyst, whose properties were investigated for alkene epoxidation with H2O2 (30 wt%)/NaHCO3 (0.2 M) as a green terminal oxidizing reagent. The supported Eco-Mn? catalyst demonstrated a high efficiency for styrene epoxidation, with only 0.31 mol% of Mn, a much lower content of Mn than in previously described Mn-derived heterogeneous catalysts. Whereas Fe was also present in the supported Eco-Mn? catalyst, comparison experiments showed that Fe had only a limited role in the catalysis. The water content in the reaction medium had a beneficial effect, increasing the reaction efficiency. The supported Eco-Mn? catalyst was recycled four times without any loss of activity. Comparison of its properties to those of heterogeneous catalysts made by incorporation of commercial MnCl2.4H2O and FeCl3.6H2O highlighted the superior catalytic activity of polymetallic species present in the biosourced catalyst. The substrate scope of the method was extended to various alkenes, including bulky natural products, which were epoxidized with high yields (up to 99%), sometimes much higher than those obtained with already described Mn-derived heterogeneous catalysts. Finally, by simple adjustments of reaction conditions, the method allowed controlled access to aldehydes by oxidative cleavage of various styrene-derived substrates (up to 93% yield). The method thus constitutes a valuable alternative not only to classical epoxidation reagents, but also to oxidative cleavage of styrene-derived molecules, which usually involves toxic and hazardous reagents.

Equipe: Département CP2S : Chimie et électrochimie des matériaux

2014

Articles:

Turgut, C., Sinha, G., Mether, L., Lahtinen, J., Nordlund, K., Belmahi, M. and Philipp, P.
Analytical Chemistry, 86:11217-11225
2014

Equipe: Département CP2S : Expériences et Simulations des Plasmas Réactifs - Interaction plasma-surface et Traitement des Surfaces ESPRITS

ZHOU, T., COLIN, M., CANDOLFI, C., Boulanger, C., DAUSCHER, A., Santava, E., HEJTMANEK, J., BARANEK, P., AL RAHAL AL ORABI, R., POTEL, M., Fontaine, B., GOUGEON, P., Gautier, R. and LENOIR, B.
Chemistry of Materials, 26(16):4765-4775
2014

Resume: We present a detailed study of the evolution of the electrical, galvanomagnetic, and thermodynamic properties of polycrystalline AgxMo9Se11 compounds for 3.4 ? x ? 3.8 at low temperatures (2?350 K). In agreement with density functional theory calculations, the collected data show an overall gradual variation in the transport properties from metallic to semiconducting behavior on going from x = 3.4 to 3.8. The results evidence subtle variations in the electronic properties with the Ag content, typified by both positive and negative phonon-drag effects together with thermopower and Hall coefficient of opposite signs. Analysis of the data suggests that these features may be due to peculiarities of the dispersion of the valence bands in the vicinity of the chemical potential. A drastic influence of the Ag content on the thermal transport was evidenced by a pronounced change in the temperature dependence of the specific heat below 10 K. Nonlinearities in the Cp(T3) data are correlated to the concentration of Ag atoms, with an increase in x resulting in a more pronounced departure from a Debye law. The observed behavior mirrors that of ionic conductors, suggesting that AgxMo9Se11 for x ? 3.6 might belong to this class of compounds.

Equipe: Département CP2S : Chimie et électrochimie des matériaux

Jana, A., Briquet, L., WIRTZ, T., Philipp, P. and Henrion, G.
Nuclear Instruments and Methods in Physics Research B: Beam Interactions with Materials and Atoms, 326:341-344
2014

Resume: The deposition of multiple carbon atoms on a crystalline silicon (Si) surface is modelled at 5 eV energy by using molecular dynamics simulations combined with a third generation force field that includes bond breaking and formation. Force field parameters are taken from a previous work. These simulations allow for atomic scale insights into the deposition mechanisms and an easier comparison with experimental observations. The results, including distributions of implantation depth, carbon concentrations, sticking coefficients, radial distribution function, and angular distributions are compared for different incidence angles. Due to the deposition of carbon atoms inside the silicon structure, silicon carbide starts to form. The crystalline structure has been investigated for different conditions to get a better understanding of the damaging and growth mechanisms. It is found that a lot of deformation is accumulated in the area of deposition near to the surface but underneath the surface the silicon has still a more crystalline structure. The variation of the silicon (carbide) structu re slightly depends on the angle of incidence. For the conditions used for these simulations, the sticking probability is always high and varies between 95% and 100%, which can be attributed to the high affinity of carbon for silicon.

Equipe: Département CP2S : Expériences et Simulations des Plasmas Réactifs - Interaction plasma-surface et Traitement des Surfaces ESPRITS

Wang, Y., Ghanbaja, J., SOLDERA, F., Boulet, P., Horwat, D., MUECKLICH, F. and Pierson, J. F.
ACTA MATERIALIA, 76:207-212
2014
ISSN: 1359-6454

Equipe: Centre de Compétences : X-Gamma rayons X et spectroscopie

Mangin, S., Gottwald, M., Lambert, C.-H., Steil, D., Uhlír, V., Pang, L., Hehn, M., Alebrand, S., Cinchetti, M., Malinowski, G., Fainman, Y., Aeschlimann, M. and Fullerton, E.E.
Nature Materials, 13(3):286-292
2014

Equipe: Département P2M : Nanomagnétisme et Electronique de Spin

Turgut, C., WIRTZ, T., Belmahi, M. and Philipp, P.
Surface and Interface Analysis, 46:357-359
2014

Equipe: Département CP2S : Expériences et Simulations des Plasmas Réactifs - Interaction plasma-surface et Traitement des Surfaces ESPRITS

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