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Coupling experiment and simulation analysis to investigate physical parameters of CO2 methanation in a plasma catalytic hybrid process
Bo Wang Maria Mikhail Maria Elena Galvez Simeon Cavadias Michael Tatoulian Patrick Da Costa Stéphanie Ognier
First published - 17 9 - https://doi.org/10.1002/ppap.201900261 - 2020
This study focuses on the use of a heterogeneous catalyst Ni/Ce0.58Zr0.42O2 to study the Sabatier reaction in conventional catalytic thermal heating and the dielectric barrier discharge plasma‐catalytic process. Its aim is to study the threshold temperature of the Sabatier reaction in plasma conditions. A set of experiments with different inlet flow rates is carried out in a plasma reactor to investigate the steady‐state temperature of the reaction. To estimate the threshold temperature of the Sabatier reaction more accurately, the temperature difference between the catalytic bed and the external surface of the reactor is calculated and simulated in COMSOL Multiphysics® software. Finally, the threshold temperature of the Sabatier reaction during plasma processing is assumed to be 116°C, based on the experimental data and simulation analysis.
Electrocatalytic behaviour of CeZrOx-supported Ni catalysts in plasma assisted CO2 methanation
Maria Mikhail, Patrick Da Costa, Jacques Amouroux, Siméon Cavadias, Michael Tatoulian, Stéphanie Ognier and María Elena Gálvez
Catalys Science & Technology - 10 4532-4543 - https://doi.org/10.1039/D0CY00312C - 2020
Plasma-catalytic and thermo-catalytic methanation were assayed in the presence of a CeZrOx-supported Ni catalyst, proving that high CO2 conversions and high methane yields can be obtained under dielectric barrier discharge (DBD) plasma conditions and that they are maintained with time-on-stream over 100 h operating time. The characterization of the spent catalysts through TPD-MS, ATR-FTIR, TEM and HR-TEM and XRD evidenced the coexistence of a Ni0/NiO phase together with an increased presence of Ce3+ cations and oxygen vacancies, on the surface of the catalyst submitted to plasma catalytic operation. The different facts collected through physicochemical characterization point to our catalyst behaving like a PN junction, or like a fuel cell, with a P-side, the anode, i.e. the Ni-side releasing electrodes, while the CeZrOx support, N-side and cathode, acts as an acceptor. The DBD plasma, rich in ionic species and free electrodes, acts as the electrolyte, conducting the electrodes in the right direction. Oxygen accumulation on the surface of the catalyst during thermo-catalytic methanation leads to the formation of non-reactive adsorbed species, whereas Ni-sintering is favored. Under DBD plasma conditions, electron transfer is guaranteed and the adsorption–desorption of reactants and products is favored.
Ni-Fe layered double hydroxide derived catalysts for non-plasma and DBD plasma-assisted CO2 methanation
D Moreno, MV Ognier, S Motak, Grzybek, T Da Costa, P Galvez
Catalys Science & Technology - 45 17 - DOI: 10.1016/j.ijhydene.2019.06.095 - 2020
A series of bi-metallic layered double hydroxide derived materials, containing a fixed amount of Ni promoted with various amounts of Fe were obtained by co-precipitation. The synthesized materials were characterized by X-ray diffraction (XRD), temperature-programmed reduction (H 2-TPR), temperature-programmed desorption of CO 2 (CO 2-TPD), elemental analysis and low temperature N 2 sorption and tested as catalysts in CO 2 methanation at atmospheric pressure. The obtained results confirmed the formation of mixed nano-oxides after thermal decomposition of the precursor and suggest successful introduction of both nickel and iron into the layers of Layered Double Hydroxides (LDHs). The introduction of Fe into the layered double hydroxides changed the interaction between Ni and supports matrix as proven by temperature programmed reduction (H 2-TPR). The introduction of low amount of iron influenced positively the catalytic activity in CO 2 methanation at 250 C, with CO 2 conversion increasing from 21% to 72% with CH 4 selec-tivity ranging from 97 to 99% at 250 C. No other products, except CH 4 and CO were registered during the experiments. In order to enhance the catalytic activity a non-thermal plasma created by dielectric barrier discharge was applied. The obtained results prove that * Corresponding author.
Plasma deposited high density amines on surface using (3- aminopropyl)triethoxysilane for assembling particles at sub-nano size
Xi Rao , Ali Abou Hassan , Cédric Guyon , Stephanie Ognier , Michaël Tatoulian
Reaction Chemistry & Engineering - - DOI: 110.1016/j.matchemphys.2019.121974 - 2020
Although solid particles assembling on substrate surface is one of the key points for
developing membrane reactors, the technology of organizing nano/sub nanometer building
blocks into complex structures is still a challenge to scientists in years. In this work, amine
functional groups were deposited on the surface of different substrates via plasma enhanced
chemical vapor deposition (PECVD) technology and (3-aminopropyl)triethoxysilane
monomers were used as precursors. The influence of active gas, substrates, as well as
deposition time on the physico-chemical features of as-deposited film were investigated,
respectively. The highest density of amine of 5.5% on surface was obtained when Ar was
utilized as active gas and deposition time was 40 s. Furthermore, Y type zeolite particles at
sub-nano size were synthesized and subsequently used as a model material for testing the
immobilizing ability of plasma treated surface. The results clearly confirmed that a dense
mono or multi-layer of closely packed zeolite particles could be formed on the APTES as-
deposited surface after 24 hours’ immersion and the surface area of substrate could be
improved by the deposition of zeolite.
Amination of Cyclohexane by Dielectric Barrier Discharge Processing in a Continuous Flow Microreactor: Experimental and Simulation Studies
Aurélien Lepoetre, Stéphanie Ognier, Mengxue Zhang, Julien Wengler, Safwan Al Ayoubi, Cyril Ollivier, Louis Fensterbank, Xavier Duten, Michael Tatoulian
Plasma Chemistry and Plasma Processing - - DOI: 10.1007/s11090-020-10140-9 - 2020
A miniaturized flow device has been developed to combine microfluidics technology and plasma process. In this microreactor, atmospheric pressure dielectric barrier discharges are generated in a gas in contact with a liquid phase. This study was conducted with plasma generated in ammonia in contact with a flow of liquid cyclohexane. Cyclohexylamine was synthesized with a good selectivity, and the process can be implemented to improve conversion and effectiveness. Numerical simulations confirmed that NH2 radicals are generated in the plasma and react with cyclohexyls radicals to achieve the reaction, giving a selectivity of 50% and a total molar conversion of 20% of cyclohexane. The effects of voltage and frequency on the selectivity and the experimental conversion rate were studied and discussed.
Characterization of home-made graphite/PDMS microband electrodes for amperometric detection in an original reusable glass-NOA®-PDMS electrophoretic microdevice
J.Gouyon F.d’Orlyé S.Griveau F.Bedioui A.Varenne
Electrochimica Acta - 329 135164 - doi.org/10.1016/j.electacta.2019.135164 - 2020
A new dismountable and reusable microchip for electrophoretic separation coupled to amperometric detection was developed. For this purpose, a new home made three-microbands electrode system was developed and microfabricated based on screen-printing for the inclusion of graphite/polydimethylsiloxane (C-PDMS) composite in microchannels down to 30 μm width. The composition of the composite as well as the fabrication methodology were optimized for an easy handling and an optimized electrochemical behavior. The electrochemical characterization of this composite material was first performed in bulk format (disc-shaped electrode, 6 mm diameter). It was then transposed to the micrometric scale for its integration in an original glass-NOA81®-PDMS microfluidic device allowing for reversible sealing. The microband electrodes were characterized by scanning electron microcopy and cyclic voltammetry, illustrating a good control of the microelectrode width. Then, the analytical performances of the C-PDMS composite microelectrodes were evaluated using Ru(NH3)63+ and FcMeOH as model electroactive molecules. The electrophoretic separation and quantitation of Ru(NH3)63+ were then performed in a background electrolyte made of hydrochloric acid and sodium chloride, leading to a LOD and a LOQ of 3.4 μmol L−1 and 11.3 μmol L−1, respectively. The re-openable NOA-based microdevice permits to regenerate the electrode surface by simply repositioning the microband on a new spot, allowing for robust analysis in a reusable system.
Hydrogel Matrix-Grafted Impedimetric Aptasensors for the Detection of Diclofenac
G. S. Kassahun, S. Griveau, S. Juillard, J. Champavert, A. Ringuedé, B. Bresson, Y. Tran*, F. Bedioui, and C. Slim
Langmuir - 36(4) 827–836 - doi.org/10.1021/acs.langmuir.9b02031 - 2020
Driven by the growing concern about the release of untreated emerging pollutants and the need for determining small amounts of these pollutants present in the environment, novel biosensors dedicated to molecular recognition are developed. We have designed biosensors using a novel class of grafted polymers, surface-attached hydrogel thin films, on conductive transducers as a biocompatible matrix for biomolecule immobilization. We showed that they can be dedicated to the molecular recognition of diclofenac (DCL). The immobilization of the aptamer onto surface-attached hydrogel thin films by covalent attachment provides a biodegradable shelter, providing the aptamer with excellent environments to preserve its active and functional structure while allowing the detection of DCL. The grafting of the aptamer is obtained using the formation of amide bonds via the activation of carboxylic acid groups of the poly(acrylic acid) hydrogel thin film. For improved sensitivity and higher stability of the sensor, a high density of the immobilized aptamer is enabled. The aptamer-modified electrode was then incubated with DCL solutions at different concentrations. The performances of the aptasensor were investigated by electrochemical impedance spectroscopy. The change in charge-transfer resistance was found to be linear with DCL concentration in the 30 pM to 1 μM range. The detection limit was calculated to be 0.02 nM. The improvement of the limit of detection can be mainly attributed to the three-dimensional environment of the hydrogel matrix which improves the grafting density of the aptamer and the affinity of the aptamer to DCL.
Speciation and quantitation of precious metals in model acidic leach liquors, theoretical and practical aspects of recycling
Jérémie Gouyon, Fanny d’Orlyé, Julia Zimmerman, Sophie Griveau, Fethi Bedioui & Anne Varenne
Analytical and Bioanalytical Chemistry volume - 412 4595–4608 - doi.org/10.1007/s00216-020-02707-4 - 2020
Waste printed circuit boards are a major source of strategic materials such as platinum group metals since they are used for the fabrication of technological devices, such as hard drive discs, capacitors, and diodes. Because of the high cost of platinum, palladium, and gold (> 25 k€/kg), an economic and environmental challenge is their recycling from printed circuit boards that represent around 2% weight of electronic equipment. Hydrometallurgical treatments allow the recovery of these metals in solution, with a high recovery rate for a leaching liquor made of thiourea in hydrochloric acid. So as to develop an efficient recycling process from this leach liquor, one requires the speciation of these strategic metals, as well as their extraction and quantitation in the mixture. For this purpose, platinum, palladium, and gold were dissolved in model leach liquors made of hydrochloric acid and thiourea at low concentration. The identification of metal complexes was determined as a function of thiourea concentration (between 10 μmol/L and 10 mmol/L) by the combination of UV-visible spectrometry, cyclic voltammetry, and for the first time capillary electrophoresis. The electrokinetic method was then applied for the quantitation of trace metal analyses in leach samples from waste printed circuit boards reprocessing, demonstrating its applicability for industrializable recycling applications.

Reversible microfluidics device for precious metal electrodeposition and depletion yield studies
Jérémie Gouyon Fanny d’Orlyé Craig Simon Sophie Griveau Catherine Sella Laurent Thouin Fethi Bediouia Anne Varenne
Electrochimica Acta - 352 136474 - doi.org/10.1016/j.electacta.2020.136474 - 2020
A new low-cost reversible Glass-NOA®-PDMS microfluidic device was designed for the study of recovery yield of precious metals present in acid media mimicking leach liquors for long-term recycling objectives. It offers the unique advantage of allowing easy washing of the microchannel and renewal of the electrode surface by simply repositioning the microband electrodes which allows this type of device to have a relatively much longer lifespan than irreversibly closed ones. It consists in a re-useable microchip with four graphite microbands electrodes, prepared by screen printing, to set-up an original amperometric device for both depletion and yield quantification. One upstream working electrode is devoted to the depletion of the metallic ions through their electrolysis by electrodeposition while the second downstream working microelectrode is used as real-time detection electrode to evaluate the depletion efficiency. The dimensions of the depletion electrode and of the channel were optimized thanks to numerical simulations for a given range of flow velocities. First, the performances of the device were assessed experimentally according to flow rate and applied potential under continuous flow, and then compared to theoretical predictions using an electrochemical probe, ferrocenemethanol. The proof of concept was then demonstrated for precious metal, by electroreduction of Pd(II) and Au(III) from acidic leach liquors under continuous flow, with a depletion yield of up to 89% and 71% respectively.
Multiple Zones Modification of Open Off-Stoichiometry Thiol-Ene Microchannel by Aptamers: A Methodological Study & A Proof of Concept
Samantha Bourg, Fanny d’Orlyé, Sophie Griveau, Fethi Bedioui, Jose Alberto Fracassi da Silva, andAnne Varenne.
Electrochimica Acta - 8(2) 24 - doi.org/10.3390/chemosensors8020024 - 2020
Off-stoichiometry thiol-ene polymer (OSTE) is an emerging thermoset with interesting properties for the development of lab-on-a-chip (LOAC), such as easy microfabrication process, suitable surface chemistry for modification and UV-transparency. One of the challenges for LOAC development is the integration of all the analytical steps in one microchannel, and particularly, trace level analytes extraction/preconcentration steps. In this study, two strategies for the immobilization of efficient tools for this purpose, thiol-modified (C3-SH) aptamers, on OSTE polymer surfaces were developed and compared. The first approach relies on a direct UV-initiated click chemistry reaction to graft thiol-terminated aptamers on ene-terminated OSTE surfaces. The second strategy consists of the immobilization of thiol-terminated aptamers onto OSTE substrates covered by gold nanoparticles. The presence of an intermediate gold nanoparticle layer on OSTE has shown great interest in the efficient immobilization of aptamers, preserving their interaction with the target, and preventing non-specific adsorption. With this second innovative strategy, we proved, for the first time the concept of creating multiple functional zones for sample treatment in an open OSTE-microchannel thanks to the immobilization of aptamers in consecutive areas by the simple droplet deposition methodology. This methodological development allows further consideration of OSTE material for lab-on-a-chip designs, integrating multiple zones for sample pretreatment, based on molecular recognition by ligands, such as aptamers, in a specific zone of the microchannel and is adaptable to a large range of analytical applications for LOAC industrialization. View Full-Text

606 publications.