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8. Revealing the origin of chemical complexity in extraterrestrial matter by combining multiple characterization techniques: HR-L2MS, TOF-SIMS, and micro-Raman spectroscopy: Invited talk

Author

Pirim, Claire, Dumitru, Duca, Slavicinska, Katerina, Ferrari, Brian, Carpentier, Yvain, Vojkovic, Marin, Chazallon, Bertrand, Focsa, Cristian, Bennett, Christopher J., Laboratoire de Physique des Lasers, Atomes et Molécules - UMR 8523 (PhLAM), Université de Lille-Centre National de la Recherche Scientifique (CNRS), Physique Moléculaire aux Interfaces (PMI), Université de Lille-Centre National de la Recherche Scientifique (CNRS)-Université de Lille-Centre National de la Recherche Scientifique (CNRS), and University of Central Florida [Orlando] (UCF)

Subjects
[CHIM.THEO]Chemical Sciences/Theoretical and/or physical chemistry, [PHYS]Physics [physics], Astrochemistry -meteorites, [SDU]Sciences of the Universe [physics], Mass spectrometry imaging techniques, Micro-Raman Spectroscopy, Laser desorption ionization mass spectrometry, [PHYS.PHYS.PHYS-CHEM-PH]Physics [physics]/Physics [physics]/Chemical Physics [physics.chem-ph], Secondary ion mass spectrometry SIMS, ComputingMilieux_MISCELLANEOUS
Abstract

International audience

Published
2021

9. Multi-technique physico-chemical characterization of particles generated by a gasoline engine: Towards measuring tailpipe emissions below 23 nm

Author

Noble, J.A., Betrancourt, C., Tritscher, T., Spielvogel, J., Rahman, M., Boies, A., Lee, K.F., Bhave, A.N., Legendre, S., Lancry, O., Kreutziger, P., Rieker, M., Minutolo, Patrizia, Commodo, Mario, D’Anna, Andrea, Nuns, Nicolas, Desgroux, Pascale, Mercier, Xavier, Ngo, Linh Dan, Duca, Dumitru, Carpentier, Yvain, Noble, Jennifer, Ikhenazene, Raouf, Vojkovic, Marin, Irimiea, Cornelia, Ortega, Ismael, Lefevre, Guillaume, Yon, Jérôme, Faccinetto, Alessandro, Therssen, Eric, Ziskind, Michael, Chazallon, Bertrand, Pirim, Claire, Focsa, Cristian, Laboratoire de Physique des Lasers, Atomes et Molécules - UMR 8523 (PhLAM), Université de Lille-Centre National de la Recherche Scientifique (CNRS), Physique Moléculaire aux Interfaces (PMI), Université de Lille-Centre National de la Recherche Scientifique (CNRS)-Université de Lille-Centre National de la Recherche Scientifique (CNRS), Physicochimie des Processus de Combustion et de l’Atmosphère - UMR 8522 (PC2A), Laboratory of Atmospheric Chemistry [Paul Scherrer Institute] (LAC), Paul Scherrer Institute (PSI), International Islamic University Malaysia [Kuala Lumpur], HORIBA Scientific [France], Laboratoire Avancé de Spectroscopie pour les Intéractions la Réactivité et l'Environnement - UMR 8516 (LASIRE), Institut de Chimie du CNRS (INC)-Université de Lille-Centre National de la Recherche Scientifique (CNRS)-Centrale Lille Institut (CLIL), ANR-11-LABX-0005,Cappa,Physiques et Chimie de l'Environnement Atmosphérique(2011), Centre National de la Recherche Scientifique (CNRS)-Université de Lille, Institut de Chimie du CNRS (INC)-Université de Lille-Centre National de la Recherche Scientifique (CNRS), Institut des Sciences Moléculaires (ISM), Université Montesquieu - Bordeaux 4-Université Sciences et Technologies - Bordeaux 1-École Nationale Supérieure de Chimie et de Physique de Bordeaux (ENSCPB)-Centre National de la Recherche Scientifique (CNRS), International Centre for Diarrhoeal Disease Research, International Centre for Diarrhoeal Disease Research, Bangladesh (ICDDR,B), Laboratoire de Spectrochimie Infrarouge et Raman - UMR 8516 (LASIR), Université de Lille, Sciences et Technologies, DMPE, ONERA, Université Paris Saclay (COmUE) [Palaiseau], Université Paris Saclay (COmUE)-ONERA, Complexe de recherche interprofessionnel en aérothermochimie (CORIA), Université de Rouen Normandie (UNIROUEN), Normandie Université (NU)-Normandie Université (NU)-Institut national des sciences appliquées Rouen Normandie (INSA Rouen Normandie), and Normandie Université (NU)-Institut National des Sciences Appliquées (INSA)-Institut National des Sciences Appliquées (INSA)-Centre National de la Recherche Scientifique (CNRS)

Subjects
Atmospheric Science, 010504 meteorology & atmospheric sciences, [SDE.MCG]Environmental Sciences/Global Changes, Internal combustion engine, Nanoparticles, Physico-chemical characterization, Mass spectrometry, Emission modeling, Context (language use), 010501 environmental sciences, 01 natural sciences, 7. Clean energy, Ultrafine particle, Process engineering, Gasoline direct injection, ComputingMilieux_MISCELLANEOUS, 0105 earth and related environmental sciences, General Environmental Science, Petrol engine, [PHYS.PHYS.PHYS-AO-PH]Physics [physics]/Physics [physics]/Atmospheric and Oceanic Physics [physics.ao-ph], [PHYS.PHYS]Physics [physics]/Physics [physics], [CHIM.ORGA]Chemical Sciences/Organic chemistry, business.industry, Particulates, Characterization (materials science), 13. Climate action, Environmental science, Particle, [PHYS.PHYS.PHYS-CHEM-PH]Physics [physics]/Physics [physics]/Chemical Physics [physics.chem-ph], business
Abstract

Particulate emissions from on-road motor vehicles are the focus of intensive current research due to the impact of the ambient particulate matter (PM) levels on climate and human health. Constant improvement in engine technology has led to significant decrease in the number and mass of emitted PM, but particular concern is raised nowadays by the ultrafine particles. In this context, there is a critical lack of certification procedures for the measurement of the smallest-size ( 23 nm) particulate matter emissions. To support the engine development process as well as future certification procedures, a measurement technology for sub-23 nm particles must be designed. The development of a reliable measurement procedure entails understanding the formation and evolution of particles from the engine to the tailpipe via multiple analytical techniques and theoretical simulations. We present here extensive experimental characterization of ultrafine particles emitted by a gasoline direct injection single-cylinder engine as particle generator. The particles were sampled using a cascade impactor which allows size-separation into 13 different size bins. Chemical characterization of the collected size-selected particles was performed using mass spectrometry, which gives access to detailed molecular information on chemical classes of critical interest such as organosulphates, oxygenated hydrocarbons, nitrogenated hydrocarbons, metals, or polycyclic aromatic hydrocarbons. Additionally, the morphology of the emitted particles was probed with atomic force (AFM) and scanning electron microscopy (SEM). Tip-Enhanced Raman Spectroscopy (TERS) was applied for the first time to sub-10 nm combustion-generated particles to gather information on their nanostructure. The extensive database built from these multiple experimental characterizations has been used as input of a theoretical approach to simulate and validate engine out-emissions. These studies were performed in the framework of the H2020 PEMS4Nano project which aims to the development of a robust, reliable and reproducible measurement technology for particles down to 10 nm for both chassis dyno and real driving emissions (RDE).

Published
2020
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11. Micro-Raman investigations of the formaldehyde-ice system

Author

Chazallon, Bertrand, Lebrun, Nathalie, Toubin, Celine, and Focsa, Cristian

Subjects
Formaldehyde -- Thermal properties, Raman effect -- Research, Chemicals, plastics and rubber industries
Abstract

The study investigated the effects of freezing on the water-formaldehyde system for different concentrations and to establish related information on ice-formaldehyde interactions by using Raman spectroscopy. From the subtle changes of the bands assigned to the CO and CH group frequencies, at least two distinct crystalline phases are found to coexist with ice at different temperatures.

Published
2005

13. Hundreds of meter-long low-loss silicon-core optical fiber

Author

Kudinova, Maryna, primary, Bouwmans, Géraud, additional, Habert, Rémi, additional, Plus, Stéphane, additional, Baudelle, Karen, additional, Bernard, Rémy, additional, Chazallon, Bertrand, additional, Cassez, Andy, additional, El Hamzaoui, Hicham, additional, Vanvincq, Olivier, additional, Troles, Johann, additional, and Bigot, Laurent, additional

Published
2020
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14. Chemical discrimination of the particulate and gas phases of miniCAST exhausts using a two-filter collection method

Author

Ngo, Linh Dan, primary, Duca, Dumitru, additional, Carpentier, Yvain, additional, Noble, Jennifer A., additional, Ikhenazene, Raouf, additional, Vojkovic, Marin, additional, Irimiea, Cornelia, additional, Ortega, Ismael K., additional, Lefevre, Guillaume, additional, Yon, Jérôme, additional, Faccinetto, Alessandro, additional, Therssen, Eric, additional, Ziskind, Michael, additional, Chazallon, Bertrand, additional, Pirim, Claire, additional, and Focsa, Cristian, additional

Published
2020
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15. Ge-Sb-Te Chalcogenide Thin Films Deposited by Nanosecond, Picosecond, and Femtosecond Laser Ablation

Author

Bulai, Georgiana, Pompilian, Oana, Gurlui, Silviu, Němec, Petr, Nazabal, Virginie, Cimpoesu, Nicanor, Chazallon, Bertrand, Focsa, Cristian, Bulai, Georgiana, Pompilian, Oana, Gurlui, Silviu, Němec, Petr, Nazabal, Virginie, Cimpoesu, Nicanor, Chazallon, Bertrand, and Focsa, Cristian

Abstract

Ge-Sb-Te thin films were obtained by ns-, ps-, and fs-pulsed laser deposition (PLD) in various experimental conditions. The thickness of the samples was influenced by the Nd-YAG laser wavelength, fluence, target-to-substrate distance, and deposition time. The topography and chemical analysis results showed that the films deposited by ns-PLD revealed droplets on the surface together with a decreased Te concentration and Sb over-stoichiometry. Thin films with improved surface roughness and chemical compositions close to nominal values were deposited by ps- and fs-PLD. The X-ray diffraction and Raman spectroscopy results showed that the samples obtained with ns pulses were partially crystallized while the lower fluences used in ps- and fs-PLD led to amorphous depositions. The optical parameters of the ns-PLD samples were correlated to their structural properties., Tenké vrstvy Ge-Sb-Te byly získány ns, ps a fs pulzní laserovou depozicí (PLD) za různých experimentálních podmínek. Tloušťka vrstev byla ovlivněna vlnovou délkou Nd-YAG laseru, hustotou energie, vzdáleností mezi terčem a substrátem a depozičním časem. Výsledky topografie a chemická analýza ukázaly, že vrstvy připravené ns PLD obsahují kapky na povrch a nižší koncentraci Te a nadstechiometrii Sb. Tenké vrstvy s lepší povrchovou drsností a chemickým složením blízkým nominálním hodnotám byly deponovány ps a fs PLD. Výsledky rentgenové difrakce a Ramanovy spektroskopie ukázaly, že vzorky získané ns pulzy byly částečně krystalické, zatímco nižší hustoty energie použité při ps a fs PLD vedly k amorfním vrstvám. Optické parametry vzorků připravených ns PLD byly korelovány s jejich strukturními vlastnostmi.

Published
2020

16. Particulate and Gas Phase Separation in Simultaneous Sampling of Combustion Byproducts: New Insights into Chemical Composition by Mass Spectrometric Analysis

Author

Noble, Jennifer, Ngo, Linhdan, Dumitru, Duca, Vojkovic, Marin, Raouf Ikhenazene, Abd, Irimiea, Cornelia, Lefevre, Guillaume, Faccineto, Alessandro, Pirim, Claire, Carpentier, Yvain, Therssen, Eric, Chazallon, Bertrand, Nuns, Nicolas, Yon, Jerôme, Focsa, Cristian, Institut des Sciences Moléculaires (ISM), Université Montesquieu - Bordeaux 4-Université Sciences et Technologies - Bordeaux 1-École Nationale Supérieure de Chimie et de Physique de Bordeaux (ENSCPB)-Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS), Physicochimie des Processus de Combustion et de l’Atmosphère - UMR 8522 (PC2A), Université de Lille-Centre National de la Recherche Scientifique (CNRS), Institut Lumière Matière [Villeurbanne] (ILM), Centre National de la Recherche Scientifique (CNRS)-Université Claude Bernard Lyon 1 (UCBL), Université de Lyon-Université de Lyon, Laboratoire de Physique des Lasers, Atomes et Molécules - UMR 8523 (PhLAM), Institut des Molécules et de la Matière Condensée de Lille (IMMCL), Centrale Lille Institut (CLIL)-Centre National de la Recherche Scientifique (CNRS)-Université de Lille, Sciences et Technologies, Complexe de recherche interprofessionnel en aérothermochimie (CORIA), Centre National de la Recherche Scientifique (CNRS)-Institut national des sciences appliquées Rouen Normandie (INSA Rouen Normandie), Institut National des Sciences Appliquées (INSA)-Normandie Université (NU)-Institut National des Sciences Appliquées (INSA)-Normandie Université (NU)-Université de Rouen Normandie (UNIROUEN), Normandie Université (NU), Université Montesquieu - Bordeaux 4-Université Sciences et Technologies - Bordeaux 1 (UB)-École Nationale Supérieure de Chimie et de Physique de Bordeaux (ENSCPB)-Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS), Université Claude Bernard Lyon 1 (UCBL), Université de Lyon-Université de Lyon-Centre National de la Recherche Scientifique (CNRS), Université de Lille, Sciences et Technologies-Centrale Lille-Centre National de la Recherche Scientifique (CNRS), Université de Rouen Normandie (UNIROUEN), Normandie Université (NU)-Normandie Université (NU)-Institut national des sciences appliquées Rouen Normandie (INSA Rouen Normandie), and Institut National des Sciences Appliquées (INSA)-Normandie Université (NU)-Institut National des Sciences Appliquées (INSA)-Centre National de la Recherche Scientifique (CNRS)

Subjects
[SPI.FLUID]Engineering Sciences [physics]/Reactive fluid environment, ComputingMilieux_MISCELLANEOUS
Abstract

International audience

Published
2018

18. Supplementary material to "Chemical discrimination of the particulate and gas phases of miniCAST exhausts using a two-filter collection method"

Author

Ngo, Linh Dan, primary, Duca, Dumitru, additional, Carpentier, Yvain, additional, Noble, Jennifer A., additional, Ikhenazene, Raouf, additional, Vojkovic, Marin, additional, Irimiea, Cornelia, additional, Ortega, Ismael K., additional, Lefevre, Guillaume, additional, Yon, Jérôme, additional, Faccinetto, Alessandro, additional, Therssen, Eric, additional, Ziskind, Michael, additional, Chazallon, Bertrand, additional, Pirim, Claire, additional, and Focsa, Cristian, additional

Published
2019
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19. Chemical discrimination of the particulate and gas phases of miniCAST exhausts using a two-filter collection method

Author

Ngo, Linh Dan, primary, Duca, Dumitru, additional, Carpentier, Yvain, additional, Noble, Jennifer A., additional, Ikhenazene, Raouf, additional, Vojkovic, Marin, additional, Irimiea, Cornelia, additional, Ortega, Ismael K., additional, Lefevre, Guillaume, additional, Yon, Jérôme, additional, Faccinetto, Alessandro, additional, Therssen, Eric, additional, Ziskind, Michael, additional, Chazallon, Bertrand, additional, Pirim, Claire, additional, and Focsa, Cristian, additional

Published
2019
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22. In situ structural properties of N[sub 2]-, O[sub 2]-, and air-clathrates by neutron diffraction.

Author

Chazallon, Bertrand and Kuhs, Werner F.

Subjects
*NEUTRON diffraction, *HYDRATES, *COMPRESSIBILITY, *CHEMICAL structure
Abstract

The crystal structures of type II N[sub 2-], O[sub 2-], and air-clathrate hydrates have been studied under their thermodynamic conditions of stability by neutron powder diffraction. The isothermal compressibilities were deduced from the refined lattice constants and found to be significantly different for N[sub 2] and O[sub 2] clathrate hydrates. The water host lattice structure rearranges as a function of pressure with a resulting change of the volume ratio of small and large cages. The cage fillings were established on an absolute scale for the first time. The large cages were found to be partly occupied by two molecules. The results are compared with predictions based on the statistical thermodynamic theory of van der Waals and Platteeuw. While the filling follows the predicted trend significant differences exist in detail. [ABSTRACT FROM AUTHOR]

Published
2002
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23. Gas hydrate technology: state of the art and future possibilities for Europe

Author

Klar, Assaf, Deerberg, Dipl.-Ing Georg Janicki, Schicks, Judith, Minshull, Timothy, Riedel, Michael, Fietzek, Peer, Mosch, Thomas, Tinivella, Umberta, De, Maria, La Fuente Ruiz, Gatt, Peter, Schwalenberg, Katrin, Schwalenberg@Bgr, Katrin, De, Katja, Heeschen, Joerg Bialas, Pinkert, Shmulik, Tang, Anh Minh, Kvamme, Bjorn, Erik@Gfz-Potsdam, Erik Spangenberg, English, Niall, Chazallon Bertrand, Parlaktuna, Mahmut, Sourav Kumar, and Wallmann, Klaus

Published
2017
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25. Measuring non-volatile particles properties in the exhaust of an aircraft engine

Author

Ortega, Ismael, Delhaye, David, Ouf, Francois-Xavier, Ferry, Daniel, Focsa, Christian, Irimiea, Cornelia, Carpentier, Yvain, Chazallon, Bertrand, Parent, Philippe, Laffon, Carine, Penanhoat, Olivier, Harivel, Nadine, Gaffie, Daniel, Vancassel, Xavier, ONERA - The French Aerospace Lab [Palaiseau], ONERA-Université Paris Saclay (COmUE), Institut de Radioprotection et de Sûreté Nucléaire (IRSN), Centre Interdisciplinaire de Nanoscience de Marseille (CINaM), Aix Marseille Université (AMU)-Centre National de la Recherche Scientifique (CNRS), Laboratoire de Physique des Lasers, Atomes et Molécules - UMR 8523 (PhLAM), Université de Lille-Centre National de la Recherche Scientifique (CNRS), Snecma-SAFRAN group, and ONERA - The French Aerospace Lab [Châtillon]

Subjects
SOOT, 13. Climate action, PARTICULATE MATTER, PARTICULE, MOTEUR AVION, [SPI.FLUID]Engineering Sciences [physics]/Reactive fluid environment, AIRCRAFT ENGINE EMISSIONS, NVPM, MESURE, MEASUREMENTS, EMISSION, 7. Clean energy, SUIE
Abstract

The steady growth of air traffic and its foreseen expansion during future years have raised concerns about its potential impact on climate and ground-level air quality. So far, the smoke number has been used to evaluate the non-volatile particulate matter amount emitted by aircraft engines, but it is a poor proxy for modern engine emissions. Therefore, new sampling and measurement techniques have recently been tested on aircraft engine emissions, especially as a new ICAO particle emission standard is currently being developed. Number and mass of emitted particles are generally used, but are not sufficient to fully characterize soot emissions and further address atmospheric impact issues. Chemical composition is crucial to evaluate their atmospheric reactivity. This paper presents a complete set of techniques that have been used to characterize soot emissions from an aircraft engine in a comprehensive manner. It reports results from a campaign on a PowerJet SaM146 engine, performed within the framework of the MERMOSE (Mesure et Etude de la Reactivite des emissions de MOteurS aEronautiques) project. It emphasizes the influence of the engine regime, ranging from 30% to 100% of the takeoff thrust, on the various particle properties investigated, including the size, number, morphology and chemical composition., AerospaceLab Journal, Issue 11, June 2016; ISSN: 2107-6596

Published
2016
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29. Chemical discrimination of the particulate and gas phases of miniCAST exhausts using a two-filter collection method.

Author

Ngo, Linh Dan, Duca, Dumitru, Carpentier, Yvain, Noble, Jennifer A., Ikhenazene, Raouf, Vojkovic, Marin, Irimiea, Cornelia, Ortega, Ismael K., Lefevre, Guillaume, Yon, Jérôme, Faccinetto, Alessandro, Therssen, Eric, Ziskind, Michael, Chazallon, Bertrand, Pirim, Claire, and Focsa, Cristian

Subjects
SECONDARY ion mass spectrometry, QUARTZ, POLYCYCLIC aromatic hydrocarbons, CARBONACEOUS aerosols, ATMOSPHERIC chemistry, CRYSTAL filters, SURFACE chemistry
Abstract

Combustion of hydrocarbons produces both particulate and gas phase emissions responsible for major impacts on atmospheric chemistry and human health. Ascertaining the impact of these emissions, especially on human health, is not straightforward because of our relatively poor knowledge of how chemical compounds are partitioned between the particle and gas phases. Accordingly, we propose to couple a two-filter sampling method with a multi-technique analytical approach to fully characterize the particulate and gas phase compositions of combustion by-products. The two-filter sampling method is designed to retain particulate matter (elemental carbon possibly covered in a surface layer of adsorbed molecules) on a first quartz fiber filter while letting the gas phase pass through, and then trap the most volatile components on a second black carbon-covered filter. All samples thus collected are subsequently subjected to a multi-technique analytical protocol involving two-step laser mass spectrometry (L2MS), secondary ion mass spectrometry (SIMS), and micro-Raman spectroscopy. Using the combination of this two-filter sampling/multi-technique approach in conjunction with advanced statistical methods we are able to unravel distinct surface chemical compositions of aerosols generated with different set points of a miniCAST burner. Specifically, we successfully discriminate samples by their volatile, semi-volatile and non-volatile polycyclic aromatic hydrocarbon (PAH) contents and reveal how subtle changes in combustion parameters affect particle surface chemistry. [ABSTRACT FROM AUTHOR]

Published
2019
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30. Ab initio calculations of the H2CO + H2O reaction

Author

Delcroix, Pauline, HANOUNE, Benjamin, Chazallon, Bertrand, Duflot, Denis, Physicochimie des Processus de Combustion et de l’Atmosphère - UMR 8522 (PC2A), Université de Lille-Centre National de la Recherche Scientifique (CNRS), and Laboratoire de Physique des Lasers, Atomes et Molécules - UMR 8523 (PhLAM)

Subjects
[CHIM.THEO]Chemical Sciences/Theoretical and/or physical chemistry, [PHYS.PHYS.PHYS-CHEM-PH]Physics [physics]/Physics [physics]/Chemical Physics [physics.chem-ph], ComputingMilieux_MISCELLANEOUS
Abstract

International audience

Published
2013

31. Ab initio molecular dynamics of formaldehyde aqueous solutions

Author

Delcroix, Pauline, HANOUNE, Benjamin, Chazallon, Bertrand, Cardini, G., Physicochimie des Processus de Combustion et de l’Atmosphère - UMR 8522 (PC2A), Université de Lille-Centre National de la Recherche Scientifique (CNRS), Laboratoire de Physique des Lasers, Atomes et Molécules - UMR 8523 (PhLAM), Università degli Studi di Firenze [Firenze], Università degli Studi di Firenze = University of Florence [Firenze] (UNIFI), and Università degli Studi di Firenze = University of Florence (UniFI)

Subjects
[CHIM.THEO]Chemical Sciences/Theoretical and/or physical chemistry, [PHYS.PHYS.PHYS-CHEM-PH]Physics [physics]/Physics [physics]/Chemical Physics [physics.chem-ph], ComputingMilieux_MISCELLANEOUS
Abstract

International audience

Published
2013

32. Guest Partitioning and Metastability of the Nitrogen Gas Hydrate

Author

Petuya, Claire, Damay, Françoise, Chazallon, Bertrand, Bruneel, Jean-Luc, and Desmedt, Arnaud

Abstract

Gas clathrate hydrates or gas hydrates are made of H-bonded water molecules forming cages, within which gaseous (guest) molecules are encapsulated. The formed clathrate structures, which may be metastable, depend on the nature and on the partitioning of the guest molecules in the water cage. This work focuses on the structural and vibrational properties of nitrogen hydrate in its two clathrate forms (namely, SI and SII) in the thermodynamic ranges 50–200 bar and 150–270 K, together with a comprehensive analysis of the transformation from SI to SII of this gas hydrate. The thermal expansion of both structures has been measured at 1 bar, and the melting of the nitrogen hydrate has been measured at ca. 210 K at 1 bar. Moreover, the SI structure is metastable in the studied pressure region: from time-dependent neutron powder diffraction analysis, it is shown that the SI structure transforms over time to the SII structure with a rate of (1.37 ± 0.17) × 105s–1at 100 K and at 1 bar. The transformation is also characterized by an induction time (i.e., the lifetime of the pure SI structure) of 0.49 day. We have also investigated the guest partitioning of the nitrogen hydrate using high-resolution Raman scattering. Vibrational bands of nitrogen molecules encapsulated in large cages are measured at lower wavenumbers than the one associated with encapsulation in small cages (by 1.1 cm–1in SI and 0.8 cm–1in SII). In the case of the thermodynamically stable SII phase, the dependence of the guest partitioning has been characterized as a function of the pressure–temperature conditions. Variation of the relative cage filling is demonstrated. While the small cages remain singly occupied according to previous neutron diffraction analysis, this variation is attributed to large cages of the nitrogen hydrate that easily catch or release nitrogen guest molecules. This study thus provides new opportunities for preparing nitrogen gas hydrates with a “targeted” structure and relative cage filling not only by varying the pressure and temperature but also by playing with the structural metastability.

Published
2024
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33. Capture du CO2 par voie Hydrate : résultats de l'ANR SECOHYA

Author

Herri, Jean-Michel, Bouchemoua, Amina, Cameirao, Ana, Ouabbas, Yamina, Kwaterski, Matthias, Dalmazzone, Didier, Deschamps, Johnny, Bouchafaa, Wassila, Broseta, Daniel, Daniel-David, Delphine, Mohammadi, Amir H., Eslamimanesh, Ali, Belandria, Veronica, Chazallon, Bertrand, Laboratoire Georges Friedel (LGF-ENSMSE), École des Mines de Saint-Étienne (Mines Saint-Étienne MSE), Institut Mines-Télécom [Paris] (IMT)-Institut Mines-Télécom [Paris] (IMT)-Université de Lyon-Centre National de la Recherche Scientifique (CNRS), Centre Sciences des Processus Industriels et Naturels (SPIN-ENSMSE), Institut Mines-Télécom [Paris] (IMT)-Institut Mines-Télécom [Paris] (IMT), Département Géochimie, environnement, écoulement, réacteurs industriels et cristallisation (GENERIC-ENSMSE), Institut Mines-Télécom [Paris] (IMT)-Institut Mines-Télécom [Paris] (IMT)-SPIN, Laboratoire des Procédés en Milieux Granulaires (LPMG-EMSE), Institut Mines-Télécom [Paris] (IMT)-Institut Mines-Télécom [Paris] (IMT)-Centre National de la Recherche Scientifique (CNRS), Département PROcédés Poudres, Interfaces, Cristallisation et Ecoulements (PROPICE-ENSMSE), Unité de Chimie et Procédés (UCP), École Nationale Supérieure de Techniques Avancées (ENSTA Paris), Laboratoire des Fluides Complexes et leurs Réservoirs (LFCR), TOTAL FINA ELF-Université de Pau et des Pays de l'Adour (UPPA)-Centre National de la Recherche Scientifique (CNRS), CEP/Fontainebleau, Centre Énergétique et Procédés (CEP), MINES ParisTech - École nationale supérieure des mines de Paris, Université Paris sciences et lettres (PSL)-Université Paris sciences et lettres (PSL)-MINES ParisTech - École nationale supérieure des mines de Paris, Université Paris sciences et lettres (PSL)-Université Paris sciences et lettres (PSL), Centre Thermodynamique des Procédés (CTP), Laboratoire de Physique des Lasers, Atomes et Molécules - UMR 8523 (PhLAM), Université de Lille-Centre National de la Recherche Scientifique (CNRS), Mines Paris - PSL (École nationale supérieure des mines de Paris), and Université Paris sciences et lettres (PSL)-Université Paris sciences et lettres (PSL)-Mines Paris - PSL (École nationale supérieure des mines de Paris)

Subjects
[SPI.GPROC]Engineering Sciences [physics]/Chemical and Process Engineering, Capture CO2, Thermodynamique
Abstract

International audience; Nous présentons dans ce papier les résultats principaux de l’ANR SECOHYA qui se termine à la fin de l’année 2011 et qui a consisté pendant quatre années à étudier la structure, la thermodynamique et la cinétique de cristallisation des hydrates de gaz en présence d’ammonium quaternaire.

Published
2011

35. Investigation on the geochemical dynamics of a hydrate-bearing pockmark in the Niger Delta

Author

Ruffine, Livio, Caprais, Jean-claude, Bayon, Germain, Riboulot, Vincent, Donval, Jean-pierre, Etoubleau, Joel, Birot, Dominique, Pignet, Patricia, Rongemaille, Emmanuelle, Chazallon, Bertrand, Grimaud, Sylvie, Adamy, Jerome, Charlou, Jean-luc, Voisset, Michel, Ruffine, Livio, Caprais, Jean-claude, Bayon, Germain, Riboulot, Vincent, Donval, Jean-pierre, Etoubleau, Joel, Birot, Dominique, Pignet, Patricia, Rongemaille, Emmanuelle, Chazallon, Bertrand, Grimaud, Sylvie, Adamy, Jerome, Charlou, Jean-luc, and Voisset, Michel

Abstract

A joint industrial project with IFREMER and Total provides insights into the tectonic setting and the geochemistry of a large active pockmark offshore W-Africa in the Niger Delta. The study combines both geophysical (seismic) and geochemical data to infer the dynamics of a 300 m wide pockmark located at 667 m water depth. Two Calypso cores, one at the centre and one outside the pockmark, along with three box-cores, two inside the pockmark and one outside, were collected to study the geochemistry of gas hydrates, carbonates and pore waters. Two seismic lines, a 3D high resolution random line and a 2D high resolution seismic line, provide a good description of the plumbing of the system. The integrated results depict a very active pockmark characterized by several gas charged-bodies, a well identified BSR marking a hydrate accumulation zone, charged from deeper sources via a network of faults. Hydrates and carbonate concretions have been detected inside the pockmark while only the latter has been found outside. The hydrate analyses show that the hydrate-forming gases are of thermogenic origin, albeit overwhelmingly composed of methane. Pore-water analyses reveal the occurrence of anaerobic oxidation of methane coupled with sulphate reduction at shallow depth (∼200 cm). The chloride concentration profile exhibits both values lower than that of seawater which is inherent to hydrate dissociation after core recovery and positive anomalies (values 7% higher than that of seawater background) at the lowermost part of the core. The latter evidence suggests current or recent hydrate formation at this area. The carbonate dating provides additional temporal information and indicates that this pockmark has been active since ∼21 kyr.

Published
2013
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38. Investigation on the geochemical dynamics of a hydrate-bearing pockmark in the Niger Delta

Author

Ruffine, Livio, primary, Caprais, Jean-Claude, additional, Bayon, Germain, additional, Riboulot, Vincent, additional, Donval, Jean-Pierre, additional, Etoubleau, Joel, additional, Birot, Dominique, additional, Pignet, Patricia, additional, Rongemaille, Emmanuelle, additional, Chazallon, Bertrand, additional, Grimaud, Sylvie, additional, Adamy, Jérome, additional, Charlou, Jean-Luc, additional, and Voisset, Michel, additional

Published
2013
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43. Chemical physics of air clathrate hydrates

Author

Kuhs, Werner F., Klapproth, Alice, Chazallon, Bertrand, Kuhs, Werner F., Klapproth, Alice, and Chazallon, Bertrand

Abstract

International Symposium on Physics of Ice Core Records. Shikotsukohan, Hokkaido, Japan, September 14-17, 1998.

Published
2000

48. CO2Capture Using Semi-Clathrates of Quaternary Ammonium Salt:Structure Change Induced by CO2and N2Enclathration.

Author

Chazallon, Bertrand, Ziskind, Michael, Carpentier, Yvain, and Focsa, Cristian

Subjects
*CLATHRATE compounds, *QUATERNARY ammonium salts, *CARBON sequestration, *MOLECULAR structure, *NITROGEN analysis, *AMMONIUM bromide
Abstract

Semi-clathrates of tetrabutylammoniumbromide (TBAB) are investigated for their potential application inthe CO2capture context based on hydrate technology. Thethree-phase lines of semi-clathrates of CO2–TBAB–H2O and N2–TBAB–H2O areestablished simultaneously with their structure using in situ Ramanscattering performed at high pressure. The preferred crystal phaseobtained at ambient pressure from solutions of 5 and 40 wt % TBABinitial concentrations is shown to change upon enclathration of CO2or N2, or by applying a higher pressure on thesystem. Deep in the stability field, metastable hydrate phases areoccurring at the onset of the formation and correspond to the onesexpected under ambient pressure conditions. Depending on the pressure,they progressively transformed into the most stable ones when approachingequilibrium and dissociation points. Besides, it is shown that a 5wt % TBAB original solution forms preferentially a mixed structureof both type B and type A at low gas pressure with CO2asthe guest gas. A new structure is spectroscopically characterizedat pressures higher than ∼2 MPa CO2. Type A is demonstratedto be stable at 5 wt % initial TBAB concentration with N2as the guest molecule and pressure between 8 and 12 MPa. These structuraldata address new insights on the relationship between the hydrophilic-anionand hydrophobic-cation intercalation with a guest gas producing hydrophobicinteraction in a distorted water lattice. [ABSTRACT FROM AUTHOR]

Published
2014
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