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Spectroscopie X haute résolution appliquée à l'étude des fluides hydrothermaux

Author: Mohammed IrarJean-Louis HazemannLaurent TrucheRodolphe VuilleumierManuel MuñozAll authors
Publisher: 2017.
Dissertation: Thèse de doctorat : Physique des matériaux : Université Grenoble Alpes (ComUE) : 2017.
Edition/Format:   Computer file : Document : Thesis/dissertation : English
Summary:
Les connaissances des propriétés des fluides hydrothermaux, c'est-à-dire des solutions aqueuses à haute température (T) et haute pression (P), sont essentielles dans les domaines des sciences de la terre, chimie prébiotique, industrie nucléaire ou encore des sciences environnementales. Près du point critique (Pc, Tc) et dans les conditions pseudocritiques (i.e. à la densité critique au dessus de la Tc-Pc),
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Details

Genre/Form: Thèses et écrits académiques
Material Type: Document, Thesis/dissertation, Internet resource
Document Type: Internet Resource, Computer File
All Authors / Contributors: Mohammed Irar; Jean-Louis Hazemann; Laurent Truche; Rodolphe Vuilleumier; Manuel Muñoz; Marie-Christine Boiron; Elena Bazarkina; Communauté d'universités et d'établissements Université Grenoble Alpes.; École doctorale physique (Grenoble).; Institut Néel (Grenoble).
OCLC Number: 1029557743
Notes: Titre provenant de l'écran-titre.
Description: 1 online resource
Responsibility: Mohammed Irar ; sous la direction de Jean-Louis Hazemann.

Abstract:

Les connaissances des propriétés des fluides hydrothermaux, c'est-à-dire des solutions aqueuses à haute température (T) et haute pression (P), sont essentielles dans les domaines des sciences de la terre, chimie prébiotique, industrie nucléaire ou encore des sciences environnementales. Près du point critique (Pc, Tc) et dans les conditions pseudocritiques (i.e. à la densité critique au dessus de la Tc-Pc), les propriétés des fluides changent de manière radicale. Ces modifications ont lieu à différentes échelles: à l'échelle macroscopique (changements de densité et de compressibilité), à l'échelle mésoscopique (processus d'agglomération entre les différentes clusters) et enfin à l'échelle moléculaire (organisation local entre les atomes et les molécules, par exemple les liaisons hydrogène, H).Cette étude est centrée sur les effets de la solvatation aqueuse de différents électrolytes en fonction de la température, pression et concentration. L'étude expérimentale a été conduite par les mesures d'Absorption X, technique de choix pour mesurer d'une part l'évolution de la densité du fluide et d'autre part sonder l'environnement atomique local autour des solutés. Cette étude a été faite sur l'eau pure et sur différentes solutions salines à différentes pressions (jusqu'à ~1.3Pc) et à température variable (jusqu'à ~2Tc), pour passer du domaine liquide au domaine supercritique, dans une cellule permettant de découpler totalement l'effet de la pression et de la température.Nous avons obtenu des preuves expérimentales du déplacement du point critique et de l'isochore et de leur dépendance en fonction de la concentration en sel pour NaCl (0,3, 0,5 et 1,0 moles NaCl par kilogramme d'eau). Nous avons également observé une anomalie de densité dans la région supercritique (SC) et l'apparition d'une séparation des phases liquide-vapeur pour certaines solutions aqueuses. L'augmentation de la densité relative dans cette zone critique est plus prononcée pour Cs>Rb>K>Na>Li pour les bromures et les chlorures. Le changement structural dans cette région a été suivi par spectroscopie XANES haute résolution au seuil K du brome pour différents bromures d'alcalin. L'interprétation des spectres XANES indiquent clairement un changement drastique dans la structure locale du fluide au moment de l'apparition de cette anomalie pouvant être interprétée par l'apparition des paires ioniques.Ces nouvelles observations sont a relier au changement structurale du solvant et principalement à l'évolution de son pouvoir de solvatation lié à l'évolution des liaisons hydrogène à hautes T-P.

Knowledge of the properties of hydrothermal fluids, i.e. aqueous solutions at high temperature (T) and high pressure (P), are essential in the fields of earth sciences, prebiotic chemistry, nuclear industry and environmental sciences. Near the critical point (Pc, Tc) and under the pseudocritic conditions (i.e. at the critical density at T-P above Tc-Pc), the fluid properties change radically. These changes take place at different scales: the macroscopic scale (density and compressibility changes), the mesoscopic scale (agglomeration process between different clusters) and finally, the molecular scale (local organization of atoms and molecules, for example hydrogen bonds, H).This study focuses on the solvation effects in different electrolytes as a function of temperature, pressure and concentration. The experimental study was carried out by X-ray absorption measurements, the technique suitable for probing both fluid density evolution and local atomic environment around the solutes. This study was carried out on pure water and salt solutions at different pressures (up to ~ 1.3Pc) and temperatures (up to ~ 2Tc), to pass from the liquid to the supercritical domain, using a cell permitting to completely decouple the effects of pressure and temperature.We have obtained experimental proofs of the displacement of the critical point and the isochore and their dependence on the salt concentration in the case of NaCl (0.3, 0.5 and 1.0 moles NaCl per kilogram of water). We have also observed a density anomaly in the supercritical region (SC) and the appearance of liquid-vapor phase separation for some aqueous solutions. The relative density increase in the critical zone is more pronounced for Cs>Rb>K>Na>Li for bromides and chlorides. The structural change in this region was followed by high-resolution XANES spectroscopy at the K-threshold of bromine for various alkali bromide. The interpretation of the XANES spectra clearly indicates a drastic changes in the fluid structure related to this anomaly, which can be interpreted by the appearance of ionic pairs.These new observations are in link with water structure and solvation properties evaluation and consequently with hydrogen bonding changes under high T-P.

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<http:\/\/www.worldcat.org\/oclc\/1029557743<\/a>> # Spectroscopie X haute r\u00E9solution appliqu\u00E9e \u00E0 l\'\u00E9tude des fluides hydrothermaux<\/span>\n\u00A0\u00A0\u00A0\u00A0a \nschema:MediaObject<\/a>, bgn:Thesis<\/a>, schema:CreativeWork<\/a>, bgn:ComputerFile<\/a> ;\u00A0\u00A0\u00A0\nbgn:inSupportOf<\/a> \"Th\u00E8se de doctorat : Physique des mat\u00E9riaux : Universit\u00E9 Grenoble Alpes (ComUE) : 2017.<\/span>\" ;\u00A0\u00A0\u00A0\nlibrary:oclcnum<\/a> \"1029557743<\/span>\" ;\u00A0\u00A0\u00A0\nlibrary:placeOfPublication<\/a> <http:\/\/id.loc.gov\/vocabulary\/countries\/fr<\/a>> ;\u00A0\u00A0\u00A0\nschema:about<\/a> <http:\/\/experiment.worldcat.org\/entity\/work\/data\/4863214860#Thing\/rx<\/a>> ; # RX<\/span>\n\u00A0\u00A0\u00A0\nschema:about<\/a> <http:\/\/experiment.worldcat.org\/entity\/work\/data\/4863214860#Topic\/fluides_supercritiques_proprietes_physico_chimiques<\/a>> ; # Fluides supercritiques--Propri\u00E9t\u00E9s physico-chimiques<\/span>\n\u00A0\u00A0\u00A0\nschema:about<\/a> <http:\/\/experiment.worldcat.org\/entity\/work\/data\/4863214860#Topic\/spectrometrie_exafs<\/a>> ; # Spectrom\u00E9trie EXAFS<\/span>\n\u00A0\u00A0\u00A0\nschema:about<\/a> <http:\/\/dewey.info\/class\/530\/<\/a>> ;\u00A0\u00A0\u00A0\nschema:about<\/a> <http:\/\/experiment.worldcat.org\/entity\/work\/data\/4863214860#Thing\/exafs<\/a>> ; # EXAFS<\/span>\n\u00A0\u00A0\u00A0\nschema:about<\/a> <http:\/\/experiment.worldcat.org\/entity\/work\/data\/4863214860#Thing\/spectroscopie<\/a>> ; # Spectroscopie<\/span>\n\u00A0\u00A0\u00A0\nschema:about<\/a> <http:\/\/experiment.worldcat.org\/entity\/work\/data\/4863214860#Thing\/hydrothermal<\/a>> ; # Hydrothermal<\/span>\n\u00A0\u00A0\u00A0\nschema:author<\/a> <http:\/\/experiment.worldcat.org\/entity\/work\/data\/4863214860#Person\/irar_mohammed_1988<\/a>> ; # Mohammed Irar<\/span>\n\u00A0\u00A0\u00A0\nschema:contributor<\/a> <http:\/\/experiment.worldcat.org\/entity\/work\/data\/4863214860#Person\/vuilleumier_rodolphe<\/a>> ; # Rodolphe Vuilleumier<\/span>\n\u00A0\u00A0\u00A0\nschema:contributor<\/a> <http:\/\/experiment.worldcat.org\/entity\/work\/data\/4863214860#Person\/hazemann_jean_louis<\/a>> ; # Jean-Louis Hazemann<\/span>\n\u00A0\u00A0\u00A0\nschema:contributor<\/a> <http:\/\/experiment.worldcat.org\/entity\/work\/data\/4863214860#Organization\/communaute_d_universites_et_d_etablissements_universite_grenoble_alpes<\/a>> ; # Communaut\u00E9 d\'universit\u00E9s et d\'\u00E9tablissements Universit\u00E9 Grenoble Alpes.<\/span>\n\u00A0\u00A0\u00A0\nschema:contributor<\/a> <http:\/\/experiment.worldcat.org\/entity\/work\/data\/4863214860#Person\/boiron_marie_christine_1961<\/a>> ; # Marie-Christine Boiron<\/span>\n\u00A0\u00A0\u00A0\nschema:contributor<\/a> <http:\/\/experiment.worldcat.org\/entity\/work\/data\/4863214860#Organization\/institut_neel_grenoble<\/a>> ; # Institut N\u00E9el (Grenoble).<\/span>\n\u00A0\u00A0\u00A0\nschema:contributor<\/a> <http:\/\/experiment.worldcat.org\/entity\/work\/data\/4863214860#Person\/munoz_manuel_1975<\/a>> ; # Manuel Mu\u00F1oz<\/span>\n\u00A0\u00A0\u00A0\nschema:contributor<\/a> <http:\/\/experiment.worldcat.org\/entity\/work\/data\/4863214860#Person\/truche_laurent_1982<\/a>> ; # Laurent Truche<\/span>\n\u00A0\u00A0\u00A0\nschema:contributor<\/a> <http:\/\/experiment.worldcat.org\/entity\/work\/data\/4863214860#Person\/bazarkina_elena_1982<\/a>> ; # Elena Bazarkina<\/span>\n\u00A0\u00A0\u00A0\nschema:contributor<\/a> <http:\/\/experiment.worldcat.org\/entity\/work\/data\/4863214860#Organization\/ecole_doctorale_physique_grenoble<\/a>> ; # \u00C9cole doctorale physique (Grenoble).<\/span>\n\u00A0\u00A0\u00A0\nschema:datePublished<\/a> \"2017<\/span>\" ;\u00A0\u00A0\u00A0\nschema:description<\/a> \"Les connaissances des propri\u00E9t\u00E9s des fluides hydrothermaux, c\'est-\u00E0-dire des solutions aqueuses \u00E0 haute temp\u00E9rature (T) et haute pression (P), sont essentielles dans les domaines des sciences de la terre, chimie pr\u00E9biotique, industrie nucl\u00E9aire ou encore des sciences environnementales. Pr\u00E8s du point critique (Pc, Tc) et dans les conditions pseudocritiques (i.e. \u00E0 la densit\u00E9 critique au dessus de la Tc-Pc), les propri\u00E9t\u00E9s des fluides changent de mani\u00E8re radicale. Ces modifications ont lieu \u00E0 diff\u00E9rentes \u00E9chelles: \u00E0 l\'\u00E9chelle macroscopique (changements de densit\u00E9 et de compressibilit\u00E9), \u00E0 l\'\u00E9chelle m\u00E9soscopique (processus d\'agglom\u00E9ration entre les diff\u00E9rentes clusters) et enfin \u00E0 l\'\u00E9chelle mol\u00E9culaire (organisation local entre les atomes et les mol\u00E9cules, par exemple les liaisons hydrog\u00E8ne, H).Cette \u00E9tude est centr\u00E9e sur les effets de la solvatation aqueuse de diff\u00E9rents \u00E9lectrolytes en fonction de la temp\u00E9rature, pression et concentration. L\'\u00E9tude exp\u00E9rimentale a \u00E9t\u00E9 conduite par les mesures d\'Absorption X, technique de choix pour mesurer d\'une part l\'\u00E9volution de la densit\u00E9 du fluide et d\'autre part sonder l\'environnement atomique local autour des solut\u00E9s. Cette \u00E9tude a \u00E9t\u00E9 faite sur l\'eau pure et sur diff\u00E9rentes solutions salines \u00E0 diff\u00E9rentes pressions (jusqu\'\u00E0 ~1.3Pc) et \u00E0 temp\u00E9rature variable (jusqu\'\u00E0 ~2Tc), pour passer du domaine liquide au domaine supercritique, dans une cellule permettant de d\u00E9coupler totalement l\'effet de la pression et de la temp\u00E9rature.Nous avons obtenu des preuves exp\u00E9rimentales du d\u00E9placement du point critique et de l\'isochore et de leur d\u00E9pendance en fonction de la concentration en sel pour NaCl (0,3, 0,5 et 1,0 moles NaCl par kilogramme d\'eau). Nous avons \u00E9galement observ\u00E9 une anomalie de densit\u00E9 dans la r\u00E9gion supercritique (SC) et l\'apparition d\'une s\u00E9paration des phases liquide-vapeur pour certaines solutions aqueuses. L\'augmentation de la densit\u00E9 relative dans cette zone critique est plus prononc\u00E9e pour Cs>Rb>K>Na>Li pour les bromures et les chlorures. Le changement structural dans cette r\u00E9gion a \u00E9t\u00E9 suivi par spectroscopie XANES haute r\u00E9solution au seuil K du brome pour diff\u00E9rents bromures d\'alcalin. L\'interpr\u00E9tation des spectres XANES indiquent clairement un changement drastique dans la structure locale du fluide au moment de l\'apparition de cette anomalie pouvant \u00EAtre interpr\u00E9t\u00E9e par l\'apparition des paires ioniques.Ces nouvelles observations sont a relier au changement structurale du solvant et principalement \u00E0 l\'\u00E9volution de son pouvoir de solvatation li\u00E9 \u00E0 l\'\u00E9volution des liaisons hydrog\u00E8ne \u00E0 hautes T-P.<\/span>\" ;\u00A0\u00A0\u00A0\nschema:description<\/a> \"Knowledge of the properties of hydrothermal fluids, i.e. aqueous solutions at high temperature (T) and high pressure (P), are essential in the fields of earth sciences, prebiotic chemistry, nuclear industry and environmental sciences. Near the critical point (Pc, Tc) and under the pseudocritic conditions (i.e. at the critical density at T-P above Tc-Pc), the fluid properties change radically. These changes take place at different scales: the macroscopic scale (density and compressibility changes), the mesoscopic scale (agglomeration process between different clusters) and finally, the molecular scale (local organization of atoms and molecules, for example hydrogen bonds, H).This study focuses on the solvation effects in different electrolytes as a function of temperature, pressure and concentration. The experimental study was carried out by X-ray absorption measurements, the technique suitable for probing both fluid density evolution and local atomic environment around the solutes. This study was carried out on pure water and salt solutions at different pressures (up to ~ 1.3Pc) and temperatures (up to ~ 2Tc), to pass from the liquid to the supercritical domain, using a cell permitting to completely decouple the effects of pressure and temperature.We have obtained experimental proofs of the displacement of the critical point and the isochore and their dependence on the salt concentration in the case of NaCl (0.3, 0.5 and 1.0 moles NaCl per kilogram of water). We have also observed a density anomaly in the supercritical region (SC) and the appearance of liquid-vapor phase separation for some aqueous solutions. The relative density increase in the critical zone is more pronounced for Cs>Rb>K>Na>Li for bromides and chlorides. The structural change in this region was followed by high-resolution XANES spectroscopy at the K-threshold of bromine for various alkali bromide. 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<http:\/\/experiment.worldcat.org\/entity\/work\/data\/4863214860#Person\/munoz_manuel_1975<\/a>> # Manuel Mu\u00F1oz<\/span>\n\u00A0\u00A0\u00A0\u00A0a \nschema:Person<\/a> ;\u00A0\u00A0\u00A0\nschema:birthDate<\/a> \"1975<\/span>\" ;\u00A0\u00A0\u00A0\nschema:deathDate<\/a> \"\" ;\u00A0\u00A0\u00A0\nschema:familyName<\/a> \"Mu\u00F1oz<\/span>\" ;\u00A0\u00A0\u00A0\nschema:givenName<\/a> \"Manuel<\/span>\" ;\u00A0\u00A0\u00A0\nschema:name<\/a> \"Manuel Mu\u00F1oz<\/span>\" ;\u00A0\u00A0\u00A0\u00A0.\n\n\n<\/div>\n
<http:\/\/experiment.worldcat.org\/entity\/work\/data\/4863214860#Person\/truche_laurent_1982<\/a>> # Laurent Truche<\/span>\n\u00A0\u00A0\u00A0\u00A0a \nschema:Person<\/a> ;\u00A0\u00A0\u00A0\nschema:birthDate<\/a> \"1982<\/span>\" ;\u00A0\u00A0\u00A0\nschema:deathDate<\/a> \"\" ;\u00A0\u00A0\u00A0\nschema:familyName<\/a> \"Truche<\/span>\" ;\u00A0\u00A0\u00A0\nschema:givenName<\/a> \"Laurent<\/span>\" ;\u00A0\u00A0\u00A0\nschema:name<\/a> \"Laurent Truche<\/span>\" ;\u00A0\u00A0\u00A0\u00A0.\n\n\n<\/div>\n
<http:\/\/experiment.worldcat.org\/entity\/work\/data\/4863214860#Person\/vuilleumier_rodolphe<\/a>> # Rodolphe Vuilleumier<\/span>\n\u00A0\u00A0\u00A0\u00A0a \nschema:Person<\/a> ;\u00A0\u00A0\u00A0\nschema:familyName<\/a> \"Vuilleumier<\/span>\" ;\u00A0\u00A0\u00A0\nschema:givenName<\/a> \"Rodolphe<\/span>\" ;\u00A0\u00A0\u00A0\nschema:name<\/a> \"Rodolphe Vuilleumier<\/span>\" ;\u00A0\u00A0\u00A0\u00A0.\n\n\n<\/div>\n
<http:\/\/experiment.worldcat.org\/entity\/work\/data\/4863214860#Thing\/exafs<\/a>> # EXAFS<\/span>\n\u00A0\u00A0\u00A0\u00A0a \nschema:Thing<\/a> ;\u00A0\u00A0\u00A0\nschema:name<\/a> \"EXAFS<\/span>\" ;\u00A0\u00A0\u00A0\u00A0.\n\n\n<\/div>\n
<http:\/\/experiment.worldcat.org\/entity\/work\/data\/4863214860#Thing\/hydrothermal<\/a>> # Hydrothermal<\/span>\n\u00A0\u00A0\u00A0\u00A0a \nschema:Thing<\/a> ;\u00A0\u00A0\u00A0\nschema:name<\/a> \"Hydrothermal<\/span>\" ;\u00A0\u00A0\u00A0\u00A0.\n\n\n<\/div>\n
<http:\/\/experiment.worldcat.org\/entity\/work\/data\/4863214860#Thing\/rx<\/a>> # RX<\/span>\n\u00A0\u00A0\u00A0\u00A0a \nschema:Thing<\/a> ;\u00A0\u00A0\u00A0\nschema:name<\/a> \"RX<\/span>\" ;\u00A0\u00A0\u00A0\u00A0.\n\n\n<\/div>\n
<http:\/\/experiment.worldcat.org\/entity\/work\/data\/4863214860#Thing\/spectroscopie<\/a>> # Spectroscopie<\/span>\n\u00A0\u00A0\u00A0\u00A0a \nschema:Thing<\/a> ;\u00A0\u00A0\u00A0\nschema:name<\/a> \"Spectroscopie<\/span>\" ;\u00A0\u00A0\u00A0\u00A0.\n\n\n<\/div>\n
<http:\/\/experiment.worldcat.org\/entity\/work\/data\/4863214860#Topic\/fluides_supercritiques_proprietes_physico_chimiques<\/a>> # Fluides supercritiques--Propri\u00E9t\u00E9s physico-chimiques<\/span>\n\u00A0\u00A0\u00A0\u00A0a \nschema:Intangible<\/a> ;\u00A0\u00A0\u00A0\nschema:name<\/a> \"Fluides supercritiques--Propri\u00E9t\u00E9s physico-chimiques<\/span>\" ;\u00A0\u00A0\u00A0\u00A0.\n\n\n<\/div>\n
<http:\/\/experiment.worldcat.org\/entity\/work\/data\/4863214860#Topic\/spectrometrie_exafs<\/a>> # Spectrom\u00E9trie EXAFS<\/span>\n\u00A0\u00A0\u00A0\u00A0a \nschema:Intangible<\/a> ;\u00A0\u00A0\u00A0\nschema:name<\/a> \"Spectrom\u00E9trie EXAFS<\/span>\" ;\u00A0\u00A0\u00A0\u00A0.\n\n\n<\/div>\n
<http:\/\/id.loc.gov\/vocabulary\/countries\/fr<\/a>>\u00A0\u00A0\u00A0\u00A0a \nschema:Place<\/a> ;\u00A0\u00A0\u00A0\ndcterms:identifier<\/a> \"fr<\/span>\" ;\u00A0\u00A0\u00A0\u00A0.\n\n\n<\/div>\n
<http:\/\/www.theses.fr\/2017GREAY060\/document<\/a>>\u00A0\u00A0\u00A0\nrdfs:comment<\/a> \"Acc\u00E8s au texte int\u00E9gral<\/span>\" ;\u00A0\u00A0\u00A0\u00A0.\n\n\n<\/div>\n
<http:\/\/www.worldcat.org\/title\/-\/oclc\/1029557743<\/a>>\u00A0\u00A0\u00A0\u00A0a \ngenont:InformationResource<\/a>, genont:ContentTypeGenericResource<\/a> ;\u00A0\u00A0\u00A0\nschema:about<\/a> <http:\/\/www.worldcat.org\/oclc\/1029557743<\/a>> ; # Spectroscopie X haute r\u00E9solution appliqu\u00E9e \u00E0 l\'\u00E9tude des fluides hydrothermaux<\/span>\n\u00A0\u00A0\u00A0\nschema:dateModified<\/a> \"2020-05-20<\/span>\" ;\u00A0\u00A0\u00A0\nvoid:inDataset<\/a> <http:\/\/purl.oclc.org\/dataset\/WorldCat<\/a>> ;\u00A0\u00A0\u00A0\u00A0.\n\n\n<\/div>\n\n

Content-negotiable representations<\/p>\n