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Pvtx Properties of Saline Aqueous Fluids at High PT Conditions From Research Collection Doctoral Thesis PVTx properties of saline aqueous fluids at high P-T conditions from acoustic velocity measurements using Brillouin scattering spectroscopy Author(s): Mantegazzi, Davide Publication Date: 2012 Permanent Link: https://doi.org/10.3929/ethz-a-007582357 Rights / License: In Copyright - Non-Commercial Use Permitted This page was generated automatically upon download from the ETH Zurich Research Collection. For more information please consult the Terms of use. ETH Library DISS. ETH NO. 20358 PVTx properties of saline aqueous uids at high P-T conditions from acoustic velocity measurements using Brillouin scattering spectroscopy A dissertation submitted to ETH ZURICH for the degree of Doctor of Sciences presen ted by Davide Mantegazzi Diplom in Naturwissenschaften ETH ETH Zürich born on January 8, 1983 citizen of Riva San Vitale (TI) accepted on the recommendation of examiner Prof. Dr. C. Sanchez-Valle ETH Zurich co-examiner PD Dr. T. Driesner ETH Zurich co-examiner Prof. Dr. R.J. Bodnar Virginia Tech. (VA) co-examiner Prof. Dr. L.W. Diamond UNI Bern 2012 Abstract Saline aqueous fluids play a fundamental role in several geological processes. Despite the great importance of these fluids for the heat and mass transport i for their contribution to geodynamical cycles, their thermodynamic data are limited to low pressure conditions, typically below 0.5 GPa (ca. 15 km depth). The lack of PVTx properties for saline aqueous fluids at higher pressure considerably limits the quantitative modelling of fluid-rock interactions at pressure and t crust and the upper mantle. The goal of this study was to determine experimentally the equation of state and thermodynamic properties of several model saline aqueous fluids at elevated pressure and temperature conditions. The densities of the fluids are determined from acoustic velocity measurements performed in an externally heated membrane-type diamond anvil cell (mDAC) using Brillouin scattering spectroscopy. The maximal pressure and temperature conditions investigated in this study, i.e. 800 °C and 4.5 GPa, are representative for cold subduction zone settings at shallow to intermediate depths. The compositions of the saline water-rich fluids investigated, namely chlorined, sulphate-, carbonate and bicarbonate-bearing binary aqueous solutions, are reasonable analogs for aqueous fluids involved in geological processes, including metasomatism and melt production at subduction zones, hydrothermal alteration of the seafloor and ore deposits formation. The choice of solute concentrations, which range between 0m and 3m (mol/kg H 2O), was made in order to represent realistic concentrations of natural geological fluids, and were also influenced by the availability of literature data on the investigated compositions. The acoustic velocities V P(P,T,x) measured using Brillouin spectroscopy were inverted to calculate the density (P,T,x) of the solution of interest following basic thermodynamic relationships. Successively, the experimentally derived density data were fitted with an equations of state (EoS) which were then used to derive all other thermodynamic properties of geological interest ( i.e. , coefficient of thermal expansion, isobaric heat capacity, adiabatic bulk modulus and compressibility, isothermal bulk modulus and compressibility, partial molar properties and water fugacity). In case of multi-concentration systems the molality- dependence of the PVTx data were provided. The effects of salt-addition on the thermodynamic properties of the pure solvent ( i.e. water) were discussed, and the main iii changes were ascribed to the structure breaking/making behaviour of the dissolved electrolyte species. We have provided the first equation of state and constraints on the thermodynamic properties of H2O-NaCl fluids up to 800 °C and 4.5 GPa. The results were used to evaluate the effect of dissolved NaCl species on the location of dehydration reaction boundaries in subducting oceanic slabs. We find that the transition from greenschist to blueschist metamorphic facies shifts toward shallower depths when the activity of water decreases due to the presence of NaCl species dissolved in the fluid. The partial molar volumes and compressibility in the carbonate-bicarbonate aqueous systems obtained from the acoustic velocity measurements were used to determine the effect nd - 2- + of pressure on the 2 dissociation reaction of carbonic acid (HCO 3 = CO 3 + H ) up to 300 °C and 3 GPa. The volume of reaction Vr is negative in the investigated P-T range, indicating 2- - that carbonate ions (CO 3 ) are favoured over the bicarbonate ions (HCO 3 ) at high pressure and temperature conditions, in agreement with experimental and theoretical studies. This 2- implies that CO 3 ions may be the dominant dissolved carbon species in subduction zone fluids. We have shown that the experimental set-up and the numerical data treatment proposed in this study is a powerful tool to determine the thermodynamic properties of saline water-rich solutions up to pressure and temperature conditions relevant for the lower crust and the upper mantle. This technique can be applied to all other binary water-salt and molecular systems, and the continuous development of the DAC technique may extend the pressure and temperature range investigated to deeper Earth conditions. iv Riassunto I fluidi acquosi salini svolgono un ruolo chiave in numerosi processi geologici. Nonostante la loro grande importanza come vettori di trasporto per calore ed elementi disciolti e la loro influenza sui cicli geodinamici della Terra, la conoscenza delle loro proprietà termodinamiche è limitata a condizioni di bassa pressione, tipicamente sotto i 0.5 GPa, che corrispondono ad una profondità di circa 15 km. La mancanza di dati termodinamici per le soluzioni acquose saline a più alte pressioni, limita in modo considerevole la modellizzazione quantitativa delle interazioni tra fluidi e rocce a condizioni di pressione e temperature rilevanti per gli strati della crosta terrestre inferiore e del mantello terrestre superiore. Questo manoscritto presenta per la prima volta le proprietà termodinamiche di numerosi fluidi acquosi salini di riferimento ad alte pressioni e temperature, determinate da misurazioni di velocità acustica compiute in una cella ad incudine di diamante con membrana (membrane- type diamond anvil cell, abbreviata mDAC) usando la spettroscopia Brillouin. La temperatura e la pressione sperimentale massimale, 800 °C e 4.5 GPa, corrispondono a condizioni di bassa e media profondità in una zona di subduzione a basso gradiente geotermico. Le composizioni dei fluidi acquosi salini studiati in questa tesi di dottorato, - 2- corrispondenti a sistemi binari contenenti acqua e ioni cloruro (Cl ), acqua e solfati (SO 4 ), 2- - acqua e carbonati (CO 3 ) e infine acqua e bicarbonati (HCO 3 ), modellizzano alcuni dei più importanti fluidi geologici, che ricoprono un ruolo fondamentale in processi come il metasomatismo e la generazione di magma calc- idrotermale del fondo oceanico e la formazione di giacimenti minerari. Le concentrazioni molali dei fluidi investigati, che variano da 0 m a 3 m (moli sale / kg H 2O) , sono realistiche per alcuni fluidi geologici naturali, e la loro scelta è stata dettata anche dalla disponibilità di dati nella letteratura scientifica già pubblicata precedentemente. Le velocità acustiche V P(P,T,x) misurate con la spettroscopia Brillouin sono state invertite secondo principi termodinamici base per calcolare la densità (P,T,x) dei fluidi acquosi salini. Successivamente, i valori di densità calcolati dai dati sperimentali sulle velocità acustice sono stati modellizzati con equazioni di stato (EoS) di tipo polinomiale. Da queste EoS sono state derivate tutte le altre importanti proprietà termodinamiche. Specificatamente, queste propietà sono: coefficiente di espansione termale, calore specifico isobarico, bulk modulus e compressibilità adiabatici, bulk modulus e compressibilità isotermici, volume molare parziale, fugacit e velocità acustica. Nei sistemi acqua- v sale, dove gli esperimenti sono stati condotti in più concentrazioni molali, la dipendenza dei dati termodinamici dalla molalità è stata inclusa nelle EoS. I cambiamenti subiti dalle proprietà termodinamiche del solvente (acqua) in seguito n soluzione sono stati descritti e ricondotti distruttivo o costruttivo degli ioni sulla struttura molecolare del solvente. Il presente studio presenta per la prima volta le proprietà termodinamiche del sistema binario H 2O-NaCl fino a 800 °C e 4.5 GPa. Gli esperimenti sono stati condotti in più dalla molalità è stata determinata. Questi valori di fugacità sono stati successivamente usati per modellizzare una tipica reazione di disidratazione che avviene nelle rocce basiche della crosta oceanica durante la loro subduzione, alle condizioni di transizione dalla facies a scisti verdi alla facies a scisti blu. I risultati di questo lavoro mostrano che la reazione di disidratazione avviene a temperature e pressioni diverse a dipendenza della concentrazione salina del fluido rilasciato durante il metamorfismo progrado. Infatti, si sposta a profondità minori. Le misure sperimentali effettuate nei sistemi contenenti ioni disciolti di carbonato e bicarbonato hanno permesso di determinare la dipendenza dalla pressione della seconda - 2- costante di equilibrio dell 3 = CO 3 + H+) fino a condizioni di 200 °C e 3 GPa. I risultati di questi esperimenti suggeriscono che a 2- condizioni di alte pressioni gli ioni di carbonato CO
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