Clustering in supercritical fluid mixtures

Kim, Sunwook; Johnston, Keith P.

doi:10.1002/aic.690331004

Cited by 254 publications

(248 citation statements)

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“…In more recent work, Johnston and co-workers (17,18,20,27,32) showed quantitatively that the local fluid density about the solute is greater than the bulk density. In these papers, results were presented for CQ2, C 2 H 4 , CF 3 H, and CF 3 C1.…”

Section: Spectroscopic Investigations Of Supercritical Fluidsmentioning

confidence: 99%

“…Steady-state solvatochromic techniques provide a reasonable means to study solvation processes in supercritical media (5,(17)(18)(19)(20)(21)(22)(23)(24)(25)(26)(27)(28)(29)(30)(31)(32)(43)(44)(45)(59)(60)(61)(62)(63)(64)(65)(66)(67)(68). But, unless the interaction rates between the solute species and the supercritical fluid are slow, these "static" methods cannot be used to study solvation kinetics.…”

Section: Spectroscopic Investigations Of Supercritical Fluidsmentioning

confidence: 99%

“…Local densities were recovered by comparison of the observed spectral shift (or position) to that expected for a homogeneous polarizable dielectric medium. Clustering manifests itself in deviation from the expected linear McRae continuum model (17,18,20,27,32,56,57). These data were subsequently interpreted using an expression derived from Kirkwood-Buff solution theory (20).…”

Section: Spectroscopic Investigations Of Supercritical Fluidsmentioning

confidence: 99%

“…Some of these efforts have used optical spectroscopy (17)(18)(19)(20)(21)(22)(23)(24)(25)(26)(27)(28)(29)(30)(31)(32)(33)(34)(43)(44)(45) and others have used chromatographic methods as a tool to probe the aforementioned interactions. Many of these experimental studies have been advanced by theoretical calculations and modelling (35-42).…”

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confidence: 99%

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Fundamental Studies and Applications of Supercritical Fluids

McNally

Bright

1992

ACS Symposium Series

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Section: Spectroscopic Investigations Of Supercritical Fluidsmentioning

confidence: 99%

Section: Spectroscopic Investigations Of Supercritical Fluidsmentioning

confidence: 99%

Section: Spectroscopic Investigations Of Supercritical Fluidsmentioning

confidence: 99%

mentioning

confidence: 99%

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Fundamental Studies and Applications of Supercritical Fluids

McNally

Bright

1992

ACS Symposium Series

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“…These experimental studies are based on the solubility of solids and on partial molar properties of dilute solutes in near-critical solvents [32,40,49,51,52] and also on spectroscopic techniques which provide information on solvation (short ranged interactions) and solvent structure [43,45,53,54,55,56,57,58,59].…”

Section: Solute Solubilitymentioning

confidence: 99%

Thermodynamic Aspects of Supercritical Fluids Processing: Applications of Polymers and Wastes Treatment

Cansell

Rey

Beslin

1998

Rev. Inst. Fr. Pét.

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La mise en Ïuvre des fluides supercritiques est d'un intŽr•t croissant dans de nombreux domaines : pour la sŽparation (sŽparation et purification en pŽtrochimie, industrie alimentaire) et la chromatographie par fluides supercritiques (sŽparation analytique et prŽ-paratoire, dŽtermination des propriŽtŽs physicochimiques), comme milieux rŽactifs aux propriŽtŽs continžment ajustables allant du gaz au liquide (polyŽthyl•ne de faible densitŽ, Žlimination des dŽchets, recyclage des polym•res), en gŽologie et en minŽralogie (volcanologie, Žnergie gŽothermique, synth•se hydrothermique), dans la formation des particules, fibres et substrats (produits pharmaceutiques, explosifs, rev•tements), pour le sŽchage des matŽriaux (gels).Cet article prŽsente les propriŽtŽs physicochimiques exceptionnelles des fluides supercritiques en rapport avec leurs applications en ingŽnierie. Apr•s un bref rappel des concepts fondamentaux relatifs au comportement critique des fluides purs, nous dŽvelop-pons d'une mani•re plus dŽtaillŽe les propriŽtŽs physicochimiques ajustables des fluides dans le domaine supercritique. La deuxi•me partie de lÕarticle dŽcrit les applications en ingŽnierie des fluides supercritiques relatives aux rŽactions chimiques et au traitement des polym•res. Chaque prŽsentation d'application est divisŽe en deux parties : la premi•re rappelle les concepts de base et le contexte gŽnŽral ainsi que les propriŽtŽs physicochimiques, la seconde dŽveloppe les applications en ingŽnierie se rapportant au domaine concernŽ. THERMODYNAMIC ASPECTS OF SUPERCRITICAL FLUIDS PROCESSING: APPLICATIONS TO POLYMERS AND WASTES TREATMENTSupercritical fluid processes are of increasing interest for many fields: in supercritical fluid separation (petroleum-chemistry separation and purification, food industry) and supercritical fluid chromatography (analytical and preparative separation, determination of physicochemical properties); as reaction media with continuously adjustable properties from gas to liquid (lowdensity polyethylene, waste destruction, polymer recycling); in This paper presents the unusual physicochemical properties of supercritical fluids in relation to their engineering applications. After a short report of fundamental concepts of critical behavior in pure fluids, we develop in more details the tunable physicochemical properties of fluid in the supercritical domain. The second part of this paper describes the engineering applications of supercritical fluids relevant of chemical reactions and polymer processing. Each application presentation is divided in two parts: the first one recalls the basic concepts including general background, physicochemical properties and the second one develops the engineering applications relevant of the advocated domain. ASPECTOS TERMODINçMICOS DEL TRATAMIENTO DE LOS FLUIDOS SUPERCRêTICOS : APLICACIONES PARA LOS TRATAMIENTOS DE LOS POLêMEROS Y DE LOS RESIDUOSLa implementaci-n de los fluidos supercr'ticos presenta un interŽs cada vez mayor en numerosos campos : para la separaci-n (separaci-n y purific...

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Direct Measurements of the Enthalpy of Solution of Solid Solute in Supercritical Fluids: Study on the CO2-Naphthalene System

et al. 2001

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A setup for a calorimeter for simultaneously measuring the solubility and the solution enthalpy of solid solutes in supercritical fluids (SCFs) has been established. The enthalpy of solution of naphthalene in supercritical CO2 was measured at 308.15 K in the pressure range from 8.0-11.0 MPa. It was found that the enthalpy of solution (deltaH) was negative in the pressure range from 8.0 to 9.5 MPa, and the absolute value decreased with increasing pressure. In this pressure range, the dissolution of the solute was enthalpy driven. However, the deltaH became positive at pressures higher than 9.5 MPa, and the dissolution was entropy driven. Monte Carlo simulation was performed to analyze the local structural environment of the solvated naphthalene molecules in supercritical CO2 under the experimental conditions for the calorimetric measurements. By combining the enthalpy data and the simulation results, it can be deduced that the energy level of CO2 in the high compressible region is higher than that at higher pressures, which results in the large negative enthalpy of solution and the larger degree of solvent-solute clustering in the high compressible region.

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Clustering in supercritical fluid mixtures

Cited by 254 publications

References 29 publications

Fundamental Studies and Applications of Supercritical Fluids

Fundamental Studies and Applications of Supercritical Fluids

Thermodynamic Aspects of Supercritical Fluids Processing: Applications of Polymers and Wastes Treatment

Direct Measurements of the Enthalpy of Solution of Solid Solute in Supercritical Fluids: Study on the CO2-Naphthalene System

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