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The present article summarizes experimental and theoretical considerations required for a proper use of dynamic light scattering (DLS) for the measurement of transport properties of fluids. It addresses not only recent advancements of the method, but also aims to provide recommendations to researchers who intend to apply the technique in the future. As outlined in this study, DLS is based on the analysis of scattered light governed by microscopic statistical or periodic fluctuations that originate from the thermal movement of molecules and/or particles at macroscopic thermodynamic equilibrium. The dynamics of these hydrodynamic fluctuations in the bulk of fluids or at their phase boundaries are related to the underlying diffusive processes and, thus, to the associated transport properties, and are reflected by the time-dependent correlation function of the scattered light intensity. The fundamentals of this type of detection, known as photon correlation spectroscopy (PCS), will be discussed in the present contribution in some more detail. It is emphasized that the experiments need to be designed carefully in accordance with theory in order to assign the measurement signals to the corresponding hydrodynamic fluctuations. If the necessary conditions are fulfilled, DLS allows the accurate determination of several transport properties including kinematic and dynamic viscosity, thermal diffusivity, mutual diffusivity, and sound attenuation, which may be accessed together with other thermophysical properties such as speed of sound and surface or interfacial tension. In some instances, also the simultaneous determination of several transport properties is possible. With the exception of the sound attenuation, expanded uncertainties for the mentioned transport properties down to 1 % can be achieved for various types of fluid systems over a wide range of thermodynamic states up to elevated temperatures and pressures as well as in the vicinity of critical points. This performance and versatility of the DLS technique is documented in the present study by highlighting measurement examples from recent thermophysical property research on different classes of working fluids relevant for process and energy technology.
The present article summarizes experimental and theoretical considerations required for a proper use of dynamic light scattering (DLS) for the measurement of transport properties of fluids. It addresses not only recent advancements of the method, but also aims to provide recommendations to researchers who intend to apply the technique in the future. As outlined in this study, DLS is based on the analysis of scattered light governed by microscopic statistical or periodic fluctuations that originate from the thermal movement of molecules and/or particles at macroscopic thermodynamic equilibrium. The dynamics of these hydrodynamic fluctuations in the bulk of fluids or at their phase boundaries are related to the underlying diffusive processes and, thus, to the associated transport properties, and are reflected by the time-dependent correlation function of the scattered light intensity. The fundamentals of this type of detection, known as photon correlation spectroscopy (PCS), will be discussed in the present contribution in some more detail. It is emphasized that the experiments need to be designed carefully in accordance with theory in order to assign the measurement signals to the corresponding hydrodynamic fluctuations. If the necessary conditions are fulfilled, DLS allows the accurate determination of several transport properties including kinematic and dynamic viscosity, thermal diffusivity, mutual diffusivity, and sound attenuation, which may be accessed together with other thermophysical properties such as speed of sound and surface or interfacial tension. In some instances, also the simultaneous determination of several transport properties is possible. With the exception of the sound attenuation, expanded uncertainties for the mentioned transport properties down to 1 % can be achieved for various types of fluid systems over a wide range of thermodynamic states up to elevated temperatures and pressures as well as in the vicinity of critical points. This performance and versatility of the DLS technique is documented in the present study by highlighting measurement examples from recent thermophysical property research on different classes of working fluids relevant for process and energy technology.
One concept for the safe storage and transport of molecular hydrogen (H2) is the use of hydrogen carrier systems which can bind and release hydrogen in repeating cycles. In this context, the liquid system based on isopropanol and its dehydrogenated counterpart acetone is particularly interesting for applications in direct isopropanol fuel cells that are operated with an excess of water. For a comprehensive characterization of diluted aqueous solutions of isopropanol or acetone with technically relevant solute amount fractions between 0.02 and 0.08, their liquid density, liquid viscosity, and interfacial tension were investigated using various light scattering and conventional techniques as well as equilibrium molecular dynamics (EMD) simulations between (283 and 403) K. Polarization-difference Raman spectroscopy (PDRS) was used to monitor the liquid-phase composition during surface light scattering (SLS) experiments on viscosity and interfacial tension. For comparison purposes and to expand the database, capillary viscometry and dynamic light scattering (DLS) from bulk fluids with dispersed particles were also applied to determine the viscosity while the pendant-drop (PD) method allowed access to the interfacial tension. By adding isopropanol or acetone to water, density and, in particular, interfacial tension decrease significantly, while viscosity shows a pronounced increase. The behavior of viscosity and interfacial tension is closely related to the strong hydrogen bonding between the unlike mixture components and the pronounced enrichment of both solutes at the vapor–liquid interface, as revealed by EMD simulations. For an aqueous solution with an isopropanol amount fraction of 0.04, minor variations in interfacial tension and viscosity were found in the presence of pressurized H2 up to 7.5 MPa. Overall, the results from this study contribute to an extended database for diluted aqueous solutions of isopropanol or acetone, especially at temperatures above 323 K.
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