SODI-DSC - Diffusion and Soret Coefficients Measurement for Improvement of Oil Recovery (DCMIX1)
  1. 2011 • ISS Increments 29-30
  2. 2011 • ISS "PromISSe"- long-duration mission
Physical Sciences:
  • Fluid physics
SODI (Selectable Optical Diagnostic Instrument)
Olivier Minster
S. van Vaerenbergh (1), F. Dubois (1), Z. Saghir (2), F. Montel (3), J.P. Caltagirone (4), G. Galliéro (4), M. Azaeiz (4), A. Shapiro (5), J.L. Daridon (6)
MRC - Microgravity Research Centre
Université Libre de Bruxelles
Chimie-Physique EP, CP165/62
50 avenue F.D. Roosevelt
1050 Bruxelles
Ryerson University
Department of Mechanical and Industrial Engineering
350 Victoria Street
Ontario M5B 2K3
Division Production-Exploitation
CSTJF - Le Centre Scientifique et Technique Jean Féger
avenue Larribau
64018 Pau cedex
Laboratoire TREFLE
16, av. Pey-Berland
33607 Pessac Cedex
Technical University of Denmark
Anker Engelundsvej 1
DK-2800 Kgs. Lyngby
Université de Pau
Av. de l´université
BP 576
64012 PAU Cedex

Diffusive processes are ubiquitous in daily life and in natural processes, and play a key role in the transformation and mixing of fluid mixtures. In this context, the term diffusion is used to describe the relative motion of a species with respect to the other and can be caused by a concentration (isothermal diffusion) or temperature (thermal diffusion) across the mixture or by a potential gradient (as sedimentation).

A very peculiar natural laboratory where mixing processes in fluid mixtures have a high scientific and industrial interest is the one of oil reservoirs, where all the above mentioned effects contribute to the distribution of the component of the mixture that forms crude oils. Among them, a role is played by thermal diffusion caused by temperature gradient that develops inside reservoirs, assessing around an average value of 3ºC/100 m.

The prediction of hydrocarbon composition is an important factor that contributes to the reservoirs exploitation strategies. Since the cost of resources increases with depth, the oil companies are interested in reliable thermodynamical models that allow the characterisation of an entire reservoir using a reduced number of exploratory wells. To better model the complex behaviour of crude oils, a better prediction of the thermal diffusion or Soret effect could be included. To this extent, there is a need of an experimental determination of the diffusion and thermal diffusion coefficients of crude oils.

To summarise, the purpose of the DSC experiment is:
1. to measure the isothermal and thermal diffusion coefficient of a ternary system that is representative of the three main families of crude oils;
2. To validate a measurement technique to be used by petroleum industries or in a ISS application program at low residual gravity level;
3. to refine numerical models of oil reservoirs using diffusion data from the experiment
4. to refine and obtain mixing rules allowing to predict diffusion coefficients form a n component mixtures from the ones with n-1 components

It is mandatory to perform diffusion limited experiments at a very low gravity level, in order not to perturb the long duration processes and to be able to obtain reliable values that can be used in numerical models.

previous experiments in microgravity
The team has an extensive experience in space experiments. What follows is a list of project related with diffusion and Soret coefficient measurement:
- Soret Coefficient Measurement Experiment (Legros and Van Vaerenbergh), EURECA mission, 1992;
- Diffusion coefficients in crude oils (DCCO) (Legros, Van Vaerenbergh, Dubois, Montel, Shapiro, Caltagirone, Saghir and Piercey), ISS 5S “Odissea” mission, 2002;
- Diffusion and Soret Coefficient Measurements for Improvement of Oil Recovery (SCCO-1, SCCO-2 and SCCO-3), (J.C. Legros, F. Montel, A.Shapiro, J.P Caltagirone, Z. Saghir, G. Piercey), FOTON M1, M2, M3 missions.
- Thermovibrational convection in microgravity (TEVICON) (Shevtsova, Mialdun, Ryzhkov, Melnikov), 46th Parabolic Flight Campaign in 2007 and 48th ESA Parabolic Flight Campaign in 2008
- Solutovibrational convection in microgravity (SOVICON) (Shevtsova, Mialdun, Gaponenko, Melnikov), 50th ESA Parabolic Flight Campaign, 2009
- Influence of Vibration on Diffusion in Liquids (IVIDIL) (Shevtsova, Saghir), SODI IVIDIL experiment on the International Space Station, 2009

VIPIL-FARADAY II - Vibration in liquids
60th ESA Parabolic Flight Campaign - 2014

Vibrational phenomena in liquids - VIPIL
59th ESA Parabolic Flight Campaign - 2013

SODI-IVIDIL - Selectable Optical Diagnostics Instrument-Influence of VIbrations on DIffusion of Liquids
ISS Increment 19 - 21/22  2009

SOluto-VIbrational CONvection in reduced gravity (SOVICON)
50th ESA Parabolic Flight Campaign - 2009

TEVICON-1 - Thermo-vibrational convection in reduced gravity
48th ESA Parabolic Flight Campaign - 2008

TEVICON - Transient time of thermal-vibrational convection in reduced gravity
46th ESA Parabolic Flight Campaign - 2007

link to project website of the E-USOC

The DSC experiment will be performed in SODI.

The Selectable Optical Diagnostic Instrument (SODI) instrument is an interferometer that shines a laser beam through liquid mixtures and compares it to another beam that does not pass through the sample.By comparing the time it takes to pass through the sample and air, researchers can record the mixing process itself.
The liquids of interest are mixtures of different liquids and colloids, liquids with minute particles suspended in them. Most liquids can be considered colloids, from milk to oil. Never at rest, the components move continuously, influenced by movement (such as shaking and mixing), gravity and changes in temperature.
Researchers want to understand how these factors destabilise the mixtures but investigating the process on Earth is hampered by the pull of gravity. Running an experiment on the International Space Station removes gravity from the mix and allows us to focus on a single factor in the equation: temperature.
A number of liquids have been investigated over the years with the SODI hardware, all placed inside the European-built microgravity science glovebox on the Space Station. Once setup by an astronaut and containers holding the mixtures are inserted, the experiments are controlled from Earth.

The DSC experiment will be performed in two different cells: the primary cells that are probed by MZI (Mach Zehnder Interferometry) and the companion cells that are filled with tracer particles and are probed by digital holography for PIV (Particle Image Velocimetry).

• Experiment protocol (primary cell): the sample is thermalised at a temperature of 45 ºC (35 degC for optional runs). The MZI images acquisition is switched on and the isothermal condition is checked by MZI. Then, a temperature difference of 10 ºC (minimum requirement by design, any higher value that can be validated by test will be implemented) is applied to the sample (Thot=50 ºC, Tcold=40ºC). After a transient time, the Soret separation phase begins. The MZI image acquisition rate changes with time. Then, the thermal gradient is removed and the temperature of the cell is brought back to the isothermal condition. After a transient time, the isothermal diffusion relaxation phase starts. The MZI image acquisition rate changes with time. This forms an experimental run.

• Experiment protocol (companion cell): the companion cell experimental procedure follows exactly the one for the primary cell.

• Parameters measured:
– temperature of the primary cell. The temperature is controlled with an accuracy better than 0.1 K and measured with a resolution of 0.01 K
– temperature of the companion cell. Performance of the control and measurement system: same as above.
– power dissipated by the TECs (Thermo Electric Cooler) both in the primary and in the companion cell;

• Number of samples the experiment is performed in parallel in the primary and in the companion cell. The primary cells are filled with a mixture of THN (Tetraline), IBB (Isobutylbenzene) and C12 (Dodecane) or a binary mixture of water/n-penthanol. The companion cell is filled with IBB. The primary and companion cells shall be visibly bubble free after filling.

UPDATE on experiment implementation
On 7 November 2011 ISS Flight Engineer Satoshi Furukawa installed the SODI-DSC hardware in the Microgravity Science Glovebox in the US-American Destiny laboratory. The first science run was started on 9 November 2011. Until January 2012 about 50 scientific runs could be completed. On 16 January 2012 ESA astronaut André Kuipers completed the experiment by removing the experiment hardware from the Microgravity Science Glovebox (MSG) and stowing it.

The main goal of the DSC experiment is an accurate determination of the four isothermal diffusion coefficients and the two thermal ones for the 10 samples.

The post flight scientific activity will be:
– a comparison between the measured diffusion coefficients and the ones obtained in numerical models from fitting of segregation data of specific reservoirs assuming reservoir equilibrium.
– The establishment of mixing rules.
– A refinement of petroleum reservoir models.
– The dissemination of results to industrial partners.
– The assessment of future model requirements.

from Reference Document [12]
S. Kozlova, A. Mialdun, I. Ryzhkov, T. Janzen, J. Vrabec, V. Shevtsova, (2019), "Do ternary liquid mixtures exhibit negative main Fick diffusion coefficients?", Physical Chemistry Chemical Physics, 21, 4, DOI: 10.1039/C8CP06795C, pp. 2140-2152.

Experimental data on Fick diffusion coefficients of ternary and higher mixtures depend on the reference frame; those which are in common use are associated with the average velocity either with respect to volume, mass or mole number. In this study, the dependence of diffusion coefficients on the reference frame is thoroughly analyzed for three ternary mixtures of different types. The first one, tetralin–isobutylbenzene–dodecane, can almost be considered as ideal, the second one, cyclohexane–toluene–methanol, exhibits liquid–liquid phase separation and the third one, water–ethanol–triethylene glycol, contains three associating species and is also strongly non-ideal. Experimental diffusion coefficient data sampled in the volume reference frame are transformed to the molar and mass reference frames. The required partial molar volumes are derived from present density measurements. Four additional mixtures are considered along a single or two composition paths. A highlight of this study is the existence of a strong similarity of the main diffusion coefficients in the volume and mass reference frames for all considered mixtures. When the excess volume is small, the coefficients in the molar reference frame are also similar. However, for the mixture with a large excess volume (containing water), the diffusion coefficients in the molar reference frame differ significantly, even indicating negative main diffusion coefficients. It is shown that negative main diffusion coefficients appear due to relatively large experimental uncertainties of cross diffusion coefficients, which are propagated and amplified by frame transformation.

from Reference Document [13]
T. Triller, D. Sommermann, M. Schram, I.F. Sommer, E. Lapeira, M.M. Bou-Ali, W. Köhler, (2019), "The Soret effect in ternary mixtures of water+ethanol+triethylene glycol of equal mass fractions: Ground and microgravity experiments", The European Physical Journal E, 42, 27.

Measurements of the Soret and thermodiffusion coefficients of a symmetric ternary mixture with equal mass fractions of water, ethanol, and triethylene glycol have been performed by two-color optical beam deflection (2-OBD) and the thermogravitational column technique (TGC) in the laboratory and under microgravity conditions in the Selectable Optical Diagnostics Instrument (SODI) aboard the International Space Station. The results from all three experimental techniques agree within the experimental error bars, which result mainly from the inversion of the contrast factor matrices. TGC shows by far the lowest, 2-OBD the highest error amplification. The microgravity measurements are in between. The agreement with the microgravity results shows that thermosolutal convection could be well controlled in the 2-OBD experiments by a proper orientation of the temperature gradient. Despite the different condition numbers, the results are invariant under the choice of the independent compositions. Based on the orientation of the confidence ellipsoid in the ternary composition diagram, not all coefficients are equally affected by experimental errors. Although there are appreciable uncertainties for water and ethanol, the Soret and the thermodiffusion coefficients of triethylene glycol could be obtained with a good accuracy due to the favorable orientation of the confidence ellipsoid. We have found that water behaves thermophobic, corresponding to a positive Soret coefficient, whereas both ethanol and triethylene glycol are thermophilic with negative Soret coefficients. This resembles the behaviour of the binary system ethanol/water above the ethanol concentration of the sign change.

Reference Document [14] 
Galand, Q., Van Vaerenbergh, S., Köhler, W., Khlybov, O., Lyubimova, T., Mialdun, A., Ryzhkov, I., Shevtsova, V., Triller, T., (2019), "Results of the DCMIX1 experiment on measurement of Soret coefficients in ternary mixtures of hydrocarbons under microgravity conditions on the ISS", The Journal of Chemical Physics151, https://doi.org/10.1063/1.5100595, pp. 134502.
includes a comprehensive study of possible data processing sequences for the interpretation of interferometric Soret experiments in ternary systems. Several data processing methodologies are discussed. A significant concentration dependence of the Soret coefficients is observed. In the present study, we have obtained large and positive values for THN and negative ones for IBB in all investigated systems. A linear relation between the Soret coefficients of two components is derived for each system and allows validating experimentally the coefficients measured in other experiments.
J.P. Garandet, J.P. Praizey, S. Van Vaerenbergh, T. Alboussière, (1997), "On the problem of natural convection in liquid phase thermotransport coefficients measurements", Physics of Fluids, vol 9, n.3, pp. pp. 510-518.
L. MONTEL, J.C. LEGROS, M.Z. SAGHIR, A. SHAPIRO, J.L. DARIDON, G. GALLIéRO, S. Van Vaerenbergh, (2005), "DSC program : multicomponent processes in crudes", ESA, SP 1290, pp. 202-213.
M. Khawaja, S. Van Vaerenbergh, M.Z. Saghir, (2005), "Theoretical analysis and comparison with experimentation of the molecular diffusion and thermal diffusion coefficients for a ternary hydrocarbon mixtures", Journal of non Equilibrium thermodynamics, vol 30, pp. pp. 359-374.
S. Van Vaerenbergh, J.C. Legros, T. Karapantios, K. Kostoglou, Z. Saghir, (2006), "Multicomponent transport studies of crude oils and asphaltenes in DSC program", Microgravity Science and technology, XVIII-3/4.
I.I. Ryzhkov, V.M. Shevtsova, (2007), "On thermal diffusion and convection in multicomponent mixtures with application to the thermogravitational column", Physics of Fluids, vol 19, 027101.
Q. Galand, S. Van Vaerenbergh, F. Montel, (2008), "Measurement of Diffusion Coefficients in binary and ternary mixtures by the Open Ended Capillary Technique and the DSC microgravity experiment", Energy Fuels, 22, 2, DOI: 10.1021/ef7004332, pp. 770-774.
G. Galliero, F. Montel, (2008), "Nonisothermal gravitational segregation by molecular dynamics simulations", Physical Review E, 78, pp. 041203.
S. VanVaerenbergh, S. Srinivasan, M.Z. Saghir, (2009), "Thermodiffusion in multicomponent hydrocarbon mixtures: Experimental investigations and computational analysis", Journal of Chemical Physics, 131, 11, DOI:10.1063/1.3211303, pp. 114505.
S. Srinivasan, M.Z. Saghir, (2009), "Measurements on thermodiffusion in ternary hydrocarbon mixtures at high pressure", Journal of Chemical Physics, 131, DOI:10.1063/1.3236745, pp. 124508.
R. Jurado, J. Pallarès, J. Gavaldà, X. Ruiz, (2018), "On the impact of the ISS reboosting maneuvers during thermodiffusion experiments of ternary liquid systems: Pure diffusion", International Journal of Thermal Sciences, 132, DOI: https://doi.org/10.1016/j.ijthermalsci.2018.05.040, pp. 186-198.
T. Janzen, J. Vrabec, (2018), "Diffusion Coefficients of a Highly Nonideal Ternary Liquid Mixture: Cyclohexane-Toluene-Methanol", Industrial and Engineering Chemistry Research, 57, 48, DOI: 10.1021/acs.iecr.8b04385, pp. 16508-16517.
S. Kozlova, A. Mialdun, I. Ryzhkov, T. Janzen, J. Vrabec, V. Shevtsova, (2019), "Do ternary liquid mixtures exhibit negative main Fick diffusion coefficients?", Physical Chemistry Chemical Physics, 21, 4, DOI: 10.1039/C8CP06795C, pp. 2140-2152.
T. Triller, D. Sommermann, M. Schram, I.F. Sommer, E. Lapeira, M.M. Bou-Ali, W. Köhler, (2019), "The Soret effect in ternary mixtures of water+ethanol+triethylene glycol of equal mass fractions: Ground and microgravity experiments", The European Physical Journal E, 42, 27.
Q. Galand, S. Van Vaerenbergh, W. Köhler, O. Khlybov, T. Lyubimova, A. Mialdun, I. Ryzhkov, V. Shevtsova, T. Triller, (2019), "Results of the DCMIX1 experiment on measurement of Soret coefficients in ternary mixtures of hydrocarbons under microgravity conditions on the ISS", The Journal of Chemical Physics, 151, https://doi.org/10.1063/1.5100595, pp. 134502.
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Experiment concept diagram. The sample is visualized by means of an Interferometry set-up where the cell is probed by two wavelengths. A temperature gradient perpendicular to the optical path is applied to the cell.

ISS030-E-155917 (16 January 2012) European Space Agency astronaut Andre Kuipers, Expedition 30 flight engineer, prepares to place Diffusion Soret Coefficient (DSC) hardware in stowage containers in the Destiny laboratory of the International Space Station. Credit: NASA/ESA
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