The present work demonstrates that by the analysis of the dynamics of non-equilibrium fluctuations using the shadowgraph method, the thermal diffusivity, the Fick diffusion coefficient, the kinematic viscosity, and the Soret coefficient of a binary mixture can be determined from a single thermodiffusion experiment. The study was performed for a mixture consisting of equal masses of 1,2,3,4-tetrahydronaphthalene and n-dodecane in a newly developed shadowgraph apparatus at temperatures up to 373 K and pressures up to 40 MPa. The obtained results are mainly discussed in the light of their uncertainties at varying thermodynamic states for evaluating the benefits, drawbacks, and potentials of the apparatus. The Fick diffusion coefficient and the thermal diffusivity obtained with average expanded uncertainties of 2.8% and 6.6% agree with literature data and measurements for the same mixture taken by heterodyne dynamic light scattering. Current limitations of the method are reflected by the distinctly larger uncertainties of the kinematic viscosity and the Soret coefficient. Corresponding reasons and potential measures to overcome the limitations are discussed.

1.
R.
Skorpa
,
T. J. H.
Vlugt
,
D.
Bedeaux
, and
S.
Kjelstrup
,
J. Phys. Chem. C
119
,
12838
(
2015
).
2.
Greener Fischer-Tropsch Processes for Fuels and Feedstocks
, edited by
P. M.
Maitlis
and
A.
de Klerk
(
WILEY-VCH Verlag GmbH & Co. KGaA
,
Weinheim, Germany
,
2013
).
3.
S. R.
De Groot
and
P.
Mazur
,
Non-Equilibrium Thermodynamics
, Dover Books on Physics (
Dover Publications
,
New York
,
1984
).
4.
J. D.
Figueroa
,
T.
Fout
,
S.
Plasynski
,
H.
McIlvried
, and
R. D.
Srivastava
,
Int. J. Greenhouse Gas Control
2
,
9
(
2008
).
5.
G. T.
Rochelle
,
Science
325
,
1652
(
2009
).
6.
S.
Hollinger
and
M.
Lücke
,
Phys. Rev. E
57
,
4238
(
1998
).
7.
K.
Ghorayeb
,
A.
Firoozabadi
, and
T.
Anraku
,
SPE J.
8
,
114
(
2003
).
8.
W.
Wu
,
T.
Klein
,
M.
Kerscher
,
M. H.
Rausch
,
T. M.
Koller
,
C.
Giraudet
, and
A. P.
Fröba
,
J. Phys. Chem. B
123
,
8777
(
2019
).
9.
P.
Blanco
,
M.
Mounir Bou-Ali
,
J. K.
Platten
,
P.
Urteaga
,
J. A.
Madariaga
, and
C.
Santamaria
,
J. Chem. Phys.
129
,
174504
(
2008
).
10.
C. R.
Wilke
and
P.
Chang
,
AIChE J.
1
,
264
(
1955
).
11.
A. P.
Fröba
and
A.
Leipertz
,
Diffus. Fundam. 2
2
,
63-1
(
2005
).
12.
W.
Wu
,
T.
Klein
,
M.
Kerscher
,
M. H.
Rausch
,
T. M.
Koller
,
C.
Giraudet
, and
A. P.
Fröba
,
J. Phys. Chem. B
124
,
2482
(
2020
).
13.
S.
Wiegand
,
H.
Ning
, and
H.
Kriegs
,
J. Phys. Chem. B
111
,
14169
(
2007
).
14.
A.
Königer
,
B.
Meier
, and
W.
Köhler
,
Philos. Mag.
89
,
907
(
2009
).
15.
A.
Mialdun
and
V.
Shevtsova
,
J. Chem. Phys.
134
,
044524
(
2011
).
16.
D. A.
Weltz
,
Nature
390
,
233
(
1997
).
17.
J. M. O.
de Zárate
and
J. V.
Sengers
,
Hydrodynamic Fluctuations in Fluids and Fluid Mixtures
, 1st ed. (
Elsevier
,
2006
).
18.
J. M.
Ortiz de Zárate
,
C.
Giraudet
,
H.
Bataller
, and
F.
Croccolo
,
Eur. Phys. J. E
37
,
77
(
2014
).
19.
H.
Bataller
,
C.
Giraudet
,
F.
Croccolo
, and
J. M.
Ortiz de Zárate
,
Microgravity Sci. Technol.
28
,
611
(
2016
).
20.
I.
Lizarraga
,
C.
Giraudet
,
F.
Croccolo
,
M. M.
Bou-Ali
, and
H.
Bataller
,
Microgravity Sci. Technol.
28
,
545
(
2016
).
21.
R.
Cerbino
,
A.
Vailati
, and
M.
Giglio
,
Philos. Mag.
83
,
2023
(
2003
).
22.
R.
Cerbino
,
Shadowgraphic Study of Convection in a Colloidal Suspension
(
University degli Studi di Milano
,
2005
).
23.
A.
Vailati
and
M.
Giglio
,
Nature
390
,
262
(
1997
).
24.
F.
Croccolo
,
L.
García-Fernández
,
H.
Bataller
,
A.
Vailati
, and
J. M.
Ortiz De Zárate
,
Phys. Rev. E
99
,
012602
(
2019
).
25.
C.
Soret
,
Arch. Sci. Phys. Nat.
2
,
48
(
1879
).
26.
C.
Ludwig
,
Akad. Wiss. Wien Math.-Naturwiss.
20
,
539
(
1856
).
27.
R.
Schmitz
and
E. G. D.
Cohen
,
J. Stat. Phys.
40
,
431
(
1985
).
28.
C.
Giraudet
,
H.
Bataller
,
Y.
Sun
,
A.
Donev
,
J. M.
Ortiz de Zárate
, and
F.
Croccolo
,
Europhys. Lett.
111
,
60013
(
2015
).
29.
C.
Giraudet
,
H.
Bataller
,
Y.
Sun
,
A.
Donev
,
J. M.
Ortiz de Zárate
, and
F.
Croccolo
,
Eur. Phys. J. E
39
,
120
(
2016
).
30.
S.
Hartmann
,
G.
Wittko
,
W.
Köhler
,
K. I.
Morozov
,
K.
Albers
, and
G.
Sadowski
,
Phys. Rev. Lett.
109
,
065901
(
2012
).
31.
A.
Shojaei
,
M.
Fahimian
, and
B.
Derakhshandeh
,
Compos. Sci. Technol.
67
,
2665
(
2007
).
32.
A. G.
Avval
and
S. M.
El-Ghazaly
, in
2018 Texas Symposium on Wireless and Microwave Circuits and Systems
(
IEEE
,
2018
), pp.
1
4
.
33.
J. P.
McCullough
,
H. L.
Finke
,
J. F.
Messerly
,
S. S.
Todd
,
T. C.
Kincheloe
, and
G.
Waddington
,
J. Phys. Chem.
61
,
1105
(
1957
).
34.
A.
Lalnez
,
M. M.
Rodrigo
,
E.
Wilhelm
, and
J. P. E.
Grolier
,
J. Chem. Eng. Data
34
,
332
(
1989
).
35.
M. L.
Huber
,
A.
Laesecke
, and
R.
Perkins
,
Energy Fuels
18
,
968
(
2004
).
36.
E. F.
May
,
W. J.
Tay
,
M.
Nania
,
A.
Aleji
,
S.
Al-Ghafri
, and
J. P.
Martin Trusler
,
Rev. Sci. Instrum.
85
,
095111
(
2014
).
37.
B.
Chu
,
Laser Light Scattering: Basic Principles and Practice
, 2nd ed. (
Academic Press
,
1991
).
38.
A. P.
Fröba
,
Dynamic Light Scattering (DLS) for the Characterization of Working Fluids in Chemical and Energy Engineering
(
Friedrich-Alexander-University Erlangen- Nuremberg
,
2009
).
39.
T.
Klein
,
W.
Wu
,
M. H.
Rausch
,
C.
Giraudet
,
T. M.
Koller
, and
A. P.
Fröba
,
J. Phys. Chem. B
122
,
7122
(
2018
).
40.
G.
Cerchiari
,
F.
Croccolo
,
F.
Cardinaux
, and
F.
Scheffold
,
Rev. Sci. Instrum.
83
,
106101
(
2012
).
41.
F.
Croccolo
,
D.
Brogioli
,
A.
Vailati
,
M.
Giglio
, and
D. S.
Cannell
,
Appl. Opt.
45
,
2166
(
2006
).
42.
F.
Croccolo
,
F.
Scheffold
, and
H.
Bataller
,
C. R. Mec.
341
,
378
(
2013
).
43.
F.
Croccolo
,
D.
Brogioli
,
A.
Vailati
,
M.
Giglio
, and
D. S.
Cannell
,
Phys. Rev. E
76
,
041112
(
2007
).
44.
C.
Giraudet
,
H.
Bataller
, and
F.
Croccolo
,
Eur. Phys. J. E
37
,
107
(
2014
).
45.
H.
Bataller
,
C.
Miqueu
,
F.
Plantier
,
J.-L.
Daridon
,
T. J.
Jaber
,
A.
Abbasi
,
M. Z.
Saghir
, and
M. M.
Bou-Ali
,
J. Chem. Eng. Data
54
,
1710
(
2009
).
46.
J. K.
Platten
,
M. M.
Bou-Ali
,
P.
Costesèque
,
J. F.
Dutrieux
,
W.
Köhler
,
C.
Leppla
,
S.
Wiegand
, and
G.
Wittko
,
Philos. Mag.
83
,
1965
(
2003
).
47.
G.
Wittko
and
W.
Köhler
,
Philos. Mag.
83
,
1973
(
2003
).
48.
J. K.
Platten
,
M. M.
Bou-Ali
, and
J. F.
Dutrieux
,
Philos. Mag.
83
,
2001
(
2003
).
49.
M.
Gebhardt
,
W.
Köhler
,
A.
Mialdun
,
V.
Yasnou
, and
V.
Shevtsova
,
J. Chem. Phys.
138
,
114503
(
2013
).
50.
H.
Matsuura
and
Y.
Nagasaka
,
Rev. Sci. Instrum.
89
,
024903
(
2018
).
51.
M.
Arko
and
A.
Petelin
,
Soft Matter
15
,
2791
(
2019
).
52.
A.
Oprisan
,
A.
Rice
,
S. A.
Oprisan
,
C.
Giraudet
, and
F.
Croccolo
,
Eur. Phys. J. E
40
,
14
(
2017
).
53.
M.
Piszko
,
W.
Wu
,
S.
Will
,
M. H.
Rausch
,
C.
Giraudet
, and
A. P.
Fröba
,
Fuel
242
,
562
(
2019
).
54.
R.
Kita
and
S.
Wiegand
,
Macromolecules
38
,
4554
(
2005
).
55.
K. J.
Zhang
,
M. E.
Briggs
,
R. W.
Gammon
, and
J. V.
Sengers
,
J. Chem. Phys.
104
,
6881
(
1996
).
56.
Y.
Kishikawa
,
S.
Wiegand
, and
R.
Kita
,
Biomacromolecules
11
,
740
(
2010
).
57.
G.
Wittko
and
W.
Köhler
,
Europhys. Lett.
78
,
46007
(
2007
).
58.
P.
Kolodner
,
H.
Williams
, and
C.
Moe
,
J. Chem. Phys.
88
,
6512
(
1988
).

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