The Journal of Supercritical Fluids 134 (2018) 21–27

Contents lists available at ScienceDirect

The Journal of Supercritical Fluids

journal homepage: www.elsevier.com/locate/supflu

Current theoretical opinions and perspectives on the fundamental T

description of supercritical fluids
⁎
Tae Jun Yoon, Youn-Woo Lee
School of Chemical and Biological Engineering and Institute of Chemical Processes, Seoul National University, 1 Gwanak-ro, Gwanak-gu, Seoul 151-744, Republic of Korea

G RA P H I C A L AB S T R A C T

A R T I C L E I N F O A B S T R A C T

Keywords: We briefly overview the theoretical advances for the fundamental description on the supercritical fluids since the
Supercritical gas-liquid boundary late 1980s. The concept of supercritical gas-liquid boundary and its importance are introduced. The current state
Density inhomogeneity of the state-of-art theories about supercritical gas-liquid boundary (Integral Equation Approximation,
Integral equation approximation Fluctuation Theory of Solutions, and molecular simulations) are examined. Based on these principles and the
Fluctuation theory of solutions
remarkable progresses in the field of supercritical fluids, the direction of future research and promising meth-
Molecular simulation
odologies are given. The future researches on the fundamental descriptions of supercritical fluids are expected to
play a crucial role in extending the knowledges and utilizing supercritical fluid technologies.

1. Introduction
In recent 40 years, supercritical fluid science and technology have
bloomed. Supercritical fluids have been widely utilized in the physical
and/or chemical processes such as extraction, impregnation, pre-
cipitation, extrusion, drying, chromatography, leaching, power gen-
eration, and hydrothermal synthesis [1–8]. This versatility of super-
critical fluids stems from their duality. they can have both gas-like and
liquid-like properties depending on the thermodynamic conditions, and
these thermophysical and transport properties are instantaneously
tunable.
The idea that supercritical fluid is not a single homogeneous fluid,
but an inhomogeneous fluid at molecular level where gas-like and
liquid-like structure coexists starts from the Bernal’s metal ball ex-
periments [9,10]. From his experiments, Bernal classified fluids into
four categories including gas, associated gas, expanded liquid and li-
quid and defined a hypercritical line between associated gas and ex-
panded liquid. This idea was firstly verified by the experimental mea-
surements of the critical anomalies around the critical point by Sengers
and Voronel [11]. These behaviors cannot be understood from the
viewpoint of mean-field theory. Thus, the theory of critical phenomena
and fluid polyamorphism theory were employed and supported by
spectroscopic measurements, which showed that large density fluctua-
tion becomes maximum at a certain set of thermodynamic states
[12–18]. This set of thermodynamic states, called hypercritical line by
Bernal, is later defined the supercritical gas-liquid boundary, Widom

⁎
Corresponding Author.
E-mail address: ywlee@snu.ac.kr (Y.-W. Lee).

https://doi.org/10.1016/j.supflu.2017.11.022
Received 8 September 2017; Received in revised form 23 November 2017; Accepted 23 November 2017
Available online 24 November 2017
0896-8446/ © 2017 Elsevier B.V. All rights reserved.
T.J. Yoon, Y.-W. Lee
line [19–21], or pseudo-boiling line [8,22–24], which is under active
investigation by physicists, chemists and chemical engineers.
Supercritical gas-liquid boundary is of great importance in the
fundamental aspect and the application of supercritical fluid technol-
ogies. In the fundamental viewpoint, the existence of the supercritical
gas-liquid boundary leads to the following fundamental questions. How
do we define liquid-like and/or gas-like properties of supercritical
fluids? Seeking answers for these questions will result in a revised phase
diagram. From the aspects of application, this revised phase diagram is
used to reduce operating costs and maximize the efficiency of processes
because the supercritical gas-liquid boundary could be a reference state
for tuning the thermodynamic properties. Ultimately, theoretical un-
derstanding of supercritical fluids will lead to the rational design of
global equation of state for the prediction/correlation of thermo-
physical properties of supercritical fluids [25,26]. For example, an ad-
dition of kernel term to traditional (i.e., van der Waals type) and mo-
lecular-based (i.e., Statistical Associating Fluid Theory (SAFT),
perturbed hard chain theory) EoS leads to more accurate description of
supercritical fluids for a wide range of thermodynamic condition. Thus,
theoretical advances on the fundamental properties of supercritical
fluids are expected to give physical insights and solid backgrounds for
building this type of EoS in rational and efficient ways. This direction of
researches is reviewed in the article written by Vega in this special
issue.
So far, theoretical researches for understanding the supercritical
gas-liquid boundary have extensively exploited the statistical mechan-
ical theories (the Integral Equation Approximation (IEA) and the
Fluctuation Theory of Solutions (FST)) and molecular simulations since
late 1980s. Initially, these studies have been heavily contributed to
purely fundamental journals related to chemical physics and physical
chemistry, but number of relevant publications has increased con-
tinuously in The Journal of Supercritical Fluids (Fig. 1). This increase
substantiates that understanding the fundamental aspects of super-
critical fluids would enable us to provide an optimal solution for the
process design and analysis.
Therefore, in this work, a brief history of the theories relevant to the
supercritical gas-liquid boundary since late 1980s will be explored. An
extensive review on the hundreds of the publications is avoided.
Fundamental descriptions on the thermophysical and transport prop-
erties of supercritical fluids so far can be referred in textbooks [27–29],
and in-depth extensive reviews on the methodologies mentioned in this
work can be found in other literatures [30–32]. Instead, some historical
cornerstones and recent important publications are highlighted. Then, a
perspective on the future direction and prospective tools for the theo-
retical exploration of supercritical fluids will be covered.
2. History and current state
2.1. Integral equation approximations
IEA and FST could be regarded as main successful applications of
the statistical mechanics on the phase behavior of supercritical fluids.
Fig. 1. An increase in the publications dealing with molecular simulations and statistical
mechanical theory in The Journal of Supercritical Fluids. The statistical data was obtained
from Scopus with the combined search words “molecular simulation” or “fluctuation
theory” in the article title, abstract and keywords and “The Journal of Supercritical
Fluids” in the source title.
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The Journal of Supercritical Fluids 134 (2018) 21–27
IEA is a numerical procedure for the structural analysis of a system
based on correlation functions. Homogeneous IEA has been mainly used
to describe liquid structure and solution thermodynamics. It consists of
homogeneous Ornstein-Zernike Equation and the closure relations such
as the Percus-Yevick (PY) and Hypernetted Chain (HNC) closures. By
solving simultaneous equations, the pair correlation functions and the
direct correlation functions can be obtained. The correlation function
obtained from IEA is used to estimate the thermodynamic properties
based on FST [32]. FST provides an expression for the pair correlation
function integral, which is also called Kirkwood-Buff Integral (KBI). FST
can be directly related to the experimental data at any solution com-
position by the inversion procedure proposed by Ben-Naim and Smith
[33,34].
IEA in conjunction with the FST was mainly used in studies dealing
with the divergence of partial molar volume of a solute (v͠ 2∞) in dilute
supercritical mixtures in the 1990s. The sign of divergence seemed to be
related with the extent of intermolecular energy. Hence, Debenedetti
proposed to classify solutes into three categories depending on the ex-
tent of the interaction energy; attractive, repulsive and weakly attrac-
tive solutes [35]. The formation of distinct cluster structure was first
proposed as a physical mechanism behind the divergence in the partial
molar volume [17]. However, in the early 1990s, IEA yielded that the
divergence did not mainly come from the strong attraction and/or re-
pulsive forces between solute and supercritical fluids [36]. Rather,
earlier studies from the IEA showed that the large density fluctuation in
neat supercritical fluids was mainly responsible for the divergence. To
resolve the controversy, Chialvo and Cummings decomposed v͠ 2∞ into
short-range and long-range contributions by relating FST with IEA [37].
This approach distinguished the short-range contribution to the diver-
gence from the long-range contribution, but did not provide the origin
of high-density domain around an attractive solute. Thus, Ruckenstein
and Shulgin modified the definition of excess number of molecules
around a solute molecule to describe the density inhomogeneity, and
hypothesized that the density inhomogeneity around a solute mainly
originates from the pre-existent density fluctuation [38]. The low ac-
curacy of homogeneous IEA made it hard to apply the method for the
quantitative analysis of the near-critical system. Hence, Egorov et al.
recently improved the accuracy by introducing the inhomogeneous
Ornstein-Zernike Equation proposed by Attard [39,40]. These theore-
tical advances not only provide a physicochemical explanation on the
solvation mechanism, but also be readily applied to model the solubility
of solute in supercritical fluids. The employment of FST for the pre-
diction of solute solubility was largely endeavored by Ruckenstein and
Shulgin [41]. Based on the FST formulations, they developed analytic
expressions for the prediction of solute solubility in neat supercritical
fluids and their mixtures. Abbott and Schimizu demonstrated how FST
methodologies can provide a physical insight to understand the solva-
tion mechanism in supercritical CO2/co-solvent mixture as well as be
easily implemented as an user-friendly application (app) [42]. In
summary, statistical mechanical theories and their applications to su-
percritical fluid systems led us to analyze how this inhomogeneous
system works and provided useful tools to predict and/or correlate the
experimental results.
2.2. Molecular simulations
Along with the statistical mechanical theories, Monte Carlo (MC)
and classical Molecular Dynamics (MD) simulations have been widely
utilized for the characterization of the supercritical fluid system. In
time-independent MC simulations, the configurations of molecules can
be obtained by generating random numbers. Basically, the Metropolis
algorithm is the most common method to generate the configurations in
MC simulations [43]. In the Metropolis algorithm, new configurations
are generated from an old configuration by applying various molecular
motions (e. g., translation, vibration, rotation, and switching) to the
system. This new configuration can be either accepted or rejected by
T.J. Yoon, Y.-W. Lee
comparing the energies of old and new configurations. MD simulation,
on the other hand, is a time-dependent simulation. In MD simulations,
an initial configuration of molecules and their momenta are given. Then
the simultaneous equations of motion are numerically calculated for a
given period. The time step is usually on the order of femtoseconds. In
both classical MC and MD simulations, a forcefield, a set of interatomic
potential parameters, has been used to describe the phase behavior. The
basic principles of molecular simulations are included in well-known
textbooks [44–46].
In early stage, molecular simulations in the field of supercritical
fluids focused to obtain useful thermophysical properties such as the
density, solubility, diffusion coefficient, dielectric constant and visc-
osity. Supercritical CO2 and H2O have been extensively investigated
because of their wide industrial and academic uses. For supercritical
CO2 simulations, EPM, TraPPE and Zhang forcefields are frequently
used to model the interatomic potential [47–50]. For supercritical H2O,
SPC and TIP series forcefields have been mainly used [51,52]. Gen-
erally, water models are not satisfactory compared to CO2 models. For
instance, TIP4P/2005 had the closest critical point to the experimental
data, but showed approximately 10% deviation from the experimental
measurements [53]. Thus, modeling the hydrogen-bond induced asso-
ciation is difficult. In addition to property estimations [50,54–56], a
theory for the density inhomogeneity around the supercritical gas-li-
quid boundary is being established via molecular simulations. Com-
pared to IEA, molecular simulations require large computational costs,
but provide a large amount of data that cannot be obtained using IEA.
This collection of data, along with the emergence of the data science, is
now expected to be a powerful source for the theoretical improvement
to describe thermodynamic behavior around the supercritical gas-liquid
boundary.
Molecular simulation researches about the supercritical gas-liquid
boundary can be classified into two categories. First, a lot of researches
have been contributed to the specification of the location of super-
critical gas-liquid transition region. Brazhkin and his collaborators
showed that supercritical gas-liquid boundaries (Widom line and
pseudo-boiling lines) defined from different response functions are only
consistent with each other near the critical point (Tc < T < 1.3Tc)
[57–61]. This inconsistency among supercritical gas-liquid boundaries
was recently explained by May and Mausbach [20]. A noteworthy idea
on the similarity law of pseudo-boiling line was proposed by Banuti and
Ihme. They maintained that pseudo-boiling lines follow three-para-
meter corresponding state principle, which states that pseudo-boiling
lines of all substances are identical when they are compared at the same
reduced temperature, reduced pressure and the acentric factor [22,23].
This idea has a great potential to be utilized for engineering purpose,
which is dealt in the Future direction section.
Although supercritical gas-liquid boundary enables us to char-
acterize where the gas-like to liquid-like transition occurs, it does not
reflect the continuity of structural transition. In addition to the super-
critical gas-liquid boundary, therefore, Woodcock, Finney and Heyes
have focused on the thermodynamic boundaries of supercritical gas-
liquid transition region, also called supercritical mesophase [10,62,63].
Based on the rigidity calculation, they defined two percolation transi-
tion loci that bound the supercritical gas-liquid transition region. As
shown in Fig. 2, supercritical gas-liquid boundaries defined from the
response functions and correlation length and percolation transition
loci are sometimes overlapped, and they are not consistent with each
other. These results lead us to the following question. How can we
quantify the gas-like fraction and liquid-like fraction of supercritical
fluids inside the supercritical transition region? Can we define the su-
percritical mesophase consistently?
The answers are now sought by the second type of researches which
focus on the local geometric features of supercritical fluids. At initial
stage, these investigations defined some useful local quantities that
characterize the density inhomogeneity in terms of FST by Samios and
Maroncelli [64,65]. Based on these definitions, Tucker and co-workers
23
The Journal of Supercritical Fluids 134 (2018) 21–27
Fig. 2. Supercritical gas-liquid boundaries and percolation transition loci of Lennard-
Jones fluid obtained from the correlation length, response function maxima and the ri-
gidity discontinuity. Supercritical gas-liquid boundaries were obtained from the article of
Brazhkin et al. [57]. For percolation transition loci, the percolation transition pressures
were calculated from the density data given by Woodcock and Heyes [62].
first introduced a concept of distribution for the characterization of the
local densities [66,67]. From the two-dimensional Lennard-Jones fluid
simulation, Tucker et al. found that the shape of the local density dis-
tribution changes from right-skewed to almost symmetric distribution
as the bulk density increases at a fixed temperature. They divided the
high- and low-density region in the two-dimensional supercritical fluid
and described that the convergence behaviors of the pair correlation
functions from two domains were quite different. Independent from
these studies, Jedlovszky and his colleagues used Voronoi tessellation
to investigate the density inhomogeneity in supercritical fluids [68,69].
They discovered that the local density distribution defined from the
Voronoi polyhedrons changes from right-skewed to almost symmetric
as the pressure increased as Tucker et al. observed in the local density
distribution defined from the local coordination number [68,69]. They
also argued that the geometric characteristics of the Voronoi polyhedral
are related with the criticality. Thus, the local densities defined from
two independent studies were almost equal. The first statistical model
based on the local density distribution for the estimation of liquid-like
and gas-like fraction of supercritical fluids in the field of molecular si-
mulations was recently proposed by Lee et al. [70]. Lee et al. discovered
that the local density distributions of supercritical CO2 obtained from
Voronoi tessellation can be decomposed into gas-like and liquid-like
distributions. Thus, a statistical mixture model was built. This model
made it possible to quantify the gas-like fraction of supercritical system
and describe continuous structural transition in supercritical meso-
phase. They recently applied this statistical model for dilute naphtha-
lene/CO2 mixture to verify the hypothesis stated by Ruckenstein and
Shulgin [71]. They extended this hypothesis to a general type of solute
based on the classification proposed by Debenedetti et al.
From the perspective of the data science, these theoretical ad-
vancements in the field of molecular simulations can be viewed as a
long-term data science process (Fig. 3). Data science defines how a
collection of data can be transformed into a data product. This process
consists of the data collection, data processing, exploratory data ana-
lysis (EDA), model establishment, data visualization, and data product.
In terms of the data science process, response function and rigidity
analysis and geometric analysis on the inhomogeneity of supercritical
fluids can be described as EDA, a summary of the main characteristics
of the data for building a statistical model and/or hypothesis test [72].
Recent work by Lee and his colleagues can be regarded as the first trial
T.J. Yoon, Y.-W. Lee
to establish an integrated model that can explain the continuity of
structural transition as well as the specification of transition loci in
supercritical fluids. Therefore, the future direction and perspectives in
the field of molecular simulations can be expected from the data sci-
entific viewpoint.
3. Challenges
3.1. Integral equation approximations
The inhomogeneous Ornstein-Zernike Equation showed high accu-
racy for the estimation of the phase behavior near the critical point.
However, there are some limitations in applying the IEA to general
supercritical system. First, it is hard to apply the IEA methodology for
the polyatomic molecules [73]. Therefore, coarse-grained molecules
were used for the IEA calculation, or the molecular Ornstein-Zernike
Equation was proposed outside the field of supercritical science and
technology [74,75]. Another challenging aspect of IEA and FST is that
most of the studies mainly focus on the mean properties of the system.
As mean-field approximation fails near the critical point, this analysis
cannot give a concrete answer to the critical anomalies. Thus, the
theory of distributions should be introduced to describe the system near
the supercritical gas-liquid boundary. IEA is also vulnerable when ap-
plied to a pure fluid system. When a solute is inserted in a system, the
surrounding supercritical fluid molecules can be easily characterized
due to the existence of a solute. On the other hand, the identification of
local environment of neat fluid system is comparatively obscure: only
the mean local coordination number can be obtained [76]. Therefore,
the necessity for the introduction of statistical methods is receiving
attention from the FST. For instance, Smith and his collaborators ex-
tended the FST methodology to deal with triplet and quadruplet
number and energy fluctuations [77,78]. They found that the triplet
number fluctuation of three neat fluids (H2O, CO2, and SF6) has a ne-
gative sign in vapor, gas and supercritical gas-like region, and a positive
sign in the liquid and supercritical liquid-like region. They also pro-
vided the expressions for a non-Gaussian behavior of thermodynamic
variables in terms of the FST. Likewise, FST is heading towards the
general theory of supercritical fluids by considering the triplet and
quadruplet fluctuations. Independent from the IEA and FST, these
fluctuation behaviors are also considered in the field of the molecular
simulations in conjunction with data science.
3.2. Molecular simulations
As seen in Section 2.2., molecular simulations have been conducted
for the theoretical development as well as property estimation of su-
percritical fluids. To estimate thermophysical properties, the exact force
fields for various kinds of supercritical fluids and solutes are essential.
The force fields for supercritical CO2 show satisfactory results for many
systems, but there are few forcefields available for other common su-
percritical fluids such as dimethyl ether (CH3OCH3), fluoroform (CHF3)
and nitrous oxide (N2O) and their performances are yet to be verified
[79]. The large computational cost can also be a bottleneck for the
property estimation. For instance, most of the compounds of industrial
24
The Journal of Supercritical Fluids 134 (2018) 21–27
Fig. 3. Theoretical advances about the supercritical
gas-liquid transition as a data science process. It is
expected that the molecular simulation techniques
will be popularly used for understanding and pre-
dicting the thermophysical and transport properties
of supercritical fluids.
interest have low solubility in neat supercritical fluids; the number of
supercritical fluid molecules should be large (105 − 106 molecules)
enough to dissolve a solute molecule, which slows down the compu-
tation speed. Thus, coarse-grained (implicit) solvent models are em-
ployed for the simulation at the expense of accuracy of simulations. For
the characterization of the supercritical gas-liquid transition region, the
recently proposed statistical mixture model is fitted well to simulation
data near the critical region [70]. However, this does not mean that the
model provides an adequate description of the local density distribu-
tions in the whole thermodynamic regions as well. Also, the simplicity
of the model can be a double-edged sword; it comes at the price of
accuracy. Therefore, it is expected that other statistical models and/or
methodologies are required for the improvement of the model.
4. Future Directions/Perspectives
From the challenging issues and data science process, several pro-
spective methodologies and research themes can be expected. First, IEA
will have a significant influence in the computation and estimation of
pure supercritical fluid systems and their solutions if the molecular
Ornstein-Zernike Equation in conjunction with the inhomogeneous
fluid hypothesis can be developed. In property estimation using the
molecular simulations, the accurate forcefields that can be applied for a
wide range of pressures, temperatures, and concentrations are needed.
Therefore, the refinement of force fields and/or the use of alternative
methods such as the density functional theory (DFT) and quantum
mechanical (QM) calculations will be promising in improving the es-
timation results even at a large computational expense. This large
computational expense is believed to be relieved by a development of
the specialized hardware.
Data science process (Fig. 3) tells us that the development and the
utilization of the statistical models for the description of the general
structure of supercritical fluids can also be attractive research themes.
The simplicity of the first statistical model indicates that the refinement
of the methodology is necessary for a more accurate estimation and/or
prediction of the liquid-like and gas-like properties over the whole su-
percritical region. Alternative models can be obtained by using both the
artificial neural networks and/or other algorithmic methods. After an
accurate theoretical model is established, the goal will be to make a
data product. Data product, in this case, would be (1) a refinement in
the statistical mechanical theories and (2) a powerful engineering
model. First, as mentioned before, FST is expanding its research area
from the pair correlations to triplet and quadruplet fluctuations. As
these properties are not easily obtained from experimental results, it
would be expected that molecular simulation data will be used to verify
and modify the theory. Second, the engineering models based on clas-
sical thermodynamics is expected to be greatly improved when the
aforementioned methodologies are exploited like the crossover theory
applied for classical and modern molecular-based EoS [13]. Ultimately,
these theoretical advances will give us physical insights and meth-
odologies that lead to the improvement in the design and operation of
the supercritical fluid process. For instance, the similarity law suggested
by Banuti et al. can be used to obtain the thermophysical properties of a
supercritical fluid with very few experimental data. This scaling
T.J. Yoon, Y.-W. Lee
relationship gave a physical insight to develop an engineeringly useful
empirical scaling relations that can be found in the following work by
Hobold and da Silva which is published in The Journal of Supercritical
Fluids in 2018. They suggested the dimensionless heat and momentum
transfer equations and empirical correlations based on the corre-
sponding state principle. By using these correlations, they solved the
heat and momentum transfer equations of CO2 utilizing the water EoS
without any transport properties of supercritical CO2. Compared to the
solution obtained from the CO2 EoS, the statistical error was quite sa-
tisfactory. This indicates that a characterization of supercritical gas-li-
quid boundary makes it possible to predict the thermophysical prop-
erties without a requirement to build an exact EoS [80].
For research themes, the utilization of the IEA and molecular si-
mulations can be extended to the various systems of industrial and
academic interests. First, it is highly expected that the divergence of
response functions can be explained based on the thermodynamics of
fluid polyamorphism [81]. In this theory, the free energy of a system is
given as a combination of the free energy contribution terms of gas-like,
liquid-like and their mixing energy. The divergence of various quan-
tities is explained by this mixing term. When more advanced mixture
model and local density/energy relation is established, the fraction of
gas-like and liquid-like molecules of supercritical fluids at any ther-
modynamic system would be easily obtained from this model and used
to characterize the thermodynamic mixing quantities (Gibbs free en-
ergy, entropy, enthalpy). Second, most of the researches on the super-
critical gas-liquid boundary were limited to the model systems (Len-
nard-Jones fluid, square well fluid and hard sphere fluid) and neat
fluids. Thus, supercritical gas-liquid boundary of mixtures is under in-
vestigation. For example, Raju et al. firstly studied the pseudo-boiling
lines of supercritical mixture [24]. They observed that the number of
pseudo-boiling lines depend on the magnitude of intermolecular in-
teractions between two species. When two substances are well miscible,
a single pseudo-boiling line is obtained. On the contrary, two pseudo-
boiling lines are obtained when they are immiscible. It is expected that
geometric features of these mixtures would be dependent on the large
density fluctuation of supercritical fluids. Thus, the IEA/FST and mo-
lecular simulations in conjunction with data science methodologies
would play an important role for the characterization of supercritical
gas-liquid boundary of supercritical mixture. This will results in the
design of a new mixing rule, and this mixing rule would be used to
predict the entrainer effect in supercritical fluids, one of the most im-
portant but not fully understood mechanism widely utilized in super-
critical extraction, chromatography, precipitation, etc. [82–85]. The
other interesting phenomenon related to the criticality would be critical
Casimir force. The critical Casimir force is a weak attractive interaction
between narrow slits induced by large density fluctuation of the system.
It has been mainly observed and measured in liquid mixtures, and
firstly measured in neat near-critical CO2 recently [86]. This surface
force is regarded to be important for the supercritical fluids in the
confined geometry, but the measurement is not easy [87]. Thus, mo-
lecular simulations in conjunction with data science approaches can be
adopted to explain the occurrence of this surface force and characterize
the system. Lastly, supercritical solid/liquid boundary, also called the
Frenkel line, is also an attractive research theme that can have a great
impact in applications [60,61,88]. Since the process technology has
been remarkably advanced, it is expected that high-pressure super-
critical processes ( > 103bar) can be industrially operated in near fu-
ture. As this high-pressure phase equilibria cannot be easily made using
conventional high-pressure pump, it is expected that molecular simu-
lations will play a key role to expect the thermophysical behavior of
supercritical fluids [61]. In summary, a process in establishing a theory
for the fundamental aspects of supercritical fluids is actively ongoing.
This exciting field will greatly contribute to our understanding on the
supercritical fluids, and applying the marvelous supercritical science
and technologies to a variety of chemical processes for the everlasting
well-being and sustainable future of mankind.
25
The Journal of Supercritical Fluids 134 (2018) 21–27
Acknowledgements
We appreciate Professor Erdogan Kiran for inspiring us to contribute
to this special issue, and his great support to The Journal of
Supercritical Fluids. In addition, authors would like to thank Professor
Won Bo Lee and Mr. Min Young Ha at Seoul National University for
productive advice and discussion on the contents of this manuscript. We
also thank for Ms. Hee Jeong Park and Mr. Dong Eui Kwon for their
generous advice and correction on the grammar and expressions of this
article.
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