Chinese Journal of Chemical Engineering 27 (2019) 1236–1246

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Chinese Journal of Chemical Engineering

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Review

Process intensification in vapor–liquid mass transfer: The state-of-the-art☆

Hong Li, Chuanhui Wu, Zhiqiang Hao, Xingang Li, Xin Gao ⁎
School of Chemical Engineering and Technology, National Engineering Research Center of Distillation Technology, Collaborative Innovation Center of Chemical Science and Engineering (Tianjin), Tianjin
University, Tianjin 300072, China

a r t i c l e i n f o a b s t r a c t

Article history: The concept of process intensification (PI) has absorbed diverse definitions and stays true to the mission—“do
Received 14 June 2018 more with less”, which is an approach purposed by chemical engineers to solve the global energy & environment
Received in revised form 4 July 2018 problems. To date, the focus of PI has been on processes mainly involving vapor/liquid systems. Based on the
Accepted 17 August 2018
fundamental principles of vapor–liquid mass transfer process like distillation and absorption, there are three
Available online 25 August 2018
strategies to intensify interphase mass transfer: enhancing the overall driving force, improving the mass transfer
Keywords:
coefficient and enlarging the vapor–liquid interfacial area. More specifically, this article herein provides an
Mass transfer overview of various technologies to strengthen the vapor–liquid mass transfer, including application of
Transport process external fields, addition of third substances, micro-chemical technology and usage of solid foam, with the
Two-phase flow objective to contribute to the future developments and potential applications of PI in scientific research and
Process intensification industrial sectors.
Microwave field ©2018 The Chemical Industry and Engineering Society of China, and Chemical Industry Press Co.,Ltd. All rights reserved.
Foam

1. Introduction Fundamentally, there is something about PI of vapor–liquid mass

The science and art of process intensification (PI) have evolved into
an important component of varied aspects of chemical science and
engineering over the last three decades [1]. PI can be comprehended
as “do more with less” [2], in which the “more” and the “less” are
summarized in Table 1 along with some examples.
On the other hand, vapor–liquid mass transfer has found extensive
application in chemical engineering problems. Moreover, it is inextrica-
bly linked to reaction engineering, separation engineering, and many
other sub-disciplines of chemical engineering. It is fair to say that the
mass transfer rate and efficiency determine the cost and potential profit
of a vapor–liquid mass transfer equipment. For example, the application
of high gravity vapor–liquid contactors (rotating packed bed) from the
Dow Chemical Company for the production of hypochlorous acid
achieved a 10% growth of yield, meanwhile, the investment cost and
operating cost was 70% and 30% lower than conventional tower,
respectively [3–5]. With that level of improvement, it is understandable
why groups in the Americas, Asia, and Europe are advocating the
usage of PI in vapor–liquid mass transfer process [6]. Fig. 1 shows
the rate of growth in the publication (Data from the Web of Science
Core Collection).
☆ Supported by the National Key Research and Development Program of China
(2018YFB0604903), National Natural Science Foundation of China (21776202, 21336007),
Major Science and Technology Program for Water Pollution Control and Treatment
(2015ZX07202-013).
⁎ Corresponding author. Fax: +86 22 27404705.
E-mail address: gaoxin@tju.edu.cn (X. Gao).
transfer always comes back to the overall driving force, the mass trans-
fer coefficient and the vapor–liquid interfacial area. For example, the ex-
tremely high mass transfer coefficient was the main reason for the
unexceptionable performance of rotating packed bed. According to
reference [7], the equivalent rate law of vapor–liquid mass transfer
can be expressed as follow:


N i ¼ K L A C i − C i ð1Þ
In Eq. (1), Ni is the mass transfer rate of component i, KL is termed as
the overall mass transfer coefficients (determined by the liquid side
mass transfer coefficient, kL and the vapor side mass transfer coefficient,
kG), A is the vapor–liquid interfacial area, Ci is the bulk concentrations of
i in liquid phase, and the asterisked quantities are the concentrations in
equilibrium with the bulk concentration of vapor phase. Eq. (1) is
widely adopted in vapor–liquid mass transfer, where (Ci − C ⁎i ) are
called the overall driving force. Besides, it is more generally to use the
overall volumetric mass transfer coefficient KLa where the vapor–liquid
specific interfacial area a is lumped together with KL.
In this paper, authors have reviewed various PI approaches in vapor–
liquid mass transfer process. These technologies include external
field (microwave field, electric field, magnetic field, ultrasonic field
and high-gravity field), third substance (surfactants, micro- and
nano-particles), micro-chemical technology and solid foam. Meanwhile,
typical vapor/liquid system such as distillation, evaporation, physical
absorption and chemical absorption are involved. More importantly,
the mechanisms of different approaches are summarized by analyzing
the changes of the mass transfer coefficient, a and the overall driving

https://doi.org/10.1016/j.cjche.2018.08.005
1004-9541/© 2018 The Chemical Industry and Engineering Society of China, and Chemical Industry Press Co., Ltd. All rights reserved.
 H. Li et al. / Chinese Journal of Chemical Engineering 27 (2019) 1236–1246 1237

Table 1
The interpretation of PI

Types of PI “More” “Less” Examples

Structural intensification Production or quality Size of plants Microreactor

Energetic intensification Energy efficiency Energy consumption Rotating packed bed
Temporal intensification Productive rate Time Microwave heating
Functional intensification Functionality Number of unit operations Reactive distillation

force. As will be explained in this tutorial review, there are many better
reasons why the chemical engineers are nowadays incorporating
dedicated process intensification into vapor–liquid mass transfer.
2. External Field
2.1. Microwave field
Microwave field has been used in some vapor–liquid mass transfer
process such as distillation and dehydration, and then has received con-
siderable attention as an efficient method due to its excellent controlla-
bility, higher selectivity, better heating rates and more energy efficiency
compared with other forms of energy [8–11]. In general, the effects of
microwave irradiation on vapor–liquid mass transfer could be divided
into thermal effects and non-thermal effects [11–13]. Thermal effects,
consists of superheating [11,14,15] (also called overheating) and selec-
tive absorption of irradiation by polar substances [16], could affect
heating rate in a way different from the classical heating. Non-thermal
effects (also called not purely thermal and specific microwave effects)
are still a controversial topic which appears mostly in chemical reaction.
Thermal effects are the main effects response for the enhancement of
vapor–liquid mass transfer.
Some recent applications of microwave-assisted drying are pre-
sented in Table 2. Comparing with conventional drying method,
microwave-intensified drying significantly promoted the drying
efficiency and showed other advantages like operation and control
simplification, product quality raising, etc. This is because the water
molecule is a polar molecule whose electric loss tangent is large.
The electric loss tangent [24], as shown in Eq. (2), is designed to
describe and compare the capacity of different microwave absorbents
to be heated.
ε″
tan δ ¼
ε0
80
vapor/liquid system
other systerms
60
Number of Publications
In Eq. (2) The dielectric constant ε′ characterizes the ability of a di-
electric material to store electrical potential energy under the influence
of microwave field, the dielectric loss ε″ describes the efficiency of
absorbed energy dissipates into heat [25]. Specifically, the dielectric
constant of water is about 80 (20 °C) [26] and the dielectric loss of
water is about 9.889 (20 °C) [16].
Recently, microwave irradiation has also been exploited to intensify
distillation and reactive distillation [16,24,25,27,28]. For instance, Alt-
man et al. [16] found that the vapor phase becomes richer in the compo-
nent with lower boiling temperature when the microwave directly
irradiate to the vapor–liquid interface, and they believed it was the
higher temperatures and turbulence caused by superheating locally at
the top liquid surface encouraged molecules to set off easier into
vapor phase, thus enhanced the vapor–liquid mass transfer. This re-
search was followed by Gao et al. [25], who demonstrated that the
vapor–liquid equilibrium and even the azeotropic point of benzene-
ethanol were shifted in the presence of microwave. Though the relative
volatility of the two substances reduced, it is noteworthy that the driv-
ing force of vapor–liquid mass transfer is directly influenced by the
vapor–liquid equilibrium and it is possible to adjust the vapor–liquid
mass transfer driving force of different systems by microwave. More
systems under microwave irradiation were examined and the mecha-
nisms involved therein were analyzed by Li et al. [27,29] According to
their mechanism conjecture, microwave-intensified separation
depended on five characteristics: dielectric properties, boiling-point se-
quence, microwave power, enthalpy of vaporization and intermolecular
force. In summary, we sorted out some binary systems studied in liter-
atures and the results are showed in Table 3.
As can be seen from Table 3, different binary systems showed
different performances under microwave irradiation, and it is remarked
that Werth et al. [24] pointed out that a dedicated microwave equip-
ment which gave reliable measurement would be necessary for future
investigations. The microwave equipment they used [24] was the
ð2Þ
commercial microwave oven for synthetic chemistry CEM Discover
(2.45 GHz), as shown in Fig. 2. In contrast, the dedicated microwave
equipment Gao et al. [25] and Li et al. [27] used was presented in
Fig. 3. Additionally, there is not a confirmed interpretation for the inten-
sification of microwave on vapor–liquid mass transfer yet. Further
investigations are suggested to focus on the interacting mechanism
between microwave with certain binary systems and try to present a
uniform theory.

2.2. Electric field

40
Though the number of literatures closely related to the intensifica-
tion of vapor–liquid mass transfer by application of electric field is
relatively small, authors try to summarize the effects of electric field
into two parts: one is to increase the driving force and the other is to
20
improve the volumetric mass transfer coefficient.

2.2.1. Driving force enhancement

0 Electrohydrodynamic (EHD) drying is one of the typical techniques
2000 2002 2004 2006 2008 2010 2012 2014 2016 2018 that utilize electric fields. A schematic diagram is shown in Fig. 4 [30].
Publication year Ionic wind (identified as the movement of the air ions in a strong
electric field) appears when a high voltage is applied to two electrodes
Fig. 1. Publications whose topic including process intensification and mass transfer for the of different shapes, e.g. needle-to-plate or wire-to-plate [31]. The
period of 2000–2017. maximum ionic wind velocity was reported usually on the magnitude
1238 H. Li et al. / Chinese Journal of Chemical Engineering 27 (2019) 1236–1246

Table 2
Examples of microwave-intensified drying

Raw material Operating condition Products' quality Publication

year

Hydrometallurgy mud Microwave intensity 12.5 W·g−1, Dehydration rate 99.5% 2015 [17]
drying time 3 min
Detoxified starfish Microwave intensity 4 W·g−1, Average drying rate 2.95%·min−1, 2015 [18]
vacuum degree −0.090 mPa energy consumption 11.8 W·h·g−1,
Chinese wolfberry Microwave intensity 406 W, Moisture content b12.5% 2015 [19]
drying time 15 s
Grass carp fillets Microwave intensity 600 W, drying time 9 min Moisture content 0.1000 g·g−1 2016 [20]
Municipal sewage sludge Microwave intensity 400, 650, 1000 W Moisture content 10% 2016 [21]
Germinated brown rice Electric current 100 mA, drying time 20 s, Moisture content b14% 2017 [22]
intermittent time 60 s, 2 layer
Carrots Microwave intensity 2.83 W·g−1, Moisture content b13% (dry basis), 2017 [23]
drying time 2.3 h average drying rate 0.2189 kg·h−1,
vitamin C content (51.71 ± 0.27) mg·g−1

of several meters per second, thus introduced a convection near the
ground electrode where the wet materials placed [32,33]. This aerody-
namic effect decreases the local vapor concentration of water and sub-
sequently enhances the dehydration rate. Lai et al. [34] found that the
enhancement in drying rate increases linearly with the applied voltage,
and the EHD drying rate was 3–4 times more efficient than conventional
thermal drying. Besides, due to the no-thermal property, EHD drying
has been regarded as an attractive candidate for drying heat-sensitive
materials [35]. In addition, it was reported the energy introduced by
electric field (14.7–700 kJ·kg−1) could consume more efficiently than
thermal evaporation (2200–2300 kJ·kg−1) [36]. However, EHD drying
is not a profoundly explored method of drying since there exists com-
bined effect of electric charge, heat and mass transfers in a multiphase
environment. The general theory of vapor–liquid mass transfer in the
presence of electric field is so complex and has not yet been developed.
On the other side, Blankenship et al. [37] examined the effects
of electric fields on vapor–liquid equilibria of isopropanol and water,
and found an a positive deviation in phase composition, as the
vapor phase became richer in the component with the lower boiling
temperature. Specifically, the separation factor, or relative volatility,
was enhanced up to 10%. This phenomenon shows the possibility that
vapor–liquid mass transfer can be enhanced by electric field with
increasing the overall mass transfer driving force.
2.2.2. Increase the overall volumetric mass transfer coefficient
As mentioned in Section 1, the overall volumetric mass transfer coef-
ficient composed of the overall mass transfer coefficient and a. Applying
an external electric field could increase a by shrinking the bubble size
[38–40]. Tsouris et al. [39] performed a laboratory-scale experiment of
electrodistillation of 2-propanol and water, and they found the average
bubble size in a distillation stage decreased from 4.4 mm at 0 kV to
1.8 mm at 14 kV, resulting in increases of plate efficiency and distillate
flow rate. Furthermore, Elperin and Fominykh [41] thought that electric
charges accumulated at the interface interacted with electric field and
caused a circulatory flow around the bubbles. This disturbance near
the interface could enlarge the mass transfer coefficient. Li et al. [42]
compared the KL of ozone mass transfer with and without external elec-
tric field, and the result showed an increase of 89.11% at 2 kV voltage.
Since much attention is payed to the application of EHD drying,
authors suggest to put more efforts into foundation works such as the
investigation pf microscopic mechanism of vapor–liquid mass transfer
intensification in electric field.
2.3. Magnetic field
Magnetic field applied to liquid phase can directly change the phys-
ical properties of the fluid, including surface tension force and viscosity,
which have influence on the liquid flow pattern and mass transfer
coefficient. In addition to this, a synergistic effect of magnetic field and
tiny magnetic particles was utilized to facilitate vapor–liquid mass
transfer, too.
Magnetic field could change the intermolecular force, and conse-
quently has impacts on viscosity and surface tension of liquid phase
[43,44]. In general, lowering the liquid surface tension served to in-
crease a, and viscosity has influences on the liquid flow pattern and
mass transfer coefficient as well [45–47]. The micro mechanism had
been discussed by Niu et al. [43] On the one hand, the additional Lorentz
force exerted on the polar molecules increases the molecular average

Table 3
Binary systems under microwave irradiation

Binary system Effects of microwave on separation

1-Propanol/n-propyl propionate [16] Significant impact

Propionic acid/n-propyl propionate [16] Significant impact
1-Propanol/propionic acid [16] Significant impact
Ethanol/benzene [25] Significant impact
Bis(2-ethylhexyl) phthalate/isooctane [25] No significant impact
Ethanol/dimethyl carbonate [24] No significant impact
Ethanol/ethyl methyl carbonate [24] No significant impact
Ethanol/diethyl carbonate [24] No significant impact
Cyclohexane/isopropanol [27] Significant impact
Cyclohexane/ethanol [27] No significant impact
Ethanol/isopropanol [27] No significant impact
Ethyl acetate/methanol [27] Significant impact
Fig. 2. Lab scale distillation setup with a CME Discover [24].
 H. Li et al. / Chinese Journal of Chemical Engineering 27 (2019) 1236–1246
Fig. 3. Photo of the apparatus used in [27].
diameter of them, leading to surface tension and viscosity decreases. On
the other hand, magnetic field may break the balance of hydrogen bond
(if existed) between molecules, which also results in the decrease in the
viscosity of the magnetized system. Niu et al. [48] had studied the effects
of an external magnetic field on falling film absorption for ammonia–
water through their macroscopic mathematical absorption model, in
which considered the changes of physical properties. Numerical results
showed positive effects of magnetic field on the absorption process and
the absorbability increased by 5.9% when the magnetic induction inten-
sity at the solution's inlet is 3 Tesla. However, Niu et al. believed a superior
performance would be found if increasing the strength of magnetic field.
Subsequently, it was experimentally confirmed that a magnetic field with
the same direction as the falling film enhanced the absorption rate, and
the absorption performance was enhanced with the increase in magnetic
induction intensity [49]. In contrast, the external magnetic field against
the direction of falling film showed negative effects [50]. The precise
mechanism of magnetic field on water might remain controversial until
now, but the enhancement of water evaporation in a magnetic field
was less disputed [51–55]. Guo et al. [56] verified the enhancement of
water evaporation in a magnetic field, and they came up with an equation
about water evaporation.

and their effects on vapor–liquid mass transfer are summarized in
W evaporation ¼ f ðAÞ þ f ðBÞ þ f B0
Fig. 4. Diagram of electrohydrodynamic drying [30].
1239
where Wevaporation is the amount of water evaporation, A is the vapor–
liquid interfacial area, B is the magnetic field, and B′ is the field gradient.
Nowadays, with the rapid development of nanotechnology,
nanomagnetic particles have gradually been applied for the en-
hancement of absorption and evaporation [50,57–62]. Though the
addition of nanomagnetic particles have been confirmed to exert a pos-
itive effect on vapor–liquid mass transfer (discussed in Section 3.2),
some scientists had verified a coupling effects of external magnetic
field on CO2 absorption with nanoferrofluid [50,58,60]. However,
the mechanism behind requires further studies. Wu et al. [61] found
that apart from the small-size effect and surface effect resulted from
the nanoparticles, there existed a combined effect between the Fe3O4-
water nanoferrofluid and the external magnetic field, which gave rise
to collision of bubbles and nanoparticles, thereby squeezed bubbles
into small volume to enlarge a. The enhancement effects increase with
increasing magnetic field intensity, and the maximum of the effective
absorption ratio (identified as the ratio of the corresponding ammonia
absorption rate of the nanoferrofluid-based solution under an external
magnetic field to that of the pure ammonia-water solution without an
external magnetic field under the same conditions) was about 1.0812
at an external magnetic field intensity of 280 mT. Darvanjooghi et al.
[57] experimentally found that both alternating current (AC) and direct
current (DC) magnetic field could further enhance the mass transfer
coefficient and then the mass transfer rate of carbon dioxide in
Fe3 O 4-water nanofluid. And among AC and DC magnetic field, the
former was better. Fig. 5 showed the average mass transfer coeffi-
cient in different magnetic fields. Moreover, their mathematical
model indicated that applying magnetic field caused a thinner
diffusion layer, a faster renewal surface rate, a higher diffusivity
coefficient, and most importantly, a superior mass transfer coefficient.
Great progress has been made in the mechanism study of mag-
netic field and coupling effects of magnetic-coupled nanofluid
absorption process, but most of literatures are talking about the
macro-behavior of mass transfer, few mentioned the mechanism
behind, especially the coupling effects. There is a long way to go
before industry application.
2.4. Ultrasonic field
Many literatures had confirmed the intensification of ultrasound on
vapor–liquid mass transfer process [63–70]. Types of sonochemical
equipment, investigated system, power density, resonance frequency
ð3Þ
Table 4.
Fig. 5. Average mass transfer coefficient exposed to different magnetic fields (KL, Theoretical:
experimental mass transfer coefficient, K L, Experimental : theoretical mass transfer
coefficient) [57].
1240 H. Li et al. / Chinese Journal of Chemical Engineering 27 (2019) 1236–1246

Table 4
Summary of vapor–liquid mass transfer processes under ultrasonic field

Sonochemical equipment System Power density/W·ml−1 Resonance frequency Effects Publication year

T-shape microreactor with CO2–water – 1.7 mHz Up to 34% enhancement in liquid side 2017 [63]
piezoelectric transducer volumetric mass transfer coefficient, kLa
T-shape microreactor with CO2–NaOH solution – 1.7 mHz Up to 31% enhancement in kLa and Up to 30% 2017 [63]
piezoelectric transducer enhancement in a
Microreactor plate with Langevin-type CO2–water 0.07–0.3 20 kHz 3–20 times enhancement in kLaa 2016 [65]
transducer
a
Microreactor plate with CO2–water 0.13–1.4 20 kHz 3.3–5.7 times enhancement in kLa 2015 [66]
Langevin-type transducer
Bubble columns with ultrasonic horn Air–water 0.016–0.46 20 kHz Average 26.53% ± 5.42% enhancement in KLa 2012 [67]
Autoclave reactor with cup-horn Nitrogen–water – 20 kHz Typical 10 times enhancement in KLaa 2008 [69]
Glass reactor with ultrasonic horn Air–water 0.01–0.125 20 kHz ~50%–110% 2004 [70]
Enhancement in KLa
Ultrasonic bath with three transducers Air–water 0.01–0.125 20 kHz ~5%–11% 2004 [70]
Enhancement in KLa
a
Where kLa is approximately equal to the KLa.

As we can see from Table 4, both low and high frequency ultrasound packing and it has become another spot to investigate the intensifica-
could promote the vapor–liquid mass transfer process, and all of the lit- tion of vapor-side mass transfer controlled processes [96,97].
eratures have mentioned the promotion of the volumetric mass transfer HiGee technology is becoming increasingly mature over the last
coefficient by ultrasound. The largest enhancement of kLa already three decades. Hydrodynamics, micromixing, intensification mecha-
achieved was 20 times in the ultrasonic microreactor designed and fab- nism and modeling of rotating bed have been systematically investi-
ricated by Dong et al. [65,66] On the one hand, some researchers gated. Recently, many works are focus on intensification of different
thought that ultrasonic irradiation provides mechanical effects such as zones in the RPB. Since Guo [98] divided the RPB into end effect zone
cavitation [69,70] and surface wave oscillation [63–67] to reduce the [99], bulk zone and cavity zone, Yang et al. [100] verified the existence
size of gas bubbles subsequently increased a. The Danckwerts method of end effect close to the inner edge of packing where the effective
was used to determine the interfacial area of chemical absorption by interfacial area reached 7500 m−1. In addition, they also mentioned
Akbari et al. [63], and a maximum increase of 30% was found under the noticeable contribution of cavity zone to the overall mass transfer
the ultrasound wave. On the other hand, the ultrasound-induced cavita- [100]. After then, Luo et al. [101] came up with an idea to insert several
tion microstreaming might accelerate the interface renewal rate and artificially created end effect zones inside the bulk zone to promote
further enhanced the mass transfer coefficient [65,67,71]. mass transfer. On the other hand, Guo et al. [102] measured the
Similar to mechanically agitation, inappropriate designs and opera- vapor–liquid interfacial area of cavity zone experimentally, and
tions of the external ultrasonic field would lead to a situation where found it took up around 30% of the whole RPB. Then, Sang et al. [103]
low energy efficient and bad control happens [70,72,73]. Dealing with developed a model to guide a reasonable structure design of cavity zone.
above-mentioned problems, better design is required. Thanks to the Specific researches on different zones of HiGee contactors, especially
ideal environment for investigation provided by microreactor, combina- on end effect zone, are expected to continue for some time. Besides,
tion of ultrasound field and microreactors is expected to be one of the there are other barriers ahead need to be challenged, like the usage of
emerging and promising ways to study the microscopic mechanism of modern detecting techniques, model development and simulation,
ultrasound–bubble interaction [66,74–76]. mechanical stability issues [104], the lack of scale-up principles and so
forth. Considering that HiGee technologies have already found its
2.5. High-gravity field place in China [78,105,106], authors look forward to see more industrial
applications of HiGee gas–liquid contactors worldwide in the future.
High-gravity (HiGee) technology imitates a high-gravity field
(100–1000 times larger than gravitational acceleration of the earth)
by centrifugal force, aiming to augment mass transfer and throughput
and subsequently realize PI (significant size reduction) [6,77–80].
Higher mass transfer coefficients and larger a were achieved through
the formation of thinner liquid films and smaller droplets in the HiGee
vapor–liquid contactors [81].
Though many patents [82–88] and literatures [89–95] in relation to
the designs of HiGee vapor–liquid contactors (mainly the rotor designs)
have been filed and published, respectively, their basic working princi-
ples are similar with each other. Taking the universally mentioned
device—the rotating packed bed (RPB) as an example, liquid is intro-
duced to the center of the rotor through a distributor and is thrown
out into the packing as shown in Fig. 6. Then it is broken and split into
fine droplets, ligaments, and thin liquid films by the shearing force
caused by high-speed packed rotor. These kinds of liquid inside packed
rotor own a thinner liquid film and smaller size which significantly
enlarge the liquid phase mass transfer coefficient and a, respectively.
Liquid droplets, ligaments and films meet gas in counter-current,
co-current or cross-current to realize the mass exchange between
vapor phase and liquid phase. By the way, HiGee design using split pack-
ing innovated by Chandra et al. [95] could even enhance the vapor-side
mass transfer coefficient by promoting vapor–liquid slip inside the Fig. 6. Working principle of a rotating packed bed [6].
 H. Li et al. / Chinese Journal of Chemical Engineering 27 (2019) 1236–1246
3. Third Substance
3.1. Surfactant
Surfactants are compounds that lower surface tension (or interfacial
tension) between multiphase. Modulating surface tension with addition
of surfactants in the vapor and/or liquid phase could produce an effect
on vapor–liquid mass transfer process, specially, most of the related
works relate to absorption process of aqueous solution.
Usually, surfactants are organic compounds, which are amphiphilic,
in other words, they contain both hydrophobic groups and hydrophilic
groups. This kind of nature makes them tending to accumulate in the
gas–liquid interface, and may lead to both positive effect and negative
effect on the vapor–liquid mass transfer. Generally, mass transfer
interfacial area [107–110] increases with the addition of surfactant,
while simultaneously the liquid side mass transfer coefficient decreases
[109,111,112]. Jia et al. [113] observed that the average bubble size
decreased and corresponding a increased when different surfactants
(n-octyltrimethylammonium bromide (OTABr), sodium dodecyl ben-
zene sulfonate (SDBS) and Tween 80) were employed. Meanwhile,
they found a trend of kLa and kLa decreasing with the increase of the
surfactant concentration. kL is supposed to be more sensitive than a to
these additives, resulting in the overall effect on kLa. Therefore, the ef-
fects of surfactants on mass transfer coefficient are worth studying.
García-Abuín et al. [114] studied various surfactants with different
hydrocarbonate chain lengths, and observed two effects—Marangoni
effect and barrier effect when surfactants with smaller hydrocarbonate
chain length were employed. It is well known that Marangoni effect was
caused by the surface tension gradients, and was the positive way to in-
duce turbulence and enhance the liquid side mass transfer coefficient.
[115] On the other hand, the barrier effect was the dominating negative
effect where the chain length is long or/and surfactant concentration is
high. However, similar experiments performed by Jia et al. [113] showed
no Marangoni effect at low concentrations of OTABr, but barrier effect
existed. In conclusion, it is less disputed that the addition of surfactants
does influence the vapor–liquid mass transfer, but controversies remain
on the exact effects and mechanisms.
However, other low surface tension compounds like alcohols and
alkanes can also be regarded as surfactants based on the definition of
surfactants. Ramezani et al. [116] investigated the bubble size distri-
bution in an air–water multiphase Taylor–Couette vortex bioreactor
and they found the presence of ethanol as a low surface tension sub-
stance decreased the bubble size significantly (a 1.5% reduction of
surface tension could result in 10%–25% reduction of bubble diame-
ters). Apparently, under the same gas velocity, smaller bubble size
produced larger a. Moreover, they believed that the enhancement
of a was stronger than the negative effect on kL, because they found
that the addition of ethanol produces an increase on the value of
k L a at low surfactant concentrations. Moraveji et al. [117] who
added methanol, ethanol, propanol, and butanol into water, respec-
tively, also obtained similar results. Besides, Zhang et al. [118] sup-
ported the PI effect of dispersed organic phase by texting some
other alcohol and alkane. In addition, adding ethanol to vapor
phase was found more effective [119]. Further investigation per-
formed by Jia et al. [120] showed that k L increases initially and
decreases afterwards with the addition of ethanol into the gas, and
it was caused by the local Marangoni effect and Rayleigh effect. The
addition of a third component in the vapor phase seems to be an
effective way to intensify vapor–liquid mass transfer, but the
above-mentioned works are more like primary works and creative
work and could be made through molecular simulation to reach a
better understand of this complex process.
Both amphiphilic surfactants and dispersed organic substances
could change a and mass transfer coefficient but in different extent.
The addition of aforementioned surfactants to intensify vapor–liquid
mass transfer process is still a technique that needs more mechanism
1241
study. Much more kinds of surfactants should be measured in differ-
ent system in order to find a universal rule based on surface tension.
3.2. Fine particles
It has been confirmed that adding some fine solid particles
facilitate the process of gas solute into the liquid bulk, and is one
of the PI approaches in vapor–liquid mass transfer process [121].
Micrometer-sized particles were used firstly. Ramachandran and
Sharma [122] found that the absorption rate of carbon dioxide to
aqueous slurry of lime was significantly enhanced by adding extra
fine lime particles. Alper et al. [123] also thought that the effect of
fine activated carbon particles on absorption cannot be ignored,
and they postulated a possible transport mechanism for interpreta-
tion. Some metal oxide fine particles were employed to evaluate
the enhancement of carbon dioxide absorption under Taylor flow
by Cai et al. [124]. Mena et al. [125] investigated the relationship
between the characteristics of solid particles (mean diameter,
loading and type) and the vapor–liquid mass transfer, and found
that when 9.5 μm hollow glass spheres were used, k L a increased
with the solid loading (≤ 3 vol%).
Due to the ongoing development in nanotechnology in recent years,
nanometer-sized particles between 1 and 100 nm in diameter, called
nanofluid nanoparticles [126], were stably dispersed into a base liquid
to enhance and mass transfer. Typical nanoparticles include metals,
oxides, carbides, or carbon nanotubes. Esmaeili-Faraj and Esfahany
[127] studied the absorption of hydrogen sulfide and carbon dioxide
by using exfoliated graphene oxide (EGO) or synthesized silica (SS) as
nanoparticles and water as the base liquid. They calculated and found
that diffusivity coefficient of EGO-nanofluid and SS-nanofluid was
respectively 1.42- and 1.52-fold that for the base water, the liquid
film thickness of EGO-nanofluid and SS-nanofluid was respectively
1/4- and 2/3-fold that for the base water, and the mass transfer
coefficient, kL , was respectively 4.64- and 2.07-fold that for the
base water. 1% volume fraction γ-Al2O3 nanoparticles was added to
water and nearly a 50% increase of CO2 absorption rate was achieved
by Samadi et al. [50]. Olle et al. [128] took magnetite (Fe3O4) nanoparti-
cles to investigate the oxygen-transfer enhancement. Both a and kL
increased, and they reported up to 6-fold enhancement of kLa at
nanoparticle volume fractions below 1%. Moreover, Lee et al. [129] in-
vestigated the combined CO2 absorption/regeneration performance en-
hancement of Al2O3/methanol and SiO2/methanol nanoabsorbent
and found that SiO2/methanol nanoabsorbent maintained a higher
level of absorption rates and regeneration rate than pure methanol
throughout the experimental cycle. In contrast, the overall performance
of Al2O3/methanol nanoabsorbent was encumbered by the decreasing
regeneration rate.
There is no definitively correct interpretation for the mechanism of
enhancing vapor–liquid mass transfer performance by fine particles
till date, but there are three major models which are supported by spe-
cific experiments or numerical analysis. They are shuttle effect models
considering the adsorption of gas to fine particles [123,130], hydrody-
namic effect model considering Brownian motion of the fine particles
[131,132] and bubble-breaking effect model considering larger a [133,
134]. These mechanisms are not isolated, instead jointly contribute to
the improvement of the vapor–liquid mass transfer performance [129].
In fact, only a few studies have been conducted to explore the vapor–
liquid mass transfer enhancement in the presence of fine particles, and
most of them just deal with the measurement of macroscopic experi-
ment data. Future studies should take the microscopic mass transfer
into consideration. On the other hand, there are various ways for
nanofluid preparation which set up a barrier in quantitative analysis be-
tween different researches [135]. However, the trend of development of
nanofluid-manufacturing technology and nanoparticles-dispersion
stability would accelerate the research of nanoparticle enhancing
vapor–liquid mass transfer.
1242 H. Li et al. / Chinese Journal of Chemical Engineering 27 (2019) 1236–1246
4. Micro-chemical Technology
Microchannels in micro-chemical technology are usually defined as
miniaturized channels fabricated by using, at least partially, methods
of micromechanical technology and precision engineering [136]. Due
to the large surface-to-volume ratios that inherent in microchannels,
remarkably intensification of vapor–liquid mass transfer can be
realized. Yue et al. [137] found that both higher superficial liquid
and vapor velocities showed positive effects on enhancing kLa in a
Y-type rectangular microchannel (Fig. 7) with a hydraulic diameter
of 667 μm. k L , a and k L a were measured up to 1.6 × 10 −3 m·s −1 ,
9 × 103 m2·m−3 and 21 s−1, respectively. Moreover, they developed
dimensionless empirical correlations for slug flow pattern:
ShL  a  dh ¼ 0:084 Re0:213
G Re0:937
L Sc0:5
L ð4Þ
where ShL and ScL refer to liquid side Sherwood number and Schmidt
number, respectively. ReGS and ReLS are superficial Reynolds numbers in
vapor side and liquid side, respectively. Moreover, follower researchers
[138–140] demonstrated the good prediction accuracy of this correlation.
As we can see, a and kLa are at least 1–2 order of magnitude larger in
microchannel reactors compared with that in classical vapor–liquid
mass transfer units, such as bubble columns [141] (50–600 m2·m−3;
0.005–0.24 s−1), spray columns [142] (75–170 m2·m−3; 0.015–
0.022 s−1), stirred tank [142] (100–2000 m2·m−3; 0.03–0.4 s−1)
and the emerging commercial system Advanced-Flow Reactor [143]
(160–1300 m2·m−3; 0.2–3 s−1). However, it is worth taking a moment
to flag the fact that the high kLa is mainly caused by the large a in
micro-devices, while the kL itself is still comparable to that in some con-
ventional equipment, such as static mixers [144] (1 × 10−3 − 4.5
× 10−3 m·s−1) and tube reactors [141] (1 × 10−4 − 1 × 10−3 m·s−1).
Therefore, further improvement of the individual kL was studied by
structure optimization [143–145] and intervention of external en-
ergy [64,65]. Obviously, the flow and mass transfer performance in
these microchannels are more complex which draw higher demand
for investigation.
Obviously, micro-chemical technology shows a great potential for
many industrially relevant mass transfer operations. However, experi-
ence of the macro-world sometimes fails when being simply transferred
to micro-chemical processes, therefore newly designed experiments
and revised models should be conducted under different flow pattern,
especially Taylor flow.
5. Solid Foam
Solid foam material (either ceramic or metal-based) has been exten-
sively reported in chemical engineering, especially used as contacting
material, structured catalyst or catalyst support, owing to its advanta-
geous properties such as high porosity, high a, low pressure drop.
Meanwhile, solid foam has also been recognized as a promising material
for intensifying the vapor–liquid mass transfer process.
Fig. 7. Y-type vapor–liquid microchannel contactor [137].
The vapor–liquid mass transfer in commercial aluminum foam pack-
ing was studied by Stemmet et al. [146–148] They firstly predicted the
kLa to be relatively high, ranging up to 6 s−1 for the solid foam packing
in count-current flow condition using the penetration theory [147] and
latterly experimentally determined the kLa ranging from 0.1 to 1.3 s−1
when operated in co-current condition [148]. However, the semi two-
dimensional column Stemmet et al. used was questioned by Lévêque
et al. [149] They placed a chunk of silicon carbide (SiC) foam cylinder
(Fig. 8) inside a distillation column and found that the mass transfer
performance with 4–5 theoretical stages per meter was outstanding
compared with classical packing (Sulzer M250Y, Sulzer CY and Pall
ring), but the capacity of monolithic SiC foam packing was limited by
higher wet pressure drop and lower flooding line. Nonetheless, they
pointed out a target application of ceramic foam in reactive distillation
where high liquid hold-up at low F-factors are favorable. Further
research by Li et al. [150] and the developments in catalyst coating
technology on SiC foam [151,152] also indicated that the application
of ceramic foam in reactive distillation could be a promising field.
As shown in Fig. 9, structured corrugation SiC foam packing
(SCFP-SiC), an integration of foam material into traditional corrugated
packing structure, however, is able to exploit advantages from both
parties [153,154]. Li et al. [155] found the theoretical plate number per
meter for SCFP-SiC was 50% higher than that of wire mesh corrugated
structured packing (Sulzer Mellapak 350Y). To clearly demonstrate
which factors leading to the high mass transfer performance of SCFP-
SiC, Li et al. [156] pointed out the following two conjecture characteristics:
– Due to porous material's imbibition effect (leading to transverse
flow) than packing sheet's corrugation structure, SiC foam possesses
better liquid dispersion ability, so the effective a for mass transfer
is enlarged.
– The irregular surface and special skeleton structure of SiC foam may
influence the flow pattern and increase the mass transfer coefficient,
so the vapor–liquid mass transfer performance enhanced.
In order to verify these hypothesis and better understand the
outstanding mass transfer performance of SiC foam corrugated struc-
tured packing, Li et al. [156,157] continued their works on macroscopic
liquid flow behavior in SCFP-SiC sheets by visualization research and
definition of the microscopic liquid flow patterns. Recently, they
published an article to show that most of the wetted area on the SCFP-
SiC sheets could be renewed due to the larger radial and axial dispersion
coefficients (compared with modular catalytic structured packing
KATAPAK-S) and thus majority of the wetted area was effective in
reaction and mass transfer all the time [150].
The relatively low hydrodynamic performance is of concern with the
aim to make full use of foam packing. Zhang et al. [158,159] installed
Fig. 8. β-SiC monolithic foam packing [149].
 H. Li et al. / Chinese Journal of Chemical Engineering 27 (2019) 1236–1246
Fig. 9. Structured corrugation SiC foam packing [153].
thin slices of SiC foam material on valve tray to produce a SiC foam valve
tray (Fig. 10). They found that the operating rang of SiC foam valve tray
was wider than that of some other distillation trays (F1 float valve, sieve
tray, etc.), while the mass transfer efficiency of the SiC foam valve tray
was also higher than F1 float valve tray. Another example is the SiC
foam monolithic tray (Fig. 11) [160–162] which also proved that the
SiC foam was a suitable material for distillation. More recently, Li et al.
[163] put forward a novel foam ring random packing (Fig. 12) made of
carbon foam material that takes both the advantages of random packing
and solid foam.
Foam material packing and trays are attractive candidates for regular
distillation and reactive distillation. However, there are too many
parameters in connection with the hydrodynamic and mass transfer
properties of solid foam, such as material (metal or ceramic-based),
pore size, porosity, extrusion ratio and corrugation angle (for
corrugated structured packing) [164–167]. Therefore, it is necessary
to figure out the principles for the structure optimization of solid
foam. Not only distillation but also other processes like humidification
[168], absorption [169] and multiphase reaction [170,171] should be
considered separately.
6. Summary and Perspective
A large number of studies about intensification of vapor–liquid mass
transfer have been reviewed in this article, but it should be noted
Fig. 10. SiC foam valve tray [159].
1243
Fig. 11. SiC foam monolithic tray [161].
that the above-mentioned methods are insufficient to cover all aspects
of vapor–liquid mass transfer intensification as new variations of
enhancement techniques are constantly being developed. Even so, the
basic rate laws governing mass transport are the unchanging rules we
can follow. By increasing one or more of the overall driving force, the
mass transfer coefficient and interfacial area, the vapor–liquid mass
transfer can be enhanced. Outlooks of the future of the intensification
of vapor–liquid mass transfer are provided below:
– The length scale of research develops from the level of meters to the
level of microns, even nanometers and molecular. The research of
mass transfer cannot merely be satisfied with determination of
macroscopic performance; it encourages researchers to find out
the underlying mechanism. Take the research progress of solid
foam as an example, researchers started their work at experimental
characterization of the mass transfer efficiency in terms of the height
equivalent to theoretical plate or the theoretical plate number per
meter, and now they turned to the liquid behavior on solid foam
skeleton and determination of dispersion coefficients. The use of
novel and sophisticated measurements is necessary for illuminating
the fundamental research of mass transfer.
– Interdiscipline plays an important role in intensification of vapor–
liquid mass transfer. Electromagnetism, acoustics, computer science,
Fig. 12. Carbon foam ring random packing [163].
1244 H. Li et al. / Chinese Journal of Chemical Engineering 27 (2019) 1236–1246
material science are now in the “toolbox” of chemical engineers and
inspire a series of creative works in the hand of knowledgeable
chemical engineers. We have reasons to believe that many future
breakthroughs are likely to emerge from multidisciplinary work
at the nexus of chemistry, biology, physics, mathematics and
computer science.
– Using two methods to intensify the vapor–liquid mass transfer
simultaneously may lead to additional effects. For instance, the
synergistic effects of the nanoferrofluid and an external magnetic
field which is mentioned in Section 2.3, microreactor with ultrasonic
field which is mentioned in Sections 2.4 and 4, solid foam with high-
gravity field which is mentioned elsewhere [172]. Among these
effects, the coupling of microreactor and ultrasonic field is the finest
examples, because ultrasonic field promote the mass transfer inside
microchannel, and microchannel provides an ideal environment to
study the ultrasound-bubble interaction phenomena. Future
research should study the development and usage of these hybrid
technologies.
– Foregoing PI methods have to overcome the pains of equipment
development and scale-up before successfully commercialized
and industrial application. To date, high-gravity field [77] and
microreactors [173] are ahead of other PI technologies, especially
on the invention of dedicated equipment for chemical process.
We have seen various kinds of HiGee vapor–liquid contactors built
for different process, including rotating bed with helix channels for
inorganic nanoparticles synthesis [174], rotating packed bed for de-
sulfurization [106], two-stage counter-current rotating packed bed
[91] and rotating zigzag bed [175] for separation process. Equipment
development played an important role in the industrial application
of high-gravity field, while devices for alternative energy sources
such as magnetic field, electric field, microwave and ultrasound are
relatively laggard. At Tianjin University, we are investigating the
feasibility of using microwave as a novel concept for regular
distillation and reactive distillation, so we have built specialized
laboratory-scale experimental instrument for vapor liquid equilib-
rium measurement under microwave [25] and pilot-scale continu-
ous microwave-assisted reactive distillation column [176]. These
devices alone with the novel ultrasonic microreactor [66] offer
exciting prospects for accessible industrial applications.
Nomenclature
A vapor–liquid interfacial area, m2
a vapor–liquid specific interfacial area, m2·m−3
C concentration, mol m−3
G mass transfer rate, mol·s−1
KL overall liquid side mass transfer coefficient, m·s−1
KLa overall liquid side volumetric mass transfer coefficient, s−1
kG vapor side mass transfer coefficient, m·s−1
kL liquid side mass transfer coefficient, m·s−1
kLa liquid side volumetric mass transfer coefficient, s−1
Acknowledgements
We would like to thank Weiwei Wu for providing language help and
writing assistance.
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