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Journal of the Taiwan Institute of Chemical Engineers

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Investigation of the liquid film thickness in an open-channel falling

film micro-reactor by a stereo digital microscopy
Yongchang Yang, Tao Zhang, Dan Wang, Shengwei Tang∗
Multiphase Mass Transfer and Reaction Engineering Laboratory, School of Chemical Engineering, Sichuan University, Chengdu 610065, China

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

Article history: The film thickness is a vital parameter for the falling film micro-reactor (FFMR) as a characteristic value
Received 25 January 2018 representing both the surface to volume ratio and the distance of mass and heat transfer. In this pa-
Revised 21 July 2018
per, a method and procedure using a stereo digital microscopy to study the flow pattern and liquid film
Accepted 24 July 2018
thickness in the FFMR were developed. The hydrodynamic behaviors of three liquids (deionized water,
Available online xxx
ethanol and isopropanol) have been investigated in a customer designed FFMR. Studies suggest that the
Keywords: film thickness increases with increasing flowrate and viscosity. The viscous force plays a dominant role
Falling film in the falling film process. The falling film behaviors were also analyzed by computational fluid dynamics
Micro-reactor (CFD) simulation. A new correlation for the film thickness prediction has been proposed, and its predic-
Stereo microscopy tions are consistent with the experimental data from this work and public literatures with an accuracy of
Film thickness 7% and 20%, respectively. As a result, stereo digital microscopy has been proved to be an effective device
for investigating the hydrodynamic behaviors in FFMR, and the proposed model can accurately predict
the film thickness in falling film micro-system within a wide flow regime.
© 2018 Taiwan Institute of Chemical Engineers. Published by Elsevier B.V. All rights reserved.

1. Introduction in nitrogen stripping [20], binary phase separation [21,22] and

As a combination of micro-electromechanical systems (MEMS)
and microfluidic technology with the conventional falling film con-
cept, falling film micro-reactor (FFMR) has attracted considerable
attention in recent years [1–4]. FFMR is a new-type of continuous
contact gas-liquid mass transfer device, and numerous researches
have shown that it can generate the ultra-thin stable liquid films
less than 100 μm thickness [5–8], which provides an excellent heat
and mass transfer between the phases. The Institut für Mikrotech-
nik Mainz GmbH [9,10] developed the first commercial falling film
micro-reactor and pilot scale study was carried out accordingly
[11], results shown that FFMR has incomparable advantages in
comparison with macroscopic reactors owing to the enhancement
of mass transfer between phases with the help of ultra-thin liquid
film. So far, FFMR has successfully applied in direct fluorination
[12,13], sulfonation [14], photochemical reaction [8,15], ozonolysis
reaction [16,17] and catalytic hydrogenation [18,19], especially in
studying the complex kinetics of rapid and strong exothermic
gas-liquid reactions. Moreover, it is also an efficient contactor
∗
Corresponding author.
E-mail addresses: yc.yang@stu.scu.edu.cn (Y. Yang), zhangtao@scu.edu.cn
(T. Zhang), d.wang@stu.scu.edu.cn (D. Wang), tangdynasty@scu.edu.cn (S. Tang).
physical absorption [23], etc.
The superior mass and heat transfer exhibited by FFMR is based
on the good hydrodynamic behaviors of the liquids in the mi-
crochannel, and the film thickness is a vital parameter in film-
forming process for it represents the surface to volume ratio and
the distance of mass and heat transfer. Generally, the specific gas-
liquid interface area can be calculated from the reciprocal film
thickness, which lead to as high as 10,0 0 0–48,0 0 0 m2 /m3 [24] and
is 1 or 2 orders of magnitude higher than those obtained in tra-
ditional tank reactor [10]. Gravity and inertia force are known to
have great influence on macroscopic falling film process, whereas,
surface tension and viscous force probably play a dominant role
in microscale flows [25–27]. Therefore, the film-forming behaviors
and mechanism in microchannel need to be explored in depth and
it is useful for predicting the performance of heat and mass trans-
fer, reaction as well as separation characteristics in this device.
The hydrodynamic behaviors of liquid in microchannel exert a
significant influence on interphase mass transfer process. Pertinent
parameters mainly include flow morphology, film thickness and
velocity distribution in the thin-film. Wille et al. [28] made at-
tempt to measure the liquid film thickness in microchannel and
found a deviation of around 50% between experimental and theo-
retical calculation. Yeong et al. [29] measured the liquid film thick-
ness for three different liquids including ethanol, isopropanol and
acetone by confocal laser scanning microscopy (CLSM) and laser

https://doi.org/10.1016/j.jtice.2018.07.033
1876-1070/© 2018 Taiwan Institute of Chemical Engineers. Published by Elsevier B.V. All rights reserved.

Please cite this article as: Y. Yang et al., Investigation of the liquid film thickness in an open-channel falling film micro-reactor by a
stereo digital microscopy, Journal of the Taiwan Institute of Chemical Engineers (2018), https://doi.org/10.1016/j.jtice.2018.07.033
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2 Y. Yang et al. / Journal of the Taiwan Institute of Chemical Engineers 000 (2018) 1–10

thermographic camera, and found that the liquid/solid advancing

Nomenclature and receding contact angles and the micro-channel size are the key
parameters dominating the film-forming process. Anastasiou et al.
Bo bond number [27,35] used a μ-PIV system for measuring velocity profiles and
Ca capillary number estimating the local film thickness in three open inclined micro-
CA contact angle (°) channels, which provided a new non-destructive method for mea-
Co courant number suring film thickness.
D channel depth (μm) Computational fluid dynamics (CFD) is another great tool to
Fvol volumetric force (N) study the hydrodynamics as well as the mass and heat transfer
Fr froude number characteristics in microfluidic devices. Compared with the exper-
Ff wall shear stress (N) imental study, this method is not only cheaper but also faster,
Fs gas-liquid interface shear stress (N) which has been proved to be an appropriate tool to study the
g gravitational acceleration (m/s2 ) physical phenomenon inside microfluidic devices. Al-Rawashdeh
l characteristic length (m) et al. [36] extended a rigorous 2D model to so-called pseudo-3D
p pressure (N/m2 ) model through COMSOL Multiphysics and Matlab and numerically
Q volume flowrate (ml/h) simulated the influence of liquid flow distribution, gas chamber
QN normalized volume flowrate (QN = Q/W) (m3 /(s m)) height and channel wettability on the mass transfer rate of the ab-
nair refractive index of air sorption of CO2 in NaOH aqueous solution. Subsequently, Ho et al.
nliquid refractive index of liquid [37] analyzed the liquid film thickness, velocity, pressure and shear
Re film Reynolds number profiles using the volume of fluid (VOF) model. Ishikawa et al.
t time (s) [38] examined the wavy motion of falling film experimentally and
W channel width (μm) numerically, results showed that the existence of surface deforma-
We Weber number tion was the main reason why gas phase absorption process was
U average liquid velocity (m/s) intensified.
v velocity vector (m/s) Currently, most of the hydrodynamic studies were based on
common fluid media. However, for some special fluids, especially
Greek symbols
with strong oxidizability or high viscosity, such as concentrated
α volume fraction
sulfuric acid or ionic liquid, it may be difficult to find a suitable
αw surface tension coefficient
tracer particle in the fluorescent microscopy or μ-PIV system. Ionic
μ dynamic viscosity (Pa s)
liquid has been studied broadly and is potential excellent catalyst
κ surface curvature (1/m)
for many reactions [39,40]. The hydrodynamics of sulfuric acid or
v kinematic viscosity (m2 /s)
ionic liquid are vital to the corresponding reactions [41]. However,
θ1 incident angle (°)
researchers have not found a feasible method and device to study
θ2 angle of refraction (°)
it. To close this gap, a stereo digital microscopy was adopted to
ρ density (kg/m3 )
investigate the liquid film hydrodynamic behaviors in this work,
σ surface tension (N/m)
and a new method was developed to measure the film thickness
δ film thickness (μm)
in FFMR. In addition, CFD numerical simulation was conducted to
δd measured film thickness
investigate the hydrodynamics of FFMR using the VOF model. The
δ̄d average measured film thickness
simulation was validated by the experimental data, and then a di-
δr real film thickness
mensionless model was developed to predict the film thickness in
Subscripts FFMR.
G gas phase
L liquid phase 2. Experimental materials and methods
N normalized
Nu Nusselt 2.1. Falling film micro-reactor
Ka Kapitza
To Tourvieille A single channel falling film micro-reactor was designed and
Exp experimental fabricated to study the film-forming behaviors. The reactor mainly
Sim simulation consists of three parts including stainless steel reactor plate (316 L),
upper and lower cover plate and bottom plate (PTFE), as shown in
Fig. 1. Among them, reactor plate is the core component of the
profilometer, the results were compared with the correlations es- system, and the microchannel on it was constructed by wet chem-
tablished from classical falling film theory and they found the ical etching. The cover and bottom plate were constructed on the
Kapitza correlation gave the best predictions. The results also found computer numerical control (CNC) lathe and all have oval grooves
that the liquid film is concave instead of flat, and viscosity has used for liquid distributor and collector, the O-ring was put around
more effect on the film thickness. Zhang et al. [30,31] observed the grooves for sealing the liquid, then a steady and uniform distri-
with a high-speed CCD camera and revealed that there are three bution of the liquid film can be realized by this method [13]. Be-
flow patterns in microchannel, namely, corner rivulet flow, flow sides, a cross-section of the microchannel with rectangular-shape
with dry patches and complete film flow. Previous studies didn’t was chosen in this experiment and the channel size is 1200 μm in
pay attention to the location of the three phase contact line, which width, 200 μm in depth and 100 mm in length, the reactor plate
is an important parameter for describing the morphology of the size is 62 mm, 1.5 mm and 182 mm respectively. Furthermore, a
liquid film in microchannel [32]. To address this issues, Tourvieille vent hole was also equipped to the upper cover plate to release
et al. [33] proposed a method for study of the liquid film at the the gas in the liquid distributor. The working liquid was feed into
edge of the wall by laser-induced fluorescent confocal microscopy. the reactor by a syringe pump (DB-80-ST, Beijing Spacecrafts, China)
Roques–Carmes et al. [34] investigated the liquid wettability and and thin liquid films flow downward along the vertical microchan-
the hydrodynamics of a customer designed FFMR by an infrared nel by gravity, and all the liquids gathered in the bottom collector

Please cite this article as: Y. Yang et al., Investigation of the liquid film thickness in an open-channel falling film micro-reactor by a
stereo digital microscopy, Journal of the Taiwan Institute of Chemical Engineers (2018), https://doi.org/10.1016/j.jtice.2018.07.033
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Fig. 1. Photographic view of the FFMR.

Fig. 2. Experimental set-up for the falling film hydrodynamic test.

will be withdrawn by a peristaltic pump (BQ80S-FZ10, Lead Fluid
Technology Co., Ltd, China) so as to control the liquid level in the
collector. The experimental set-up was shown in Fig. 2.
2.2. Channel profile visualization
A stereo digital microscopy (Smartzoom 5, Carl Zeiss, Germany)
was adopted to investigate the flow behavior and film thickness
in this work. This instrument has the characteristics of no-contact,
nondestructive, high precision and speed 3D imaging. The mi-
croscopy can capture the optical slices of the specimen accurately
under the specified scanning range and steps in the longitudinal
direction by the focused optical path, then these slices can be as-
sembled together through digital processing and finally a 3D mor-
phology of the specimen is displayed on a personal computer via
data acquisition system.
The objects can be photographed and analyzed quickly and ef-
fectively by Smartzoom 5. Two kinds of lighting modes are built
in this machine, which are the ring light integrated on the object
lens and the coaxial light integrated in the optical system. The lat-
ter can move with the microscopy when focusing, which is suitable
for the imaging of objects with high reflection. The 3D topogra-
phies of the channel with different lighting modes were shown
in Fig. 3. In this work, the experiments were conducted with the
coaxial light. The cross-sectional profile of the channel was shown
in Fig. 4 (black solid line) which indicates that the channel is rect-
angular.
In this study the microscopy was put down on a special metal
cradle so as to adjust the lens to the horizontal position, and then
the FFMR was fixed vertically on the microstat through a titanium
plate. Through this way the reactor can follow the movement of
the microstat during the scanning process.
2.3. Experimental set-up and research methodology
In order to measure the actual film thickness and minimize
the entrance effect, the microscopy was positioned 5 cm downward
from the liquid inlet. A 3D photo is taken for the blank channel
firstly. It can be functioning as a baseline. Another 3D photo is
taken again at the same position when the liquid film is stable af-
ter feeding.
The light reflection signal will be produced both at the film sur-
face and channel bottom due to the existence of liquid, which has
been proved by Yeong et al. [29] and Anastasiou et al. [35]. Lel’s
study indicated that the reflection signal from channel bottom is
about ten times stronger than the one from the film surface for
transparent and thinner films, which is often within the noise level
and filtered out [42]. In reality, the detected signals are from the

Please cite this article as: Y. Yang et al., Investigation of the liquid film thickness in an open-channel falling film micro-reactor by a
stereo digital microscopy, Journal of the Taiwan Institute of Chemical Engineers (2018), https://doi.org/10.1016/j.jtice.2018.07.033
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Fig. 3. 3D topography of the microchannel in: (a) ring light (b) coaxial light.

Fig. 4. Principle of film thickness measuring. (deionized water, QL = 15 ml/h.).

Table 1
Physical properties of deionized water, ethanol and isopropanol.

Fluids ρ (kg/m3 ) μ (Pa s) σ L − G (N/m) n CA (°)

Deionized Water 998.2 0.0010 0.0722 1.333 67.7

Ethanol 789.0 0.0012 0.0241 1.362 16.8
Isopropanol 785.4 0.0023 0.0213 1.377 10.1

tan θ2 / tan θ1 = δa /δr (4)

δa = δr − δd (5)

Fig. 5. Phenomenon of the reflection and refraction on liquid film surface.
channel bottom as a result of both refraction and reflection, hence
a “new” bottom would be sensed by detectors from B to B’, as
shown in Fig. 5. Compared with the baseline, the film thickness
δ d can be obtained as depicted in both Figs. 4 and 5. The relation-
ship between this measured film thickness (δ d ) and the real film
thickness (δ r ) is governed by the Snell-Descartes law.
sin θ1 · nair = sin θ2 · nliquid
nair /nliquid = sin θ2 / sin θ1
where, θ 1 , and θ 2 approch to zero,
sin θ2 / sin θ1 ≈ tan θ2 / tan θ1
nliquid
δr = δd · (6)
nliquid − nair
since nair = 1,
nliquid
δr = δd · (7)
nliquid − 1
As denoted in Eq. (7), the real film thickness δ r can be calcu-
lated from the measured film thickness δ d . Based on the measure-
ment principle, the light should be almost perpendicular to the
bottom. So the film thicknesses in the center section of microchan-
nel are measured easily and showed as solid line in Fig. 4. How-
ever, the microscopy cannot be positioned to be perpendicular to
the side walls. So the film thicknesses nearby the side walls cannot
be measured accurately in this study. It just schematically showed
as dashed lines in Fig. 4.
In this work, three fluids were adopted for the investigation
including deionized water, ethanol and isopropanol, and their
(1) physical properties are listed in Table 1. The liquid flowrates were
(2) controlled between 2–30 ml/h, and their corresponding Reynold
numbers are between 1.15–6.91, 0.76–3.80, and 0.16–0.71 for
deionized water, ethanol and isopropanol respectively. Therefore,
(3) the liquid phase is in a fully developed laminar flow, and the

Please cite this article as: Y. Yang et al., Investigation of the liquid film thickness in an open-channel falling film micro-reactor by a
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impact of channel surface roughness is negligible. All these exper-

iments were carried out at ambient conditions (∼25.0 °C). Each
experiment is repeated three times with relative standard error
less than 8% one another so as to improve the accuracy, and the
average result is used for further analysis.

3. Numerical simulations

To study the flow behaviors of the liquid phase in a systemic

manner, a two-dimensional multiphase CFD model is developed
based on the method of VOF. The VOF model can model two or
more immiscible fluids by solving a single set of momentum equa-
tions and tracking the volume fraction of each of the fluids through
the computation domain [43], which is usually used to track the
steady or transient gas-liquid interface. The numerical simulations
were performed with the CFD software ANSYS® Fluent, which Fi-
nite Volume Method (FVM) was chosen to solve the governing
equations, and a Continuum Surface Force (CSF) model proposed
by Brackbill [44] et al. was employed in the simulation for surface
tension sensitivity study as well.

3.1. Governing equations

The continuity equation is given by

∂ρ
+ ∇ · (ρv ) = 0 (8)
∂t
The momentum conservation equation is given by Fig. 6. Computation mesh and schematic diagram of FFMR geometry. (not to scale).

∂   
(ρv ) + ∇ · (ρvv ) = −∇ p + ∇ · μ ∇v + ∇vT + ρ g + Fvol
∂t
which made the falling film was easy to achieve stable state during
(9)
the calculation. Moreover, non-convergence of the continuity equa-
where Fvol is a momentum source term resulting from surface ten- tion or film break-down which mentioned in Ho’s et al. [37] work
sion in the VOF model. can be avoided. The structured and rectangular grids were used to
2ρκ∇ αL improve the calculation accuracy over the whole domain. Grid sen-
Fvol = σ (10) sitivity simulation indicated that the best results can be achieved
ρG + ρL
with 14,531 grids. Furthermore, denser grids were developed in
where κ is the surface curvature and can be computed from local gas-liquid interface, and coarser grids were adopted in gas phase
gradients in the surface normal to the interface. considering both the simulation accuracy and cost.
  The boundary conditions for free falling film hydrodynamics in-
1 n
κ =∇ · nˆ = ·∇ |n| − (∇ · n ) (11) clude gas inlet velocity at zero, gas outlet pressure at atmosphere,
|n| |n|
and no-slip wall. A Dell R730 server with Intel® Xeon® E5-2683 v3
The gas-liquid interface position can be obtained from the liq- @ 2.0 0 GHz 2.0 0 GHz (2 CPU) and 64 GB RAM was used. All simu-
uid volume fraction, and then the gas volume fraction is computed lation cases are listed in Table 2.
based on the Eq. (13)
∂
(α ρ ) + ∇ · (αL ρLv ) = 0 (12) 3.3. Solution strategy and convergence criterion
∂t L L
To show the dynamic behaviors of the gas-liquid interface, tran-
αG = 1 − αL (13)
sient simulations were performed with variable time-step about
In the above equations, physical properties in each cell such as 10−6 –10−4 s to accelerate the simulation, and the global courant
density and viscosity are volume-fraction-averaged, which can be number is 0–0.5 to ensure adequate solution accuracy and reliabil-
given by: ity. Pressure Implicit with Splitting of Operators (PISO) scheme was
selected for pressure-velocity coupling. For spatial discretization of
ρ = αL ρL + (1 − αL )ρG (14)
the pressure and momentum equation, a Pressure Staggering Op-
tion (PRESTO!) method and a second-order upwind differencing
μ = αL μL + (1 − αL )μG (15) were carried out, respectively. Under-relaxation factors of the pres-
sure and momentum were set as default, namely, 0.3 and 0.7. The
3.2. Flow geometry and boundary conditions highly precision solution Geo-Reconstruct scheme was employed
to capture the gas-liquid interface, which was the position with
The computation mesh details and schematic diagram of the VOF value of 0.5. Initially, a certain thickness of film was patched
FFMR geometry is shown in Fig. 6. In order to show the size of on the plate, which was calculated by Nusselt theory [30]. The nu-
microchannel clearly, the schematic diagram of the FFMR geom- merical solution was considered to be converged when the nor-
etry is not on actual scale. The establishment of the 2D model malized residuals for governing equations fell below 10−3 between
and grids partition were developed via ANSYS® ICEM, and a “liquid the step n and (n + 1). Meanwhile, flowrates of liquid phase at
seal” structure was added at the bottom of the model (see Fig. 6.), y = 80 mm and y = 20 mm were monitored when these values kept

Please cite this article as: Y. Yang et al., Investigation of the liquid film thickness in an open-channel falling film micro-reactor by a
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Fig. 7. Flow patterns in microchannel: (a) corner rivulet flow (b) flow with dry patches (c) complete liquid flow.

Table 2 corner rivulet flow, flow with dry patches and complete liquid flow
Flowrate sensitivity simulations.
as shown in Fig. 7, which was consistent with the works of Anas-
Case no. System VL-inlet (m/s) ReL tasiou et al. [27] and Zhang et al. [31]. However, when switching
1 Water, air 0.00579 1.15 the fluid to deionized water, the liquid film was easily broken-
2 Water, air 0.00694 1.38 up at the tube outlet as flowrates decreased gradually, also, liquid
3 Water, air 0.00810 1.61 droplets were formed and fell along the channel. This should re-
4 Water, air 0.00926 1.84 sult from the high surface tension of deionized water, which lead
5 Water, air 0.01042 2.07
to a bigger contact angle (see Table 1) with poor wetting [32].
6 Water, air 0.01157 2.30
7 Water, air 0.01736 3.45 Moreover, channel aspect ratio and channel surface characteristics
8 Water, air 0.02315 4.61 should have contributed to this difference as well.
9 Water, air 0.02894 5.76
10 Water, air 0.03472 6.91
11 Ethanol, air 0.00579 0.76 4.2. Liquid film thickness in experimental and simulation
12 Ethanol, air 0.00810 1.07
13 Ethanol, air 0.0116 1.52
Liquid film profiles with different flowrates captured by Smart-
14 Ethanol, air 0.0139 1.83
15 Ethanol, air 0.0174 2.28
zoom 5 are illustrated in Fig. 8. Apparently, it appears that the
16 Ethanol, air 0.0197 2.59 three phase contact line (TPCL) pinned at the edges of the channel
17 Ethanol, air 0.0231 3.04 and is independent of flowrates. Previous studies such as Seemann
18 Ethanol, air 0.0289 3.80 et al. [32], Zhang et al. [31] and Tourvieille et al. [33] revealed that
19 Isopropanol, air 0.00231 0.16 the location of TPCL depends heavily on how the channel is ini-
20 Isopropanol, air 0.00347 0.24 tially wetted and the channel’s aspect ratio, and that the TPCL will
21 Isopropanol, air 0.00463 0.32
be the same as this work for completely wetted channel initially.
22 Isopropanol, air 0.00579 0.40
23 Isopropanol, air 0.00694 0.47 In this work, the channel is shallow and was fully wetted initially,
24 Isopropanol, air 0.00810 0.55 hence a fixed TPCL was observed.
25 Isopropanol, air 0.00926 0.63 Due to a low aspect ratio of the channel, the meniscus in
26 Isopropanol, air 0.01042 0.71
microchannel is prominent at low flowrates (i.e., QL = 5–10 ml/h),
and the liquid surface become flatter with increasing flowrates as
shown in Fig. 8. In this study, the film thickness are determined
constant, a quasi-steady state of the falling film flow was reached from Eq. (7) based on the average measured film thickness δ̄d
and the iterative computation was terminated. within 500 μm in channel center.
The liquid film is in laminar flow under current experimental
4. Results and discussion conditions as shown in Table 2. It is assumed that there is no fluc-
tuation along the flow direction which is consistent with the sim-
4.1. Flow pattern visualization ulation results. Fig. 9 shows the volume fraction distribution con-
tours in quasi-steady state, in which the liquid phase is blue and
In order to keep the liquid film stable, the liquid will pass the gas phase is red. Between the blue and red is the transition
through the tube firstly before flowing into the channel. The wet- region from liquid and gas. It is obvious that a smooth film surface
ting behaviors and flow pattern in microchannel can then be in- with no wave is adhered to the wall.
vestigated with varying flowrates. Taking ethanol as an example, The liquid film thickness was both measured and simulated un-
the flow in microchannel was mapped into three different regimes: der experimental conditions listed in Table 2, and the results for

Please cite this article as: Y. Yang et al., Investigation of the liquid film thickness in an open-channel falling film micro-reactor by a
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240
Three phase contact line

Channel profile/liquid film

200

thickness (microns)
Q = 5 ml/h
160
Q = 10 ml/h
Q = 15 ml/h
120
Q = 20 ml/h
Q = 30 ml/h
80
channel wall

40
0 500 1000 1500 2000
Channel width (microns)

Fig. 8. Cross-sectional profiles of the liquid film surface at various liquid flowrates. (deionized water).

140

Film thickness(microns)
120

100

Isopropanol Ethanol Water

80 Exp Exp Exp
Sim Sim Sim
Nu Nu Nu
60 Ka Ka Ka

0 1 2 3 4 5 6 7

QN (10 m /(s m))

-6 3

Fig. 10. Comparison of liquid film thickness for three liquids with different
flowrates.

Fig. 9. Contours of air-isopropanol volume fraction distribution at QL = 5 ml/h: (a)

upper (b) lower. (For interpretation of the references to color in this figure, the
reader is referred to the web version of this article.)

three liquids are illustrated in Fig. 10, where δ r is plotted versus

volume flowrates per unit width, QN .
The results suggest that the liquid flowrates are a key factor af-
fecting the film thickness. A general trend is that the increase of
liquid flowrates leads to an increased film thickness. An increas-
ing film thickness is needed to provide increasing sectional area
for an increasing flowrate. The increase of film thickness is un-
avoidable. Another point to be noted is that the film thickness
is directly related to the liquid physical properties. Taking ethanol
and isopropanol as examples, their physical properties are basically Fig. 11. Schematic diagram of: (a) 3D force balance of falling film flow in mi-
the same except viscosity, and the results indicate that higher vis- crochannel, (b) 2D force analysis for the quasi-steady liquid film flow.
cosity leads to thicker film thickness under the same conditions.
Furthermore, the liquid film thickness difference enlarged with in-
creased liquid flowrates. Here, the film thickness is measured when of film fluid decreases with increasing viscosity. For a fixed volu-
the falling film flow achieved steady. For a steady flow, all the metric flowrate, a slow flow velocity needs a large sectional area or
forces are balanced. A schematic diagram of the force balance in a thicker film. Obviously, the falling film thickness increases with
the falling film process is provided both in the form of 2D and 3D, increasing viscosity. It clearly demonstrated that the viscous force
as shown in Fig. 11. In the vertical direction, the gravity of the fluid becomes dominant for liquid film thickness in microscale.
is almost balanced with the drag force acted on the liquid-solid in-
F du
terface by the bottom wall and side walls. For a viscous fluid, it =μ (16)
has a higher viscosity. Based on the Newton’s Law of Viscosity (see A dz
Eq. (16)), the velocity gradient du
dz
decreases with increasing viscos- Moreover, deionized water and ethanol have similar viscosity
ity at a fixed shear stress F/A. It means the average falling velocity but quite different density and surface tension, thicker film is ob-

Please cite this article as: Y. Yang et al., Investigation of the liquid film thickness in an open-channel falling film micro-reactor by a
stereo digital microscopy, Journal of the Taiwan Institute of Chemical Engineers (2018), https://doi.org/10.1016/j.jtice.2018.07.033
JID: JTICE
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8 Y. Yang et al. / Journal of the Taiwan Institute of Chemical Engineers 000 (2018) 1–10

served for ethanol under the same flowrates, which implies that role at microscale [27]. The experiments also confirmed that nei-
the film thickness is affected by multiple factors. ther Nusselt correlation nor Kapitza correlation can be used to
Furthermore, good agreement is achieved between experi- predict the liquid film hydrodynamics accurately in a wide flow
ments and CFD simulation, especially at high liquid flowrates (i.e., regime since the effect of surface tension and viscous force on
QN- water = 2.5 × 10−6 –8.0 × 10−6 m3 /(s m), QN- ethanol = 3.0 × 10−6 – film behaviors are not fully considered inside their models. Obvi-
6.0 × 10−6 m3 /(s m), QN- water = 1.0 × 10−6 –2.0 × 10−6 m3 /(s m)), and ously, a new correlation with wider application for film thickness
the maximum deviation is within 2.2%, 3.7% and 4.3%, respec- prediction is required. Consequently, dimensional analysis based
tively. However, an obvious inconsistency occurs at small flowrates. on Rayleigh method was applied to study the hydrodynamic char-
As mentioned above, liquid meniscus is much steeper at low acteristics in FFMR, and five dimensionless parameters including
flowrates, causing the “stretching efforts” of side-wall is more pro- Reynolds number (Eq. (19)), Capillary number (Eq. (20)), Weber
nounced, while a 2D simulation model simplified the physical pro- number (Eq. (21)), Froude number (Eq. (22)) and Bond number
cess by assuming equal film thickness along the channel width (Eq. (23)) were selected as follows.
with focus on channel middle section only. This oversimplification μ·U QL · μ
cannot simulate the physical process, and the resulted difference is Ca = = (20)
σ W ·D·σ
reasonable. Overall, great match between experiments and simula-
tion proves that the numerical model with a “liquid seal” structure ρ · U2 · l QL2 · ρ
is creditable and correct. We = = (21)
σ W · D2 · σ
Nusselt [30] and Kapitza [35] are two widely used correlations
for falling film flow behaviors prediction in flat vertical plate. Both U2 Q2
correlations have common assumptions including laminar liquid Fr = = 3 L2 (22)
g·l W ·D ·g
flow, zero shear stress at gas-liquid interface, and equal film thick-
ness along the plate width. ρ · g · l2 ρ · g · W 2
 1/3
3 · Q · μ 1 / 3 Bo =
σ
=
σ
(23)
3 · v · Re
2
δNu = =
L
(17)
The dimensionless film thickness (δ /W) can then be given by:
g W ·ρ ·g
 1/3 δ
2.4 · v2 · Re = C · (Re )a · (Ca )b · (W e )d · (F r ) f · (Bo)g (24)
δKa = (18) W
g It is difficult to fit Eq. (24) with so many dimensionless num-
bers. Furthermore, parameters involved in We and Fr also appeared
Where, Re denotes the film Reynolds number:
in all other three dimensionless numbers, and Bo is the result of
QL · ρ two other dimensionless numbers, namely, Bo = We/Fr. Therefore,
Re = (19)
W ·μ Eq. (24) was simplified to fit the experimental data.
As shown in Fig. 10, great match is observed between simula- δ
tion and Nusselt correlation, and the maximum deviation for these = C · (Re )a · (Ca )b · (Bo)d (25)
W
three liquids are 0.41%, 0.36%, 0.24%, respectively, which makes
Fitting the experimental results by the means of the least
perfectly sense because of the similar assumptions. Also, Nusselt
square method for Eq. (25), a, b, C, and d can be regressed and
correlation predicts lower film thickness than simulation since it
the corresponding correlation is as follows:
ignored the shear stress between the gas and liquid interface,
while Kapitza correlation obviously underestimates the film thick- δ
= 1.23 · (Re )0.0026 · (Ca )0.41 · (Bo)−0.43 (26)
ness instead. W
Compared with experimental results, Fig. 10 also indicates In Eq. (26), the Re fitting parameter a is far less than b for Ca,
that Kapitza correlation is good for film thickness prediction and the reason lies in that Ca is a function of Re (Eq. (27)).
at low flowrates (i.e., QN- water = 1.0 × 10−6 –1.5 × 10−6 m3 /(s m),
QN- ethanol = 1.0 × 10−6 –1.7 × 10−6 m3 /(s m)), while Nusselt cor- μ2
Ca = Re · (27)
relation presents better predictions at higher flowrates (i.e., D·ρ ·σ
QN- water = 2.2 × 10−6 –7.0 × 10−6 m3 /(s m), QN- ethanol = 2.8 × 10−6 – This is common for data fitting when two numbers are depen-
6.0 × 10−6 m3 /(s m)). It is obvious that neither Nusselt nor Kapitza dent each other, and “over-fitting” occurs. Similar situation also oc-
can give reasonably accurate prediction in a wide flow regime, curred in Anastasiou’s et al. [27] work. Since the power index a is
which mainly lies in the fact that these two models are derived much less than b for Re and Ca respectively, the function of Re can
from conventional falling film flow. In contrast, the dominant fac- be embodied in Ca mathematically. Besides, the absolute value for
tor affecting the fluid hydrodynamics and film thickness is quite b and d is very close, hence Eq. (25) can be further simplified.
different in microchannel due to their characteristics. As shown
δ
Ca a
in Fig. 11, compared with the traditional falling film reactor, the =C· (28)
falling film liquid is confined in microscale channels and should be W Bo
treated as a 3D flow. Apart from the bottom wall, the two channel By fitting the model with data again and a new correlation was
side walls are also wetted by the liquid. The increase of solid-liquid proposed (Eq. (29)). Compared with Eq. (26), the index of Ca and
contact area leads to an enhancement of the shear stresses exerted Bo almost unchanged with or without Re, only a slightly change on
by the wall, which means viscous force instead of gravity plays a C. Therefore, the impact of Re has been reflected in Eq. (29).
more important role in microchannel. Thus, the correlations devel-
δ
Ca 0.405
oped from conventional scale will not work well for microchannel. = 1.248 · (29)
W Bo
4.3. Correlation model To examine the applicability of the new proposed film thick-
ness prediction model, experimental data from both Yeong et al.
Previous study indicates that surface tension and viscous force [29] and Tourvieille et al. [33] has been used in this model. Two
instead of inertial and gravitational forces play more important deviations, 7% and 20%, are also presented in Fig. 12. Apparently,

Please cite this article as: Y. Yang et al., Investigation of the liquid film thickness in an open-channel falling film micro-reactor by a
stereo digital microscopy, Journal of the Taiwan Institute of Chemical Engineers (2018), https://doi.org/10.1016/j.jtice.2018.07.033
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Y. Yang et al. / Journal of the Taiwan Institute of Chemical Engineers 000 (2018) 1–10 9

5. Conclusion
140
This work +7%
A procedure and method to measure the liquid film thickness in
Yeong et al. [29] +20% the falling film micro-reactor (FFMR) by a stereo digital microscopy
120
-7% was developed. Three liquids including deionized water, ethanol
Tourvieille et al. [33]
and isopropanol were used to study the hydrodynamic behaviors
in a customer designed FFMR. This method is simple, cheap, and
δ measured (microns)

100
-20% non-intrusive with good accuracy. The liquid flowrates and physi-
cal properties exert a remarkable influence on falling film behav-
80
iors, and the film thickness increases with increasing flowrate and
viscosity under given conditions. The viscous force plays a domi-
60 nant role in the falling film process.
The film-forming characteristics in microchannel were also sim-
ulated by CFD simulation, and good match has been achieved with
40
experimental data at higher liquid flowrates.
Based on the experimental results, a film thickness predic-
20 tion model is developed through the dimensional analysis, namely,
δ /W = 1.248 · (Ca/Bo)0.405 . This model has been validated by the ex-
perimental data from both this work and public domain as well
0 with an average deviation of 7% and 20%, respectively, which is
0 20 40 60 80 100 120 140
better than the prediction from Nusselt, Kapitza and Tourvieille
δ predicted (microns) models.
As a result, the established method is proved to be an effec-
Fig. 12. Parity plots of liquid film thickness model prediction vs. experimental data.
tive way to study the film thickness in FFMR as well as liquid flow
characteristics in other micro-devices. The proposed model is not
only simple, but provides better prediction with wide application
. .
for film thickness in FFMR.
.
Tourvieille [33] = .
⁄
5.2
Nusselt [30] = Notes
⁄
2.
Kapitza [35] = The authors declare no conflict of interest.
5.0
log(δ/W)

4.8
Yeong et al. [29]
Tourvieille et al. [33]
4.6
This work
4.4
-4.0 -3.5 -3.0 -2.5
log(Ca/Bo)
Fig. 13. Model comparison and validation with published experimental data.
the new model gave best match for the whole source experimen-
tal data with 7% deviation only, which proves to be a good corre-
lation with much wider flow regime application. Meanwhile, this
model also gave prediction for Yeong’s et al. and Tourvieille’s et.al
research system with a relative deviation less than 20%.
Both Yeong et al. [29] and Tourvieille et al. [33] had measured
the film thickness in a FFMR with an aspect ratio of 1/3 using dif-
ferent methods, and the latter also proposed a model to predict
the film thickness. To further validate the proposed model in this
work, Eq. (29) has been compared with the available Tourvieille,
Nusselt and Kapitza correlations based on experimental data from
Yeong et al. and Tourvieille et al.
As illustrated by Fig. 13, although all these models show the
same trend, both Nusselt and Kapitza correlations overestimate the
liquid film thickness, while Tourvieille correlation underestimate
them comparing with experimental data. However, the proposed
new correlation, Eq. (29), obtained great match covering the full
two party experimental data. As a result, this new correlation is
not only simple but also provides better prediction with wide ap-
plication for film thickness in FFMR.
Acknowledgments
This work was supported by the National Natural Science Foun-
dation of China (Grant no. 21576168).
.
= 1.248
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