Chemical Engineering Science 225 (2020) 115800

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Chemical Engineering Science

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

3D CFD modelling of liquid dispersion in structured packed bed column

for CO2 capture
Mohammad Ashraf Hossain a, Seyed Ali Nabavi a,⇑, Panneerselvam Ranganathan b, László Könözsy c,
Vasilije Manovic a,⇑
a
Centre for Climate and Environmental Protection, Cranfield University, Bedford, Bedfordshire MK43 0AL, UK
b
Department of Chemical Engineering, National Institute of Technology Calicut, Kozhikode 673601, India
c
Centre for Computational Engineering Sciences, Cranfield University, Bedford, Bedfordshire MK43 0AL, UK

h i g h l i g h t s

3D two-fluid flow models for prediction of liquid-gas hydrodynamics are developed.

Higher liquid velocity leads to overconcentration of liquid on its border.

Multiple liquid inlets increase local volume fraction and slightly increase pressure drop.

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

Article history: Structured packing has been used for gas-liquid reactions in several industrial processes, including
Received 12 February 2019 amine-based CO2 scrubbing. Accurate prediction of flow behaviour within the columns provides a better
Received in revised form 6 April 2020 understanding for process intensification and optimisation, leading to more efficient systems and reduc-
Accepted 12 May 2020
tion in capital cost. In this work, three-dimensional (3D) transient Eulerian-Eulerian two-phase flow
Available online 18 May 2020
models were developed to assess mechanical dispersion models for prediction of the liquid dispersion.
The present model showed very good agreement with experimental results, but also provided much bet-
Keywords:
ter predictions compared to two-dimensional (2D) models, indicating the anisotropic behaviour of flow.
CO2 capture
Multiphase Eulerian-Eulerian model
It was found that an increase in inlet velocity of liquid resulted in a wider dispersion, but with overcon-
Liquid dispersion centration on its border. Moreover, it was shown that multiple liquid inlets showed an increase in liquid
Structured packing hold-up, but slightly increased pressure drop along the column, compared to the single liquid inlet.
Computational fluid dynamics Ó 2020 Elsevier Ltd. All rights reserved.

1. Introduction short- to long-term strategies to reduce CO2 emissions (Met Office,

Two centuries of fossil fuel combustion to address the growing
energy demand have significantly increased the level of atmo-
spheric CO2 concentrations and contributed to global warming
and climate change (Mac Dowell et al., 2010). The atmospheric
concentration of CO2 has increased from 280 ppm in the mid-
1800s to nearly 410 ppm in 2019, and resulted in nearly 0.8 °C
increase in global mean surface temperature compared to the
pre-industrial levels (IEA, 2016; NASA, 2019). The increase in the
temperature over the period of 1901–2010 has led to a 20-cm rise
in global mean sea level. It is believed that the temperature rise
should be limited to a maximum of 2 °C by 2100 (2DS), by adopting
⇑ Corresponding authors.
E-mail addresses: s.nabavi@cranfield.ac.uk (S.A. Nabavi), v.manovic@cranfield.
ac.uk (V. Manovic).
2015), in order to prevent severe climate change events. Accord-
ingly, the UK government has targeted reducing greenhouse gas
(GHG) emissions including CO2 by at least 80%, from the 1990
baseline, by 2050 (DECC, 2012). The power sector has been recog-
nised as one of the major CO2 emitters, and accounts for almost
60% of global CO2 emissions (IEA, 2016), thus requiring immediate
attention. Carbon capture and storage (CCS) is considered as the
key mitigation approach for decarbonisation of this sector (CCC,
2015; TUC & CCSA, 2013).
Carbon capture is considered as the primary and the most
expensive step in the CCS chain. The main CO2 capture technolo-
gies are oxy-combustion, pre-combustion and post-combustion
capture (Kenarsari et al., 2013). In oxy-fuel combustion, the fuel
is combusted using oxygen instead of air; thus, the composition
of the flue gas is mainly CO2 and H2O. Upon condensation of
H2O, a relatively pure stream of CO2 can be achieved. However,

https://doi.org/10.1016/j.ces.2020.115800
0009-2509/Ó 2020 Elsevier Ltd. All rights reserved.
2 M.A. Hossain et al. / Chemical Engineering Science 225 (2020) 115800
Nomenclature
Symbol Description [Unit]
as Packing external surface area per unit volume of bed
[m2m3]
ae Effective contact area between the gas and liquid phases
[m2m3]
E1 ; E2 Ergun constants [–]
fspread Spreading factor [m]
fe Fraction of wetted area [–]
! !
F disp;k Dispersive term in the momentum equation for phase k
[Pa]
g Gravitational acceleration [ms2]
hL Liquid hold up [–]
!
Jl Local liquid flow rate [s1]
K gs Gas-solid drag coefficient [–]
K ls Liquid-solid drag coefficient [–]
K Ig Momentum exchange coefficient at gas-liquid interface
[–]
P Pressure [Pa]
Q Volume flow rate [m3s1]
the O2 supply via an air separation unit is energy-intensive and
increases the efficiency penalties of the capture system (Burdyny
and Struchtrup, 2010; Kenarsari et al., 2013). In pre-combustion
capture, the fuel is mainly converted to CO and H2 through a gasi-
fication or gas reforming process. CO is then converted to CO2
through gas shift reactions to produce a CO2/H2 stream. Upon
removal of CO2, H2 is used as fuel in air-fired combustion pro-
cesses. This approach benefits from high CO2 partial pressure that
facilitates the CO2 capture process (Rubin et al., 2012). In post-
combustion capture (PCC), CO2 is captured from flue gases prior
to release into the atmosphere. Although the partial pressure of
CO2 in flue gas is relatively low (typicaly less than 0.15 bar), which
causes relatively high energy penalties, PCC systems can be retro-
fitted to existing power stations without extensive modifications.
Thus, PCC is considered as the most viable short- to medium-
term carbon capture approach (D’Alessandro et al., 2010;
Kenarsari et al., 2013).
Chemical solvent scrubbing using mainly monoethanolamine
(MEA) in packed columns is considered as the most commercially
proven PCC approach (Rochelle, 2009). Although MEA is inexpen-
sive and has relatively high CO2 capture capacity, the MEA-based
PCC process is energy-intensive due to required high energy
demand in the regeneration step, causing high efficiency penalties.
In addition, due to the low surface area-to-volume ratio of MEA
solution in the packed column, compared to solid-based capture
systems, large reactors are required that additionally increase the
capital costs and energy penalties (D’Alessandro et al., 2010; da
Silva and Booth, 2013; Yu, 2012). CO2 uptake in MEA scrubbing
is a mass transfer process with chemical reaction. Therefore, a
reduction in the energy penalties can be achieved by the intensifi-
cation of the MEA scrubbing process through increasing the mass
and heat transfer, so that a smaller reactor can be utilised (Reay,
2008). So far, a few intensification strategies, such as utilising
rotating bed reactors (Kang et al., 2014; Visscher et al., 2013) and
structured packing (Razi et al., 2012), have been proposed and
applied.
Structured packing has been widely used in industrial applica-
tions for distillation, scrubbing, and stripping and, due to several
advantages, such as low pressure drop, good wettability, and high
capacity and efficiency, has been considered for MEA scrubbing
(Razi et al., 2012). The initial and key factor in understanding the
qL Liquid load [m3m2h1]
r Radial position from reactor centre [m]
Re Reynolds number [–]
!
R I;k Average momentum transfer at interphase wall [Pa]
S Spreading tensor [–]
!
S porous;k Average momentum transfer at the wall for phase k [Pa]
t Time [s]
!
uk Velocity vector of phase k [ms1]
u d;g Drift velocity of gas [–]
!
u d;l Drift velocity of liquid [–]
V Volume [m3 ]
Z Streamwise distance from liquid inlet [m]
aL Volume fraction of liquid [–]
aG Volume fraction of gas [–]
e Porosity [–]
q Density [kgm3]
s Viscous stress tensor [Pa]
l Dynamic viscosity [Pas]
mass transfer and chemical reactions in structured packing and
further structural optimisation mainly depends on accurate predic-
tion of hydrodynamics of the structured packed column.
Computational fluid dynamics (CFD) is a powerful tool for flow
field-based quantification of measures that are hard to achieve
through experiments, and has already been used to study CO2-
MEA scrubbing within structured packing at different scales
(Sebastia-Saez et al., 2015a). The investigation of liquid scrubbing
within structured packing has been performed in three distinct
but complementary scales: micro-, meso-, and macro-scale
(Raynal and Royon-Lebeaud, 2007). Micro-scale studies have been
performed in millimetre-sized domains, mainly focused on predic-
tion of liquid-gas interface profile, liquid hold-up, and reactive
mass transfer (Sebastia-Saez et al., 2015b, 2014, 2013). Meso-
scale research has looked at gas-liquid flow behaviour (mainly
pressure drop, liquid hold-up and interfacial area), and mass trans-
fer over a set of representative elementary units (REUs) of struc-
tured packing (centimetre-sized domains) (Chen et al., 2009;
Sebastia-Saez et al., 2015a). On the other hand, macro-scale inves-
tigations have been focused on the hydrodynamics and chemical
reactions within the entire column (metre-sized domains), and
have been mainly used to study liquid dispersion and design opti-
misation (Lappalainen et al., 2009; Fourati et al., 2013; Pham et al.,
2015; Kim et al., 2016).
In the macro-scale, bulk parameters such as porosity and per-
meability appear due to volumetric averaging of micro-scale prop-
erties such as pore size and pore space geometry. The averaging is
done on a scale which is larger than the pore sizes, and results in
the formation of a dispersion for both gas and liquid phases. In
addition, due to the presence of the porous zone, required resis-
tance terms need to be considered, which can be implemented
by relevant closure laws (Whitaker, 1973). The liquid spreading
profile within the structured packing is affected by four basic
mechanisms, namely: capillary dispersion; mechanical dispersion;
gas-liquid momentum transfer; and porous resistance. Capillary
dispersion is associated with the pressure gradient at the liquid-
gas interface, and might be neglected in macro-scale modelling
due to its insignificant effect (Fourati et al., 2013). Mechanical dis-
persion is a macro-scale-based mechanism, and occurs due to
advection of momentum by phases, which induces a random veloc-
ity field through the porous media (Koch et al., 1989). Gas-liquid
 M.A. Hossain et al. / Chemical Engineering Science 225 (2020) 115800 3

!
 !
! !

momentum transfer is attributed to the induced shear stress at the @
ak qk u k þ r  ak qk u k u k
@t
interface of the gas-liquid flow due mainly to drag force (Iliuta ð2Þ
! !
¼
 ! ! ! !
et al., 2004). Porous resistance is associated with viscous and iner- ¼ ak r p þ r  ak sk þ ak qk g þ aek S porous;k þ e R I;k þ F disp;k
tial resistances through the porous media that result in the loss of
!
viscous and kinetic energy (Wu et al., 2008). where p is the pressure, u is the velocity vector, q is the density, g is
It is necessary and complementary to obtain an in-depth under- ¼
the gravitational acceleration, and s is the average viscous stress
standing of the gas-liquid flow in the structured packing at all
tensor. The volume fraction of phase k, ak , is calculated as
three scales. Macro-scale modelling can reveal the average distri-
ak ¼ V k =V, in which, V k is the volume of phase k in a given occupied
bution of liquid within the entire column (Fourati et al. 2013).
volume V. Since both liquid and gas phases are mathematically con-
Solomenko et al. (2015) developed a series of 2D axisymmetric
sidered as interpenetrating continua, there is no overlapping of the
and 3D Eulerian-Eulerian CFD models and validated them with P
phases and ak ¼ 1: The porosity, e, is calculated as
c-ray tomography experimental data. The models were used to ! !
simulate the spreading of liquid in a gas-liquid co-current e ¼ ðV g þ V l Þ=V. S porous;k (porous resistance force), R I;k (gas-liquid
!
trickle-bed reactor. Fourati et al. (2013) developed a 2D axisym- momentum exchange force), and F disp;k (gas-liquid dispersion force)
metric Eulerian-Eulerian CFD model and implemented porous are source terms, discussed in detail below. Two proposed mechan-
resistance, gas-liquid momentum exchange, and dispersion forces. ical dispersion models, Cases 2 and 3, were implemented and com-
The structured packing was considered as a porous zone and the pared with no dispersion scenario (Case 1). The same porous
model was validated with their experiments. Relatively acceptable resistance and gas-liquid momentum transfer models were used
agreement between the experiment and the numerical model in all cases. The summary of the models is tabulated in Table 1.
implied that the porous zone can be considered as structured pack-
ing. Further, Lim and co-workers (Kim et al., 2016; Pham et al., 2.1.1. Porous resistance force
2015) extended the Fourati et al. (2013) model by incorporating The liquid-solid and gas-solid interaction forces are quantified
mass transfer and chemical reaction to investigate CO2 removal based on the approach proposed by Iliuta et al. (2004) and Iliuta
from natural gas in an absorber reactor with structured packing. and Larachi (2005) and are expressed by Eqs. (3) and (4)
The accurate prediction of CO2-MEA hydrodynamics in struc- ! ! 
tured packing is the key step for realistic modelling of mass trans- S porous;g ¼ ð1  f e ÞK gs  u g  ð3Þ
fer and chemical reaction, and further optimisation of the absorber
! ! 
reactor design. Despite those CFD models developed to predict S porous;l ¼ f e K ls  u l  ð4Þ
and/or improve the hydrodynamics of CO2-MEA scrubbing in
structured packing, there remains a considerable discrepancy where K gs and K ls are gas-solid and liquid-solid drag coefficients,
between the numerical models and experimental data. calculated by Eqs. (5) and (6), respectively.
In this work, 3D transient multiphase Eulerian-Eulerian numer-  
a  E1 ea2s b  E2 eas ! 
ical models were implemented to predict and explore the hydrody- K ls ¼  2 lL þ ql u l ð5Þ
36 al 6 al
namics of MEA scrubbing within a structured packed bed. For
prediction of the liquid dispersion in a counter-current gas-liquid  
a  E1 a2s b  E2 as  
flow, two different models of mechanical dispersion were imple- K gs ¼  lg þ qg ag !
u g ð6Þ
mented and assessed. In addition, the model was compared with 36 e 6 e
the 2D models presented in the literature, to determine the aniso- E1 andE2 are Ergun coefficients, and for Mellapak 250X they are
tropic behaviour of fluid flow. Moreover, the validated model was 160 and 016, respectively (Iliuta and Larachi, 2005). The modifica-
further used to study the effect of liquid nozzles on the flow beha- tion factors for the Ergun coefficients, a and b, are assumed in this
viour within the column. study to be 1 (Fourati et al., 2013).f e is the fraction of wetting area,
defined as the ratio of the effective contact area between the gas
2. Governing equations and numerical method and liquid phases (ae Þ to the specific surface area of the structured
packing (as ). lg and lL are the dynamic viscosities of gas and liquid,
2.1. Governing equations respectively, and, qg and ql are the densities of gas and liquid,
respectively. In addition, f e , representing the fraction of wetted
The hydrodynamics of gas-liquid flow through structured pack- area, is introduced to define wetting of the solid surface inside
ing was studied using a 3D multiphase Eulerian-Eulerian approach the packed bed column for a two-phase gas-liquid counter-
(two-fluid model). In this modelling, the following is assumed: (i) current flow. It is assumed that f e = 1, indicating that the walls
both gas and liquid phases are incompressible and Newtonian; are fully wetted by the liquid and there is no shear stress due to
(ii) the capillary dispersion is negligible (due to the large size of the presence of gas.
the reactor (Fourati et al., 2013); (iii) the liquid and gas velocity
profiles at inlets are uniform; (iv) porous media are isotropic; 2.1.2. Gas-liquid momentum exchange
and (v) neither mass transfer nor chemical reactions were consid- The gas-liquid momentum exchange force is expressed by Eq.
ered. In addition, Sulzer Mellapak 250 (M250X) was considered as (7)
the structured packing, and all packing factors were adopted from

! ! !
the experimental and numerical studies performed by Fourati et al. R exc;lg ¼ f e K lg u g  u l ð7Þ
(2012, 2013).
In the two-fluid model, a set of continuity and momentum
equations is solved for each individual phase.
Table 1
The continuity equation for phase k (k can be liquid, l, or gas, g) Cases investigated in this work.
is
Mechanical dispersion
@

!
ðak qk Þ þ r  ak qk u k ¼ 0 ð1Þ Case 1 No dispersion
@t Case 2 Lappalainen et al. (2009)
Case 3 Mewes et al. (1999)
The momentum equation for phase k is
4 M.A. Hossain et al. / Chemical Engineering Science 225 (2020) 115800

where K lg is the coefficient of momentum exchange, which is imple- volume-based commercial software ANSYSÒ Fluent v. 14.5. The
mented based on the correlation developed by Iliuta and Larachi discretised momentum equation was approximated using both
(2005) and is given by Eq. (8) second-order upwind and QUICK schemes. Since the discrepancy
  between the obtained solutions by the two schemes was negligi-
c  E1 a2s d  E2 as ! 
K lg ¼  þ qg u g  !
u l ð8Þ ble, the second-order upwind scheme was used to carry out the
36 eag 6 e simulations. The pressure-velocity coupling was achieved by the
where c and d are the modification factors for the Ergun coeffi- SIMPLE scheme. One of the limitations of the Eulerian-Eulerian
cients, assumed in this study to be 1 (Fourati et al., 2013). approach is associated with maintaining the numerical stability
Special attention should be taken when this model is being of the simulations. To mitigate any numerical instability and
implemented. Namely, for very small ag (in the absence of gas), ensure that the simulations converge, a constant time-step of 10-
5
! s was selected, and relaxation factors of pressure = 0.3, density = 1,
K lg tends to infinity, and results in nonphysical R exc;gl and poor
body forces = 1, momentum = 0.5, and volume fraction = 0.3 were
hydrodynamic prediction. To avoid this issue, the following algo-
used.
rithm is implemented and is given by Eq. (9)
A schematic of simulated geometries for single and multiple liq-
8
 
< K ¼ cE1  a2s þ dE2 as q !u 
!
u  for ag > 0:0001
uid inlets is presented in Fig. 1. A series of hexahedral-based
lg 36 eag 6 e g g l
ð9Þ meshes were constructed using ICEM CFD Meshing Software. A
: K lg  0 for ag  0:0001 grid dependency study was performed by constructing three
meshes with size of 11456, 210235, and 313,841 mesh elements
for single liquid inlet, and 36294, 284544, and 383,218 for multiple
2.1.3. Dispersion forces liquid inlets, respectively. As shown in Fig. 2c and d, the discrepan-
For Case 2, the gas and liquid mechanical dispersion forces in cies in results between cases with 210,235 and 313,841 mesh ele-
the structured packing are calculated by Eqs. (10) and (11), respec- ments for single inlet, and cases with 284,544 and 383,218 mesh
tively (Lappalainen et al., 2009) elements for multiple inlets, were negligible. Moreover, the axial
!

! ! ! variation of the liquid volume fraction and dimensionless pressure
F disp;g ¼ ag K gs u d;g þ eK lg u d;g  u d;l ð10Þ
drop (DP/DPmax) obtained from CFD simulation is plotted in Fig. 2e

 and f. It can be seen that both medium and fine meshes predict a
! ! ! !
F disp;l ¼ al K ls u d;l  eK lg u d;g  u d;l ð11Þ similar trend, whereas a large discrepancy is observed in the coarse

! !
where u d;g and u d;l are the gas and liquid drift velocities, calculated
by Eqs. (12) and (13), respectively.
 
! 
 u g 
f spread  ag 
!  !
u d;g ¼  rag ð12Þ
ag
! !
! f spread  u l  !
u d;l ¼  r al ð13Þ
al
where f spread is the spread factor, and in this study is assumed as
3.7 mm (Fourati et al., 2012).
For Case 3, the mechanical dispersion model, Eq. (14), proposed
by Mewes et al. (1999) is implemented. The reason for implement-
ing this correlation is to enable a comparison between mechanical
dispersion and the spread tensor approach for prediction of the liq-
uid dispersion in counter-current gas-liquid flow.
! ¼ ¼ !
F disp;l ¼ fðS ðal u l ÞÞ ð14Þ
¼
In Eq. (14) S is the liquid spreading tensor. No closure law was
¼
found for approximation of S; thus, in this study, it is assumed as a
constant value of 3.7 mm, as it was proposed by Fourati et al.
¼
(2013). f is the resistance tensor arising from the wall shear stress,
and calculated by Eq. (15) (Fourati et al., 2013):
 
¼ K ls ¼ ! ! 
f¼ ðS  r  J l Þ ð15Þ
e
! ! !
where J l is the local liquid flow rate ( J l ¼ al  r u l Þ, and K ls is cal-
culated by Eq. (5). The detailed derivations of the closure sub-
models are provided by Fourati et al. (2013).

2.2. Numerical method

Fig. 1. Schematic of simulated geometry with single and multiple inlets, along with
boundary conditions. The height of the reactor is 760 mm, the diameter of the
The governing equations were solved by utilising an unsteady reactor is 400 mm, and liquid inlet diameter (Din) is 24 mm. Z is the distance from
pressure-based segregated algorithm established in the finite- the liquid inlet.
 M.A. Hossain et al. / Chemical Engineering Science 225 (2020) 115800 5

Fig. 2. Mesh structure of structured packing with (a) single liquid inlet; and (b) multiple liquid inlets. Grid independency analysis of the radial liquid volume fraction (c)
single liquid inlet at Vin,l = 1.2 m/s; and (d) multiple liquid inlets, Vin,l = 0.09 m/s, liquid flow rate is constant at 0.54 kg/s, Z = 4.17 Din, and Din = 24 mm. Grid independency
analysis of the (e) liquid volume fraction, and (f) dimensionless pressure drop (DP/DPmax) along the height of the column for a single inlet.

simulation. Therefore, the mesh sizes of 210,235 and 284,544 for
single and multiple inlet cases, respectively, were selected for the
simulations. The simulations were performed using 48 CPU cores
in Delta high-performance computing facility at Cranfield Univer-
sity. Summaries of boundary conditions, and fluid properties used
for the simulations are in Tables 2 and 3, respectively.
3. Results and discussion
3.1. Validation and assessment of numerical model
Fig. 3 shows the quantitative comparison of the radial distribu-
tion of average liquid volume fraction of various Cases (1–3) with
the experimental (Fourati et al., 2012) and numerical data (Fourati
et al., 2013) at Z = 13.7Din and Z = 20.0Din, with a liquid loading, ql ,

Table 2 Table 3
Summary of boundary conditions. Fluid properties of liquid and gas phases.

Boundaries Type q (kg/m3) m (mPas)

Liquid/Gas inlet Velocity inlet Liquid phase Water 997 0.001
Cylinder wall No-slip wall Gas Phase Air 1.105 1.00  105
Outlets Pressure outlet Liquid phase 30 wt% MEA 1012 2.48
Structured packing Porous zone Gas phase Carbon dioxide 1.79 1.37  10-2
6 M.A. Hossain et al. / Chemical Engineering Science 225 (2020) 115800
of 16 m3/m2/h, and inlet velocity of gas of 1.05 m/s (corresponding
to a gas capacity factor of 1.16 Pa0.5). The details of the experimen-
tal setup can be found in the work of Fourati et al. (2012). Amongst
the developed CFD models in this study, Case 2 showed very good
agreement with experimental data. The poor prediction of Case 1 is
due to the fact that liquid dispersion is not considered in the
model. Case 3 resulted in slight under-prediction of the average
liquid volume fraction compared to the experimental data of
Fourati et al. (2012). The liquid saturation profile predicted by Case
3 shows a lesser spread in the radial position. This implies that the
models of mechanical dispersion proposed by Mewes et al. (1999)
with the specified liquid spreading tensor based on the advection–
diffusion model of flow resistance tensor may not be capable of
accurately predicting the mechanical dispersion in structured
packing. The Mewes model was originally developed and tested
for trickle-bed and monolithic reactors and the model was
extended to apply in the structural packed bed column. However,
its validation with the experimental data was not reported quanti-
tatively (Mahr and Mewes, 2007). The proposed dispersion model
is based on both the flow resistance tensor and liquid spreading
tensor. The flow resistance tensor depends on velocity as well as
the volume fraction. One of the limitations of this model when con-
sidered to be extended to the structured packing is modelling
approach of the flow resistance and liquid spreading tensor values.
Fig. 3. Validation of developed CFD models with existing experimental and
numerical data: radial distribution of average liquid volume fraction at (a)
Z = 13.7 Din; and (b) Z = 20.0 Din. Din = 24 mm, Vin,l = 1.2 m/s and Vin,g = 1.05 m/s.
In this work, the anisotropic spreading tensor of liquid was
replaced by an isotropic scalar factor for model simplification,
i.e., a constant value of liquid spreading tensor of 3.7 mm, proposed
by Fourati et al. (2013), was used. An advection–diffusion-based
model equation was used for the resistance tensor. Thus, further
modification needs to be considered in the exact method of liquid
spreading and the flow resistance tensor predictions for the Eule-
rian simulation of structured packing. It should be highlighted that
the liquid dispersion within the packed bed column can be mod-
elled based on mechanical dispersion, spread tensor and tortuosity.
The current simulations were developed based on mechanical dis-
persion (Lappalainen et al., 2009) and the spread tensor approach
(Mewes et al., 1999). Also, the advection–diffusion model used
for the spread factor calculation needs to be developed in a more
conservative form. A comparison of liquid spreading profiles repro-
duced by Cases 1–3 is presented in Fig. 4. A narrow distribution of
liquid along the column in Case 1 was observed. It is evident that
Cases 2 and 3 showed a wider liquid spatial distribution. Moreover,
Case 2 resulted in a noticeably more accurate reproduction of
experimental data compared with the 2D axisymmetric CFD model
developed by Fourati et al. (2013), specifically in the lower range of
radial distance (r) of 0–0.05 m. This can be attributed to the 3D nat-
ure of multiphase flow through structured packing and the distri-
bution of flow anomalies, highlighting the necessity of 3D models
for accurate prediction of hydrodynamics.
3.2. Effect of operational condition and geometry
Since Case 2 showed the best agreement with experimental
data, the proposed approach by Lappalainen et al. (2009) for
mechanical dispersion was used in further investigation of the flow
behaviour in the packed column. The effect of liquid loading on the
liquid hold-up in a packed column with a single inlet for liquid is
presented in Fig. 5a. In the same plot, the empirical relation
between liquid hold-up and liquid loading reported by Billet
(2015) and Fourati et al. (2012) is also considered to verify the pre-
sent model for the prediction of liquid hold-up quantitatively. The
liquid hold-up (hL) is calculated using Eq. (16) (Pham et al., 2015)
P
i al;i DV i
hL ¼ P ð16Þ
i DV i
where DV i is the cell volume. An increase in liquid loading from
15.5 to 80.3 m3/m2/h caused the liquid hold-up to rise from 0.02
to 0.05. This is mainly attributed to the dynamic hold-up and accu-
mulation of larger amounts of liquid along the packed column at
Fig. 4. Simulated 30 wt% MEA/CO2 flow behaviour within a structured packed bed
using the developed CFD models in this study. Vin,l = 1.2 m/s, Vin,g = 1.05 m/s and
Din = 24 mm.
 M.A. Hossain et al. / Chemical Engineering Science 225 (2020) 115800 7

DP 3
¼ 0 h 0i ð19Þ
l 4f 0 1  q u2 d0
0 4:65 g g p


where
   c=3
0 hL
f0 ¼ f0 1e 1 =ð1  eÞ ð20Þ
e

5 3
f0 ¼ þ þ 0:45 ð21Þ
Reg Re0:5
g

 
hL
 ¼e 1
0
ð22Þ
e
 
 Re5g  2Re30:5
g
c¼ ð23Þ
f0

8h
i91=3
0
< 1   1  heL =
dp ¼ dp ð24Þ
: ð1  eÞ ;

dp ¼ 6ð1  eÞ=as ð25Þ

Fig. 5. Variation of (a) liquid hold-up and (b) wet pressure drop as a function of
liquid loading for a single-inlet packed column. Vin,l = 1.2 – 6.2 m/s, Vin,g = 1.05 m/s
and Din = 24 mm.
higher liquid loading. The liquid hold-up predicted by the present
model based on the experimental data of Fourati et al. (2012) and
Tsai et al. (2011) matches the empirical correlation proposed by
Billet (2015), Eq. (17)
 1=3
as
hL ¼ 0:555 u2l 4:65 ð17Þ
ge
where ul is the liquid velocity. However, the correlation reported by
Fourati et al. (2012), Eq. (18), over-predicts liquid hold-up.
 1=3
lL
hL ¼ 0:0209 q0:4 ð18Þ
lwl
In Eq. (18) mw is the dynamic viscosity of water. A similar obser-
vation is reported by Fourati et al. (2012) who experimentally
measured and developed a correlation for liquid hold-up in a
packed column with a single inlet for liquid. They found that the
averaged liquid hold-up is almost two times higher than that pre-
sented in the literature. Fig. 5b shows the effect of liquid load on
wet pressure drop obtained in this study as well as a correlation
reported by Stikkelman et al. (1989), Eq. (19)
The condition used for wet pressure drop prediction is the same
as that used in liquid hold-up prediction. It was found that the wet
pressure drop increased when the liquid loading was raised from
15.5 to 80.3 m3/m2/h. At a constant gas velocity, increasing liquid
loading leads to an increase in liquid volume fraction and reduces
the available cross-sectional area for gas flow, consequently result-
ing in a higher pressure drop. In addition, pressure drop occurs due
to friction at the gas-liquid interface and the induced drag when in
contact with the reactor wall. Therefore, a rise in liquid loading
causes an increase in the liquid velocity at the gas-liquid and
wall-liquid interfaces, which elevates the shear stress and, conse-
quently, the pressure drop. It was also found that the wet pressure
drop obtained from the present model matches with the Eq. (19)
for the lower liquid loading, but underpredicts for the higher liquid
loading.
The wet pressure drop along the column in the multiple liquid
inlets case was validated with the experimental data of Tsai et al.
(2011) who studied CO2 absorption within several structured pack-
ings including M250X. At a liquid loading of ~24.4 m3/m2/h and gas
capacity factor of 1.16 (Pa)0.5, the predicted pressure drop by the
model was 0.24 mbar/m, which was in very good agreement with
the measured experimental pressure drop of 0.22 mbar/m.
The radial distribution of the liquid volume fraction along the
column, as a function of inlet velocity of liquid (Vin,l), is presented
in Fig. 6. It can be clearly seen that an increase in the inlet velocity
of liquid from 1.2 to 6.2 m/s resulted in a wider radial distribution
of liquid. However, the variations in radial distribution of liquid
reduced when the inlet velocity of liquid exceeded 2.9 m/s. It
was also noticed that at a constant Z, the liquid volume fraction
was relatively low at the centre of the column, and overconcen-
trated at its border. This behaviour was intensified with inlet veloc-
ity of liquid, and the largest liquid volume fraction at its border
was observed at Vin,l of 6.2 m/s for Z = 0.1 – 0.5 m. Moreover, the
radial distribution of liquid in all cases was anisotropic, implying
the necessity of 3D models for exploring the liquid-gas interaction
within packed columns. The anisotropic fluid flow behaviour was
confirmed experimentally by Fourati et al. (2012). From a mod-
elling perspective, the reason for the anisotropic behaviour of the
liquid inside the structured packing can be associated with the dis-
persion term in the momentum equation, i.e., Eq. (11) for the
Lappalainen et al. (2009) model and Eq. (14) for the Mewes et al.
8 M.A. Hossain et al. / Chemical Engineering Science 225 (2020) 115800

Fig. 6. Evolution of cross-sectional liquid volume fraction contours along the reactor for Case 2 at inlet velocity of liquid (Vin,l) of (a) 1.2 m/s; (b) 2.9 m/s; (c) 4.3 m/s; (d) 6.2 m/
s. Vin,g = 1.05 m/s and Din = 24 mm.

(1999) model. To demonstrate that the observed dispersion pat- Table 4

tern does not stem from any numerical instability, the radial distri-
bution of the liquid volume fraction along the column for the case
without a dispersion term (Case 1) is also provided in Fig. 7. It can
be seen that the same anisotropic pattern, similar to Case 2 (Fig. 6),
associated with liquid dispersion in structured packing, is
captured.
Table 4 presents the comparison of liquid hold-up and wet pres-
sure drop for the packed column with single and multiple liquid
inlets (13 nozzles) of the same diameter (Din = 24 mm, Fig. 1)
and liquid mass flow rate of 0.54 kg/s. It was found that increasing
the number of liquid inlets from 1 to 13 resulted in almost three
times larger liquid hold-up and raised the wet pressure drop from
98 to 310 Pa/m. A comparison between the radial distribution of
volume fraction along the reactor with single and multiple liquid
inlets is presented in Fig. 8. The packed column with a single liquid
inlet was characterised with relatively low volume fraction, but a
wider radial distribution of the liquid, which is associated with sig-
nificantly larger inlet velocity (1.2 m/s) compared to that of multi-
ple inlets (0.09 m/s). On the other hand, the column with multiple
Effect of the number of liquid nozzles on the liquid hold-up and wet pressure drop
based on Case 2. For single liquid inlet Vin,l = 1.2 m/s, and for multiple liquid inlets
Vin,l = 0.09 m/s. In both cases liquid mass flow rate is constant at 0.54 kg/s.
Vin,g = 1.05 m/s and Din = 24 mm.
Number of liquid nozzles 1 13
Liquid hold-up (–) 0.018 0.062
Wet pressure drop (Pa/m) 98 310
liquid inlets featured a narrow radial distribution of liquid and rel-
atively overconcentrated liquid fraction at the centre of the trajec-
tory for each inlet. Therefore, the increased liquid hold-up and
pressure drop along the column with multiple inlets can be attrib-
uted to multiple regions with a narrow liquid spreading and over-
concentrated liquid regions at the centre.
It should be noted that during CO2 capture, a larger liquid vol-
ume fraction can potentially enhance CO2 uptake. However, a nar-
row region of liquid with high volume fraction at the centre of the
trajectory for each inlet, in the case of multiple inlets, may reduce

Fig. 7. Evolution of cross-sectional liquid volume fraction contours along the reactor for Case 1 (no dispersion term). Vin,l = 1.2 m/s, Vin,g = 1.05 m/s, Din = 24 mm and Vin,
g= 1.05 m/s. Contours as in Fig. 6.
 M.A. Hossain et al. / Chemical Engineering Science 225 (2020) 115800
Fig. 8. Effect of number of liquid inlets (N) on cross-sectional contours of liquid volume fraction along the reactor (Case 2): (a) N = 1, Vin,l = 1.2 m/s; (b) N = 13, Vin,l = 0.09 m/s.
In both cases liquid flow rate is constant at 0.54 kg/s. Vin,g = 1.05 m/s and Din = 24 mm. Contours as in Fig. 6.
the mass transfer rate of CO2 into the amine solution due to the
maldistribution of liquid. Thus, for future work, physical and reac-
tive mass transfer need to be implemented in this model to provide
a better understanding of such behaviours.
4. Conclusions
3D transient Eulerian-Eulerian two fluid models were devel-
oped by implementing different models for mechanical dispersion
in order to further improve the predictability of liquid dispersion
within a structured packing. The results showed that the model
proposed by Lappalainen et al. (2009) provided a better prediction
of the liquid dispersion when compared with the model developed
by Mewes et al. (1999) based on spread tensor approach. In addi-
tion, the liquid dispersion was shown to be highly anisotropic,
which implied the necessity of utilising 3D models. Thus, much
better agreement with experimental data was achieved compared
to previously developed 2D models. It was found that increasing
the liquid velocity from 1.2 to 2.9 m/s considerably widened the
radial distribution of the liquid. Further increase in velocity to
6.2 m/s did not have significant effect on the liquid distribution
profile, but led to a shift in liquid hold-up from the centre of the
column to its border. Moreover, the average liquid hold-up and
wet pressure drop predicted by the present model were compared
with the empirical correlations available in the literature. An
increase in the number of liquid inlets from 1 to 13, at constant liq-
uid mass flow rate, increased liquid hold-up, but formed several
narrow overconcentrated liquid regions, which increased pressure
drop from 98 to 310 Pa/m. Although an increase in liquid hold-up
in the column can be beneficial, the presence of overconcentrated
narrow regions, observed when multiple liquid nozzles were used,
may reduce mass transfer due to the maldistribution of liquid.
Therefore, in future work physical and reactive mass transfer
should be implemented in such models to address these
uncertainties.
CRediT authorship contribution statement
Mohammad Ashraf Hossain: Investigation, Writing - original
draft. Seyed Ali Nabavi: Writing - original draft, Writing - review
& editing, Visualization, Project administration. Panneerselvam
Ranganathan: Validation, Writing - review & editing. László
Könözsy: Methodology, Software, Conceptualization. Vasilije
Manovic: Supervision, Writing - review & editing.
9
Declaration of Competing Interest
The authors declare that they have no known competing finan-
cial interests or personal relationships that could have appeared
to influence the work reported in this paper.
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