Journal of Environmental Chemical Engineering 9 (2021) 106519

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Journal of Environmental Chemical Engineering

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

Unravelling CO2 capture performance of microalgae cultivation and other

technologies via comparative carbon balance analysis
Yoke Wang Cheng a, b, Jeremy Sheng Ming Lim c, Chi Cheng Chong a, b, Man Kee Lam a, c, *,
Jun Wei Lim a, d, Inn Shi Tan e, Henry Chee Yew Foo e, Pau Loke Show f, Steven Lim g
a
HICoE-Centre for Biofuel and Biochemical Research, Institute of Self-Sustainable Building, Universiti Teknologi PETRONAS, 32610 Seri Iskandar, Perak, Malaysia
b
Department of Chemical Engineering, School of Engineering and Computing, Manipal International University, 71800 Putra Nilai, Negeri Sembilan, Malaysia
c
Chemical Engineering Department, Universiti Teknologi PETRONAS, 32610 Seri Iskandar, Perak, Malaysia
d
Department of Fundamental and Applied Sciences, Universiti Teknologi PETRONAS, 32610 Seri Iskandar, Perak Darul Ridzuan, Malaysia
e
Department of Chemical and Energy Engineering, Faculty of Engineering and Science, Curtin University, CDT 250, 98009 Miri, Sarawak, Malaysia
f
Department of Chemical and Environmental Engineering, Faculty of Science and Engineering, University of Nottingham Malaysia, Jalan Broga, 43500 Semenyih,
Selangor Darul Ehsan, Malaysia
g
Department of Chemical Engineering, Lee Kong Chian Faculty of Engineering and Science, Universiti Tunku Abdul Rahman, 43000 Selangor, Malaysia

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

Editor: Teik Thye Lim Microalgae cultivation, absorption, adsorption, and membrane separation are widely applauded as promising
technologies to sequester CO2 from flue gas. Herein, comparative carbon balance was used to elucidate their CO2
Keywords: capture performance in the aspects of CO2 emission rates (direct, indirect, total, and net), CO2 removal effi­
Carbon capture ciencies (apparent and actual), and CO2 removal rate per power input ratio. Screening criteria for effective CO2
Microalgae cultivation
capture system rule out energy-intensive sorption processes, put forward low energy membrane separation, and
Sorption
disclose alterable competency of microalgae cultivation. For CO2 capture from flue gas, microalgae (Chlorella
Membrane separation
vulgaris) cultivation in open raceway ponds was only inferior to membrane separation. To improve microalgal
CO2 capture, the sensitivity analysis was performed by replacing original microalgae species (C. vulgaris) or
cultivation system (open raceway pond). The microalgal CO2 capture in open raceway ponds became worse
following the substitution of C. vulgaris with alternatives (Botryococcus braunii, Chlorella kessleri, Chlorella pyr­
enoidosa, Scenedesmus obliquus, Spirulina sp., or Tetraselmis suecica). For microalgal (C. vulgaris) CO2 capture, the
competent cultivation systems included open raceway pond and airlift photobioreactor, while the bubble col­
umn, flat panel, or tubular photobioreactors were classified as non-competent systems. In short, microalgal
(C. vulgaris) CO2 capture was technically feasible in open raceway pond or airlift photobioreactor; further, the use
of airlift photobioreactor was preferred for better CO2 capture and microalgae biomass production. Due to the
necessity of a huge working volume, the low scalability of microalgae cultivation could hamper the industrial
application of microalgal CO2 capture from flue gas.

1. Introduction [4] are preferred for biomass-to-bioenergy valorisation; however, these

Global warming is daunting as drastic climate change (i.e., heat and
cold waves) inflicts catastrophic life loss and crop failure. Since the In­
dustrial Revolution, anthropogenic activities (mainly electricity gener­
ation from fossil fuels) largely augment global carbon dioxide (CO2)
emission [1]. As the most abundant greenhouse gas (76%), CO2 is almost
inseparable from the alarming global warming [2]. By virtue of low CO2
emission, thermochemical conversions like pyrolysis [3] and reforming
conversions and the combustion of carbonaceous biofuels still emit CO2.
Hence, carbon capture system is an indispensable facility in both fossil
fuels-based and biofuels-based power plants to lessen CO2 emissions
from power generation. To date, the adequate post-combustion carbon
capture technologies are absorption, adsorption, membrane separation,
and microalgae cultivation [5,6], where their respective pros and cons
are summarized in Table 1.
Absorption preferably utilizes Lewis base solvents (i.e., amines,

* Corresponding author at: HICoE-Centre for Biofuel and Biochemical Research, Institute of Self-Sustainable Building, Universiti Teknologi PETRONAS, 32610 Seri
Iskandar, Perak, Malaysia.
E-mail address: lam.mankee@utp.edu.my (M.K. Lam).

https://doi.org/10.1016/j.jece.2021.106519
Received 11 July 2021; Received in revised form 19 September 2021; Accepted 4 October 2021
Available online 8 October 2021
2213-3437/© 2021 Elsevier Ltd. All rights reserved.
Y.W. Cheng et al. Journal of Environmental Chemical Engineering 9 (2021) 106519

Table 1 characterization, wastewater treatment [12], growth kinetics [13], and

Pros and cons of common post-combustion carbon capture technologies [5,6].
No. Carbon Pros
capture
technology
1 Absorption • Strong affinity of CO2
towards Lewis base solvents
• Efficient CO2 removal even
for low CO2 partial pressure
• > 90% CO2 absorption
efficiency with
monoethanolamine
• Commercialized technology
2 Adsorption • Reusable, thermal stable,
and/or renewable
adsorbents
• Low operational cost and
ease of handling
• Possible tailoring of active
sites for high CO2 selectivity
• High process maturity
3 Membrane • Energy wise and
separation environmentally benign
process
• Low capital cost
• High CO2 selectivity
• Low-energy membrane
regeneration
• Physical CO2 isolation
4 Microalgae • Valorisation of CO2 into
cultivation microalgae biomass
• Possible further processing
of microalgae biomass into
valuable biofuels and
biochemicals
• Possible integration of
wastewater as cultivation
medium
• Unnecessary flue gas
pretreatment
• Phycoremediation of SO2
and NOx
parametric study [14]. Hence, the CO2 capture ability of microalgae
Cons cultivation was rarely benchmarked against other post-combustion CO2
capture technologies, leaving vagueness of its performance. Since such
benchmarking study is scarce, a comparative carbon balance analysis
• High-energy solvent was conducted herein, on the same mass basis of flue gas, to evaluate the
regeneration CO2 capture performance of microalgae cultivation (Chlorella vulgaris in
• Progressive solvent an open raceway pond), absorption (monoethanolamine solvent),
degradation by SO2 in
flue gas
adsorption (activated carbon adsorbent), and membrane separation
• Amines-induced (polymeric membrane). Scrutinization of CO2 capture performance was
equipment corrosion done by assessing CO2 emission rates (direct, indirect, total, and net),
• Formation of harmful CO2 removal efficiencies (apparent and actual), and CO2 removal rate
amine compounds
per power input ratio. By considering indirect CO2 emission,
• High production cost
of activated carbon high-energy carbon capture technologies may escalate CO2 emission
• Saturation of active rather than CO2 reduction [15].
sites by moisture in C. vulgaris cultivation in an open raceway pond represents micro­
wet flue gas algae cultivation used in the aforesaid benchmarking. C. vulgaris is a
• Low CO2 adsorption
capacity and
common freshwater microalgae species, which able to efficiently
selectivity sequester CO2 from flue gas under photoautotrophic [16] or mixotrophic
• High-energy [17] cultivation modes. Open raceway pond is a low-energy cultivation
adsorbent system that was successfully commercialized for microalgae cultivation
regeneration
[18]. Microalgal CO2 biofixation is affected by the microalgae species,
• Membrane fouling by
flue gas contaminants cultivation systems, and growth conditions (i.e., temperature, pH,
• Precooling and turbidity, salinity, light intensity, trophic modes, and culture nutrients)
pressurization of flue [5]. Regrettably, most microalgal CO2 biofixation studies are incompa­
gas are required rable owing to diverse combinations of growth conditions. By changing
• Costly thermal
microalgae species or cultivation systems, a sensitivity analysis of
resistant ceramic
membranes microalgal CO2 capture was executed to predict any possible process
• Periodical cleaning amelioration. Painstaking assumptions were made to minimize un­
and replacement of certainties caused by inconsistent growth conditions. By dint of high
membranes
CO2 tolerance and efficient CO2 capture, six alternative microalgae
• Low process maturity
• Low flue gas feeding species were put forward to replace the C. vulgaris, namely freshwater
rate microalgae (Botryococcus braunii [19], Chlorella kessleri [20], Chlorella
• Preacclimation of pyrenoidosa [21], Scenedesmus obliquus [22], Spirulina sp. [23]) and
microalgae might be marine microalgae (Tetraselmis suecica [24]). Four common closed
required
photobioreactors (bubble column, airlift, flat panel, and tubular) [25,
• High contamination
risk in open 26] were proposed as alternative cultivation systems in lieu of the open
cultivation system raceway pond. A comparison of pros and cons between aforesaid
• Temperature microalgae cultivation systems was explicitly presented in Table 2.
fluctuation of outdoor
cultivation system
• Low process maturity 2. Methodology
2.1. System boundary, goals, and scope

aqueous ammonia, alkaline solvents, or imidazole-derived ionic liquids)
as absorbents to absorb CO2 (Lewis acid) in flue gas; however, solvent
regeneration by thermal stripping is energy-intensive to overcome large
enthalpy of vaporization [7]. Adsorption often employs porous and
moisture-insensitive solid adsorbents (i.e., activated carbon, zeolites,
and silica) to physically bind CO2 on their surface; furthermore, the
temperature swing adsorption (TSA) is favoured over pressure swing
adsorption (PSA) for effective CO2 desorption [8]. Membrane separation
sequesters CO2 from precooled flue gas using a CO2-permeable mem­
brane, but the membrane plugging issue and the need for pressurization
restrict its application [9]. Given photosynthetic CO2 biofixation,
microalgae cultivation garners enormous attention as it bridges CO2
mitigation and microalgae production [10]. In relative to the multicel­
lular terrestrial crops, the unicellular microalgae could harness solar
energy and sequester CO2 more efficiently [11] to accumulate various
biometabolites, viz. carbohydrates, proteins, lipids, and photosynthetic
pigments [5]. Further processing or upgrading of biochemical-laden
microalgae biomass generates versatile valuable bioproducts, which
include feeds, biofuels, biopolymers, nutraceuticals, and colouring
agents [5].
In the literature, most microalgal CO2 biofixation studies are often
standalone with a primary focus on biomass productivity, metabolite
Fig. 1(A) depicts the life cycle for reutilization of CO2 from fossil
fuels-based power plant operation, which involves fossil fuel extraction,
fossil fuel transportation, CO2 generation, CO2 separation, CO2 separa­
tion, CO2 transportation, and CO2 utilization. For coherence with cur­
rent study, the system boundary was confined to the CO2 separation,
where the comparative carbon balance analysis was implemented.
The first goal was to compare the CO2 capture performance of
microalgae cultivation (Chlorella vulgaris in an open raceway pond) with
other typical post-combustion CO2 capture technologies, namely ab­
sorption (monoethanolamine absorbent), adsorption (activated carbon
adsorbent), and membrane separation (polymeric membrane). For
simplicity, the CO2 capture processes were hereafter quoted without
specifying respective supporting items (which are the same unless
otherwise stated). The second goal was to evaluate any improvement of
microalgal CO2 capture by altering the (i) microalgae species (B. braunii,
C. kessleri, C. pyrenoidosa, S. obliquus, Spirulina sp., or T. suecica instead of
C. vulgaris) and (ii) cultivation systems [closed photobioreactors (bubble
column, airlift, flat panel, or tubular) in lieu of open raceway pond].
To achieve both goals, the identified scope was to scrutinize CO2
capture performance of the above-said post-combustion carbon capture
technologies, which was expressible in terms of CO2 emission rates
(direct, indirect, total, and net), CO2 removal efficiencies (apparent and

2
Y.W. Cheng et al. Journal of Environmental Chemical Engineering 9 (2021) 106519

Table 2
Volumetric power input, pros, and cons of common microalgae cultivation systems [25–28].
No. Microalgae cultivation systems Volumetric power input, Pros Cons
PV (W/m3)

1 Open raceway pond 13.97[25] • Low energy input • Low productivity of biomass and
• Simple paddle wheel operation for biometabolites
mixing • High contamination risk
• Moderate mixing and mass • Restricted to robust microalgae
transfer • Land-intensive with shallow
• Low capital cost and operational depth requirement
cost • Poor light path if great depth
• Small degree of wall growth
• Easy cleaning and maintenance
• Low hydrodynamic shear stress
• Less susceptible to
photoinactivation
• Large illumination area to volume
ratio
• Easy scale-up

2 Bubble column photobioreactor 40[25] • Moderate energy input
• Simple aeration for mixing
• Good mixing and mass transfer
• Small degree of wall growth
• Low hydrodynamic shear stress
• Less susceptible to
photoinactivation
• High productivity of biomass and
biometabolites
• Low contamination risk
• Not restricted to robust
microalgae
• Land-saving if compactly packed
• High capital cost and operational
cost
• Difficult cleaning and
maintenance
• Small illumination area to volume
ratio
• Scale-up needs multiple units
• Poor light path if large diameter

3 Airlift photobioreactor 8[26] • Low energy input and operational • High capital cost
cost • Difficult cleaning and
• Simple aeration and draft tube for maintenance
better mixing • Small illumination area to volume
• Excellent mixing and mass ratio
transfer • Scale-up needs multiple units
• Small degree of wall growth • Poor light path if large diameter
• Low hydrodynamic shear stress
• Less susceptible to
photoinactivation
• High productivity of biomass and
biometabolites
• Low contamination risk
• Not restricted to robust
microalgae
• Land-saving if compactly packed

4 53[25] • Moderate energy input • High degree of wall growth

• Simple aeration for mixing
(continued on next page)

3
 • Good mixing and mass transfer

Y.W. Cheng et al. Journal of Environmental Chemical Engineering 9 (2021) 106519

Table 2 (continued )
No. Microalgae cultivation systems Volumetric power input, Pros Cons
PV (W/m3)

Flat panel photobioreactor • Low hydrodynamic shear stress • Highly susceptible to

• High productivity of biomass and
biometabolites
• Low contamination risk
• Not restricted to robust
microalgae
• Land-saving if compactly packed
• Large illumination area to volume
ratio
• Good light path
photoinactivation
• High capital cost and operational
cost
• Difficult cleaning and
maintenance
• Difficult scale-up
• High risk of thermal denaturation

5 Tubular photobioreactor 2500[25] • Good mixing and mass transfer
• Large illumination area to volume
ratio
• High productivity of biomass and
biometabolites
• Low contamination risk
• Not restricted to robust
microalgae
• Land-saving if compactly packed
• Good light path
• High energy input
• Energy-intensive pump operation
for mixing
• High capital cost and operational
cost
• High degree of wall growth
• Difficult cleaning and
maintenance
• High hydrodynamic shear stress
• Highly susceptible to
photoinactivation
• Difficult scale-up

actual), and CO2 removal rate per power input ratio.
2.2. Carbon balance analysis of carbon capture systems
Since CO2 separation was the only focus in the present study, the
development of mass (for CO2 only) and energy balances should be
restricted to the boundary of CO2 capture systems. Fig. 1(B) provides the
carbon balance diagram of CO2 capture system. Total CO2 emission rate
(ṁCO2 ,total ; Eq. (1)) is the sum of direct (ṁCO2 ,di ) and indirect (ṁCO2 ,ind )
CO2 emission rates. Direct and indirect CO2 emission rates separately
indicate CO2 production rate from the fossil fuels-based power plant
operation and the carbon capture operation. The carbon emission factor
(CEF) is a useful indicator which informs the ratio of indirect CO2
emission rate (ṁCO2 ,ind ) to the power input (P). Thus, ṁCO2 ,ind (Eq. (2))
can be readily estimated from the multiplication of CEF with the re­
ported power input of carbon capture system in the literature. According
to Takahashi and Louhisuo [29], the average global CEF on 2020 was
circa 789.20 kg CO2/MWh.
ṁCO2 ,total = ṁCO2 ,di + ṁCO2 ,ind
ṁCO2 ,ind = P × CEF
where ṁCO2 ,total , ṁCO2 ,di , ṁCO2 ,ind = total, direct, indirect CO2 emission
rate, respectively (kg/h), P = power input (MW), and CEF = carbon
emission factor (kg/MWh).
Net CO2 emission rate (ṁCO2 ,net ) is the resultant CO2 emission rate
after CO2 separation, which indicates the CO2 discharge rate from CO2
capture system into the atmosphere. Through CO2 mass balance on CO2
capture system, the deduction of desirable CO2 removal rate (ṁCO2 ,r )
from ṁCO2 ,total enables the computation of ṁCO2 ,net (Eq. (3)). Herein, the
same ṁCO2 ,r was used as the mass basis to ensure a fair comparison be­
tween CO2 capture systems, and its value was deduced from the pro­
duction rate and composition of flue gas. A simulation study of Hussain
and Hagg [30] suggested the flue gas production rate (ṁflue gas ) of the
fossil fuels-based power plant to be 1000,000 kg/h. From Zhang et al.
[31]’s work, the unknown trace contents of NOx, SO2, and particulates in
flue gas were not reported; therefore, the volume compositions of flue
gas were adapted after reasonably normalizing their sum from 99.98 to
100 vol%. Thereafter, the volume compositions of flue gas were con­
verted into the weight compositions through mole relations by assuming
the ideal gas validity (molar volume = 22.4 L/m3). As shown in Table 3,
(1)
the flue gas carries 20.57 wt% CO2. By using Eq. (4), the desirable ṁCO2,r
(2) that calculated from ṁflue gas and weight composition of CO2 in flue gas
(xCO2 ) was 205,700 kg/h.

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Y.W. Cheng et al. Journal of Environmental Chemical Engineering 9 (2021) 106519

Fig. 1. (A) System boundary of current comparative carbon balance study and (B) Carbon balance diagram of CO2 capture system.

ṁCO2 ,net = ṁCO2 ,total - ṁCO2 ,r (3)

Table 3
Compositions of flue gas.
ṁCO2 ,r = (xCO2 /100)ṁflue gas (4)
Component Molar mass (g/mol) Composition

Volume (vol%) Weight (wt%) where ṁCO2 ,net = net CO2 emission rate (kg/h), ṁCO2 ,r = CO2 removal
rate (kg/h), xCO2 = weight composition of CO2 in flue gas (wt%), and
O2 32 3.65 3.98
CO2 44 13.73 20.57 ṁflue gas = flue gas production rate (kg/h).
H2O 18 9.73 5.96 In this work, two kinds of CO2 removal efficiencies, specifically
Ar 40 0.01 0.01 apparent (XCO2 ,ap ; Eq. (5)) and actual (XCO2 ,ac ; Eq. (6)) CO2 removal ef­
N2 28 72.88 69.48
ficiencies were used to narrate the extents of CO2 capture that achieved
by carbon capture system. The main difference between XCO2 ,ap and
XCO2 ,ac is the consideration of ṁCO2 ,ind , where XCO2 ,ap ignores ṁCO2 ,ind
while XCO2 ,ac considers ṁCO2 ,ind . Despite the prevalence of XCO2 ,ap in
literature, the XCO2 ,ac shows greater reliability in describing the extent of
CO2 capture because of its comprehensiveness. Meanwhile, the XCO2 ,ap

Fig. 2. Adapted process flow diagram of Zhang et al. [31]’s aqueous MEA-based CO2 absorption.

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Y.W. Cheng et al. Journal of Environmental Chemical Engineering 9 (2021) 106519

Table 4 particular absorption, adsorption, membrane separation, and micro­

Summary of Zhang et al. [31]’s simulation for aqueous MEA-based CO2 algae cultivation. Instead of direct adoption, the relevant data was
absorption. adapted to fit the current work along with some appropriate assump­
No. Parameters Value tions. From most published simulation works, the literature values of
[( ) ]
(A) Manipulated variables power input (Plit ) and CO2 removal rate ṁCO2,r lit was often traceable.
1 Inlet flue gas flow rate (kg/h) 2814,480
By assuming constant P/ṁCO2 ,r ratio (Eq. (7)), the power input of carbon
2 CO2 composition of flue gas (wt%) 20.57
3 Inlet CO2 flow rate (kg/h) 578,938 capture system could be estimated for the specified carbon removal rate
4 Apparent CO2 removal efficiency (%) 90 of 205,700 kg/h. Here, the CO2 removal rate per power input ratio
5 MEA concentration of lean MEA stream (wt%) 28 (ṁCO2 ,r /P) was also evaluated to ascertain the energy effectiveness of
6 Temperature of lean MEA stream (◦ C) 40
CO2 capture systems.
7 Pressure of lean MEA stream (bar) 1.113
8 CO2-to-MEA molar ratio of lean MEA stream (mol CO2/mol 0.27
( )
P P
MEA) = (7)
9 CO2-to-MEA molar ratio of rich MEA stream (mol CO2/mol MEA) 0.46
ṁCO2 ,r ṁCO2 ,r lit
10 Number of stages in CO2 absorber 10 ( )
11 Murphree efficiency of CO2 absorber 30 where Plit = literature power input (MW) and ṁCO2,r lit = literature
12 Number of stages in CO2 stripper 15 CO2 removal rate (kg/h).
(B) Responding variables
13 CO2 removal rate (kg/h) 521,044
14 Electrical power input of gas blower (MW) 8.20 2.3.1. Absorption
15 Electrical power input of MEA solvent pumps (MW) 10.00 For absorption, the highly efficient and low price monoethanolamine
16 Electrical power input of steam generation (MW) 130.91 (MEA) absorbent [5] was selected to sequester CO2 from the flue gas.
17 Electrical power input of CO2 compression (MW) 45.80
Evidently, Knudsen et al. [33]’s pilot-scale study on aqueous MEA
18 Thermal power input of reboiler heating (MW) 484.60
19 Thermal power input of condenser cooling (MW) 188.50 (30 wt%)-based absorption column could abate > 90% of CO2 from the
20 Thermal power input of lean liquid cooling (MW) 234.00 flue gas. Thus, Zhang et al. [31]’s simulation study on aqueous
21 Thermal power input of CO2 compressor cooling (MW) 78.30 MEA-based CO2 absorption was retrieved herein to ease comparison,
22 Total power input of CO2 absorption (MW) 1056.21 and the adapted process flow diagram was furnished as Fig. 2. Before
CO2 absorption, the flue gas underwent desulphurization, denitrifica­
tion, and water washing to get rid of competitive absorbate (SOx and
NOx) and to reduce its temperature. In the absorber, pretreated flue gas
and aqueous MEA flowed counter-currently, and their direct contact
favoured CO2 absorption. Thereafter, the MEA-lean treated gas and the
CO2-rich MEA solvent left the absorber through the top exit and the
bottom exit, respectively. The MEA-lean gas was washed with water for
MEA recovery while the CO2-rich MEA solvent was preheated to trigger
CO2 stripping in the stripper. Finally, the entrapped water in stripped
CO2 stream was condensed and recycled back into the stripper [31].
By inputting all the manipulated variables (Table 4), Zhang et al.
[31] ran the simulation of aqueous MEA-based CO2 absorption with
Aspen Plus® software to estimate the total power input. Since MEA is an
amine, amines property package was used as the thermodynamic model
to characterize CO2 absorption and stripping [31]. For stimulation of
multistage liquid-vapor equilibrium, simple RadFrac column was uti­
lized to model both absorber and stripper, but the latter was additionally
equipped with a CO2 condenser and a steam reboiler [31]. Considering
the low efficiency of absorber, Murphree efficiency was used to stimu­
Fig. 3. Process illustration of Zhao et al. [35]’s temperature swing activated
late non-ideal deviations from equilibrium CO2 separation [31]. The
carbon-based CO2 adsorption.
important responding variables in Table 4 are CO2 removal rate, elec­
trical power inputs (i.e., gas blower, MEA solvent pumps, steam gener­
definition allows the computation of ṁCO2 ,di from the desirable ṁCO2 ,r . ation, and CO2 compressor), and thermal power inputs (i.e., reboiler
ṁCO2 ,r heating, condenser cooling, lean liquid cooling, and CO2 compressor
XCO2 ,ap = × 100 % (5) cooling).
ṁCO2 ,di
In this study, the system boundary was confined to the CO2 separa­
ṁCO2 ,r tion, so the electrical power input of CO2 compression and the thermal
XCO2 ,ac = × 100 % (6)
ṁCO2 ,total power input of CO2 compressor cooling could be omitted when
computing the total power input of CO2 capture. From thermodynamic
where XCO2 ,ap and XCO2 ,ac = apparent and actual CO2 removal efficiency context, the conversion of electrical power to thermal power must be
(%), respectively. non-ideal with some power losses, and the ratio of output power (ther­
mal power) to input power (electrical power) is often known as the
electrical efficiency (η) [34]. Regrettably, Zhang et al. [31] did not
2.3. Power input estimation of carbon capture systems specify the η of each equipment in their simulation. By assuming η was
unity, the electrical and thermal power inputs were equivalent. Except
For carbon capture systems, the power input could be computed by the power inputs of CO2 compression, all the remaining power inputs
process simulation or even estimated by literature analysis [32]. Since were summed up to determine the total power input of CO2 absorption,
this study involves four major CO2 capture systems, the process simu­ viz. 1056.21 MW for a specified CO2 removal rate of 521,044 kg/h.
lation will be very tedious, especially on the establishment of various To achieve desired ṁCO2 ,r of 205,700 kg/h, the required power input
energy balances. For simplicity, the literature analysis was adopted to of CO2 absorption was estimated as 416.98 MW via Eq. (7). From the
estimate the power input of selected carbon capture systems, in

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Y.W. Cheng et al. Journal of Environmental Chemical Engineering 9 (2021) 106519

Table 5 va = vt exp[α(T-Tt )] = vt exp[(T-Tt )/T] (9)

Summary of Zhao et al. [35]’s simulation for temperature swing activated
carbon-based CO2 adsorption. ( )
Psat
No. Parameters Value
A = RTln (10)
Pe
(A) Manipulated variables
1 Limiting volumetric adsorbate uptake, q0 (m3/g) 1.09 × 10− 6
where q = amount of CO2 uptake (mg/g), q0 = limiting volumetric
2 Characteristic energy, E (J/mol) 4957.91 adsorbate uptake (m3/g), va = specific volume of adsorbed CO2 (m3/g),
3 Structural heterogeneity parameter, n 1.24 vt = specific volume of CO2 at triple point (m3/g), A = adsorption po­
4 Specific volume of CO2 at triple point, vt (m3/g) 0.8486 × 10− 6
tential (J/mol), E = characteristic energy (J/mol), n = structural het­
5 Temperature of CO2 at triple point, Tt (K) 216.6
erogeneity parameter, α = thermal expansion coefficient, 1/T (K− 1),
6 Adsorption temperature, TL (K) 293
T = adsorption temperature (K), Tt = temperature of CO2 at triple point
7 Desorption temperature, TH (K) 348
(K), Psat = saturation vapor pressure (Pa), Pe = equilibrium pressure of
8 Ambient temperature, T0 (K) 293 CO2 at adsorption temperature (Pa), and R = universal gas constant
9 Shaft work, WS (kJ/kg) 0 (8.314 J/mol⋅K).
10 Specific heat capacity of activated carbon, Cp,AC (kJ/kg⋅K) 0.825 ( ) ( ) ( )
(B) Responding variables T0 T0 T0
Win = WS + QH 1- - QL 1- = QH 1- (11)
11 Apparent CO2 removal efficiency (%) 81.86 TH TL TH
12 Work input of CO2 adsorption, Win (MJ/kg) 0.72
13 Heat input of CO2 desorption, QH (MJ/kg) 4.56 where Win = work input (kJ/kg), WS = shaft work (kJ/kg), QH = heat
14 Total specific energy input of CO2 adsorption, e (MJ/kg) 5.28 input of CO2 desorption (kJ/kg), QL = heat output of CO2 adsorption
(kJ/kg), T0 , TH , and TL = ambient, desorption, and adsorption temper­
atures, respectively.
90% XCO2 ,ap of CO2 absorption, the ṁCO2 ,di of absorption herein was
reckoned as 228,556 kg/h through Eq. (5). QSE + QLA
QH = (12)
q2 - q3
2.3.2. Adsorption ∫ ∫ ∫
Adsorption seizes CO2 from the flue gas through the surface binding
T3 T2 T3
QSE = Cp,AC dT + q2 Cp,a dT + qCp,a dT (13)
of solid adsorbents. Through desorption, the CO2-saturated adsorbents T1 T1 T2
are regenerable either by lowering pressure (pressure swing) or raising ∫
temperature (temperature swing) [8]. Despite its longer regeneration
q3
QLA = Had dq = Had,avg (q2 - q3 ) (14)
time, the temperature swing adsorption is preferred over the pressure q2
swing adsorption because of its better CO2 recovery [35]. Among
various adsorbents, activated carbon is highly favoured by dint of its where QSE = sensible heat of adsorbed CO2 (kJ/kg), QLA = latent heat of
high CO2 adsorption capacity [36] and renewable attribute (viable adsorbed CO2 (kJ/kg), T1 , T2 , and T3 = temperature (K) before pre-
synthesis from biomass wastes) [37]. For the comparison herein, Zhao heating, desorption, and pre-cooling, respectively, q, q2 , and q3
et al. [35]’s thermodynamic simulation on temperature swing activated = amount of CO2 uptake at a specific time, before adsorption, and after
carbon-based CO2 adsorption (Fig. 3) was retrieved. The inner tubes of desorption (mg/g), respectively, Cp,AC and Cp,a = specific heat capacity
adsorption column allowed the admission of cooling water or saturated of activated carbon and adsorbed CO2 (kJ/kg⋅K), separately, Had = heat
steam to realize pre-cooling or preheating operations, separately [35]. of adsorption (kJ/mol), and Had,avg = average Had (kJ/mol).
CO2 adsorption was operated in four-step cyclic operations, viz. (i) CO2 ( ( ) )1-n2n
adsorption at 20 ◦ C (with cooling to suppress its exothermicity), (ii) pre α2 (1-n) q0
Cp,a = Cp,f + ET ln ; [for T < Tc (304 K)] (15)
heating of CO2-saturated adsorber, (iii) CO2 desorption at 75 ◦ C under n2 qe va
N2 purging (with heating to counteract its endothermicity), and (iv) ( )( ( ) )1-n2n
pre-cooling of column to 20 ◦ C [35]. (1-n) E q0
Cp,a = Cp,g (T, Pe ) + ln -2R; [for T > Tc (304 K)]
Aside from inputting all the manipulated variables (Table 5), Zhao n2 T qe va
et al. [35] also made some assumptions to simplify their thermodynamic (16)
simulation, such as (i) uniform temperature of adsorber, (ii)
non-competitive adsorption, and (iii) identical equilibrium CO2 con­ where Cp,f and Cp,g = specific heat capacity of liquid CO2 and gaseous
centration between adsorber and adsorbents. The Dubinin-Astakhov CO2 (kJ/kg⋅K), singly.
(D-A) isotherm [Eq. (8) with the aid Eqs. (9)-(10)] was utilized to ⎡ ⎤
( ( ))1n ( ( ))1-n n
model the amount of CO2 uptake (q) as a function of temperature and ⎣ q0 αT q0 ⎦ + hfg ; [for T < Tc (304K)]
Had = E ln + ln
pressure [35]. Both liquid and gaseous properties of bulk CO2 were qe va n qe va
directly retrieved from the NIST Reference Fluid Thermodynamic and
(17)
Transport Properties Database (REFPROP 9.0). Without any shaft work
(WS = 0), the work input of CO2 adsorption (Win ) could be computed via ⎡ ⎤
Eq. (11) under the assumption of identical adsorption and ambient ⎢
( (
q0
) )1n
αT
( (
q0
) )1-n n
⎥
temperatures (T0 = TL ). For adsorbent regeneration, the required heat Had = E⎣ ln
qe va
+
n
ln
qe va
⎦ + 2RT; [for T
input of CO2 desorption (QH ; Eq. (12)) was the sum of sensible heat (QSE ;
Eq. (13)) and latent heat (QLA ; Eq. (14)). To estimate QSE and QLA , the > Tc (304 K)] (18)
heat of adsorption (Had) and specific heat capacity of adsorbed CO2 (Cp,
a) were calculated beforehand, in which their formulae depends on where qe = amount of CO2 uptake during equilibrium (mg/g) and hfg
subcritical [Eqs. (15) and (17)] or supercritical [Eqs. (16) and (18)] CO2 = heat of vaporization of CO2 (kJ/mol).
conditions. Zhao et al. [35]’s thermodynamic analysis revealed that the tem­
( ) ( )n perature swing activated carbon-based CO2 adsorption would require
q0 A
q = exp- (8) 0.72 MJ/kg Win and 4.56 MJ/kg QH to accomplish 81.86% XCO2 ,ap . By
va E
assuming the η was unity, the Win and QH were equivalent, whereby

7
Y.W. Cheng et al. Journal of Environmental Chemical Engineering 9 (2021) 106519

Fig. 4. Adapted process flow diagram of Zhang et al. [31]’s two-stage polymeric membrane CO2 separation.

membrane separation was incapable of attaining effective CO2 abate­

Table 6
Summary of Zhang et al. [31]’s simulation for two-stage polymeric membrane
CO2 separation.
No. Parameters
(A) Manipulated variables
1 Inlet flue gas flow rate (kg/h)
2 CO2 composition of flue gas (wt%)
3 Inlet CO2 flow rate (kg/h)
4 Apparent CO2 removal efficiency (%)
5 CO2 permeance [Nm3/(m2⋅bar⋅h)]
6 N2 permeance [Nm3/(m2⋅bar⋅h)]
7 O2 permeance [Nm3/(m2⋅bar⋅h)]
8 H2O permeance [Nm3/(m2⋅bar⋅h)]
ment from flue gas, but this downside can be resolved using the
two-stage membrane separation with the trade-off of its competitive
capital cost [31]. Both ceramic and polymeric membranes are highly
Value efficient (82–88% XCO2 ,ap ) membranes for CO2 separation [9], but the
polymeric membranes are relatively cheaper. Herein, Zhang et al. [31]’s
2814,480 simulation study on two-stage polymeric membrane CO2 separation was
20.57
retrieved, along with its adapted process flow diagram in Fig. 4. By
578,938
90 virtue of high flux and CO2 selectivity, the polyvinylamine/poly(phe­
1 nylene oxide) (PVAm/PPO) composite hollow fibre membranes were
0.005 used as the membrane module in both stages [31]. Zhang et al. [31]
0.02 adopted crossflow filtration mode for the membrane filtration, probably
2.25 × 10− 9

9 Vacuum pressure (bar) 0.2

because of its lower fouling propensity than dead end filtration mode
10 Pressure of second membrane (bar) 2 [38].
11 Total area of membrane module 1 (×106 m2) 15.3 Before membrane separation, the flue gas underwent desulphuriza­
12 Total area of membrane module 2 (×106 m2) 2 tion, denitrification, and water washing to alleviate potential fouling
13 CO2 fraction in permeate of membrane module 1 (mol%) 65
and thermal deterioration issues of polymeric membranes [31]. There­
(B) Responding variables
14 CO2 removal rate (kg/h) 521,044 after, the pretreated flue gas was pressurized by a compressor to induce
15 Electrical power input of compressor 1 (MW) 72.61 a large transmembrane pressure, which was conducive to the membrane
16 Electrical power input of vacuum pump 1 (MW) 33.94 separation. Inside the first membrane module, the PVAm/PPO mem­
17 Electrical power output of expander 1 (MW) 32.54 brane selectively allowed the permeation of CO2 while blocking other
18 Electrical power input of compressor 2 (MW) 12.46
19 Electrical power input of vacuum pump 2 (MW) 20.57
gases, thus forming CO2-lean gas and CO2-rich gas at the retentate side
20 Electrical power output of expander 2 (MW) 3.1 and permeate side, respectively [31]. At the retentate outlet, expander
21 Total power input of membrane separation (MW) 103.94 was installed to recover some electrical power from pressurized
CO2-lean gas through high pressure-driven shaft work. Meanwhile,
vacuum pump was connected to the permeate side to maximize the
their summation gave the total specific energy input (e) of CO2
transmembrane pressure [31]. Under aforesaid configurations, a second
adsorption, viz. 5.28 MJ/kg. Through Eq. (19), the power input can be
pair of compressor, membrane module, vacuum pump, and expander
estimated from the multiplication of total specific energy input with
were installed to further purify the CO2-rich gas for CO2 [31].
ṁCO2 ,r . Thus, CO2 adsorption needed a power input of 301.69 MW to
By inputting all the manipulated variables (Table 6), Zhang et al.
achieve the desirable ṁCO2 ,r of 205,700 kg/h. From the 81.86% XCO2 ,ap
[31] ran the simulation of two-stage polymeric membrane CO2 separa­
of CO2 adsorption, the ṁCO2 ,di of adsorption herein was predicted as 251, tion with the Aveva PRO/II® software, wherein the selected membrane
283 kg/h through Eq. (5). model was high flux asymmetric membrane in cross flow configuration.
( ) For membrane separation, the required power inputs of compressors and
1h
P = eṁCO2 ,r (19) vacuum pumps were partially fulfilled by the power outputs of ex­
3600 s
panders. As shown in Eq. (20), the subtraction of total power outputs
∑ ∑
where e = total specific energy input (MJ/kg). ( Pout ) from total power inputs ( Pin ) gave the power input of
membrane separation. From the work of Zhang et al. [31], it was un­
2.3.3. Membrane separation derstood that a power input of 103.94 MW was required to accomplish a
At low energy expenditure, membrane separation employs a CO2- ṁCO2 ,r of 521,044 kg/h.
permeable membrane to permit the passage of CO2 while restricting the ∑ ∑
P = Pin - Pout (20)
passage of other flue gas components. Further, membrane separation
offers environmentally benign CO2 capture at a low capital cost; how­
where Pin and Pout = power input and power output of individual
beit, low flux and fouling issue are its typical setbacks [9]. The one-stage
operation, respectively.

8
Y.W. Cheng et al.
As predicted by Eq. (7), the membrane separation would require a
power input of 41.03 MW to accomplish the specified ṁCO2,r of
205,700 kg/h. From the 90% XCO2 ,ap of membrane CO2 separation, the
ṁCO2 ,di of membrane separation was predicted as 228,556 kg/h via Eq.
(5).
2.3.4. Microalgae cultivation
Microalgal CO2 capture from flue gas was debuted on 1990s [39].
Unlike other post combustion CO2 capture processes, microalgal CO2
biofixation strongly relies on the wellness of living microalgae.
Considering the pollutant-laden attribute of flue gas (CO2, NOx, and
SO2), the potential inhibition of microalgae growth through acid toxicity
has raised some scepticism on the efficiency of microalgal CO2 capture
[40]. Nevertheless, the excellent phycoremediation of simulated [41,42]
and industrial [43,44] flue gases using microalgae was well documented
in literature. Out of these works, Moheimani [44]’s investigation on
industrial-scale microalgae cultivation using in-situ untreated flue gas
was ground-breaking as it affirmed high feasibility of microalgal CO2
capture from raw flue gas. To date, there are several strategies to bolster
the microalgal CO2 capture, which include long term acclimation [42],
utilization of automated pH controller system [41], and selection of
robust microalgae [44].
Despite conventional flue gas pretreatment seems unnecessary [44],
the flue gas herein was assumed to undergo sequential desulphurization,
denitrification, and water washing before being used for microalgae
cultivation. After pretreatment, the pretreated flue gas has moderate
CO2 concentration (13.73 vol%) and temperature (50 ◦ C) as well as
trace content of impurities (circa 32 ppm SO2 and 63 ppm NOx) [31],
which was more conducive to microalgae cultivation by ruling out acid
toxicity and thermal denaturation. With the sole focus on CO2 capture
system, the power input of pretreatment was disregarded for microalgae
cultivation, in analogous to the simulation work of Zhang et al. [31]’s
absorption, Zhao et al. [6]’s adsorption, and Zhang et al. [31]’s mem­
brane separation (Sections 2.3.1–2.3.3).
For the prevention of thermal denaturation, an extremely low
feeding rate of flue gas was assumed in lieu of further cooling of flue gas,
so multiple cultivation units were required to accommodate the huge
discharge rate of flue gas. At the expense of higher capital cost, this
approach not only avoided the remarkable temperature rise of the
cultivation medium, but also prolonged the residence time of CO2 in
cultivation system for better CO2 capture. Through the referral to most
microalgal CO2 capture research in Table S.1 (Supplementary Data), the
typical cultivation temperature range of 25 – 30 ◦ C and the conventional
photoautotrophic cultivation mode was adopted. In the comparative
carbon balance analysis, the representative microalgae cultivation was
microalgae (C. vulgaris) cultivation in open raceway pond, judging from
the prevalence of aforesaid microalgae species and the maturity of
selected cultivation system [18]. For stabilized CO2 capture ability, the
microalgae growth was assumed to be kept constant at the stationary
phase throughout the cultivation, such that the cell death offset the cell
growth. Constant volume process was assumed for the microalgae
cultivation, wherein the evaporative water loss was continuously
nullified by medium replenishment [11].
For microalgal CO2 capture, Klinthong et al. [45]’s review has
highlighted the critical urge to evaluate two important parameters,
specifically XCO2 ,ap and CO2 biofixation rate (RCO2 ). XCO2 ,ap indicates the
percentage of mass of CO2 removed relative to the mass of CO2 supplied,
and its presence ensures the relevance of microalgae cultivation with
other CO2 capture systems. For constant volume cultivation, Eq. (21)
shows that XCO2 ,ap can be reduced to the percentage of CO2 concentra­
tion difference between inlet and outlet streams relative to CO2 con­
centration of inlet stream. By knowing the XCO2 ,ap , the ṁCO2 ,di of
microalgae cultivation can be calculated from the pre-set ṁCO2 ,r via Eq.
(5). Meanwhile, RCO2 narrates the photosynthetic efficiency of micro­
algae in fixing the carbon of CO2 into the carbon of microalgae biomass.
9
Journal of Environmental Chemical Engineering 9 (2021) 106519
Through carbon balance (Eq. (22)), RCO2 was reckoned from the biomass
productivity (B) and the carbon mass fraction of microalgae biomass
(xC ). Through Eq. (23), the working volume (VW ) of cultivation system
was computed from the division of ṁCO2 ,di with RCO2 ; thereafter, its
multiplication with the volumetric power input (PV ) gave the power
input (P).
ṁCO2 ,in - ṁCO2 ,out CCO2 ,in - CCO2 ,out
XCO2 ,ap = × 100 % = × 100 %
ṁCO2 ,in CCO2 ,in
(21)
where ṁCO2 ,in and ṁCO2 ,out = inlet and outlet mass flow rates of CO2 (kg/
h), respectively, and CCO2 ,in and CCO2 ,out = inlet and outlet mass con­
centrations of CO2 (kg/m3), respectively.
RCO2 = xC × B ×
MWCO2
×
1d
= 0.153(xC × B) (22)
MWC 24 h
where RCO2 = CO2 biofixation rate (kg/(m3⋅h)), xC = carbon mass
fraction of dried microalgae biomass measured by the ultimate analysis
(wt%), B = biomass productivity (g/(L⋅d)), MWCO2 and MWC = molar
mass of CO2 (44 g/mol) and carbon (12 g/mol), respectively.
ṁCO2 ,di P
VW = = (23)
RCO2 PV
where VW = working volume (m3) and PV = volumetric power input
(W/m3).
Following an exhaustive literature survey, the cultivation conditions
and CO2 capture parameters of various microalgae species (C. vulgaris
and six alternatives) were summarized in Table S.1 (Supplementary
Data). Despite decades of research on microalgal CO2 biofixation, only a
finite number of articles considered the evaluation of XCO2 ,ap and RCO2
(usually either one); thus, such valuable data was in dearth. According
to the Table S.1, none of the cultivation conditions was similar or
comparable between different studies. Hence, the underlying effects of
various cultivation parameters, such as the reactor, medium, trophic
mode, temperature, pH, photoperiod, light intensity, and CO2 volume
concentration (VCO2 ), on the XCO2 ,ap and RCO2 of microalgae species
remain puzzled. While the modelling of growth kinetics is relatively
mature, it is a saddening fact that not a single universal equation able to
estimate the XCO2 ,ap and RCO2 in a sophisticated manner. Besides, the
incoherence of CO2 capture with the microalgae growth [46] compli­
cates the development of any meaningful regression models.
As reflected by Table S.1, most microalgal CO2 capture studies
strived to discover the effects of VCO2 on the XCO2 ,ap and RCO2 , with a
sporadic interest in the effects of light intensity. With the inexistence of
useful multivariate regression models for microalgal CO2 capture, both
XCO2 ,ap and RCO2 were simplified as a function of VCO2 by assuming the
trivial effects of other cultivation conditions. Here, the specified VCO2 of
flue gas was 13.73 vol% (cf. Table 3), but none of the XCO2 ,ap and RCO2
values in Table S.1 were assessed at the desired VCO2 . Henceforth, the
linear interpolation and extrapolation methods were used to estimate
the XCO2 ,ap and RCO2 values for 13.73 vol% VCO2 after extracting the
relevant data (in bold text) from the Table S.1. For more reliable data
estimation, some interpretations were furnished below as the guidance
for the selection of literature data from Table S.1.
For data estimation, interpolation was preferred over extrapolation
because its accuracy was relatively higher in securing a valid estimate
[47].
If data estimation was made across references, the selected studies
should have comparable light intensity to obviate its influence. When
multiple references were available, the outliers should not be considered
due to the intrinsic limitation of microalgal CO2 capture. Since the CO2
biofixation is genetically expressed, the CO2 capture ability of same
microalgae species should not be too deviated unless certain genetic
alterations are made.
Y.W. Cheng et al. Journal of Environmental Chemical Engineering 9 (2021) 106519

Table 7 (XCO2 ,ap and RCO2 ) of C. vulgaris and six alternatives were estimated for
Estimated CO2 capture parameters of selected microalgae species in this study. 13.73 vol% VCO2 and being summarized in Table 7. Microalgae
No. Microalgae VCO2 (vol RCO2 [kg/ XCO2 ,ap Ref.4 (C. vulgaris) cultivation in open raceway ponds could attain 40.64%
species %)1 (m3⋅h)]1,2,3 (%)1,2,3 XCO2 ,ap and 0.0378 kg/(m3⋅h) RCO2 . From the specified ṁCO2 ,r of
205,700 kg/h, the ṁCO2 ,di of microalgae cultivation was computed as
1 Chlorella vulgaris 2 0.0250 N/A [49]
13 0.0370 N/A [49] 506,152 kg/h through Eq. (5), which translatable into the required VW
5 N/A 44.29 [48] of 13,390,253 m3 after dividing ṁCO2 ,di with RCO2 via Eq. (23). Such
10 N/A 42.20 [48] huge VW of cultivation system validated the need for multiple parallel
13.73 0.0378a, c 40.64a, c Herein
units of raceway ponds to capture CO2 from flue gas, which indicated the
10 N/A 58.53 [50]
15 N/A 78.02 [50] high capital cost of microalgae cultivation. Considering an average PV of
13.73 0.0378a, d 73.07b, d Herein 13.97 W/m3 for open raceway pond (cf. Table 2), the microalgae
2 Botryococcus 10 0.0042 N/A [51] cultivation would require a power input of 187.06 MW to achieve a
braunii ṁCO2 ,r of 205,700 kg/h.
15 0.0030 N/A [51]
10 N/A 3.77 [19]
20 N/A 10.77 [19]
2.4. Sensitivity analysis of microalgal CO2 capture
13.73 0.0033b, c 6.38b, c Herein
3 Chlorella kessleri 6 0.0024 N/A [20]
10 0.0027 N/A [20] In Section 2.3.4, microalgae (C. vulgaris) cultivation in open raceway
5 N/A 44.29 [48] ponds was used as the representative microalgae cultivation for
10 N/A 42.20 [48]
benchmarking of its CO2 capture performance against other post-
13.73 0.0030a, c 14.57a, c Herein
4 Chlorella 10 0.0108 N/A [22]
combustion carbon capture technologies. Following the validation of
pyrenoidosa process feasibility (cf. Section 3.1), the sensitivity analysis of microalgal
20 0.0093 N/A [22] CO2 capture was conducted by replacing the original microalgae species
10 N/A 95.10 [21] (C. vulgaris) or cultivation system (open raceway ponds) to foresee any
15 N/A 95.90 [41]
possible amelioration. Similar computational algorithms in Section
13.73 0.0102b, c 95.70b, c Herein
5 Scenedesmus 10 0.0120 N/A [22] 2.3.4 were applied in this section.
obliquus Firstly, the performance of microalgal CO2 capture in the open
20 0.0103 N/A [22] raceway ponds using C. vulgaris and six alternatives were compared to
7 N/A 15 [52] reveal the most potent microalgae species for CO2 capture. The selection
20 N/A 14.23 [53]
13.73 0.0114b, c 14.60b, c Herein
of C. vulgaris [16], B. braunii [19], C. kessleri [20], C. pyrenoidosa [21],
6 Spirulina sp. 10 0.0187 N/A [54] S. obliquus [22], Spirulina sp. [23], and T. suecica [24] were based on
15 0.0166 N/A [54] their experimentally proven high CO2 tolerance and efficient CO2 cap­
6 N/A 9.23 [55] ture. Upon the alteration of microalgae species, the performance of
12 N/A 5.45 [55]
microalgal CO2 capture would be different in response to different
13.73 0.0171b, c 4.36a, c Herein
7 Tetraselmis 5 0.0046 N/A [24] intrinsic RCO2 and XCO2 ,ap of microalgae (cf. Table 7). Despite the prev­
suecica alence of open raceway pond, the RCO2 and XCO2 ,ap of various microalgae
15 0.0043 N/A [24] cultivations using raceway ponds were rarely reported. Due to this
11 N/A 37 [44]
constraint, the RCO2 and XCO2 ,ap of alternative microalgae species were
13.67 N/A 65 [56]
13.73 0.0043b, c 65.63a, c Herein assumed to be applicable for open raceway ponds. In Section 3.2.1,
C. vulgaris was identified as the most potent microalgae species for CO2
Remarks: N/A indicates not applicable or not available.
1 capture.
Abbreviations: CO2 volume concentration (VCO2 ) and CO2 biofixation rate
Secondly, the performance of microalgal (C. vulgaris) CO2 capture
(RCO2 ).
2
Estimation methods: extrapolation (a) and interpolation (b).
using open raceway pond and four common closed photobioreactors
3
Types of cultivation systems: open raceway pond (c) and closed photo­ (bubble column, airlift, flat panel, and tubular) were compared to the
bioreactors (d). best cultivation system for CO2 capture. Considering the scarcity of CO2
4
Reference (Ref.): the detailed cultivation conditions varied in different capture parameters, two assumptions were made to ease the analysis,
studies (cf. Table S.1). specifically (i) negligible influence of cultivation systems on RCO2 and
(ii) similar XCO2 ,ap for all closed photobioreactors. Hence, microalgal
The microalgae cultivation was conducted under photoautotrophic (C. vulgaris) CO2 capture using different closed photobioreactors shared
mode at the temperature of 25 – 30 ◦ C and the pH of 6 – 8. Due to the the same RCO2 (0.0378 kg/(m3⋅h)) and XCO2 ,ap (73.07%) for bioremedi­
scarcity of data, an exception was allowed for the mixotrophic cultiva­ ation of flue gas with 13.73 vol% CO2. Under aforesaid assumption, only
tion of C. pyrenoidosa in final effluent of wastewater treatment plant open raceway pond would have different XCO2 ,ap from all the closed
[21]. However, the usage of such low strength wastewater could photobioreactors. Here, the change of cultivation systems mainly
reasonably approximate its cultivation mode as photoautotrophy. affected the performance of microalgal CO2 capture through PV varia­
No strict specification on the cultivation medium, photoperiod, and tion (cf. Table 2).
light intensity because these parameters were easily adjusted to favour
the growth of desired microalgae. Adequate light intensity was assumed 3. Results and discussion
to avoid photoinhibition and poor microalgae growth.
Microalgal CO2 capture using open (raceway ponds) or closed 3.1. Comparison of post-combustion CO2 capture systems
(photobioreactors) systems should attain different XCO2 ,ap . Regrettably,
XCO2 ,ap of microalgae (C. vulgaris) cultivation in open raceway ponds According to British Petroleum Company PLC, the global primary
were not reported. For sensible prediction, the XCO2 ,ap of C. vulgaris energy consumption in 2019 was circa 583.9 EJ, which consisted of
cultivation was assumed to be identical with the XCO2 ,ap of Chlorella sp. 84.3% fossil energy, 11.4% renewable energy, and 4.3% nuclear energy
cultivation in open raceway pond [48]. [57]. This concise fact discloses the virtually inextricable relationship
Following aforesaid in-depth guidance, the CO2 capture parameters between electricity generation and fossil fuels combustion although the
continuous channelling of venture capitals and private equities into the

10
Y.W. Cheng et al.
Fig. 5. Performance of different CO2 capture systems: (a) CO2 emission rates
(direct, indirect, total, and net) and (b) CO2 removal efficiencies (apparent and
actual) and CO2 removal rate per power input ratio.
research and development of renewables [58]. Since fossil fuel com­
bustion was indispensable for electricity generation, the CO2 capture
from flue gas remained a great challenge in confronting global warming.
Here, four post-combustion carbon capture technologies, viz. absorp­
tion, adsorption, membrane separation, and microalgae cultivation were
subjected to a comparative carbon balance analysis. For a fair compar­
ison, the specified ṁCO2 ,r of 205,700 kg/h was used as the mass basis. For
an illustration of step-by-step computation, the results of comparative
carbon balance analysis for different post-combustion CO2 capture sys­
tems were summarized in Table A.1 (cf. appendices) sequentially.
Fig. 5 delineates the performance of different CO2 capture systems in
terms of the CO2 emission rates (direct, indirect, total, and net), CO2
removal efficiencies (apparent and actual), and CO2 removal rate per
power input ratio. As less efficient CO2 capture systems have poorer
apparent CO2 removal efficiency (XCO2 ,ap ), they must be operated under
relatively greater CO2 direct emission rate (ṁCO2 ,di ) than the efficient
one to attain the same CO2 removal rate (ṁCO2 ,r ). Based on the ṁCO2 ,di ,
the CO2 capture systems was ranked as membrane separation (229 ×103
kg/h) = absorption (229 ×103 kg/h) < adsorption (251 ×103 kg/h)
< microalgae cultivation (506 ×103 kg/h) following a contrariwise
XCO2 ,ap trend. In accordance with Leung et al. [9]’s review, the high
XCO2 ,ap of absorption (90%) [31], adsorption (81.86%) [35], and mem­
brane separation (90%) [31] was anticipated, which alluded to high
chemical reactivity between MEA with CO2, excellent CO2 binding af­
finity of highly porous activated carbon, and high CO2 selectivity of
PVAm/PPO composite membrane, respectively. From transport phe­
nomena perspective, most gas-liquid systems generally exhibit a better
mass transfer rate than the gas solid systems [59], so aqueous
MEA-based CO2 absorption outperformed activated carbon based CO2
adsorption with a higher XCO2 ,ap . Moreover, the relatively lower XCO2 ,ap
of CO2 adsorption plausibly hints at the existence of dead volume (un­
utilized region) in adsorption bed [35]. Compared to other
11
Journal of Environmental Chemical Engineering 9 (2021) 106519
Fig. 6. Performance of microalgal CO2 capture in open raceway ponds using
different microalgae species: (a) CO2 emission rates (direct, indirect, total, and
net) and (b) CO2 removal efficiencies (apparent and actual) and CO2 removal
rate per power input ratio.
post-combustion CO2 capture systems, microalgal (C. vulgaris) CO2
capture in open raceway pond achieved a remarkably lower XCO2 ,ap
(40.64%). Such inferiority of microalgal CO2 capture could be attributed
to (i) the engagement of fragile living microalgae, (ii) the presence of
microalgal cell wall (additional mass transfer barrier) that restrains CO2
diffusion [18], and (iii) the vulnerability of microalgae to acid toxicity
(H2CO3 formation) with surplus CO2 [60].
Here, the indirect CO2 emission rate (ṁCO2 ,ind ) quantifies the CO2
discharge rate of CO2 capture systems owing to the operational expen­
diture of electrical energy. As shown in Eq. (2), ṁCO2 ,ind is directly
proportional to the power input (P) of CO2 capture systems since the
carbon emission factor (CEF) is solely a constant value. With respect to
both ṁCO2 ,ind and P, the CO2 capture systems are ascendingly arranged,
viz. membrane separation (32 ×103 kg/h; 41.03 MW) < microalgae
cultivation (148 ×103 kg/h; 187.06 MW) < adsorption (238 ×103 kg/h;
301.69 MW) < absorption (329 ×103 kg/h; 416.98 MW). This result
was in line with the simulation work of Anselmi et al. [61], which
affirmed the energy consumption of polymeric membrane separation
< activated carbon-based adsorption < aqueous MEA-based absorption
in capturing CO2 from flue gas. Nevertheless, Zanco et al. [62]’s tech­
noeconomic study affirmed that both membrane separation and
adsorption were only cost competitive at the small scale operation and
poor CO2 recovery, and they recommended absorption as the most
cost-competitive CO2 capture system regardless of plant size and CO2
recovery rates.
In this work, membrane separation was the most energy-efficient
CO2 capture systems, considering its (i) zero heating approach and (ii)
partial fulfilment of total power input (due to compressors and vacuum
pumps) by expanders through high pressure-driven shaft work [31].
Y.W. Cheng et al. Journal of Environmental Chemical Engineering 9 (2021) 106519

Table A.1
Result summary of comparative carbon balance analysis for different post-
combustion CO2 capture systems.
Parameters CO2 capture systema

Absorption Adsorption Membrane Microalgae

separation cultivation
CO2 removal rate, 205,700 205,700 205,700 205,700
ṁCO2 ,r (kg/h)
Apparent CO2 90.00 81.86 90.00 40.64
removal
efficiency,
XCO2 ,ap (%)
Direct CO2 228,556 251,283 228,556 506,152
emission rate,
ṁCO2 ,di (kg/h)
CO2 biofixation N/A N/A N/A 0.0378
rate, RCO2 (kg/
m3⋅h)
Working volume, N/A N/A N/A 13,390,253
VW (m3)
Power input, P 416.98 301.69 41.03 187.06
(MW)
Indirect CO2 329,081 238,094 32,381 147,629
emission rate,
ṁCO2 ,ind (kg/h)
Total CO2 emission 557,636 489,376 260,936 653,781
rate, ṁCO2 ,total
(kg/h)
Net CO2 emission 351,936 283,676 55,236 448,081
rate, ṁCO2 ,net
(kg/h)
Actual CO2 36.89 42.03 78.83 31.46
removal
efficiency,
XCO2 ,ac (%)
CO2 removal rate 493.31 681.83 5013.40 1099.64
Fig. 7. Performance of microalgal (C. vulgaris) CO2 capture using different per power input
cultivation systems: (a) CO2 emission rates (direct, indirect, total, and net) and ratio, ṁCO2 ,r /P
(b) CO2 removal efficiencies (apparent and actual) and CO2 removal rate per (kg/h⋅MW)
power input ratio.
Remarks: N/A indicates not applicable or not available.
a
CO2 capture systems: aqueous MEA-based CO2 absorption (absorption),
According to Subramanian et al. [63]’s simulation, single stage mem­ temperature swing activated carbon-based CO2 adsorption (adsorption), two-
brane separation gave very poor electrical efficiency (34.90 – 46.20%), stage polymeric CO2 membrane separation, and microalgae (Chlorella vulgaris)
which opposed the favourable low power input of Zhang et al. [31]’s cultivation in open raceway pond (microalgae cultivation).
two-stage membrane separation that adopted herein. Henceforth,
two-stage membrane separation was surmised to be more superior over (2 groups) exhibits more amine groups than MEA (1 group), CO2 ab­
single stage membrane separation in capturing the CO2 from flue gas. As sorption using ethylenediamine requires a lower solvent amount than
the CO2 capture system with second-lowest energy input herein, the MEA to attain the similar XCO2 ,ap , thereby renders its lower heating
microalgae cultivation in open raceway ponds only expends the power and cooling requirements. The normal boiling point of ethylenediamine
to continuously rotate paddle wheel for medium recirculation, biomass (116 ◦ C) is lower than MEA (170 ◦ C); therefore, thermal stripping of
resuspension, and CO2 dispersion [32]. Considering the heating neces­ ethylenediamine is easier than MEA following its lower enthalpy of
sity of thermal-driven sorbent regenerations, it is unsurprised that both vaporization. It is surmised that the replacement of MEA with ethyl­
absorption [31] and adsorption [35] required high power input to enediamine in absorption can reduce ṁCO2 ,ind through a milder power
operate. For the sorbent regenerations, the stripping of CO2 from input, but the high price of ethylenediamine restrains its potential
aqueous MEA in absorption was surmised to be more energy-consuming application. As validated by Roussanaly et al. [67]’s technoeconomic
than the desorption of CO2 from activated carbon in adsorption. analysis, the methanol-based physical absorption has higher energy ef­
Aqueous MEA-based CO2 absorption is a chemical absorption process ficiency than the membrane separation at the cost of poor CO2 capture.
that necessitates the formation of stable carbamate [64]; hence, the Despite being energy-efficient, the physical absorption is impotent to
stripping requires high energy to break down strong chemical bonds. In outcompete the aqueous MEA-based chemical absorption in CO2
contrast, the activated carbon-based CO2 adsorption is merely a physical abatement. Based on Plaza et al. [68]’s study, the vacuum temperature
adsorption process that governed by weaker van der Waals forces and swing adsorption accomplished a higher XCO2 ,ap than the temperature
hydrogen bonds [65]; therefore, the CO2 desorption needs a lower en­ swing adsorption at a lower desorption temperature. Hence, the power
ergy input. Despite similar cyclic cooling-heating operations, the ab­ input of CO2 adsorption could be possibly reduced by integrating a
sorption expends additional energy for MEA recovery through pumping vacuum system to decrease the desorption pressure.
operation [31], different from the static activated carbon bed in the The ṁCO2 ,total represents total CO2 emission rate from power plant
adsorption [35]. operation (ṁCO2 ,di ) and carbon capture activity (ṁCO2 ,ind ). As ṁCO2,r and
For the same XCO2 ,ap of 90%, Rabensteiner et al. [66]’s pilot-scale CEF are constants, the ṁCO2 ,di is inversely proportional to XCO2 ,ap while
study proved that the CO2 absorption using aqueous ethylenediamine the ṁCO2 ,ind is directly proportional to P. Hence, high XCO2 ,ap and low P of
needed a lower power input than aqueous MEA. Since ethylenediamine carbon capture system are conducive to lessen the ṁCO2 ,total . Based on

12
Y.W. Cheng et al. Journal of Environmental Chemical Engineering 9 (2021) 106519

Table A.2
Result summary of comparative carbon balance analysis for microalgal CO2 capture in open raceway ponds using different microalgae species.
Parameters Microalgae species

Chlorella Botryococcus Chlorella Chlorella Scenedesmus Spirulina sp. Tetraselmis

vulgaris braunii kessleri pyrenoidosa obliquus suecica

CO2 removal rate, ṁCO2 ,r (kg/h) 205,700 205,700 205,700 205,700 205,700 205,700 205,700
Apparent CO2 removal efficiency, XCO2 ,ap 40.64 6.38 14.57 95.70 14.60 4.36 65.63
(%)
Direct CO2 emission rate, ṁCO2 ,di (kg/h) 506,152 3224,138 1411,805 214,943 1408,904 4717,890 313,424
CO2 biofixation rate, RCO2 (kg/m3⋅h) 0.0378 0.0033 0.0030 0.0102 0.0114 0.0171 0.0043
Working volume, VW (m3) 13,390,253 977,011,494 470,601,693 21,072,797 123,588,080 275,899,995 72,889,242
Power input, P (MW) 187.06 13,648.85 6574.31 294.39 1726.53 3854.32 1018.26
Indirect CO2 emission rate, ṁCO2 ,ind (kg/ 147,629 10,771,673 5188,442 232,330 1362,574 3041,832 803,613
h)
Total CO2 emission rate, ṁCO2 ,total (kg/h) 653,781 13,995,811 6600,247 447,273 2771,478 7759,722 1117,037
Net CO2 emission rate, ṁCO2 ,net (kg/h) 448,081 13,790,111 6394,547 241,573 2565,778 7554,022 911,337
Actual CO2 removal efficiency, XCO2 ,ac 31.46 1.47 3.12 45.99 7.42 2.65 18.41
(%)
CO2 removal rate per power input ratio, 1099.64 15.07 31.29 698.74 119.14 53.37 202.01
ṁCO2 ,r /P (kg/h⋅MW)

Remarks: N/A indicates not applicable or not available.

Table A.3
Result summary of comparative carbon balance analysis for microalgal (C. vulgaris) CO2 capture using different cultivation systems.
Parameters Microalgae cultivation system

Open raceway Bubble column Airlift Flat panel Tubular

pond photobioreactor photobioreactor photobioreactor photobioreactor

CO2 removal rate, ṁCO2 ,r (kg/h) 205,700 205,700 205,700 205,700 205,700
Apparent CO2 removal efficiency, XCO2 ,ap (%) 40.64 73.07 73.07 73.07 73.07
Direct CO2 emission rate, ṁCO2 ,di (kg/h) 506,152 281,511 281,511 281,511 281,511
CO2 biofixation rate, RCO2 (kg/m3⋅h) 0.0378 0.0378 0.0378 0.0378 0.0378
Working volume, VW (m3) 13,390,253 7447,378 7447,378 7447,378 7447,378
Power input, P (MW) 187.06 297.90 59.58 394.71 18,618.44
Indirect CO2 emission rate, ṁCO2 ,ind (kg/h) 147,629 235,099 47,020 311,506 14,693,676
Total CO2 emission rate, ṁCO2 ,total (kg/h) 653,781 516,610 328,531 593,017 14,975,187
Net CO2 emission rate, ṁCO2 ,net (kg/h) 448,081 310,910 122,831 387,317 14,769,487
Actual CO2 removal efficiency, XCO2 ,ac (%) 31.46 39.82 62.61 34.69 1.37
CO2 removal rate per power input ratio, 1099.64 690.51 3452.56 521.14 11.05
ṁCO2 ,r /P (kg/h⋅MW)

Remarks: N/A indicates not applicable or not available.

the ṁCO2 ,total , the carbon capture systems is sortable as membrane sep­
aration (261 ×103 kg/h; 87.6% ṁCO2 ,di + 12.4% ṁCO2 ,ind ) < adsorption
(489 ×103 kg/h; 51.3% ṁCO2 ,di + 48.7% ṁCO2 ,ind ) < absorption
(558 ×103 kg/h; 41% ṁCO2 ,di + 59% ṁCO2 ,ind ) < microalgae cultivation
(654 ×103 kg/h; 77.4% ṁCO2 ,di + 22.6% ṁCO2 ,ind ). By virtue of its
highest XCO2 ,ap (90%) and lowest P (41.03 MW), membrane separation
displays the lowest ṁCO2 ,total . Despite high XCO2 ,ap (81.86 – 90%), both
absorption and adsorption exhibit moderate ṁCO2 ,total following their
high P (301.69 – 416.98 MW). Likewise, the combination of poor XCO2 ,ap
(40.64%) and low P (149.08 MW) contribute to the moderate ṁCO2 ,total
of microalgae cultivation.
Apart from low ṁCO2 ,total , a promising carbon capture system should
have ṁCO2 ,di that far exceeds the ṁCO2 ,ind (ṁCO2 ,di >> ṁCO2 ,ind ); other­
wise, the power input is just squandered as the system hardly (ṁCO2 ,di ≈
ṁCO2 ,ind ) or even failed (ṁCO2 ,ind > ṁCO2 ,di ) to offset indirect CO2 emis­
sion from its operation. Based on aforesaid criteria, membrane separa­
tion and microalgae cultivation are the two delighted choices,
attributable to the reasonable ṁCO2 ,total and fulfilment of ṁCO2 ,di > >
ṁCO2 ,ind criterion. Environmentally benign carbon capture system must
fulfil the ṁCO2 ,net < ṁCO2 ,di criterion to ensure CO2 mitigation rather
than untoward CO2 intensification following outrageous power
requirement. Meanwhile, the ṁCO2 ,net > ṁCO2 ,di trend of sorption
processes imparted that the absorption and adsorption intensify CO2
emission from power plant operation with high power usage. Here,
membrane separation and microalgae cultivation with ṁCO2 ,net < ṁCO2 ,di
are deemed as the prospective carbon capture systems.
As expected, XCO2 ,ac that regards both ṁCO2 ,di and ṁCO2 ,ind are lower
than XCO2 ,ap that solely considers ṁCO2 ,di . Herein, the difference between
XCO2 ,ap and XCO2 ,ac (XCO2 ,ap - XCO2 ,ac ) serves as a magnitude indicator for
the negative impact of ṁCO2 ,ind on carbon capture systems. Considering
the (XCO2 ,ap - XCO2 ,ac ) values, absorption (53.11%) and adsorption
(39.83%) are overwhelmed by ṁCO2 ,ind whereas membrane separation
(11.17%) and microalgae cultivation (9.18%) are slightly affected by
ṁCO2 ,ind . Unlike other CO2 capture systems, the competitively high
ṁCO2 ,r /P ratio of the membrane separation (5013.40) and microalgae
cultivation (1099.64) distinguishes them as CO2 capture systems with
great energy efficiency.
In short, membrane separation is the most feasible CO2 capture
system by virtue of its (i) excellent CO2 abatement (highest XCO2 ,ap and
XCO2 ,ac respectively grants the lowest ṁCO2 ,di and ṁCO2 ,total ), (ii) mini­
mum energy necessity (lowest P and ṁCO2 ,ind ), (iii) exceptional energy
efficiency (highest ṁCO2 ,r /P ratio), and (iv) eco-friendly attribute
(lowest ṁCO2 ,net ). Despite its inferiority to membrane separation,
microalgae cultivation emerges as an alternative promising CO2 capture

13
Y.W. Cheng et al.
system that is worthy of further study since it outcompetes both sorption
processes.
3.2. Sensitivity analysis of microalgal CO2 capture
In Section 3.1, microalgal (Chlorella vulgaris) CO2 capture using open
raceway ponds was acknowledged as a feasible CO2 capture system that
is just inferior to membrane separation. To foresee any betterment plans,
the sensitivity analysis of microalgal CO2 capture was studied by tuning
(i) microalgae species (varying XCO2 ,ap and RCO2 ) or (ii) cultivation sys­
tem (varying XCO2 ,ap and PV ). Due to the scarcity of CO2 capture pa­
rameters (RCO2 and XCO2 ,ap ), the authors would like to emphasize that the
influences of extrinsic growth conditions (i.e., medium type, pH, tem­
perature, photoperiod, and light intensity) on CO2 abatement were
neglected herein.
3.2.1. Microalgal CO2 capture in open raceway ponds using different
microalgae species
Fig. 6 portrays the performance of microalgal CO2 capture in open
raceway ponds using seven selected microalgae species, namely
C. vulgaris, B. braunii, C. kessleri, C. pyrenoidosa, S. obliquus, Spirulina sp.,
and T. suecica. Table A.2 (cf. appendices) presents the CO2 emission rates
(direct, indirect, total, and net), CO2 removal efficiencies (apparent and
actual), and CO2 removal rate per power input ratio for each case. As
shown in Table 7, each microalgae species has dissimilar XCO2 ,ap and
RCO2 . As revealed by Eq. (24), both XCO2 ,ap and RCO2 are inversely pro­
portional to the VW and P. Therefore, high XCO2 ,ap and RCO2 are imper­
ative to reduce both working volume and power input of microalgae
cultivation.
ṁCO2 ,di ṁCO2 ,r P ṁCO2 ,ind
VW = = = = (24)
RCO2 XCO2 ,ap × RCO2 PV CEF × PV
For microalgal CO2 capture systems, both CO2 dissolution into me­
dium and microalgal CO2 biofixation contribute to the overall XCO2 ,ap
[21], and their individual contribution is vague with ever-changing
medium contents (secretion of extracellular metabolites by micro­
algae) and the absence of control medium (without microalgae). As only
CO2 abatement is concerned here, it is acceptable to utilize XCO2 ,ap for
microalgal CO2 capture systems because CO2 dissolution always pre­
cedes CO2 biofixation. To attain similar ṁCO2 ,r , the microalgal CO2
capture systems need to operate under high ṁCO2 ,di to compensate their
low XCO2 ,ap , but this inefficiency could render more CO2 being dis­
charged to the atmosphere. Since the CO2 capture is the utmost goal,
microalgal CO2 capture systems with low XCO2 ,ap and high ṁCO2 ,di must
be eliminated; thence, the impotent microalgae species are B. braunii
(6.38%; 332 ×104 kg/h), C. kessleri (14.57%; 141 ×104 kg/h),
S. obliquus (14.60%; 141 ×104 kg/h), and Spirulina sp. (4.36%;
472 ×104 kg/h). Because of similar XCO2 ,ap , microalgal CO2 capture
using T. suecica (65.63%; 31 ×104 kg/h) possesses comparable ṁCO2 ,di
with that of C. vulgaris (40.64%; 51 ×104 kg/h). Considering its highest
XCO2 ,ap (95.70%), microalgal CO2 capture using C. pyrenoidosa has a
lowest ṁCO2 ,di (21 ×104 kg/h).
Table A.2 clearly evinces that no specific relationships between
XCO2 ,ap and RCO2 . By reason of poor mass transfer across microalgae cell
wall, high XCO2 ,ap does not guarantee great RCO2 as CO2 abatement also
occurs through CO2 dissolution into medium [21]. Upon sparging of
CO2, the dissolved CO2 (CO2 + H2O) may become various inorganic
carbon species (H2CO3, HCO3-, and CO32-), and the chemical equilibria
of the species depends on the pH (cf. Eq. (25)) [60]. Since the optimal pH
range of most microalgae cultivation is 7 – 8.4, the dissolved CO2 mostly
exists as the bicarbonate (HCO3-) [5]. Further, the widely used Morais
and Costa [69]’s RCO2 equation (Eq. (22)) underrates actual RCO2 by
assuming CO2 biofixation only metabolizes CO2 as intracellular organic
carbon (primarily carbohydrates, proteins, and lipids) [49]. Upon hy­
drodynamic shear force, microalgae also fix the CO2 into secretable
14
Journal of Environmental Chemical Engineering 9 (2021) 106519
organic carbon, such as exopolymers [60] and volatile organic com­
pounds (VOC) [70], which constitute the dissolved organic carbon in the
medium [21]. Through a carbon balance, Deprá et al. [71] discovered
that microalgal (S. obliquus) CO2 capture turned CO2 into 88.89% VOC,
1.42% biomass, 0.19% bicarbonate, 0.07% exopolymers, and 9.43%
unidentified carbon compounds.
CO2 + H2 O ↔ H2 CO3 ↔ HCO-3 + H+ ↔ CO23-
+ 2H+
(25)
Despite underestimation, the wide acceptance of Morais and Costa
[69]’s RCO2 renders its suitability herein as a comparative parameter. As
shown in Eq. (24), both XCO2 ,ap and RCO2 are inversely proportional to the
P and ṁCO2 ,ind , so high XCO2 ,ap and RCO2 are vital to suppress ṁCO2 ,ind .
Microalgal CO2 capture using C. vulgaris (40.64%; 0.0378 kg/m3⋅h),
C. pyrenoidosa (95.70%; 0.0102 kg/m3⋅h), or T. suecica (65.63%;
0.0043 kg/m3⋅h) exhibits low ṁCO2 ,ind through the pairing of high RCO2
and moderate XCO2 ,ap or vice versa. In contrast, microalgal CO2 capture
using S. obliquus (14.60%; 0.0114 kg/m3⋅h) or Spirulina sp. (4.36%;
0.0171 kg/m3⋅h) has relatively greater ṁCO2 ,ind with the pairing of
moderate RCO2 and poor XCO2 ,ap . Following poor RCO2 and XCO2 ,ap ,
microalgal CO2 capture using B. braunii (6.38%; 0.0033 kg/m3⋅h) or
C. kessleri (14.57%; 0.0030 kg/m3⋅h) possess remarkably high ṁCO2 ,ind ,
which informs their incapableness as a CO2 capture system.
Based on the ṁCO2 ,total , microalgal CO2 capture in open raceway pond
using different microalgae species could be ranked as C. pyrenoidosa
(45 ×104 kg/h; 48.1% ṁCO2 ,di + 51.9% ṁCO2 ,ind ) < C. vulgaris (60 ×104
kg/h; 77.4% ṁCO2 ,di + 22.6% ṁCO2 ,ind ) < T. suecica (112 ×104 kg/h;
28.1% ṁCO2 ,di + 71.9% ṁCO2 ,ind ) < S. obliquus (277 ×104 kg/h; 50.8%
ṁCO2 ,di + 49.2% ṁCO2 ,ind ) < C. kessleri (660 ×104 kg/h; 21.4% ṁCO2 ,di +
78.6% ṁCO2 ,ind ) < Spirulina sp. (776 ×104 kg/h; 60.8% ṁCO2 ,di + 39.2%
ṁCO2 ,ind ) < B. braunii (1400 ×104 kg/h; 23.0% ṁCO2 ,di + 77.0%
ṁCO2 ,ind ). Among aforesaid microalgae species, only the cultivation of
C. vulgaris in open raceway ponds able to fulfil five basic criteria of good
CO2 capture systems, which entails low ṁCO2 ,total , ṁCO2 ,di > > ṁCO2 ,ind
(effective CO2 abatement), ṁCO2 ,net < ṁCO2 ,di (verified CO2 abatement),
XCO2 ,ac ≈ XCO2 ,ap (negligible power input), and high ṁCO2 ,r /P ratio (great
energy efficiency).
3.2.2. Microalgal (C. vulgaris) CO2 capture using different cultivation
systems
In Section 3.2.1, C. vulgaris is identified as the most potent species for
microalgal CO2 capture in open raceway ponds through the comparative
carbon balance analysis. On top of the open raceway ponds, the per­
formance of microalgal (C. vulgaris) CO2 capture in various closed
photobioreactors (i.e., bubble column, airlift, flat panel, or tubular)
were further examined here to evaluate the prospect of microalgae
cultivation as alternative CO2 capture system. Table A.3 (cf. appendices)
summarizes CO2 emission rates (direct, indirect, total, and net), CO2
removal efficiencies (apparent and actual), and CO2 removal rate per
power input ratio for all the cases. Fig. 7 depicts the performance of
microalgal (C. vulgaris) CO2 capture in different cultivation systems. By
assuming RCO2 invariancy for C. vulgaris, each cultivation system has
different XCO2 ,ap (cf. Table 7) and PV (cf. Table 2). Through Eq. (24), P is
directly proportional to PV but inversely proportional to XCO2 ,ap .
For microalgal (C. vulgaris) CO2 capture, the respective XCO2 ,ap of
open system (open raceway pond) and closed systems (closed photo­
bioreactors – bubble column, airlift, flat panel, or tubular) are 40.64%
and 73.07%. Since open raceway ponds is open system, poor light path
[27], short CO2 retention time, inconsistent microalgae growth, and
high cross contamination risk [45,72] are numerous possible reasons for
its low XCO2 ,ap . Due to poor light path [27], the photosynthetic oxygen
production of microalgae is inadequate to suppress the possible growth
of facultative anaerobes. In terms of CO2 uptake rate, CO2 acetogenesis
Y.W. Cheng et al.
of acetogens (reductive pathway) will be slower than CO2 fixation of
microalgae (light-driven reductive pathway) [73]. As closed systems,
the closed photobioreactors (PBR) provide long CO2 retention time,
better light path, low contamination risk, and high microalgae biomass
productivity [18], thus achieve a higher XCO2 ,ap . For the same ṁCO2 ,r ,
microalgal (C. vulgaris) CO2 capture in open raceway ponds must be
operated under higher ṁCO2 ,di than the closed photobioreactors to
counteract its relatively lower XCO2 ,ap .
As indicated in Eqs. (2) and (24), ṁCO2 ,ind is directly proportional to
PV but inversely proportional to XCO2 ,ap ; therefore, high XCO2 ,ap and low
PV are necessary to minimize ṁCO2 ,ind . For microalgal (C. vulgaris) CO2
capture, the ṁCO2 ,ind of different cultivation systems is ranked as airlift
PBR (5 ×104 kg/h) < open raceway pond (15 ×104 kg/h) < bubble
column PBR (24 ×104 kg/h) < flat panel PBR (31 ×104 kg/h) < tubular
PBR (1469 ×104 kg/h). Relative to open raceway pond with moderate
XCO2 ,ap (40.64%) and low PV (13.97 W/m3), airlift PBR with high XCO2 ,ap
(73.07%) and low PV (8 W/m3) exhibits a lower ṁCO2 ,ind , which ascribed
to its energy-efficient medium circulation via the integration of sparger
and draft tube [74]. By sparging gas upwards through the riser, airlift
PBR creates a huge density difference between degassed liquid (upper
region) and gassed liquid (lower region) to stimulate downward liquid
circulation through the downcomer [74]. Since same XCO2 ,ap is assumed
for closed systems, the ṁCO2 ,ind of microalgal (C. vulgaris) CO2 capture in
PBR simply increased with PV . With similar aeration requirement, flat
panel PBR (53 W/m3) exhibits a higher PV than bubble column PBR
(40 W/m3) because it needs extra power to operate water cooling system
[75]. Thin width of flat panel PBR enhances the light capture of
microalgae, but the cooling system is vital to obviate thermal denatur­
ation of microalgae upon excess photoabsorption. The tubular PBR
(2500 W/m3) resembles a huge system of multiple parallel tubes, and
high-power pumping operation is needed to maintain the flow of me­
dium [25].
For microalgal (C. vulgaris) CO2 capture, the ṁCO2 ,total of different
cultivation systems is ascendingly sorted as airlift PBR (33 ×104 kg/h;
85.7% ṁCO2 ,di + 14.3% ṁCO2 ,ind ) < bubble column PBR (52 ×104 kg/h;
54.5% ṁCO2 ,di + 45.5% ṁCO2 ,ind ) < flat panel PBR (59 ×104 kg/h; 47.5%
ṁCO2 ,di + 52.5% ṁCO2 ,ind ) < open raceway pond (65 ×104 kg/h; 77.4%
ṁCO2 ,di + 22.6% ṁCO2 ,ind ) < tubular PBR (1498 ×104 kg/h; 1.9% ṁCO2 ,di
+ 98.1% ṁCO2 ,ind ). Here, comparative carbon balance analysis put for­
ward open raceway pond and airlift PBR as the two promising cultiva­
tion systems for microalgal (C. vulgaris) CO2 capture since they fulfil all
the five criteria of good CO2 capture system, viz. low ṁCO2 ,total , ṁCO2 ,di
> > ṁCO2 ,ind , ṁCO2 ,net < ṁCO2 ,di , XCO2 ,ac ≈ XCO2 ,ap , and high ṁCO2 ,r /P
ratio. For microalgal (C. vulgaris) CO2 capture, the bubble column, flat
panel, or tubular PBR are deemed as impractical cultivation systems as
they intensify CO2 emission of power plant operation (ṁCO2 ,net >
ṁCO2 ,di ). Indeed, the performance of microalgal CO2 capture varies with
cultivation systems.
Based on screening criteria for effective CO2 capture systems,
microalgal (C. vulgaris) CO2 capture in airlift PBR is more feasible than
that in open raceway pond since it is relatively cleaner (lower ṁCO2 ,total ),
effective (lower ṁCO2 ,ind fraction), proven (larger difference between
ṁCO2 ,di and ṁCO2 ,net ), low power (smaller difference between XCO2 ,ac and
XCO2 ,ap ), and energy efficient (higher ṁCO2 ,r /P ratio). As shown in
Table A.3 (appendices), microalgal (C. vulgaris) CO2 capture in airlift
PBR (7447,378 m3) requires a smaller total working volume (VW ) than
the open raceway pond (13,390,253 m3), and their outrageously huge
VW informs the necessity of multiple parallel units. Airlift PBR has a
poorer scalability than the open raceway pond, but it is more land-
saving than the shallow cum large ponds by dint of its possible tall
height and compactly packed configuration [27]. To confront
land-intensive issue, multistorey frame can be constructed to situate
numerous open raceway ponds at the cost of limited light penetration
and higher capital cost. With a relatively complex design, airlift PBR
requires a higher capital cost than open raceway ponds, but its
15
Journal of Environmental Chemical Engineering 9 (2021) 106519
operational cost is lower. In view of lower contamination risk, micro­
algal CO2 capture using airlift PBR is more economically attractive
because it grants microalgae biomass production with higher produc­
tivity and better quality. Indeed, C. vulgaris could be a promising feed­
stock for the synthesis of biofuels and biochemicals, like biodiesel,
pharmaceuticals, nutraceuticals, and cosmetics [76]. At this point, the
microalgal CO2 capture possibly still far deviates from the industrial
expectation. Herein, comparative carbon balance analysis shows that
microalgal CO2 capture is technically fit. In near future, a tech­
noeconomic analysis should be meticulously performed to evaluate the
economic feasibility of large-scale microalgal CO2 capture from flue gas.
4. Conclusion
Comparative carbon balance analysis was executed to assess the
performance of post combustion CO2 capture systems in terms of CO2
emission rates (direct, indirect, total, and net), CO2 removal efficiencies
(apparent and actual), and CO2 removal rate per power input ratio.
Microalgal (C. vulgaris) CO2 capture in open raceway pond was bench­
marked against common technologies, namely aqueous MEA-based ab­
sorption, activated carbon-based adsorption, and polymeric membrane
separation. Herein, the five screening criteria of potential carbon cap­
ture system were outlined, viz. low ṁCO2 ,total , ṁCO2 ,di > > ṁCO2 ,ind
(effective abatement), ṁCO2 ,net < ṁCO2 ,di (proven abatement), XCO2 ,ac
≈ XCO2 ,ap (inconsiderable power input), and high ṁCO2 ,r /P ratio (high
energy efficiency). Based on aforesaid screening criteria, only mem­
brane separation and microalgae cultivation were deemed as the
promising CO2 capture systems, but microalgal CO2 capture was inferior
to membrane separation. To predict any improvements, the sensitivity
analysis of microalgal CO2 capture was scrutinized by changing the
original microalgae species (C. vulgaris) or cultivation system (open
raceway pond). For microalgal CO2 capture using the open raceway
pond, the only competent species C. vulgaris outperformed six alterna­
tives (B. braunii, C. kessleri, C. pyrenoidosa, S. obliquus, Spirulina sp., or
T. suecica). For microalgal (C. vulgaris) CO2 capture, both open raceway
pond and airlift photobioreactor were technically feasible cultivation
systems, while other closed photobioreactors (bubble column, flat panel,
or tubular) were impotent. From the viewpoint of CO2 capture and
microalgae biomass production, microalgal (C. vulgaris) CO2 capture in
airlift photobioreactor outmatched open raceway ponds. In view of large
working volume, the low scalability of microalgae cultivation could
potentially hamper the industrial application of microalgal CO2 capture
from flue gas. A technoeconomic analysis of microalgal CO2 capture
should be meticulously conducted in near future to inspect its economic
feasibility.
CRediT authorship contribution statement
Yoke Wang Cheng – Conceptualization, Methodology, Investiga­
tion, Writing – original draft, Writing – review & editing. Jeremy Sheng
Ming Lim – Conceptualization, Methodology, Investigation, Writing –
original draft, Resources. Chi Cheng Chong – Validation, Investigation,
Visualization, Writing – review & editing. Man Kee Lam – Resources,
Supervision, Investigation, Writing – review & editing, Funding acqui­
sition. Jun Wei Lim – Resources, Visualization, Supervision. Inn Shi
Tan – Resources, Visualization. Henry Chee Yew Foo – Resources,
Visualization. Pau Loke Show – Resources, Visualization. Steven Lim –
Resources, Visualization.
Declaration of Competing Interest
The authors declare that they have no known competing financial
interests or personal relationships that could have appeared to influence
the work reported in this paper.
Y.W. Cheng et al. Journal of Environmental Chemical Engineering 9 (2021) 106519

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