Journal of Environmental Management 255 (2020) 109870

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Journal of Environmental Management

journal homepage: http://www.elsevier.com/locate/jenvman

Research article

An engineering-environmental-economic-energy assessment for integrated

air pollutants reduction, CO2 capture and utilization exemplified by the
high-gravity process
Tse-Lun Chen a, b, Si-Lu Pei b, Shu-Yuan Pan c, Chia-Yii Yu d, Chen-Lu Chang d,
Pen-Chi Chiang a, b, *
a
Graduate Institute of Environmental Engineering, National Taiwan University, 1, Sec. 4, Roosevelt Road, Da-an District, Taipei City, 10617, Taiwan
b
Carbon Cycle Research Center, National Taiwan University, 71 Fan-Lan Road, Da-an District, Taipei City, 10672, Taiwan
c
Department of Bioenvironmental Systems Engineering, National Taiwan University, 1, Sec. 4, Roosevelt Road, Da-an District, Taipei City, 10617, Taiwan
d
Safety, Health & Environment Center, Group Administration, Formosa Plastics Group, No. 201, Dunhua N. Rd., Songshan Dist., Taipei City, 10508, Taiwan

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

Keywords: In this study, a high-gravity (HiGee) process incorporating CO2 and NOx reduction from flue gas in a petro­
High-gravity process chemical plant coupled with petroleum coke fly ash (PCFA) treatment was established. The performance of
Engineering performance HiGee was systematically evaluated from the engineering, environmental, economic, and energy aspects (a total
Environmental impacts
of 15 key performance indicators) to establish the air pollution, energy efficiency, waste utilization nexus. The
Cost benefit analysis
Retrofit heat recovery
engineering performance was evaluated that lower energy consumption of 78 kWh/t-CO2 can be achieved at a
Comprehensive performance evaluation capture capacity of 600 kg CO2/t-PCFA. A net emission reduction of 327.3 kg-CO2/t-PCFA could be determined
based on six environmental impact indicators. A cost-benefit analysis was conducted using operating cost,
product sale, carbon credit, and savings in air pollution fees to present a better technological selection compared
to existing carbon capture and storage plants. The waste heat recovery from the flue gas via the HiGee process
could be measured via moisture condensation and attendant elimination of white smog emissions. Retrofitted
heat recovery and energy intensity up to 131.8 kJ/t-PCFA and 0.21 kWh/t-PCFA were assessed. Finally, a
comprehensive analysis of the HiGee process based on three daily load scenarios of CO2 capture scale were
conducted, suggesting an optimal operating condition of the HiGee for generating profitability.

1. Introduction domestic standards is crucial. To increase reaction efficiency, a

Air pollution control in the energy sector, such as coal-fired power
plants, is a major public concern. Energy production and consumption
involve mostly anthropogenic sources of air pollution emissions, where
particulate matter (PM), sulfur oxides (SOx), and nitrogen oxides (NOx)
account for 85% of total emissions. The International Energy Agency has
pointed out that poverty, fossil fuel-intensive development, and urban­
ization are the three impacts of air pollution affecting human health and
climate change (IEA, 2016b). Based on spatio–temporal analysis of air
pollutant distribution, an optimal integration of high energy efficiency
and control technology should be implemented to maximize PM
reduction and mitigate climate change (Wang et al., 2017). A cost
effective technological strategy bridging monitoring enforcement and
performance evaluation to improve air quality per international and
high-gravity (HiGee) process, based on high-gravity technology, was
first developed by our group in 2017 (Pei et al., 2018b). In the HiGee
process, NOx can be oxidized with the aid of oxidants, such as KMnO4,
H2O2, CO(NH2)2, and ozone (O3) (Sun et al., 2017). The reaction
mechanism of NOx oxidation is shown by Eqs. (1)–(4), where both NO
and NO2 can be converted to the higher valence species (i.e., N2O5 and
HNO3) that exhibit a higher water solubility. NO and NOx could be
oxidized by O3 through a gas-phase reaction rather than a gas liquid
reaction. The gas-gas reaction has high selectivity, oxidation efficiency,
and reaction rate of NO ozonation could be k ¼ 8.43 � 109 �
e( 2600/RT)], without addition of catalysts (Skalska et al., 2011).
NO þ O3 →NO2 þ O2 (1)

* Corresponding author. 1, Sec. 4, Roosevelt Road, Taipei City, Taiwan 10617, Taiwan.
E-mail address: pcchiang@ntu.edu.tw (P.-C. Chiang).

https://doi.org/10.1016/j.jenvman.2019.109870
Received 4 July 2019; Received in revised form 18 October 2019; Accepted 12 November 2019
0301-4797/© 2019 Published by Elsevier Ltd.
T.-L. Chen et al.
NO2 þ O3 →NO3 þ O2 (2)
NO2 þ NO3 →N2 O5 (3)
H2 O þ N2 O5 →2HNO3 (4)
The removal mechanisms of PM in the HiGee process may include
diffusion, interception and inertial impaction. The structure of rotating
packed bed (RPB) is consisted of packing zone and cavity zone. As liquid
agent was jetted by nozzle into packing zone, the thin liquid-films and
tiny droplets can be generated in the packing zone then spreading into
the cavity zone (Pan et al., 2017). The relationship between droplet
numbers and particles motion is an importance factor of PM removal in a
rotating packed bed since the collection of larger particles may be
conducted mainly by inertial impaction and interception, while diffu­
sion of smaller particles usually occurs near the boundary layer of the
streamline.
Despite air pollution control, electricity and heat generation are the
greatest contributors to total greenhouse gas (GHG) emissions (over 13
Gt of CO2-eq in 2015) among different sectors, accounting for 42% of
total GHGs emission around the world (IEA, 2017). Particularly for
coal-fired power plants, deployment of carbon capture, utilization and
storage (CCUS) technologies are among the strategic plans for GHG
emission reduction. Several sites, such as Boundary Dam and Quest in
Canada (IEAGHG, 2015) and Sleipner in Norway (CCSA, 2017), have
successfully demonstrated the feasibility of CCUS technologies. It is
anticipated that CCUS technologies could remove ~52 Gt of CO2 emis­
sions from the electricity sector by 2050 to meet the “well-below 2 � C00
target(IEA, 2016a). Worldwide existing CCUS plants are mostly based on
chemical absorption, where amine solution is injected into a packed
tower to absorb CO2 from the exhausted gas stream (Coutris et al., 2015;
Rubin et al., 2015). The saturated absorbent is thermally regenerated in
a stripper with massive energy requirements (Bernstein et al., 2008),
and is then pumped back to the absorption packed tower (Puxty et al.,
2009). Despite amine-based absorption being effective in flue-gas CO2
emission reduction, the amine-based absorbents could be poisoned and
degraded by sulfur in the flue gas and thermal regeneration, respec­
tively, thereby reducing their lifetime of use (Davis and Rochelle, 2009;
Gouedard et al., 2012; Uyanga and Idem, 2007). Also, the amine ab­
sorbents would evaporate and leak from the system, leading to potential
environmental and health concerns (Khakharia et al., 2013).
CO2 can directly react with alkaline earth metal oxide-bearing ma­
terials (e.g., CaO and MgO, depicted by Eqs. (5) and (6)) (Lackner et al.,
1995) to form stable and insoluble carbonates via accelerated carbon­
ation (or so-called CO2 mineralization) (Lackner, 2003; Sanna et al.,
2014). Different types of industrial alkaline wastes, such as steelmaking
slags (Huijgen and Comans, 2005), air pollution control residues
(Baciocchi et al., 2009), and biomass wastes (Lopez et al., 2018) have
been utilized as the source of alkaline earth metals for CO2 minerali­
zation. The energy state of carbonate products, e.g., CaCO3 and MgCO3,
is much lower than that of gaseous CO2, indicating the thermodynamic
stability of the products (Santos et al., 2013). The reaction products can
be further used as supplementary cementitious materials in cement
mortars (Chen et al., 2016; Pan et al., 2016). In other words, numerous
benefits can be obtained from CO2 mineralization using alkaline wastes,
e.g., reduction of synthesized chemicals and environmental impact, and
value-added production of green cement for economic profits.
CaSiO3 þ CO2 →CaCO3 þ SiO2 ; ΔH ¼ 87kJ=mole (5)
MgSiO3 þ CO2 →CaCO3 þ SiO2 ; ΔH ¼ 81kJ=mole (6)
HiGee RPB is a process intensification technology which was first
proposed by Ramshaw and Mallinson in 1981 (Ramshaw, 2008) to
improve mass transfer performance. The operational cost and environ­
mental impact could be reduced from application of RPB by decreasing
the reactor size and equipment investment. To deliver greener chemical
2
Journal of Environmental Management 255 (2020) 109870
processing, the application of HiGee technology could significantly
improve processing efficiency, even under challenging conditions of
operation (Boodhoo, 2016). Regarding the reduction of air pollutant
emissions, the HiGee process could also simultaneously control air
pollution and capture and utilize CO2 to enhance environmental benefits
(Pei et al., 2017). Therefore, the HiGee process could be considered as a
higher energy efficiency means of multiple air pollutant reduction and
could substitute for traditional air pollution control equipment. On the
one hand, the NOx removal by the HiGee process is achieved by an
oxidation and absorption mechanism in ambient temperatures and
pressures with much lower energy consumption compared to selective
catalytic reduction (SCR) (Sorrels, 2016). The extra energy loss,
including pressure drop and heat escape, should be reduced due to the
completed air pollution control scheme. On the other hand, the life-cycle
approach was applied to assess the environmental impact under
different CO2 capture and utilization scales via the HiGee process. Based
on field testing, the evaluated results of the environmental impact of the
HiGee process could be more persuasive.
A holistic engineering, environmental, economic, and energy
(referred to as 4E in this paper) analysis could provide fundamental
knowledge regarding reactor design, process integration, and system
optimization for subsequent large-scale demonstration. In this study, the
HiGee process, using petroleum coke fly ash (PCFA) for integrated air
pollution control, was systematically assessed from the 4E perspective.
The engineering performance of the HiGee process was evaluated using
field data at a sub-pilot scale operation. Energy consumption, net CO2
emissions, and environmental impacts were determined by means of
life-cycle assessment (LCA), while the marginal economic cost and CO2
abatement scale were assessed by cost-benefit analysis. Energy effi­
ciency (e.g., heat-exchange efficiency) was by evaluated energy flow
analysis. Lastly, operating guidelines, cost benefits, and heat recovery
potential for integrated air pollution control using the HiGee process
were illustrated.
2. Materials and methods
In this study, the 4E performance evaluation of the HiGee process
was conducted to provide a trade-off solution for identifying the best
available operation conditions. To balance the critical importance of
HiGee for an upscale framework, the 4E perspective was applied to the
interaction of various factors among engineering performance, envi­
ronmental impact, economic cost and energy efficiency. During the
operating period, the 4E performance of each scenario was directly
evaluated from the real amounts of materials and energy consumption,
including electricity, real-time monitoring, and ex-situ measurement.
2.1. Scopes and definition of system boundary
Fig. S1 shows the procedure of a systematic approach to compre­
hensively evaluate engineering-environmental-economic-energy for the
HiGee process. Five steps including scope, inventory, indicators, anal­
ysis and interpretation were carried out. The scope is to define the sys­
tem boundary of HiGee while the inventory are addressed from on-site
operation, life cycle assessment and cost & benefit analysis. An ad hoc
committee supports the establishment of indicators among 4E aspects
and determination of weighting factors. After standardization and data
analysis, a comprehensive performance evaluation can be presented in a
radar diagram to further interpret the relationship between engineering-
environmental-economic-energy standpoints.
The sub-pilot scale HiGee was established in a petrochemical plant to
achieve integrated air pollution control using PCFA. As show in Fig. S2,
thy HiGee process consists of rotating packed bed, blower, tanks and
pump. A counter-current rotating packed bed reactor was used in the
HiGee process, with a packing size of 25.4 cm in height and 28.0 cm in
width. The exhausted steam used for the HiGee process was introduced
from a stack of the Formosa Company (Yunlin, Taiwan). The gas flow
T.-L. Chen et al. Journal of Environmental Management 255 (2020) 109870

Table 1
Key performance indicators (KPIs) and their associated weighting factors determined by Delphi method.
Aspect Key Performance Indicators (KPIs) Unit Weighting Factors

Engineering Performance EP1 CO2 Capture Capacity kg CO2/t-PCFA 0.70

EP2 NO Removal kg NO/t-PCFA 0.15
EP3 Production of Supplementary Cementitious Material t/t-PCFA 0.15
Environmental Impacts EI1 Global Warming Potential Reduction kg-CO2/t-PCFA 0.40
EI2 Fossil Depletion kg-oil/t-PCFA 0.20
EI3 Particulate Matter Formation Reduction kg-PM10/t-PCFA 0.10
EI4 Land Occupation m2/t-PCFA 0.10
EI5 Ecosystem Quality Improvement Points/t-PCFA 0.10
EI6 Risk of Human Health Reduction Points/t-PCFA 0.10
Economic Cost EC1 Save in Air Pollution Fees USD/t-PCFA 0.15
EC2 Earning of Carbon Credit USD/t-PCFA 0.40
EC3 Product Sale USD/t-PCFA 0.25
EC4 Operating Cost USD/t-PCFA 0.20
Energy EE1 Retrofit Heat Recovery kJ/t-PCFA 0.50
Efficiency EE2 Energy Intensity kWh/t-PCFA 0.50

rate of the exhaust gas stream was 1.10–1.84 m3/min, while the PCFA
where X’ xj is the standardized data matrix from the direct normalization
slurry flow rate was 0.02 m3/min. The concentration of CO2, NOx, and
pathway, comprised of standardized values xxj , and xxj and is the
0

O2 in the inflow flue gas were 12.81 � 0.03%, 31.00 � 0.31 ppm, and
5.6 � 0.01%, respectively. The O3 gas generated by a corona ozone multiplication product of the weighting factor and the original data.
generator (LAB2B, Triogen, UK) was used for flue-gas NOx removal, Otherwise, an inverse normalization was used for those whose
where the injected O3 flow rate was 0.1 L/min. At the beginning, the maximum value indicated the lowest performance:
PCFA and blowdown wastewater were mixed to form the PCFA slurry �
� � � max tyi tyi �
with high alkalinity then the gas flow rate and slurry flow rate were Tyi ¼ t’yi ¼
y¼1
� � (8)
controlled by a blower and a pump, respectively. The reaction was max tyi
y¼1 y¼1
min tyi
immediately occurred and accelerated as the flue gas and slurry were
simultaneously entered into the RPB. The retention time among the gas- where T’yi is the standardized data matrix from the inverse normaliza­
liquid-solid reaction of this heterogeneous system may not over 10 s due tion pathway, comprised of standardized values tyi , and tyi and is the
0

to the high centrifugal force in the reactor. Each experiment was con­
ducted around within 30 min when the pH value of PCFA slurry declined
to 6–7. After liquid and solid separation, the carbonated PCFA was
utilized as supplementary cementitious materials in cement mortar,
while the neutralized wastewater was reclaimed into other process.
In this study, two scenarios were established for the 4E analysis: (1)
business-as-usual (BAU) and (2) deployment of the HiGee process. In the
BAU scenario, the blowdown wastewater was chemically treated in a
wastewater treatment plant, while air pollutants (e.g., NOx and PM) and
CO2 in the exhausted steam from a hard coal-fired power plant were
emitted into the atmosphere and the PCFA was only legally disposed in
the petrochemical plant. In the scenario with the HiGee process, the
NOx, PM and CO2 emissions were treated through selective catalytic
reduction (SCR), electrostatic precipitator (ESP), flue gas desulfurization
(FGD), and then the HiGee process. In the HiGee process, the flue-gas
CO2 is directly used to neutralize and reduce the hardness of blow­
down wastewater. The flue-gas NOx can be absorbed via ozone oxidation
in the HiGee process, while PM can be removed by interception of the
packed bed or tiny droplets in RPB. The free-CaO in the PCFA can be
eliminated, which modified the chemical composition of PCFA to be
utilized as supplementary cementitious materials. The environmental
impacts assessment followed the International Organization for Stan­
dardization (ISO) 14040:2006 and 14044:2006 (IOS, 2006a,b).
To evaluate the 4E performance (i.e., engineering performance,
environmental impact, economic cost, and energy efficiency) of the
HiGee process, as presented in Table 1, the key performance indicators
among a total of 15 scenarios (from S1 to S15) were set-up via Dephil
method. Two normalizations were used to concisely conduct the data
analysis. The treatment capacity of PCFA by HiGee was roughly 2.88
tons per day, accompanied by 28.8 m3 of blowdown wastewater input.
For the items whose maximum value represents the optimum perfor­
mance, a direct normalization would be used, as expressed by Eq. (7):
� PCFA slurry reacted with CO2 in the flue gas. A total of six environ­
� � � xxj min xxj �
’ ’
X xj ¼ xxj ¼ � x¼1
� (7)
max xxj min xxj
x¼1 x¼1
multiplication product of the weighting factor and the original data.
2.2. Engineering performance evaluation
The functional unit of the HiGee for the 4E analysis was one ton of
PCFA input. The engineering performance was calculated using three
KPIs, i.e., EP1, EP2 and EP3, representing the CO2 capture capacity, NOx
removal, and production of supplementary cementitious materials,
respectively. The removal efficiency (η) of CO2 and NOx was evaluated
by Eq. (9):
Qi � ρi � Ci Qo � ρo � C0
η ð%Þ ¼ � 100% (9)
Q i � ρi � C i
where η (%) is the removal efficiency of a specific pollutant, ρ (kg/m3) is
the density of the flue gas, Ci (wt %/ppm) and C0 (wt %/ppm) are the
concentrations of pollutant in the inflow and outflow gasses, respec­
tively, and Qi (m3/min) and Qo (m3/min) are the flow rate of inflow and
outflow gasses, respectively. The daily loading of the HiGee process was
determined by Eq. (10),
Daily Loading ¼ Qi � Ci � η � t � 1440 (10)
2.3. Environmental impact assessment
The environmental impacts from the HiGee process were assessed by
the LCA using the ReCiPe midpoint/endpoint (Goedkoop et al., 2009).
For the BAU scenario, PCFA was disposed in a landfill, while blowdown
wastewater was directly discharged. Exhausted steam was emitted into
the atmosphere through conventional air pollution control equipment (i.
e., SCR-ESP-FGD). In the case of the HiGee process, PCFA and blowdown
wastewater were mixed and then pumped into the reactor, where the
mental impact indicators were determined: global warming potential
reduction (EI1), fossil depletion (EI2), PM formation reduction (EI3),
land occupation (EI4), ecosystem quality improvement (EI5), and risk of

3
T.-L. Chen et al. Journal of Environmental Management 255 (2020) 109870

human health reduction (EI6). specified temperature, which was estimated by polynomial regression as
expressed in Eq. (16),
2.4. Cost and benefit analysis Cp;m ¼ a0 þ a1 T þ a2 T2 þ a3 T3 (16)

To determine the economic performance, a cost-benefit analysis was
performed by calculating the differences between marginal costs and
revenues under various daily capture scales. As show in Fig. S3, the
marginal cost (MC, with a unit of USD/t-CO2) is defined as the additional
cost for “producing one more unit of product” in Eq. (11),
dðTotal ​ operating ​ costsÞ dðEC ​ þ ​ CU ​ þ ​ ⋯Þ
MC ¼ ¼ (11)
dðPlant ​ capture ​ scaleÞ dðCSÞ
where EC (USD) is the cost for electricity consumption, CU (USD) is the
cost for chemical use, and CS (t-CO2/day) is the daily capture scale of
CO2. The major cost of the HiGee process was electricity consumption,
where the electricity price was around 0.1 USD/kWh. The marginal
benefit, with a unit of USD/t-CO2, can be calculated by Eq. (12),
dðTotal ​ benefitÞ dðCC þ PS þ APF þ ⋯Þ
MB ¼ ¼ (12)
dðPlant ​ capture ​ scaleÞ dðCSÞ
where CC (USD/t-CO2) is the carbon credit, PS (USD/t-CO2) is the return
from product sale, and APF (USD/t-CO2) is the saved air pollution fee
along with the CO2 capture process. The revenue gain by HiGee process
included 10 USD for each ton of carbonated PCFA sales and 6.25 USD of
carbon credit (Bao et al., 2017).
In addition, it can be assumed that the implementation of HiGee
process in this study provided multi-benefits on CO2 capture and utili­
zation by mineralization and air pollution control. To compare the
economic impacts of HiGee with those of existing carbon capture and
storage (CCS) plants, an average inflation rate of 3.9% from 2005 to
2016 was considered to adjust the currency level in 2017 (World Bank,
2017). Therefore, the levelized currency value was transferred by Eq.
(13):
CVx
CV2017 ¼ (13)
ð1 þ iÞ2017 x was reduced by 99% (i.e., 600 rpm with a gas flow rate of 1.47 m3/min).
where i ( ) is the average inflation rate, CV2017 and CVx represent the
currency values in 2017 and in year x, respectively.
2.5. Evaluation of energy efficiency
The proposed integrated air pollution control via the HiGee process
can be considered as a heat exchanger with retrofit heat recovery (EE1)
and energy intensity (EE2). Due to the large amount of blowdown
wastewater utilization, the waste heat from the flue gas can be appro­
priately absorbed there by reducing the white smog emission. The heat-
exchange efficiency of a heat exchanger (θ) was calculated by Eq. (14)
(Fakheri, 2014).
m2 ​ � ​ Cp2 ​ � ​ ðT3 ​ ​ T4 Þ
θ¼ (14)
m1 ​ � ​ Cp1 ​ � ​ ðT2 ​ ​ T1 Þ
where m1 and m2 are the mass flow rates of fluids 1 and 2, respectively.
Cp1 and Cp2 are the specific heat value of fluids 1 and 2, respectively. The
terms (T2 T1) and (T3 T4) are the changes in temperature of fluids 1
and 2, respectively, involving the heat exchange. In the HiGee process,
where ao to a3 are the constants. The mean constant-pressure specific
heat value of the flue gas is the combination of products of mass fraction
and specific heat value for each composition. Table 2 presents the
thermodynamic parameters of major components in the flue gas. Based
on these parameters, the heat requirement and release during the heat
exchange process could be evaluated.
3. Results and discussion
3.1. Evaluation of engineering performance
Fig. 1 shows the capture scale and energy consumption for each
component in the HiGee process under various operating conditions, i.
e., gas flow rate and rotating speed. The influence of rotating speed on
the CO2 removal efficiency became more significant under higher gas
flows, while the highest capture scale was achieved at about 550–600
rpm under each gas flow. The energy consumption of the HiGee process
was inversely proportional to the carbon capture scale, i.e., in scenarios
with a higher amount of CO2 fixation, the energy consumption per unit
of captured CO2 was reduced. Under the 15 scenarios, it was observed
that the energy consumption for the pump and the blower totally
accounted for 80%–85%, while that of the reactor only accounted for
15%–20%. It was concluded that the height difference between the
reactor and the slurry tank was reduced, resulting in less power con­
sumption for delivering the slurry. Meanwhile, the driving force of waste
heat could push the exhaust stream into the reactor, thereby conserving
the energy consumption of the blower. By controlling the inlet gas flow
rate, the operation of the reactor would be more energy efficient.
Consequently, the highest daily load corresponded to a capture capacity
of 607 kg-CO2 per ton of PCFA, which could contribute the lowest en­
ergy consumption of 78 kWh/t-CO2. The emission concentration of NO
The reaction competition between carbonation and NO absorption
would not occur in the HiGee process, indicating the potential feasibility
of simultaneous air pollutant removal.
In addition, the carbonated PCFA via the HiGee process can be
directly utilized as supplementary cementitious material to avoid
additional costs for CO2 transport and storage (Pei et al., 2018a). Fig. 2
shows the compressive strength of blended cements developing on the
3rd, 7th, 28th, and 56th days. Although the mechanical strength of three
specimens met American Society for Testing and Materials (ASTM)
requirement, the 5% substitution of fresh and carbonated PCFA as
supplementary cementitious material exhibited better compressive
strength compared to Portland cement. It was observed that the early
Table 2
Thermodynamic parameters for evaluating energy conserved by HiGee process
in this study.
Thermodynamic Parameters Components in the Flue Gas
O2 N2 CO2
a0 ; J⋅mol 1 1 30.78 29.39 20.40
⋅K

fluids 1 and fluid 2 can be identified as inlet flue gas and blowdown a1 ; J⋅mol 1
⋅K 2 1.78 � 2.20 � 6.82 � 10–2
10–2 10–3
wastewater, respectively. For each single composition, the mean
a2 ; J⋅mol 1 3 5.00 � 10–5 3.00 � 10–6 4.00 �
constant-pressure specific heat (Cp;m TT21 ) can be calculated by Eq. (15):
⋅K
10–5
R T2 a3 ; J⋅mol 1
⋅K 4 4.00 � 5.00 � 10–9 6.00 � 10–9
Cp dT 10–8
(15)
T1
Cp;m TT21 ¼
T2 ​ ​ T1 Cp,m, J⋅mol 1 ⋅K 1
(In heat 37.04 29.51 59.97
extractor)
where T1 and T2 are lower and upper temperatures of the heat-exchange Cp,m, J⋅mol 1
⋅K 1
(In reheater) 31.94 29.18 47.97
process, respectively. Cp,m is the constant-pressure specific heat at a

4
T.-L. Chen et al.
Fig. 1. Engineering performance evaluation of HiGee at various daily CO2
capture levels and energy consumptions under 15 scenarios.
Fig. 2. Efficacy of 5% fresh and carbonated PCFA replaced as supplementary
cementitious material on compressive strength development compared to
Portland cement during different curing ages.
compressive strength of the blended cement with 5% carbonated PCFA
was 25% higher than that of Portland cement. The highest compressive
strength was achieved up to 54 MPa on the 56th day of the 5% substi­
tution of carbonated PCFA. Moreover, the changes on physical-chemical
characteristics of PCFA before and after carbonation via HiGee process
was presented in Table S1. It was found that a distinct difference in
calcium-bearing compositions. The calcium-bearing substances in PCFA
was the major reactive components for CO2 mineralization. The
decrease of free-CaO can benefit to the cement replacement.
3.2. Quantification of environmental impacts
Fig. 3 illustrates the contribution of major unit processes to GHG
emissions in terms of CO2-eq in scenario S-12 due to the electricity
consumption. Without a GHG emissions reduction strategy (i.e., BAU), a
CO2 emission of ~240 kg CO2 per t-PCFA was estimated, which was
mostly contributed by the combustion of the co-generation power plant.
In contrast, the abatement of CO2 emissions was 68% by implementing
the HiGee process, excluding the carbonated product utilized as sup­
plementary cementitious material. In the HiGee process, the flue gas
could penetrate through the equipment, leading to an emission of 9 kg
CO2 per t-PCFA. Meanwhile, the HiGee process could cause indirect
5
Journal of Environmental Management 255 (2020) 109870
Fig. 3. Significance of reduction in global warming potential (kg-CO2/t-PCFA
treated) by integrated HiGee process. (Operational conditions: 600 rpm; 1.47
m3/min; QG/Qslurry: 73.5; ηCO2: 95.6%).
GHG emissions of 68 kg CO2 per t-PCFA due to power consumption,
where the RPB accounted for 16.8%. Taking the utilization of PCFA into
account, a reduction of 87 kg CO2 per t-PCFA could be generated.
Consequently, a total emission reduction of ~250 kg CO2 per t-PCFA
could be conducted.
Fig. 4 shows the reduced environmental impacts of the HiGee process
with three types of daily captured CO2 load, based on endpoint analysis
for ecosystem quality, human health, and natural resources. It was found
that the highest abatement of climate change impact was 55.9% �
13.7% for the ecosystem, and 56.0% � 13.7% for human health at a
daily load of 607 kg CO2 per day. With increasing daily load, the
abatement on natural land transformation was observed to be from
61.7% � 1.1%–77.7% � 0.1%, while the reduction in PM formation was
at a similar level (i.e., from 63.7% � 1.1%–77.7% � 0.1%). Substantial
reduction in human toxicity could be clearly observed as well. However,
the abatement of fossil fuel depletion decreased with increasing daily
load of captured CO2 (i.e., from 137.5% � 0.9%–122.8% � 0.4%). This
could be attributed to a higher CO2 fixation balancing the emissions
from fossil fuel consumption.
3.3. Estimation of economic costs
The marginal costs and marginal benefits can be expressed as a
function of the daily load of CO2 abatement via the HiGee process. Fig. 5
illustrates the relationship between the marginal costs and marginal
benefits, compared to various CO2 abatement scales. It was found that
the intercept of the marginal cost curve (i.e., red line) was around 31.4
USD per t-CO2 indicating the payment needed for the initial cost of the
equipment. On the one hand, as the daily capture scale ascended, the
marginal cost would descend due to better energy efficiency, while it
would be enhanced at a higher abatement scale regime. On the other
hand, the marginal benefit (i.e., green line) was observed to be linear,
indicating that the intersection between marginal cost and benefit is
0.14 t-CO2 per day and 0.79 t-CO2 per day, corresponding to the
abatement costs of 14.5 USD per t-CO2 and 18.9 USD per t-CO2,
respectively. The favorable abatement scale of 0.65 t-CO2 per day for the
HiGee process could be estimated. As the abatement scale continues to
increase, the HiGee process would fail to be profitable compared to
carbon credit revenue. In this case, the installation of the HiGee process
could be strongly recommended under a range of abatement of
0.14–0.79 t-CO2 per day.
T.-L. Chen et al. Journal of Environmental Management 255 (2020) 109870

Fig. 4. Mitigation of environmental impacts for ecosystem quality, human health, and natural resource depletion under various daily CO2 capture levels using radar
plot: (a) 454 kg-CO2/day, (b) 607 kg-CO2/day, and (c) 760 kg-CO2/day.

1100 kJ mol 1 as solid CaCO3 precipitates. The waste heat from the
flue gas can be absorbed by water and the formation of calcite through
the HiGee process. By involving the daily treatment content of PCFA, the
retrofitted heat recovery and energy intensity can be calculated at
107.3–131.8 kJ per t-PCFA and 0.1 to 0.21 kWh per t-PCFA under each
scenario.

3.5. Comprehensive evaluation of HiGee process from 4E standpoints

To evaluate comprehensively the HiGee process quantifying engi­

neering performance, environmental impact, economic cost, and energy
efficiency, the daily loads of captured CO2, i.e., 454 kg-CO2/day, 607 kg-
CO2/day, and 760 kg-CO2/day, were selected as the key factor to
analyze the sensitivity. Fig. 6 shows the comprehensive evaluation of the
HiGee process quantifying engineering performance, environmental
impact, economic cost, and energy efficiency under different daily loads
of captured CO2. Results indicated that the points of energy efficiency
can be calculated from the range of 0.2–0.35 under all scenarios. It can
Fig. 5. Marginal cost and benefit of CO2 daily load in the HiGee process with explain that the KPI of retrofitted heat recovery and energy intensity in
respect to different abatement scales.
HiGee could not be significantly affected by different operating condi­
tions on the field test. The scenarios under 454 kg CO2 per day of daily
The operating costs of existing CCS plants were approximately 50.0
USD per t-CO2(Brooks et al., 2011) with the cost of CO2 transport and
storage at around 19.7 USD per t-CO2(ZEP, 2011). Therefore, by
implementing a geologic storage to inject CO2 into the depleted oil field
for the enhanced oil recovery (EOR) (Rubin et al., 2015), a storage
profits of 27.5 USD per t-CO2 was estimated, which would gain a net
expenses of 42.2 USD per t-CO2. To the contrary, the lowest operating
cost of the HiGee process, including electricity fees and oxidizer prices,
was estimated at 8.4 USDper t-CO2, based on the field tests. The profits,
including carbon credits and product sales for the HiGee process, were
61.3 USD per t-CO2, resulting in a net economic benefit of 52.9 USD per
t-CO2.

3.4. Integration of retrofitted heat recovery

The existing equipment (i.e., SCR, ESP and FGD) could contribute to
effective air pollution control with the generated waste heat, which
should be reused. The integration of retrofitted heat recovery for the
HiGee process is proposed to avoid the unfavorable white fume emitted
from the stack. The temperature of the exhaust gas needs proper control;
it should be higher than 350 K to reduce moisture condensation. As show
in Fig. S4, the equipped HiGee process was regarded as a cooling pro­
cess, with heat exchangers to reuse the waste heat and conserve energy.
The temperature and gas flow rate of the exhaust from SCR were around
570 K and 1.1–1.84 Nm3/min, respectively. After treatment with the
HiGee process, the temperature of the purified gas declined to 320 K Fig. 6. Performance evaluation of the HiGee process from engineering, envi­
with a gas flow rate of 0.98–1.75 Nm3/min. The energy of formation for ronmental, economic, and energy perspectives under different daily loads of
gaseous CO2 can be decreased from approximately 400 kJ mol 1 to CO2 capture and operating conditions.

6
T.-L. Chen et al.
load show the inefficient engineering performance (i.e., the points were
located from 0.11 to 0.16) while the higher environmental impact and
economic cost were conducted. The better engineering performance was
achieved under medium (607 kg CO2 per day) and high (760 kg CO2 per
day) daily loads, which could be calculated from 0.35 to 0.64 points. The
engineering performance of S-10 and S-15 were presented at relatively
lower points (e.g., 0.08 and 0.06). It could be attributed to the lower CO2
capture efficiency. Moreover, S-12, with a gas flow rate of 1.84 m3/min
and a rotating speed of 550 rpm, was superior with the lowest economic
cost (0.05) and environmental impact (0.1), as well as the highest en­
gineering performance (0.64) and adequate energy efficiency (0.21).
Under this circumstance, approximately 600 kg-CO2 could be captured,
which was equivalent to 207 kg CO2 fixed by one ton PCFA. In this case,
13.5 USD per ton PCFA of benefit, 114.7 kJ per ton PCFA of retrofitted
heat recovery, and 0.21 kWh per ton PCFA of energy intensity could be
retrieved. It was also found that the points of environmental impact
regularly change, accompanying those of economic cost, indicating a
strong relationship between carbon capture scale and performance in 4E
aspects. In addition, even in those scenarios with lower engineering
performance, the energy efficiency exerted by HiGee was not signifi­
cantly affected, which could be ascribed to the heat absorption capacity
of the HiGee process.
In this study, a waste-to-resource supply chain between petrochem­
ical and cement industries could be established to avoid waste treatment
and disposal, and reduce air pollutant and CO2 emissions. We also
demonstrated the feasibility of the HiGee process for treating waste­
water with high alkalinity (Chang et al., 2013). Meanwhile, the wastes,
including PCFA and air pollutants, are captured to produce valuable
products as construction material. It has been reported that the global
petroleum coke consumption is about 125 million tons (Factfish, 2016),
while assuming the ash content of petroleum coke is about 0.5% (Ber­
guerand and Lyngfelt, 2008). The global PCFA production and CO2
capture potential were thus estimated to be about 0.62 million tons and
0.13 million tons per year, respectively. Furthermore, if all the miner­
alized PCFA were utilized as supplementary cementitious material,
emission of 0.10 million tons of CO2 is expected to be avoided.
4. Conclusion
This study successfully examined effectiveness of the HiGee process
on CO2 capture along with air pollution control. The CO2 and petroleum
coke fly ash were originally low value byproducts of petrochemical in­
dustry and were valorized by the high-gravity process. Based on the field
test, t was found that the process was effective to reduce CO2 emission
from flue gas by approximately 600 kg/day with an energy intensity of
80 kWh/t-CO2. Marginal benefit and cost analysis revealed that the
optimal capture scale was 0.8 t-CO2/day at which point 24.9 USD net
profit could be retrieved for each day. Taking the reclamation of
carbonated petroleum coke fly ash as supplementary cementitious ma­
terials into account, reduction of global warming potential could reach
up to 328 kg–CO2–eq, accompanied by a comprehensive improvement
of environmental health including ecosystem quality and human health.
According to the 4E analysis, the HiGee process could be engineering
and energy feasible, economically profitable and environmentally
desirable. Economic profit including saving in air pollution fee, earning
in carbon credit and product sale amounted as high as to 13.5 USD/t-
PCFA, or 65.3 USD/t-CO2. Furthermore, the waste heat from flue gas
can be retrofitted to reduce the moisture condense, it was expected that
the not only the existing air pollution control process could be modified,
but also 70 � 5% of retrofit heat could be recovered from the exhausted
stream by the process. Based on the 4E analysis, the best operating
modulus should be scenario S-12, where a CO2 and NOx reduction can be
considerably conducted with relatively lower environmental impact and
economic cost. An integrated approach to appropriate air pollution
control, CO2 capture could with utilization of alkaline wastes and
wastewater could be achieved via the HiGee process in a petrochemical
7
Journal of Environmental Management 255 (2020) 109870
plant. In the future application of the upscaled HiGee process, several
key factors such as process integration, continuous operation, and
instrumental control and automation should be significantly concerned.
Acknowledgments
High appreciation goes to the Ministry of Science and Technology
(MOST) of Taiwan (R.O.C.) under Grant Number MOST 107-3113-E-
007-002 and 107-2221-E-002-009-MY3 for the financial support. Au­
thors also would like to appreciate the Enago for the English texts
revision. The authors are grateful to the Formosa Plastics Corp. for
providing technical support for the on-site operation.
Appendix A. Supplementary data
Supplementary data to this article can be found online at https://doi.
org/10.1016/j.jenvman.2019.109870.
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