Energy Conversion and Management: X 21 (2024) 100489

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Energy Conversion and Management: X

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Simulation of carbon dioxide direct air capture plant using potassium

hydroxide aqueous Solution: Energy optimization and CO2
purity enhancement
Zahra Zolfaghari a, Alireza Aslani a, *, Rahim Zahedi a, Sina Kazzazi b
a
Department of Renewable Energy and Environment, University of Tehran, Tehran, Iran
b
Department of Energy Engineering, Sharif University of Technology, Tehran, Iran

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

Keywords: While various methods of direct air capture (DAC) technology have been implemented, its widespread effec­
Direct Air Capture tiveness hinges on achieving optimal design and process improvements, largely owing to the high energy costs
DAC involved. Literatures reports a substantial heat demand for high-temperature aqueous solutions DAC (HT DAC),
Energy Optimization
ranging from 1420 to 2250 kWh per ton of CO2, accompanied by electricity consumption rates varying from 366
Pinch Analysis
Aqueous Solution
to 2790 kWh per ton of CO2. The present study adopts the HT DAC method with an aqueous KOH absorbent as its
focus, aiming to mitigate energy consumption. Given that a substantial portion of energy consumption in
comparable processes can be attributed to the calciner and slaker units, our research centers its attention on the
Air Separation Unit (ASU) and the steam cycle unit, investigating their impact on the system’s production ca­
pacity, the enhancement of CO2 purity, and the augmentation of equipment thermal recovery. Process optimi­
zation, results a remarkable increase in heat recovery (21.1 %) and significant reductions in utilities
consumption. The outcomes indicate that this facility has the capacity to annually capture around 1.1 million
tons of CO2 with a purity of 99 mol% for utilization across various industries. The process design necessitates
5.24 gigajoules (GJ) of heat and 343 kW-hours (kWh) of electricity per ton of captured CO2. Notably, in addition
to fulfilling the internal electricity requirements, the facility can export 8 MWh of electricity per ton of captured
CO2 to the grid.

shows an example of a process that uses an aqueous NaOH solution as a

solvent for capturing CO2 from the air. The process consists of two
Introduction interconnected cycles that co-occur. The cycle on the left is known as the
absorption cycle, where the CO2 molecules in the air come into contact
The increase in the consumption of fossil fuels and the economic with the absorbent and react with it, and Na2CO3 solution is produced.
development of countries has led to a rise in the emission of CO2 since In the reaction of this product with Ca(OH)2, the solvent is regenerated
the beginning of the industrial revolution [1]. According to the latest and goes to the first cycle to continue the capture activity. The cycle on
report, the concentration of CO2 in the air has reached its highest level, the right is known as the desorption cycle. Due to the decomposition of
approximately 418 ppm [2]. Therefore, researchers and scientists have CaCO3 produced at high temperatures, CO2 is removed from the system,
tried to prevent this increase using different and effective methods. and CaO reacts with water to regenerate Ca(OH)2.
Various methods have been proposed to deal with global warming. This industrial process captures CO2 from the ambient air using
Using carbon capture and storage (CCS) technologies is one of the best chemical processes and produces a stream of pure CO2 for use in various
ways to reduce CO2 in the environment. One of the newly emerging processes or storage, and this method helps remove CO2 from the at­
technologies in CCS is the DAC, which Lackner and his colleagues mosphere [6]. Due to the low concentration of CO2 in the air, chemical
introduced in 1999 to prevent climate change [3]. Considering that half absorbents have been widely considered in the literature to investigate
of the annual emissions of CO2 is made up of diffuse emission sources, their performance.
DAC has the potential to be able to emit greenhouse gases from these Keith et al. (2006) [7] investigated the capturing of CO2 from the air
sources and point emission sources even in low concentrations [4]. Fig. 1

* Corresponding author.
E-mail address: alireza.aslani@ut.ac.ir (A. Aslani).

https://doi.org/10.1016/j.ecmx.2023.100489
Received 17 August 2023; Received in revised form 22 October 2023; Accepted 14 November 2023
Available online 15 November 2023
2590-1745/© 2023 Published by Elsevier Ltd. This is an open access article under the CC BY-NC-ND license (http://creativecommons.org/licenses/by-nc-nd/4.0/).
Z. Zolfaghari et al. Energy Conversion and Management: X 21 (2024) 100489

evaluated the energy and cost of the DAC system using a soluble
Nomenclature absorbent and investigated the effect of using a contactor based on
NaOH spray. The results showed that drop coalescence significantly
ASP American Physical Society reduces the CO2 absorption efficiency but increases the number of water
LT Low Temperature losses, while in this design, the fan and pump energy requirements will
ASU Air Separation Unit be manageable. Nikulshina et al. (2009) [11] presented a one-cycle
MER Maximum Energy Recovery thermochemical process using a concentrated solar energy reactor as a
BCC Balanced Combination Curve source of heat supply for calcining CaCO3 and carbonating CaO for the
st Stream continuous removal of CO2 from ambient air. The results of this research
BECCS Biomass Energy with CCS stated that direct sunlight and water vapor help increase the reaction
CC Composite Curve rate and heat transfer.
Subscripts Mahmoudkhani and Keith (2009) [12] developed a new method for
CCS Carbon Capture and Storage a, b, and regenerating NaOH alkaline sorbent using titanate. This system’s energy
c constant and exergy analysis showed that the titanate cycle might significantly
DAC Direct Air Capture minimize water losses and greatly reduce the overall cost of DAC.
aq aqueous Socolow et al. (2011) [13], in a report prepared by the American
GCC Grand Composite Curve Physical Society (ASP), compared the DAC technologies with the post-
g gas combustion method of carbon capture and provided relatively more
HT High Temperature details about the energy balance and economic aspects of DAC systems.
s solid The considered system was based on the use of NaOH aqueous solvent.
By making optimistic assumptions about the technical parameters, the
DAC system’s cost is estimated to be at least 600 $/t-CO2. Holmes and
Keith (2012) [14] presented a simple method to optimize the gas–liquid
using two DAC technologies based on NaOH liquid absorbents and contactor design for DAC using slab contactors based on KOH solution
Biomass energy with CCS (BECCS). This study examines the economic and compared the obtained results with ASP estimates. The authors in
and physical limitations of two options, and according to the results of this study show that the difference between the cost assessed in this
the BECCS method, it is limited due to the availability of biomass re­ study and the costs reported in other studies is due to the choice in the
sources. In contrast, DAC technology can reach climate goals in the short method and basic design, not in the cost calculation method. Mazzotti
term. However, the limitation in the energy supply sources of this plant et al. (2013) [15] re-examined the ASP design in which they proposed
may increase the costs. The estimate made by Keith for this plant, with a three new packings to optimize the contactor unit, which differed in
lifetime of 20 years and absorption of 280,000 t-CO2, was estimated at pressure drop and price. These packings have no change in the CO2
500 $/t-CO2. Keith also pointed out that the estimated costs will be received from the atmosphere, and the proposed plan, like ASP, absorbs
significantly reduced by optimizing the system, design, and new tech­ 1 Mt-CO2 with all kinds of packings. Also, the ASP energy strategy was
nologies. Baciocchi et al. (2006) [8] designed a DAC plant using an maintained in this study, but the thermal energy required for regener­
aqueous solution absorbent with two different precipitators. In this ation in the furnace was produced from the natural gas available at the
study, the balance of materials and energy was checked, and the fac­ site. The final estimated cost was reduced to 399–376 $/t-CO2
tory’s energy needs were determined. The result indicated that calci­ depending on the costs and energy consumption of the three types of
nation of calcium carbonate has the most significant contribution to packing. Mazzotti also revised and recalculated the thermal energy de­
energy use and suggested evaluating the supply of this heat source using mand of the ASP plan and concluded that equipment investment costs
renewable sources. and annual operating costs could be reduced by 2.4 % and 3 %,
Zeman (2007) [9] studied the thermodynamics and energy con­ respectively. Optimizing the system and using the suggested packing
sumption of DAC technology at the industrial level using the wet reduced the avoided cost of the system by 7–9 %. Zeman et al. (2014)
scrubbing technique and concluded that the CO2 flow coming out of this [16] reviewed the ASP report and made different assumptions about the
process could be used for the continuous production of hydrocarbon energy penalty and costs related to the DAC system. This research
fuels for use in the transportation sector. Stolaroff et al. (2008) [10]

Fig. 1. Example of DAC process using NaOH chemical sorbent [5].

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Z. Zolfaghari et al. Energy Conversion and Management: X 21 (2024) 100489

showed that minimizing the plastic materials used in the air contactor DAC is moving forward and the cost reduction and process efficiency
and using low carbon electricity could reduce the investment and increase are significant, there are many challenges in developing this
operating costs by 2.4 % and 1 %, respectively, compared to the ASP technology. This study aims to design a DAC plant that uses a liquid
design. absorbent to capture CO2. Therefore, it is considered that the existing
Li et al. (2015) [17] surveyed the energy supply source required for plant can have the highest capture rate with optimal energy consump­
CO2 capturing from the air. Considering that the amount of CO2 in the tion. The following factors have been investigated for this process in
ambient air is low and the energy requirement for separating this order to improve it.
compound is high, this research evaluated and feasibility of using a wind 1. Using a turbine in the steam cycle to generate power from the
system to provide energy. Considering different parameters such as output steam flow.
intermittency and fluctuations of the wind power supply in the time of 2. Designing the ASU section and reducing the airflow to reduce the
change, this type of clean energy can be a suitable alternative to fossil amount of oxygen required for use in the calciner section in order to
fuels. increase the purity of the outgoing carbon dioxide.
Keith et al. (2018) [18] evaluated DAC technology using KOH so­ 3. Using pinch technology and thermal recovery in equipment.
lution as a liquid absorbent. This process could capture 75 % of atmo­
spheric CO2, capturing 1 Mt-CO2. Keith considered three scenarios in Materials and methods
this evaluation, which differed in oxygen supply, CO2 compression, and
electrical system. The cost of the DAC plant designed based on different The technologies used in DAC technology operate based on stable
assumptions ranged from 94 to 232 $/t-CO2. Krekel et al. (2018) [19] and regenerative absorbents so that they can absorb and then release
evaluated the separation of CO2 from ambient air from a technical and CO2 many times in the cycle. In addition, the solvents used for absorp­
economic point of view. Amines/imines were considered absorbents for tion include physical and chemical sorbents. Compared to physical
carbon dioxide separation in the designed system. The total energy de­ sorbents, which have lower CO2 absorption, lower selectivity properties,
mand required for the system was calculated, and this high energy de­ chemical sorbents provide better performance at low concentrations
mand is mainly caused by the compressor system compressing CO2 and [24]. Therefore, choosing the appropriate absorbent in the process
overcoming the pressure drop in the system. Also, the cost of preventing design can also affect the amount of CO2 absorption and the energy
CO2 emissions differs depending on the energy source (wind, natural consumption of the process. The solvent should be selected to be easy to
gas). These results provide higher energy demand and cost values than manage during the process, is resistant to contamination, and should not
other values stated in the literature. The economic analysis of this study be lost because its properties determine the entire process [5]. The
shows that combining DAC systems with renewable energy can reduce chemical sorbents studied so far in the HT DAC process are based on
CO2 removal costs compared to fossil fuel-consuming systems. Fasihi alkaline hydroxides (KOH and NaOH), which consists of two connected
et al. (2019) [5] conducted a literature review and technical and eco­ cycles. The two main components of a DAC process in the HT DAC
nomic analyzes of advanced DAC technologies. In this study, it is method are the air contactor and the regeneration facility. Aqueous
concluded that the costs of the DAC system can be significantly reduced solutions (such as KOH) consist of two cycles that coincide. The primary
with commercialization in the 2020 s, followed by widespread imple­ example of this method used in this research is shown in Fig. 2. The
mentation in the 2040 s and 2050 s. In the conducted analysis, it is stated number of each stream is displayed in green.
that to reach the goals of the Paris Agreement; it is necessary to increase Four basic reactions occur in this system (Eq. 1–4) [23]. The air
the capacity of DAC factories to 3 Mt-CO2/year, 470 Mt-CO2/year, 4798 contactor equipment carries out the contact between the air containing
Mt-CO2/year, and 15,402 Mt-CO2/year during the years 2020, 2030, CO2 (St. 1) and the aqueous KOH solution (St. 2). The solution absorbs a
2040, and 2050. large part of the CO2 in the air, and the airflow that has received been
Weimann et al. (2020) [20] designed a DAC system to produce depleted in CO2 exits into the atmosphere during as stream 3. Carbon
synthetic methane fuel and investigate its performance. This study dioxide molecules react with the absorbent, and a bond is established
evaluated the effect of system flexibility on the performance of fuel between them. During this exothermic reaction, potassium carbonate
synthesis, CO2 absorption, and the effects of geographical locations. The solution (K2CO3) and water are produced (Eq.1). K2CO3 produced in
results showed that electricity price and network emission factors stream 4 goes to the pellet reactor unit and is placed in contact with
determine economic and environmental performance. Marchese et al. calcium hydroxide (Ca(OH)2), which enters the reactor from stream 5 so
(2021) [21] discussed the integration of DAC technology with Fischer- that calcium carbonate (CaCO3) is produced and the absorbent is re­
Tropsch synthesis. In this project, the conversion of CO2 into synthetic generated (Eq. 2). The absorbent leaves this unit through stream 2 and
chemicals (wax) and synthetic fuels is maximized by using process and returns to the air contactor to continue the absorption process. Calcium
energy integration. The economic evaluation of the system shows that carbonate is removed from stream 6 in the calciner and is heated to
this integration can be a turning point in developing DAC factories and decompose into CO2 and calcium oxide (CaO) (Eq. 3). The decomposi­
wax production. tion reaction is endothermic and occurs at 900 ◦ C. The calciner is
Long-Innes and Struchtrup (2022) [22] re-examined the DAC plant considered oxy-fuel. Natural gas and pure oxygen (St. 7) obtained from
designed by Carbon Engineering. In this study, the places with the most the air separation unit have been used to provide the calcination heat.
heat loss were identified. It was determined that the major loss of Stream 8 contains CaO, and in combination with water (St. 10), lime
chemical exergy in the preheater cyclones and calciner unit is due to the water (Ca(OH)2) is rehydrated in the slaker unit and regenerated to be
required high temperature, the water removal system, the final CO2 used in the cycle (Eq. 4). CO2 concentrated gas (St. 9is compressed) after
compression system, and the power island. This study proposes guide­ purification, and is taken out of the system for storage or use [18,25].
lines for using renewable energy to improve and optimize the system to Air 2KOH(aq) + CO2 (g) →K2 CO3 (aq) + ΔHo = (1)
make this process a suitable option for climate measures. Contactor H2 O(l) − 95.8 kjmol− 1

Daniel et al. (2022) [23] investigated the DAC plant during research. Pelle K2 CO3 (aq) + Ca(OH)2 (s) →2KOH(aq) + ΔHo = (2)
The analysis showed that this system could also be used to generate Reactor CaCO3 (s) − 5.8 kjmol− 1

income, and even in the next few years, this technology will be profit­ Calciner CaCO3 (s) →CaO(s)+ CO2 (g) ΔHo = + (3)
able through the sale of produced CO2. It has also been proven that DAC 178.3 kjmol− 1
can have a very positive effect on reducing carbon emissions. Also, the Slaker CaOs + + H2 Oi→Ca(OH)2 − s ΔHo = (4)
− 63.9 kjmol− 1
use of renewable electricity will significantly reduce the use of fossil
fuels.
Based on the above research, although the development process of The simulated process in this research is based on the data of the DAC

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Z. Zolfaghari et al. Energy Conversion and Management: X 21 (2024) 100489

Fig. 2. Schematic diagram of DAC system with KOH absorbent.

plant designed by Keith et al. [26]. This system is currently being

Table 2
implemented commercially by Carbon Engineering [18]. This simula­
Coefficients for the chemical equilibrium constants.
tion was performed by Aspen Plus™ software (V. 11). ASPENPCD,
AQUEOUS, SOLIDS, INORGANIC, and PURE26 database and ENRTL No. Equilibrium A B C D
reaction constants
activity coefficient model for the liquid phase and RK-SOAVE equation
of state for vapor phase are used in this study. In addition to these cases, 5 K5 216.05 − 12431.7 − 35.4819 0
7 K7 231.465 − 12092.1 − 36.7816 0
other parts of the system, including gas cycle, steam cycle, ASU, and
8 K8 132.899 − 13445.9 –22.4773 0
calciner units, are modeled with Peng Robinson equation of state,
Steam-NBS, and Peng-Rob equations of state, respectively. This system
can capture 1.1 Mt-CO2/year, which delivers CO2 gas flow with 99 % flow is shown in yellow. The streams information is attached in
mol% (99.5 wt%) purity. Tables S2 to S5 in the supplementary information file.
The main point of the simulation is to perform these reactions in the
electrolytic environment, using the Electrolyte Wizard tool in Aspen Absorber and air contactor
Plus. The reactions as regards the DAC process have been specified and
listed out in Table 1. Fig. 4 shows the Absorber and air contactor unit of the system. The
The parameters for the calculation of the equilibrium constants are air contactor in Aspen Plus is not defined as a specific component; for
shown in Table 2. this reason, two mixers and one separator (Mixer-1, Mixer-2, and SEP-1)
have been used to simulate the air contactor section, which have the
Process description same function of separating CO2 from atmospheric air. The power plant
unit’s output flue gas (containing 12.75 wt% CO2) enters the absorber
The detailed process flow diagram of the whole DAC process is tower from stream 1. Stream 2 contains an aqueous solution of KOH.
shown in Fig. 3. In this section, the operation of the system’s main parts Some of this solution enters the absorber to capture the CO2 produced in
has been investigated. The characteristics of each of the main units are the power plant unit. In this unit, 63.5 % of CO2 in the incoming gas flow
presented in Table S1 in the Supplementary information file. As can be is absorbed by an aqueous KOH solution. Stream 3 exiting from the top
seen, the ASU section is designed to supply the oxygen needed for the of the absorber is combined with airflow (AIR-IN) with a flow rate of
calciner unit, and the EXP-03 turbine is used to generate power from the 250,000 ton/hour, which contains CO2 0.06 wt%, and enters the air
slaker exhaust steam to prevent energy loss and increase the energy contactor. Then, the mixture of the output stream from the absorber and
recovery of the system. In this figure, air flow containing CO2 is green, the contactor (St. 4) mixes with an aqueous KOH solution and enters the
clean air with CO2 is pale green, natural gas flow is brown, water flow is separator (Sep-01) to separate the gas and solid phase (St. 5). The air
blue, solid material flow is black, sorbent flow is black, and pure CO2 with lower CO2 content exits from the top of the separator (St. TO-AIR)
and the flow containing liquid materials exits from the bottom (St. 6).
Table 1 The amount of CO2 in the exiting air reaches 0.01 wt%. According to the
Reactions occuring in the electrolyte environment. amount of CO2 in the contactor inlet and outlet air, it is known that
reactions type 73.33 % of the CO2 in the air has been captured. In this way, the solution
absorbed 99.8 % of the carbon dioxide in the output stream resulting
+ HCO−3 ↔ CO2− + Equilibrium (5)
from the combustion in the power plant section and the air entering the
H2 O 3 + H3 O
+ 2+
CaOH ↔ Ca + OH − Equilibrium (6)
Equilibrium (7)
contactor. P-02 pump has been used to compensate for the pressure drop
2H2 O + CO2 ↔ HCO−3 + H3 O+
2H2 O ↔ OH− + H3 O+ Equilibrium (8) of stream 8 output from the contactor (this flow is rich in CO2) to reach 1
Ca(OH)2 (S) ↔ CaOH+ + OH− Salt (9) bar. MIXER-3 is used to mix the liquid solution coming out of the air
CaCO3 (S) ↔ CO2−
3 + Ca
2+ Salt (10) contactor (St. 7) with the aqueous solution coming out of the absorber
K2 CO3 →CO2−
3 + 2K
+ Dissociation (11) (St. 8). The final stream is heated in the heat exchanger (HX-01) and
CaCO3 →CO2−
3 + Ca
2+ Dissociation (12) enters the PELLET REACTOR.
KOH→OH− + K+ Dissociation (13)

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Fig. 3. Designed process.

Pellet reactor removed before sending back to the pellet reactor. For this purpose, two
filters, FILTER-1, and FILTER-2 are used to separate the remaining
Fig. 5 shows the pellet reactor unit. The exothermic reaction of amount of CaCO3. Both units can separate a certain amount of solid
K2CO3 produced in the air contactor (St. 10) with Ca(OH)2, which enters CaCO3. Therefore, the liquid flow (St. 19) is pumped to the pellet
from stream 11, occurs in a pellet reactor unit. The precipitated CaCO3 reactor. FILTER-2 is used to remove all solid CaCO3 from stream 20.
and the liquid leave the unit during stream 12 and move towards SEP- stream 21, the flow of aqueous KOH solution, returns to the absorber and
02. A larger share of CaCO3 is removed from the separator (St. 13), contactor at the outlet. Finally, stream 22 is divided into three streams
which is completely formed from the solid CaCO3 sediment, while the 23, 24, and 25. Stream 24 can be sent to the calciner for use, and stream
remaining calcium carbonate along with KOH is removed from the 23 is disposed of as waste. Stream 26 is a mixed flow of liquid and solid
separator (St. 14). A part of the stream that contains a high amount of solution CaCO3, which finally enters FILTER-3 and is separated. In this
water along with CaOH+ ,CO−3 and, OH− enters MIXER-4 as a return case, the liquid is separated, recycled to the reactor pellet, and starts
stream from flow 15 and mixed with flow 16, which consists of solid circulating again (St. 27). While almost all of the solid CaCO3 is filtered
CaCO3, and is considered as a make-up flow. Stream 17 is almost liquid in this section and transferred to the WASHER section through stream
but still contains very small amounts of solid CaCO3 that must be 28.

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Slaker

Fig. 6 shows the simulation of the slacker unit. Slaker is a reactor

used to hydrate the activated lime (CaO) from the calciner unit and
preheat the CaCO3 pellets from the pellet reactor. Stream 28 contains
solid CaCO3; by passing through the FILTER-3 along with water, stream
29–1 enters the WASHER, and the pellets formed there are washed. In
the washing process, the amount of CaCO3 reaches from 99 wt% to 0.55
wt%. Two streams come out of this unit. Stream 30 contains liquid water
almost completely and exits from the bottom of the washer, and stream
31 consists of water and solid CaCO3, which temperature reaches 300 ◦ C
in stream 33 from 57 ◦ C by two heat exchangers HE-03 and HX-02 and
enters the SUMP separator. This unit is a separator to separate the vapor
phase from liquid and solid.
Stream 33–1 in the vapor phase (pure water vapor) exits from the top
of the separator, while stream 33–2, which consists of two liquid and
solid phases, exits from the bottom of this unit, which is 99 % of this
stream consists of CaCO3 and the remaining 1 % of other compounds. In
order to separate solid CaCO3 from the other flow items, it enters
FILTER-4. CaCO3 is removed for use in the calciner as stream 34, and
other items enter SLAKER in stream 35 along with flow 33–1. The
amount of 7 t-water/hour also enters the slaker in the steam cycle sec­
tion of the power plant (St. 36). Stream 37, which contains CaO, enters
the slacker and reacts there (conversion coefficient 85 %) with water;
during this reaction Ca(OH)2 is formed. Unconverted CaO and solid Ca
(OH)2 enter the process again as stream 39. The output stream 40 con­
tains water and solid Ca(OH)2, which enters the DUST-COL unit. Also,
Solid CaO leaves stream 41.

Fig. 4. Absorber and air contactor.

Fig. 5. Pellet Reactor.

Fig. 6. Slaker unit.

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Calciner

Fig. 7 shows the process that is carried out in this reactor. The
calciner reactor is the most crucial part of the plant that operates at a
very high temperature. In this reactor, the calcination reaction of CaCO3
takes place. This reaction closes the solvent regeneration cycle and
produces a concentrated stream of CO2. This unit operates at a pressure
of 1 bar and a temperature of 900 ◦ C, requiring much heat to carry out
the reaction. The reaction in this unit is described by the Peng-Robinson
equation of state. Three streams enter this reactor; 1) Stream 42,
including solid CaCO3, which reaches 646 ◦ C by heat transfer, 2) stream
43, which is natural gas; and 3) Stream of oxygen 44 that has left the
ASU section. In the calciner, in addition to the conversion reaction of
CaCO3 to CaO (conversion coefficient 98 %), the complete combustion
reaction of methane and ethane also occurs. This combustion provides
the heat required for the calciner unit. Stream 45, which contains CaCO3
and CO2, leaves the calciner. The presence of both solids and gases inside
the reactor means that the product stream contains a solid and a gaseous
component. SEP-03 unit has been used to separate solid from gas. The
solid flow of CaO exits from the bottom of the SEP-03 unit (St. 46).
Stream 47 (900 ◦ C) exits from the top of the unit and transfers heat to the
calciner with CaCO3 flow. During this heat transfer, stream 48 reaches
450 ◦ C, enters SEP-04 along with pure water stream 29, and combines.
The liquid water comes out as stream 29–1 and enters the WASHER unit.
Stream 49 contains CO2, with a purity of 99.5 % by mass. This CO2
stream is released at a temperature of 45 ◦ C and high pressure for con­
sumption or storage.

Air separation unit

Fig. 8 shows the simulated flows and units of the ASU section. AIR-02
Fig. 8. ASU unit.
air stream reaches 9.52 ◦ C from a temperature of 21 ◦ C at constant
pressure by a cooler. The airflow has a certain amount of water that must
be separated in the ASU. For this purpose, the pure water stream (50) is Stream 54 contains nitrogen, oxygen, and a very small amount of CO2. It
separated by the SUMP-01 unit, and the amount of water that remains in is divided into two streams, 55 (15 Kg/s) and 56 (45 Kg/s). Stream 55
stream 51 must be separated by multi-stage compressors. The AIR should enter the LPC tower at a pressure of 1.3 bar. In order to reduce
BLOWER unit consists of 3 stages, and the temperature between each the pressure of this flow, a turbine has been used, which produces 1.34
stage (compressor outlet temperature) must be lower than 107.22 ◦ C. MW of power.
The pressure rises from 1 to 5.8 bar (stream 52) during these stages. The Stream 55–1 at a pressure of 1.3 bar and a temperature of − 54.52 ◦ C
amount of remaining water is separated by the ADS adsorption unit. enters the HXE along with stream 56 (35 ◦ C and 5.8 bar) and heat

Fig. 7. Calciner unit.

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exchange with two streams 57 (contains O2) and stream 58 (contains oxygen and nitrogen coming out of this unit are used at very low tem­
N2). Stream 59 exits this unit with saturated steam and a temperature of peratures. The nitrogen flow can act as a cooling fluid because it is not
− 159.21 ◦ C and enters tray 48 of the LPC unit. While stream 60 enters needed in the process, but the oxygen flow must enter at a temperature
the HPC with a temperature of − 174.03 ◦ C. Meanwhile, flow 57-A leaves of 625 ◦ C to perform a combustion reaction with natural gas. Calciner
the unit and goes to the calciner, while 58–1 leaves the system. Nitrogen receives part of this energy from the HRSG of the power plant unit and
is removed from the system after cooling by C-06. This flow can be sold the rest through the flow of the hot stream output from the calciner unit.
as a by-product in various industries and be a part of the source of in­
come for the system. Steam cycle
At the top of the HPC tower, N2 leaves as stream 61 as a liquid with a
high purity of 97.5 % mol at a temperature of − 177.11 ◦ C to enter the Fig. 9 shows the flows and simulated units of the steam cycle section.
LPC tower. Stream 62 (containing N2 and O2) comes out from the bottom The pure water flow is pumped up to a pressure of 63 bar and heated by
of this tower. The condenser of this tower is of full reflux type because the return flow from the turbine, and its temperature reaches 89 ◦ C.
there is a flow of liquid nitrogen at − 177.11 ◦ C (reflux = 0.9). With this Then it enters the HRSG unit and leaves this unit with a temperature of
ratio, the heat load reflux of the HPC tower condenser is 4.84 MW. The 475 ◦ C (St. 64). This flow enters the turbine (EXP-02) with the stream
liquid nitrogen stream from the top of the HPC tower reaches a pressure flow (St. 65) and produces 15.63 MW of power. The turbine’s output (St.
of 1.2 bar through a valve and enters the LPC tower from the top in a 66) is converted into a saturated liquid by the C-08 exchanger and
two-phase mode. The liquid stream 62 exiting from the bottom of this pumped. Stream 67 (50 ◦ C) enters HE-05 and performs heat exchange
tower also reaches a pressure of 1.3 bar after passing through a valve, at with solid Ca(OH)2 stream exiting from slacker (St. 68). During this heat
which pressure the flow is two-phase, and according to the pressure transfer, the flow temperature reaches 253 ◦ C. The amount of this stream
profile in the LPC tower, it enters the tray 47 of this tower. (7 ton/hour) enters the slacker, and the rest (St. 70) enters the HE-04
Stream 52 also enters the LPC tower at a pressure of 1.3 bar. The converter to increase the temperature and then enters the turbine
thermal load of the reboiler of the LPC tower is entirely provided by the cycle again as streams 65 and 72. This way, 4.6 MW of power is pro­
heat output from the condenser of the LPC tower. Stream of oxygen (St. duced from the EXP-03 turbine. The output of this turbine (St. 73) has
57) leaves the bottom of the LPC tower with a purity of 99.65 wt%. reached saturated liquid (St. 75) by heat transfer in HE-06 and C-09
However, a stream of nitrogen (St. 58) exits with a purity of 92.7 wt%. In exchangers. Stream 75 enters the cycle after reaching a temperature of
the ASU section, a multi-stream heat exchanger (HXE) facilitates heat 25 ◦ C. The amount of 7 ton/hour output from this cycle that enters the
exchange between two streams, one cold and one hot, commonly Slaker is provided by the cycle’s return flow (MU-H2O).
referred to as the Cold Box exchanger. Oxygen is in a liquid state at f
− 180.3 ◦ C, reaching a temperature of 35 ◦ C through heat transfer with Gas cycle
airflow. Also, on the other hand, the cold stream of nitrogen transfers
heat to deliver the incoming streams to the LPC and HPC towers. Fig. 10 shows the simulated flows and units of the gas cycle section.
The temperatures of the streams entering the towers of the ASU are The AIR-01 stream includes ambient air that enters the AIR-COMP
very low, and to bring the airflow to these temperatures, the streams of isentropic compressor, and the pressure reaches from 1 bar to 10 bar

Fig. 9. Steam cycle unit.

8
Z. Zolfaghari et al. Energy Conversion and Management: X 21 (2024) 100489

minimum possible external heating and cooling requirements are ob­

tained theoretically. The same information is available from the grand
composite curve (GCC). GCC analyzes can be performed to identify
possible integration of processes in an existing system.
The primary purpose of pinch technology is to connect hot and cold
streams using a network of heat exchangers to minimize the demand for
energy-supplying equipment while the heat recovery reaches its
maximum [29]. This design is called maximum energy recovery (MER).
An important parameter is ΔTmin, which shows the lowest temperature
difference in the heat exchanger network. The best design for the heat
exchanger network is possible by considering the amount of energy
recovered and the costs required to recover it. The best method is to
choose the best ΔTmin with the most heat recovery capability among
different types of flows, taking into account economic and heat transfer
issues. For this purpose, Aspen Energy Analyzer (V11) software was used
to evaluate the amount of energy consumption and production power of
the process and optimize this design.
Fig. 10. Gas cycle unit. In addition, Fig. 12 shows the ΔTmin by the total cost index target.
This value is based on the system flows’ data, the system’s default
in stream 76. The power consumption in this unit is 9.82 MW. This flow constants to calculate the equipment’s cost (heat exchanger), and energy
enters the combustion chamber (COMBUST) with natural gas (St. NG). costs (utility services). The temperature difference of each connection
The operating conditions are 1600 ◦ C and 10 bar. Stream 77 enters the between cold and hot streams should not be less than ΔTmin. Also, the
GT turbine, and the pressure reaches 1 bar again, producing 32.51 MW minimum difference occurs only at one point, called the pinch point.
of power. The turbine’s output (St. 78) reached a temperature of 892 ◦ C Based on the results from the figure below, it can be seen that the
and entered the HRSG unit. This unit works as a converter that during minimum optimum temperature will occur at ΔTmin = 10 ◦ C. The
heat transfer, the temperature of stream 63–2 reaches 475 ◦ C. The calculated operating cost at his temperature is 2.77 M$ (~0.445 cost/s).
temperature of this outlet flow must be reduced before entering the The target equipment’s cost is calculated by considering Eq. (14).
Absorber tower, and on the other hand, the temperature of the oxygen The considered constants are shown in Table 3.
entering the calciner must also be increased. Therefore, to increase the (( )C*Nshells )
temperature of the oxygen stream 80, this flow transfers heat with the A
CapitalCost(S) = a + b (14)
stream 57–1, and its temperature decreases. Therefore, the existing cold NShells
stream of nitrogen is used to reduce the temperature of this stream, and
finally, the rest of the required cooling is provided through a cooler (C- Where A is the targeted area of the entire network, Nshells is the number
07). of target shells, and a, b, and c are constants determined according to the
materials used in the equipment construction. Due to the lack of infor­
mation, software defaults for these constants have been considered. In
Carbon dioxide compression this equation, the values of A and Nshells are obtained through the
balanced combination curve (BCC) diagram analysis. So that in each
Fig. 11 shows the carbon dioxide compression unit. Peng Robinson enthalpy distance, the values of the area and the number of shells are
equation of state has been used to simulate this unit. A 4-stage obtained, and then they are added together to be calculated for the
compressor is used to compress carbon dioxide steam, leaving the sys­ entire network, which is called targeted values. Performing these cal­
tem at a pressure of 150 bar, a temperature of 45 ◦ C, and a purity of 99.5 culations is very heavy and time-consuming, and the software obtains
wt%. this amount. Fig. 13 shows the BCC curve resulting from this design at
ΔTmin = 10 ◦ C.
Energy analysis and optimization The design of the heat exchanger network by pinch technology
consists of two stages: targeting and design. In the targeting stage, the
As energy costs increase, innovative solutions must be developed to minimum energy and the required area of the network are determined
offset these costs. Energy evaluation using pinch analysis is a tool to before the design, and the more accurate the method used in this step is,
investigate thermal integration between processes, which can be used to the more accurate economic calculations and evaluation of the design
evaluate efficiency [27]. In a pinch analysis, streams that need to be will be possible before the design and to reach the optimal design with
heated are paired with streams that need to be cooled. Heat exchangers minimum cost. The minimum required area of the network is also
are placed between these flows, which form a heat exchanger network of calculated after determining the required energy of the network in the
different flows. With pinch analysis, it is possible to theoretically specified ΔTmin. The target area is the minimum amount of heat transfer
calculate the minimum possible external heat or external cold source area required for hot and cold streams in a heat exchanger network to
requirement for a heat exchanger network. It is also possible to deter­ achieve specified temperature values.
mine the amount of heat transferred inside the network [28]. During this It is evident from the GCC diagram depicted in Fig. 14 that there is a
analysis, different curves are created from which the system can be process pinch point at the intersection of the graph with the vertical axis,
analyzed differently. From the composite curve (CC) diagram, the known as the shifted temperature (94.6 ◦ C). The hot and cold temper­
ature shift can be calculated by applying (±ΔT2min ) to this shifted tem­
perature. Hot (102.4 MW) and cold (20.15 MW) utilities are distributed
above and below this point on the diagram, respectively. It’s clear from
the diagram the total amount of consumed hot and cold utilities. The
primary purpose of the GCC diagram is to identify utility pinch points
when using more than one hot or cold utility to meet the energy re­
quirements of the entire thermal network and specify the exact amount
Fig. 11. Carbon dioxide compression unit. of each utility, resulting in a more efficient network design with precise

9
Z. Zolfaghari et al. Energy Conversion and Management: X 21 (2024) 100489

Fig. 12. Determining the minimum optimal temperature.

cold composite curves is called the process pinch point, as it is shown on

Table 3
the diagram. The area to the right of this point is called the heat sink
Values of constants used in the design.
since the hot utility is used there to compensate for the energy deficit.
constants value Furthermore, the remaining area to the left of this point is related to the
a 1000 heat source, and the distribution of cold utility is conducted there to
b 800 receive the energy surplus. The area between the hot and cold composite
c 0.8
curves on the diagram demonstrates the total recovered energy
ROR 10 %
PL 5 years
throughout the network (176.58 MW). It must be taken into consider­
ation that heat exchangers with the largest heat transfer areas are placed
adjacent to the process pinch point since the minimal temperature dif­
energy distribution throughout. ference within the streams occurs in this area. Therefore, the network
The CC diagram proposed in Fig. 15 comprises the hot and cold design in this section must be carried out accurately since a wrong
process streams, so-called composite curves, indicated separately, and it stream match would contribute to a less efficient network design.
is used to calculate other types of elements in the whole network Needless to say, ΔTmin between two curves guarantees a technically and
compared to the CC diagram illustrated in Fig. 14. The total amount of economically feasible heat exchanger network [30].
required hot and cold utility can solely be calculated, and the specific The green arrow shows the amount of internal thermal energy that
amount of each utility, through using more than one utility, cannot be can be easily recovered by using heat exchangers and thus reducing the
calculated from this diagram. The minimal distance between the hot and need to use external sources.

Fig. 13. Balanced Combination Curve.

10
Z. Zolfaghari et al. Energy Conversion and Management: X 21 (2024) 100489

Fig. 14. GCC diagram of heat exchangers network.

Fig. 15. CC diagram of heat exchangers network.

Results and discussion design spec tool to gain less O2 flow rate with high mass purity. The
results illustrated that the O2 flow rate was reduced by 36.65 %, from
The main focus of this research has been on the design and 58.5 ton/hr to 37.062 ton/hr. However, this reduction in O2 flow rate
improvement of the DAC plant. Based on the results reported in this causes a bit more heat requirement in the calciner for about 0.34 % to
study [26], the CO2 mass purity exits the compression phase was about have the calcium carbonate decomposition reaction occur because it is
83.3 % because of excess O2 and a tiny amount of N2, which entered the an endothermic reaction. However, it significantly affects CO2 purity
calciner unit to produce the power requirement of the calcium carbonate increase and ASU power requirement reduction. This can be a limitation
decomposition reaction to calcium and CO2. Excess O2 in the calciner of this process which by O2 flow rate reduction in the calciner, the heat
unit cause more power consumption in the ASU because with more O2 requirement of this unit is increased, but to have high CO2 purity, it
separation in this unit, more flow rate of air must be compressed. To should happen. This energy increase in the calciner unit can be fulfilled
have a high purity of CO2 in terms of mass fraction, first, the O2 mass by other solutions such as using renewable energies rather than the hot
flow rate and purity requirements have been achieved by sensitivity utility. This reduction in the flow rate of the exited stream from the
analysis in the Aspen Plus, then by the design of ASU unit beside this calciner unit also causes less energy requirement in the CO2 compression
process beneath specific thermodynamic conditions, the O2 needed was part.
obtained. The energy performance of this has been examined in comparison
There was essential to reduce the airflow rate in the ASU by using the with other studies. Table 4 shows DAC technology’s electricity and heat

11
Z. Zolfaghari et al. Energy Conversion and Management: X 21 (2024) 100489

demand based on the available literature. As can be seen, the heat de­

0.558177

5.834087

2.891646
mand to supply the thermal energy required by the system (mainly

24.18368

52.90859
25.15531

32.57457
0.90455

0.79815

145.8088
supplied through natural gas in the calciner and combustion tower
units) is in the range of 1420–2250 kWh/t-CO2. Also, the electricity

MW
demand for this technology is estimated in the range of 2366––2790
kWh/t-CO2. The electrical energy requirement of the system comes from

HE-01
HE-02
HE-03
HE-04
HE-05
HE-06
HRSG
C-05
C-06
the power required by the compressors, air blowers, and CO2 compres­

Unit
sion. Carbon Engineering published material on its website in 2018 that
included the use of a system that was entirely powered by electricity and

6.42177648
required a total of 1500 kWh/t-CO2 for electricity and heating demand.

157.254217
150.832441
The published research of Keith et al. shows a significant improve­
ment in supplying the energy demand of technology and presents three

MW
different scenarios. In the first scenario, the required thermal energy and
electricity are generally provided by natural gas, steam turbine, and gas

176.5792
turbine (8.81 GJ of natural gas or 2450 kWh/t-CO2). While in the second
scenario, the required electricity is supplied from the grid, and the gas

Unit

H-02
HX-01
turbine is removed. In this case, the energy consumption is 5.25 GJ of
natural gas and 366 kWh of electricity. While in the third scenario, the
CO2 compression unit is removed, and it is assumed that the produced

1.32096244
2.44675817
4.37635112

9.38338766

4.07118503
3.66387703
4.38417682
8.94354827
69.5592795
19.1520923
4.4795622

131.781180
carbon dioxide is freely available, and as a result, the costs of the
compressor and its electricity demand are avoided.
Compared to the previous studies, the energy analysis of the current

MW
study shows that considering the ASU section and CO2 compression, the
system’s electricity demand will be 343 kWh, and the thermal energy

102.4357291
Heat Recovery
demand will be 1455 kWh (5.24 GJ). which will be discussed in this
section.
In this research, the energy required for the process, the energy

Unit
C-01
C-02
C-03
C-04
C-07
C-08
C-09
C-10
C-11
C-12
C-13
consumption of the units, energy production, and hot and cold utilities
before and after network optimization are summarized in Table 5. It is
considered that the system’s total power is generated from the turbines Hot Utility Consumption
used in the process. Therefore, the first column shows the amount of
power produced by steam and gas turbines. Based on the results,

34.85978896
9.82428912
3.99321167
4.35281965
4.35110319
0.07394771
0.00069238
0.14469729
0.16720847
3.57489052
3.40555619
3.33382371
3.08477057

45.5070105
approximately 1.344 MW of electricity is produced from EXP-01 in the
ASU part, and 15.631 and 4.598 MW of power are provided in the steam

9.2
cycle part and mainly 32.50 MW in the gas cycle part. In total, 54.08 MW
MW

of power is produced in the system, which, taking into account the air
compressor consumption and providing the energy consumption of this
Cold Utility Consumption

unit, the net power produced by the power plant will be 42.28 MW. The

20.14882627
noteworthy point is the use of the EXP-03 turbine, which has produced
approximately 4.59 megawatts of power in the process using the output
steam of the slaker unit. This power can also be used in the required
Unit

COMP-01
COMP-02
COMP-03
COMP-04
BLOW-S1
BLOW-S2

P-02
P-03
P-04

Air contactor
AIR-COMP

BLOW-S3
P-01

parts of the system and prevents unnecessary waste of energy.

The energy consumption column shows the energy consumption of
air compressor units, ASU section blowers, pumps, CO2 compression
section compressors, and air contactors. The energy consumption of the
air contactor unit is considered based on reference information. In total,
Power Consumption

the approximate unit consumption of the air compressor is MW 9.8,

84.71039173

while the energy demand of the air blowers will be MW 12.7. Also, the
1.344981

4.598858

21.10326
15.63167

32.50894

54.0844

highest power consumption is in the CO2 compression unit, which re­

Annual consumption and energy production of the system.

quires 13.4 MW. The pumps used in the system are about 0.38 MW; in
MW

fact, they use less than 1 MW of electricity. The cold Utility consumption
Sum of values after optimization at ΔTmin = 10 ◦ C

Table 4
The energy required for the HT DAC system.
aqueous solution energy demand reference
Reducing energy consumption (%)

Electricity (kWh/t-CO2) Heat (kWh/t-CO2)

NaOH 440 1678 [8]

NaOH 764 1420 [9]
NaOH 1199 2461 [10]
NaOH 494 2250 [13]
energy saving (%)
Power Production

NaOH 2790 – [17]

KOH 1500 – [31]
KOH – 2450 [18]
KOH 366 1458 [18]
EXP-01
EXP-02
EXP-03
Table 5

KOH 77 1458 [18]

Unit

sum
GT

KOH 343 1455 This study

12
Z. Zolfaghari et al. Energy Conversion and Management: X 21 (2024) 100489

column shows the system’s cooling unit consumption. Coolers are used effectively, which can significantly reduce system costs. The results of
in the system to cool and reduce the temperature of the flows. The plant system optimization considering ΔTmin = 10 ◦ C can be seen in the table.
in this research consumes a total of 131.781 MW of energy. The highest If the cooling demand can be satisfied by a conventional cold flow, the
power consumption is in C-08. The output flow from the EXP-02 turbine heating demand that is not satisfied by internal heat recovery must be
enters the cooler at a temperature of 100 ◦ C and a pressure of 1 bar, supplied from an external source.
leaving it as a saturated liquid at 50 ◦ C. The heat transfer during this After optimization, the energy consumption of cold sources
cooling is approximately 69.55 MW. decreased to 84.7 % and reached 20.14 MW. At the same time, 18.03
The consumption of each of the heaters is also shown separately in MW of the system’s cooling needs can be supplied by cooling water and
the Hot Utility Consumption column, which in total uses 157.254 MW of 2.118 MW by refrigerant (cooling water and refrigerant are from two
energy in these two units. H-02 unit has the highest consumption of external cold heat sources). However, this amount has reached 102.4
heating energy. This unit increases the flow temperature from 60 ◦ C to MW with a decrease of 34.85 % for hot sources (an external source of
300 ◦ C to heat the incoming flow to the SUMP unit. The heat recovery Fired Heat has been used to provide heating consumption). Also, the
column shows the exchangers. In total, MW 145.8, heat transfer occurs amount of energy recovery has reached 176.57 megawatts, with an in­
between the processes in which HE-04, HRSG, and HE-05 heat ex­ crease of 21.1 % in energy saving.
changers have the highest heat recovery capability, respectively. According to the said content, the network of existing heat ex­
The important thing in this table is the difference between the total changers has two external cold heat sources; for this reason, it can be
production power and the system’s total power consumption. 8.577 MW seen that the system has two process pinch points and utility pinch
of excess electricity produced can be sold to the power grid to points. The network design of heat exchangers, along with the areas
compensate for part of the system’s cost needs, and on the other hand, it above the pinch and below the pinch and the pinch points, are shown in
prevents the production of the same amount of electricity in the grid and Fig. 16.
prevents exceeding emission of carbon dioxide. The pair of blue dots represent the cooler, the pair of red dots
Pinch analysis is used to optimize energy recovery and minimize represent the heater, and the pair of white dots represent the heat ex­
energy consumption. The pinch point occurs at the closest point between changers. Thus, 7 coolers, 4 heaters, and 20 heat exchangers have been
cold currents and warm currents. The energy from the system’s facilities used in the network.
can be significantly reduced by designing around this point. Minimizing Table 6 below shows the designed network’s energy and surface area
energy consumption reduces the size or number of heat exchangers ratio in relation to the determined target values. The heating and cooling

Fig. 16. Network design of heat exchangers.

13
Z. Zolfaghari et al. Energy Conversion and Management: X 21 (2024) 100489

energy consumption of the network has been exactly in line with the Table 6
target values due to compliance with the rules of thermal integration. Comparison of target and designed values.
Also, the number of network heat exchangers has increased by 3.3 % Target Current Deviation due to the target
(one converter) from the targeted number of heat exchangers due to the values network values (%)
optimal simultaneous design. According to the values, it can be seen that Heating (MW) 102.4 102.4 0
the designed level is 8.8 % higher than the targeted level (this number Cooling (MW) 21.15 20.15 0.047
should be below 10 % according to the existing reference [32]). The Number of heat 30 31 0.033
table results show that the energy needs have been satisfied with the exchanger
Total area (m2) 5.07 × 104 5.525 × 104 0.088
desired thermal network due to the optimization and thermal recovery.

Conclusion Appendix A. Supplementary data

DAC technology can potentially be an essential option against Supplementary data to this article can be found online at https://doi.
climate change. This technology is in its early stage, and current costs org/10.1016/j.ecmx.2023.100489.
are alarmingly high, making deployment very difficult. Different areas
in the DAC process can significantly reduce costs with its progress. Ad­ References
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