Applied Energy 280 (2020) 116016

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Applied Energy
journal homepage: www.elsevier.com/locate/apenergy

The potential of molten metal oxide sorbents for carbon capture at high
temperature: Conceptual design
Cameron Halliday , T. Alan Hatton *
Department of Chemical Engineering, Massachusetts Institute of Technology, 77 Massachusetts Avenue, Cambridge, MA 02139, United States

H I G H L I G H T S

• Molten sorbents provide an efficient route towards low cost carbon capture.
• Unique integrated plant configuration enables efficient acid gas capture, too.
• Energy penalty could be as low as 6% points with around 90% CO2 capture.
• Cost of CO2 avoided $34/tonne ($18–56/tonne), 38% lower than amines (27–50%).

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

Keywords: Molten metal oxides represent a new opportunity for climate change mitigation through carbon capture. This
Carbon capture study presents a conceptual coal fired power plant design that utilizes these liquid phase sorbents for high
Molten sorbents temperature CO2 capture coupled with the simultaneous removal of other acid gases. To effectively recover heat
High temperature
from the process both the absorber and desorber are located within the boiler and steam is used for
Conceptual design
Preliminary economic analysis
near–isothermal regeneration of the sorbent. The potential thermodynamic opportunity was evaluated through
Process simulation process simulation, with results indicating molten sorbents could outperform the state-of-the-art amine-based
systems for CO2 capture. An energy penalty as low as 6% points was projected for systems using molten sorbents,
half that for the amine system. An initial economic evaluation confirmed the benefits of molten sorbents; for the
optimized design, levelized cost of electricity increased 39% (25%–49%) relative to that for the power plant
without carbon capture. The expected cost of CO2 avoided was $34/tonne ($18/tonne to $56/tonne) which is
38% (27%–50%) lower than that for the amine process and competitive with the social cost of CO2. Challenges
were identified with future work proposed and justified by the opportunity to mitigate climate change at a lower
cost than current systems allow.

either sequestration in the subterranean environment [7], or utilization

1. Introduction
The need to reduce CO2 emissions and address climate change con­
flicts with the industrial goals to maintain the prosperity of our societies
[1]. Electricity generation from coal and natural gas combustion pro­
duces large quantities of CO2 [2], as do hydrogen synthesis [3], cement
production [4], and metals smelting [5]. Carbon capture and storage
represents the set of technologies that enable cheap carbon based
feedstocks to be used in these industries while meeting CO2 emission
reduction targets [6]. Carbon capture and storage involves separation of
CO2 from industrial process streams, transportation to point of storage,
and subsequent exclusion from the atmosphere. Storage may be through
in industry [8]. Thermodynamic considerations and commercial de­
mand limit CO2 utilization opportunities [9], although small markets
may provide a useful revenue stream for promising initiatives [10].
Generally, a thermodynamic penalty will occur when carbon capture is
implemented. The goal within the field is to minimize this energy pen­
alty and ultimately minimize the cost of abating CO2 emissions [11]. If
abatement costs below the social cost of CO2 can be demonstrated,
implementation of carbon capture and storage could be rationalized
economically, and be convenient for many different industrial sectors
that use fossil fuels. Since CO2 capture costs are an order of magnitude
greater than transport and storage expenses [12], substantial attention
and research has been given to the development of innovative capture

* Corresponding author.
E-mail address: tahatton@mit.edu (T.A. Hatton).

https://doi.org/10.1016/j.apenergy.2020.116016
Received 9 August 2020; Received in revised form 4 October 2020; Accepted 9 October 2020
Available online 21 October 2020
0306-2619/© 2020 Elsevier Ltd. All rights reserved.
C. Halliday and T.A. Hatton Applied Energy 280 (2020) 116016

Nomenclature MW Nominal Net Electrical Output (MW/year)

OPEX Operating Expenditure
ASC Advanced Super Critical PA Primary Air
BECCS Bioenergy with Carbon Capture and Storage PE Purchased Equipment
BFW Boiler Feed Water r Discounted cash flow rate (%)
BFWH Boiler Feed Water Heater SCR Selective catalytic reduction
BFWP Boiler Feed Water Pump SPECCA Specific Primary Energy for CO2 Avoided (MJ/kg)
CAPEX Capital Expenditure SRK Soave-Redlich-Kwong
CEPCI Chemical Engineering Plant Cost Index (%) t Specific year
CF Capacity Factor (%) T Plant lifetime (years)
CW Cooling Water TCR Total Capital Requirement
EOR Enhanced Oil Recovery TOC Total Overnight Cost
EPC Engineering Procurement and Construction V’ Vapor flow rate on CO2 basis (mol/s)
FCF Fixed Charge Factor (%) X Liquid phase mole ratio (mol/mol)
FDA Forced Draft Air Y Gas phase mole ratio (mol/mol)
FGD Flue Gas Desulfurization
FWH Feed Water Heater Subscripts
HP High Pressure CCS with carbon capture and storage
ID Induced Draft e Electrical
IP High Pressure min Minimum
L’ Liquid flow rate on CO2 basis (mol/s) pt Point
LCOE Levelized Cost of Electricity ($/MWh) Ref Reference
LHV Lower Heating Value (MJ/kg) t Thermal
MEA Monoethanolamine

technologies to reduce these costs [13].
A large number of sorbent materials have been explored in the
literature [14,15]. However, recent reports have identified a new class
of materials, molten metal oxides, uniquely positioned as liquid phase
sorbents able to capture CO2 at high temperatures (around 600 ◦ C) [16].
Molten metal oxides have been studied as carriers of charge in advanced
battery and fuel cell technologies, and as carriers of heat in concentrated
solar and next generation nuclear power plants [17]. As carriers of CO2
these materials exhibit many advantages over traditional solvents
including high capacities, fast kinetics, and excellent cyclic stability. The
CO2 capture performance of a number of molten metal oxides has been
investigated, with the lithium–sodium borate (Li0.5Na0.5)xB1–xO1.5–x (x
= 0.75) identified as a strong candidate for practical designs [18]. The
maximum CO2 loading was found to be around 8 mmol/g, with enthalpy
of reaction 212 ± 13 kJ/mol, and effective CO2 diffusion coefficient on
the order of 10-9 m2/s. In terms of physical properties this sorbent has a
melting point of ~500 ◦ C, a density of around 2 g/cm3, and exhibits
shear thinning behaviour [16]. In addition to CO2, the molten sorbents
interact with other acid gasses, notably SOx and NOx [19], that are
typically present alongside CO2 in industrial emissions, providing an
opportunity to capture multiple acid gasses simultaneously [19]. It was
also shown that steam can be used as a sweep gas for the efficient
regeneration of the molten sorbents under isothermal, or near-
isothermal, conditions [20].
Here it is proposed that molten sorbents can reduce the thermody­
namic and economic cost of CO2 capture. Central to this supposition is
the concept of efficient heat recovery through high temperature opera­
tion. The role of heat recovery can be understood through consideration
of the differences between operating the capture system at high and low
temperatures, as illustrated in Fig. 1. Three steps, reaction, heat recov­
ery, and separation, describe the majority of industrial processes with
carbon capture. A reactor converts a carbon-based feedstock into a

Fig. 1. Block diagram showing carbon capture and associated energy flows with (a) separation at low temperatures (b) with separation at high temperatures.

2
C. Halliday and T.A. Hatton
valuable product, a heat recovery step converts hot exhaust gasses into
useful energy (for example driving a steam cycle), and a separation step
prevents the release of CO2 into the atmosphere.
Separation involves a reaction in which CO2 is captured by the sor­
bent in a sorber (generically an absorber or adsorber) and released in a
desorber, where the sorbent is regenerated and a high purity CO2
product is produced. A significant portion of the plant’s useful energy
output is required to regenerate the sorbent in the desorber. The reaction
of CO2 with the sorbent is reversible, such that the overall enthalpy of
reaction captures both the energy generated in the sorber and the energy
required for the desorption. Effective utilization of the energy generated
in the sorber is expected to increase efficiency, reduce the energy pen­
alty, and lower the cost of carbon capture.
Amines [21], specifically monoethanolamine (MEA), represent the
state-of-the-art in the field of carbon capture. These materials operate at
low temperatures in the sequence reaction–heat recovery–separation,
Fig. 1(a). Low temperature designs are inherently limited by the
enthalpy of reaction. The heat generated in the sorber manifests itself as
low-quality heat, which, from Carnot’s theorem, cannot be used to
generate useful energy. Most proposed sorbents operate in the same
sequence as amines, for example chilled ammonia [22], ionic liquids
[23], and amino acids [24], all of which are limited in part by inefficient
heat recovery. In an attempt to reduce the energy penalty, materials that
operate at high temperatures have been proposed [25]. When the sep­
aration is carried out upstream of the heat recovery unit at high tem­
peratures, Fig. 1(b), the temperature of the capture unit is maintained by
the flow of hot exhaust gasses, typically at 500–700 ◦ C. The exothermic
interaction between sorbent and CO2 generates high-quality heat that
may be passed through the heat recovery system and recovered along­
side the hot exhaust gasses. Likewise, the hot CO2 product generated in
the desorber contains valuable energy that may be recovered prior to its
compression and export [26]. In this way, the energy requirement re­
duces to the entropy change of separating two species, the thermody­
namic minimum [27]. To realize the benefits of separating CO2 from
other gasses close to the thermodynamic minimum energy of separation
requires sorbents that operate under the harsh conditions upstream of
the heat recovery system, for example inside the boiler. The calcium
looping process exploits capture at high temperatures [28], as do many
other solid oxides that rely on similar principles [29]. Calcium oxide
(CaO) has the advantage of low cost and extremely high capacities for
CO2 [30]. Despite strong progress at the pilot scale [31], and the ther­
modynamic advantage of high temperature operation, three factors have
limited the ability of calcium looping to outperform the amine process.
Firstly, sintering of solid oxide particles over many cycles places a heavy
burden on the system. As particles aggregate, they lose capacity and
must be replaced continually [32]. Secondly, practical heat recovery
between solid particles in solid–solid heat exchangers remains a chal­
lenge for calcium looping [33]. Thirdly, most designs rely on tempera­
ture swings in the desorber to drive the separation. To generate the very
high ~900 ◦ C temperatures requires oxy-combustion and the associated
cost, both energetic and financial, of an air separation plant.
Molten sorbents are well placed to overcome these challenges as they
combine the benefits of high temperature operation with those of liquid
sorbents. Liquids are inherently immune to morphological degradation
of the kind that limits solid oxides and can exchange heat more effec­
tively than can fluidized solid particles. Very high temperatures can be
avoided by using steam for regeneration and integrating both the
absorber and desorber into the boiler. Costs can be reduced further
through simultaneous acid gas capture. The goal of this work is to
determine the thermodynamic and economic potential of these new
materials to overcome limitations in the state-of-the-art capture tech­
nologies. Should this reveal substantial potential for molten sorbents,
then an understanding and resolution of associated issues will be worth
pursuing. This work proposes a conceptual super critical coal fired
power plant that utilizes the molten metal oxide sorbents for high
temperature carbon capture, incorporating the co-capture of multiple
3
Applied Energy 280 (2020) 116016
acid gasses, co-location of absorber and desorber inside the boiler, and
the use of steam as a sweep gas for regeneration.
2. System configuration
An Advanced Super Critical (ASC) pulverized bituminous coal plant
based on the test case presented by the DECARBit project [34], was
taken as the reference case. This represents a state–of–the–art coal fired
power plant without carbon capture. A schematic is shown in Fig. 2(a).
On the boiler side, air <1> is pre–heated by exiting flue gas and split
into Forced Draft Air (FDA) <2> and Primary Air (PA) <3>, with the
primary air used to carry fluidized coal into the boiler <4>. The com­
bustion of coal in air produces hot flue gasses and ash; bottoms ash <5>
is collected at the base of the boiler while fly ash is carried with the hot
flue gasses to the outlet of the boiler <6>. Selective catalytic reduction
(SCR) reduces NOx emissions through ammonia addition. The flue gas
passes the air pre-heater <7> and enters the bag house, where fly ash
<8> is separated from the stream. An induced draft fan maintains flow.
The flue gas passes a wet flue gas desulfurization (FGD) system to treat
SOx and generate gypsum, before exiting the stack <9>.
On the steam side High Pressure (HP) Boiler Feed Water (BFW)
<10> enters the economiser and is then heated to form steam in the
superheater <11>. Superheated steam enters the HP turbine, generating
electricity and Intermediate Pressure (IP) steam. Part of the IP steam is
extracted to pre-heat the feed water and part returned to the boiler and
reheated <13>. The reheat steam <14> is sent to the IP turbine
generating electricity and Low Pressure (LP) steam, part of which is
extracted <15> and part sent to the LP turbine <16>, generating more
electricity and condensing the steam. Various extractions of LP steam
<17> also pre-heat the feed and are ultimately collected at the
condenser <18>. Condensate <19> is pumped up to pressure <20>,
and pre-heated through a series of LP Boiler Feed Water Heaters
(BFWH). The pre-heated feed is mixed with IP extracts and returning HP
extracts <21> in a deaerator, and then pumped to HP pressure <22>
and passed through a series of HP Boiler Feed Water Heaters (BFWH),
preparing the boiler feed water for the economiser and completing the
cycle. Natural draught wet cooling towers with cooling water <23> and
associated return water <24> provide a heat sink for the plant. On
implementing carbon capture with molten sorbents, Fig. 2(b), a mini­
mum number of changes were made relative to the reference plant. The
CO2 lean molten sorbent <25> contacts the flue gas at a high temper­
ature inside the boiler, capturing CO2 and other acid gasses. The CO2
rich molten sorbent is collected <26> and pumped <27> to the
desorber, also located inside the boiler, where the sorbent is contacted
with steam. Steam strips CO2 from the sorbent leaving a CO2 lean sor­
bent <28>, which is returned to the absorber section to complete the
loop. Both the absorber and desorber are located inside the boiler to
maintain their high operating temperatures; detailed discussion of this
set-up is presented in Section 4 with additional discussion and diagrams
presented in SI1. Solids that form in the melt, notably sulfurous com­
pounds and trapped fly ash, are handled via a slipstream and sorbent
recovery section of the plant. At a high temperature, solids are up-
concentrated through cross-flow filtration and then recovered at low
temperatures. As with the conventional process, lime is used to form
gypsum. The aqueous sorbent is returned to the high temperature
absorber/desorber cycle, where the original sorbent is recovered by
boiling off the water [19]. LP steam en route to the LP turbine is
redirected to the desorber. A heat exchanger superheats the LP steam
<29> and the steam contacts the sorbent, stripping CO2 from the sor­
bent to produce a mixture of CO2 and steam <30>. The mixture is sent
to the LP turbine where the useful energy of the mixture is extracted to
generate electricity and steam is condensed. A separator attached to the
condenser splits the condensate from the wet CO2 <31>, which is passed
to the multi-stage compression train. Upon compression and inter-
cooling, the wet CO2 is dried. This produces various condensate
streams <32> that are returned to the main condensate line and a
C. Halliday and T.A. Hatton
Fig. 2. Simplified process flow diagram showing system configuration of power plant for (a) reference case without carbon capture (b) case with capture using
molten sorbents.
compressed high purity CO2 product ready for export <33>.
3. Modelling basis & assumptions
Process simulation modelling was carried out in ASPEN Hysys v9
considering operation at nominal base-load conditions. The Soave-
Redlich-Kwong (SRK) and ASME Steam fluid packages were used for
the boiler and steam sides, respectively. The material and energy bal­
ances associated with the absorber/desorber system were carried out in
Excel and implemented in ASPEN. For detailed connections and further
explanation of the process simulation modelling, refer to SI2. Technol­
ogy leveling assumptions closely follow those presented in the common
technical framework and ASC test case of the DECARBit project [34].
The proposed with and without carbon capture cases were based on the
same fuel input to a green-field inland plant with natural draught wet
cooling towers. Assumptions in Table 1 were used for both with and
without capture cases, although a small number of parameters required
modification in the capture case.
The following basis was assumed in formalizing the conceptual
4
Applied Energy 280 (2020) 116016
design. The battery limit starts with as delivered material inputs (coal,
air, water, ammonia, limestone) and ends with the flue stack outlet
(limited to 30 ppm SOx and 60 ppm NOx) or at a product’s end of life
(ash disposal, gypsum export, CO2 transport and storage). Bituminous
Douglas premium coal is supplied by rail and milled on site. ISO stan­
dard inland air and water conditions apply. Details are presented under
Material Inputs Table 1. Air is in 18.1% excess of complete combustion.
Primary air flow is double the coal flow on a mass basis for pulverized
fuel transportation with forced draft air making up the remainder. The
boiler operates under a balanced draft, with a leak across the air pre­
heater of 5.5%. Ash generated on combustion of coal comprises 80%
bottoms ash removed by a submerged chain conveyor at the furnace
base and 20% fly ash removed in the bag house by electrostatic pre­
cipitators. Without capture the boiler is equipped with low NOx axial
swirl burners, in–furnace air–staging, and a Selective Catalytic Reduc­
tion (SCR) plant for NOx reduction. Flue gas is kept above 120 ◦ C in the
air-preheater to exceed the dew point of sulfuric acid and avoid asso­
ciated corrosion issues. A downstream Flue Gas Desulfurization (FGD)
plant removes SOx to meet the 30 ppm limit and cools the stream to
C. Halliday and T.A. Hatton Applied Energy 280 (2020) 116016

Table 1
Modeling assumptions used in process simulation for both with and without carbon capture cases.
Material inputs Unit Value Process conditions Unit Value

Coal Air fans & preheater

Ultimate analysis Carbon wt% 66.52 Air excess % 18.1

Ash wt% 14.15 Air filter pressure drop kPa 1.0
Moisture wt% 8.00 Primary air pressure kPa 111.0
Oxygen wt% 5.46 Forced draft pressure kPa 106.0
Hydrogen wt% 3.78 Induced draft pressure drop kPa 10.0
Nitrogen wt% 1.56 Air preheater leak % 5.5
Sulfur wt% 0.52 Boiler Feed Water (BFW)
LHV MJ/kg 25.17 LP BFW pump pressure bar 20
Air HP BFW pump pressure bar 300
Temperature ◦
C 15.0 Feed Water Heater (FWH)
Pressure kPa 101.3 Min approach temperature C
◦
3.0
Relative humidity % 60.0 Exit temperature difference C
◦
10
Composition N2 mol% 77.30 Hot side pressure drop % 8.0
O2 mol% 20.74 Cold side pressure drop % 3.0
H2O mol% 1.01 Steam turbine
Ar mol% 0.92 HP Inlet pressure bar 270
CO2 mol% 0.03 Temperature loss ◦
C 2.0
Water Inlet temperature ◦
C 600
Temperature ◦
C 18.2 Outlet pressure bar 64
IP Inlet pressure bar 60
Power Requirements Unit Value Temperature loss ◦
C 2.0
Compression Efficiencies Inlet temperature ◦
C 620
Air Fans (polytropic) % 85.0 Outlet pressure bar 12
Water Pumps (adiabatic) % 70.0 LP Steam pressure drop % 7.0
CO2 Compressor (polytropic) % 80.0 Outlet pressure kPa 4.8
CO2 Compressor final (polytropic) % 75.0 Cooling Water (CW)
CO2 & Sorbent Pump (adiabatic) % 75.0 CW pump pressure bar 3.0
Driver efficiency % 95.0 Flue & Ash Conditions
Turbine efficiencies Flue temperature (Pre FGD) ◦
C 120
Steam turbine (adiabatic) % 89.0 Flue temperature (Post FGD) ◦
C 85
Mechanical efficiency % 99.6 Fly/bottoms ash split – 20/80
Generator efficiency % 98.5 Bottoms ash temperature ◦
C 400
Auxiliaries CO2 conditions
Coal handling kJe/kgCoal 50 Inter-stage cooling ◦
C 28
Ash handling kJe/kgAsh 200 Stage pressure drop % 1.0
Flue gas desulfurization kJe/kgSOx 5340 Export pressure bar 150

85 ◦ C. Auxiliary power requirements including coal handling, ash

Table 2
handling, and FGD are expressed as intensive properties, under Power
Parameters used for base case with carbon capture.
Requirements Table 1.
The steam cycle is a two-pass single reheat system with 600 kg/s Base case parameters Unit Value
supercritical live steam at 300 bar and 600 ◦ C, reheat steam at 620 ◦ C, Capture & release conditions
and a condenser pressure of 4.8 kPa. Assumptions around pressure Absorber temperature ◦
C 600
drops, temperature losses, and other conditions are given under Process Desorber temperature ◦
C 650
Absorber pressure drop kPa 12
Conditions Table 1. Extraction points from the HP, IP, and LP turbines Desorber pressure drop % 10
provide regenerative heating of the boiler feed water through four LP Process conditions
Boiler Feed Water Heaters (LP BFWH), a deaerator, and three HP Boiler Condenser pressure kPa 8.2
Feed Water Heaters (HP BFWH). HP and LP boiler feed water pressures 1st Compression pressure kPa 19.0
Reheat temperature C 550
and Feed Water Heater (FHW) design parameters are given under Pro­
◦

Flue gas temperature ◦

C 70
cess Conditions Table 1. The efficiencies assumed for equipment are Sorbent properties
given under Power Requirements Table 1. The driver efficiency was Specific heat capacity kJ/kg.K 1.5
applied on top of the efficiencies of fans, pumps, and compressors. The Heat of reaction kJ/mol 212
mechanical and generator efficiencies were applied on top of the steam
turbine efficiency, which was assumed to be the same for HP, IP, and LP
The Process Conditions Table 2 for the case with carbon capture
turbines.
override those on Table 1. These include the reheat temperature,
The base case parameters for the case with carbon capture are pre­
condenser pressure, and flue gas temperature which are related to the
sented in Table 2; sensitivity to these parameters is discussed in Section
absorber/desorber system, CO2 compression train, and handling of other
6. A comprehensive discussion of the capture and release conditions is
acid gasses, respectively. In the with capture case the reheat tempera­
presented in Section 4. In the base case near–isothermal operation was
ture was reduced from 620 ◦ C 550 ◦ C to make room for the absorber and
considered, assuming the absorber operates at 600 ◦ C, the desorber at
desorber as discussed in Section 4.
650 ◦ C, a pressure drop of 12 kPa across the absorber, and a 7% pressure
Within the compression train five compressors with intercooling to
drop across the desorber. The approach temperature in the sorbent and
28 ◦ C and a 1% pressure drop across each stage bring the captured CO2
steam heat exchangers were assumed to be 5 ◦ C and 20 ◦ C, respectively.
from the condenser up to 80 bar with a CO2 pump to reach the final 150
Sorbent properties based on those of the lithium–sodium borate
bar for export of high purity CO2. Water contents at the ppm level are
(Li0.5Na0.5)xB1-xO1.5-x (x = 0.75) were discussed in Section 1 and taken
required for CO2 export, which are met by a triethylene glycol dryer (not
from literature [16]. The specific heat capacity was assumed to be
modelled) located near the end of the compression train [36]. A
within 50% that of the sodium borate NaxB1-xO1.5-x (x = 0.75) [35].

5
C. Halliday and T.A. Hatton
standard staging from 1 to 4.35 to 18.65 to 80 bar was considered for the
last three compressors in the train [34]. The first two compressors in the
train are not standard items, and maximizing for overall efficiency as
discussed in Section 6, identifies the optimal pressures to be 8.2 to 19.0
to 101.3 kPa. Hence, the condenser pressure was taken as 8.2 kPa in the
base case with capture and 4.8 kPa in the case without capture.
The handling of other acid gasses (SOx and NOx) differs significantly
between the with and without carbon capture cases. It was reported that
the interaction between NOx and the molten sorbent was similar to the
interaction with CO2 [19]. Captured NOx formed liquid products and
was released on a partial pressure swing, NOx will therefore contaminate
the CO2 product stream. At the conditions considered in this study,
release takes the form of NO, NO2, O2, and/or N2 and represents ~500
ppm in the CO2 product. Upstream NOx abatement technologies remain
in place for the with capture case including low NOx axial swirl burners
and in–furnace air–staging but the downstream Selective Catalytic
Reduction (SCR) plant is removed. For modelling purposes complete
removal of NOx from the flue gas was assumed. Detailed design of the
absorber and consideration for site specific factors would identify
whether emission standards are met or if the downstream SCR plant
would need to remain in place.
It was also reported that molten sorbents capture SOx in addition to
CO2 [19], but in this case solid products formed in an irreversible re­
action. The formation of solid products introduced a very strong driving
force for capture. Furthermore, SOx competitively displaced captured
CO2 in the melt so very high capture efficiencies were predicted. Absent
any thermodynamic limitation, a system capturing ~90% CO2 would
capture ≫90% SOx. In the base case with capture, reduction to 5 ppm
SOx, or ~99% removal was considered. On reduction of the SOx con­
centration upstream of the air pre-heater, the sulfuric acid dew point is
reduced. As a result the plant may operate at lower flue gas temperatures
[37]. In the case without capture the flue gas is kept above 120 ◦ C. This
is consistent with the dew point predicted by the Verhoff model for
~430 ppm SOx and 7 mol% H2O, assuming SO3 is 2% of SOx [38]. For
the base case, with removal to 5 ppm SOx the plant could operate at a
flue gas temperature of ~70 ◦ C without corrosion issues. As part of the
sensitivity analysis in Section 6, 1 ppm SOx or 99.8% removal is
considered. This would enable a flue gas temperature of ~55 ◦ C. A case
comparable to conventional FGD with 30 ppm SOx or ~93% removal is
also considered, enabling a flue gas temperature of 85 ◦ C.
In a single pass the solid sulfur compounds that form in the sorbent
represent ~1/2000th of the stream. Therefore solids are not expected to
cause operational issues unless they accumulate. In the proposed design,
a high temperature cross-flow filter upconcentrates a slipstream of
circulating sorbent into a solids rich retentate. This limits the accumu­
lation of solids. At low temperatures gypsum and the sorbent, now in the
aqueous phase after dissolution, are recovered from the retentate with
the sorbent recycled back to the absorber. Since the flow of this stream is
relatively low it was assumed that SOx is extracted, and the sorbent
recovered at high temperatures. In effect the SOx handling system is
integrated into the CO2 capture system, significantly reducing the size of
SOx specific auxiliaries. Conservatively, the energy consumption for SOx
handling was assumed to be the same as for conventional FGD, per
Auxiliaries Table 1, to account for limestone handling etc. It was
assumed that fly ash does not significantly interact with the molten
sorbent in the absorber. However, any solid ash captured will follow
sulfur, as described above, and end up as a constituent of the gypsum
product. There is a possibility of ash causing sorbent degradation, which
would require sorbent replacement. More discussion of operational
challenges surrounding acid gas and solids handling is presented in
Section 8.
4. Absorber & desorber operation
To realize high temperature carbon capture, the absorber and
desorber must be located intimately close to the sources and users of
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Applied Energy 280 (2020) 116016
heat in the plant. In this work integration of the absorber and desorber
within the boiler is proposed. The hot exhaust gasses maintain high
temperatures while the steam cycle prevents the development of
excessively high temperatures. As discussed in Section 1 the heat
generated in the absorption section is comparable to the heat consumed
in the desorption section. If the absorber and desorber sections are
located in close proximity with perfect heat transfer between the two
then isothermal operation could be achieved. In the absence of perfect
heat transfer, the absorber, which generates heat, would operate at a
moderately higher temperature than the desorber, which consumes
heat. However, the absorber and desorber sections could be staggered,
such that the desorber is placed earlier in the path of hot exhaust gasses
and is therefore exposed to a higher temperature than the absorber
located later in the flow path, and therefore exposed to a lower
temperature.
Also integrated into the boiler are superheat and reheat steam bun­
dles, which are located at positions appropriate to the superheat and
reheat steam temperatures. The desorber takes a form similar to that of
the steam bundles, but with internal packing to maximize contact be­
tween counter flowing sorbent and steam. The high absolute pressure in
the desorber (~11 bar) compresses the system such that the desorber fits
inside the boiler despite the large flowrates of steam required. The use of
tubes similar to the superheat and reheat steam bundles maximizes heat
transfer and limits the intrusiveness of the desorber. The absorber takes
the form of a loosely packed column located on the flue gas side amongst
the desorber and steam bundles
The relative positions, and possible overlap, of these four operations
(absorber, desorber, superheat, and reheat) depends primarily on their
desired operating temperatures, see SI1 for more discussion. In this work
six cases were considered. Isothermal operation of both the absorber and
desorber at 550 ◦ C, 600 ◦ C, 650 ◦ C, and near-isothermal operation with
the absorber/desorber temperatures, 550/600 ◦ C, 600/650 ◦ C, and 550/
650 ◦ C. The limits to this approach are discussed in Section 8. The
temperature of the superheated steam remained at 600 ◦ C in the case
with capture, but the reheat temperature was reduced from 620 ◦ C to
550 ◦ C to provide energy and space for the desorber in the hotter section
of the boiler. The reheat could be placed downstream of the absorber if
needed.
Operation at the six sets of temperatures was modelled in ASPEN by
varying the relative flow rates of superheat and reheat steam, as well as
the pressures and flowrates of the regenerative steam extracts. With
knowledge of the flue gas entering the absorber section and the steam
available for desorption the coupled absorber/desorber system was
solved with the aid of equilibrium diagrams. In this Section only two
cases are discussed in detail, isothermal operation at 600 ◦ C and near-
isothermal operation at 600/650 ◦ C. The latter was taken as the base
case with capture. The full set of cases is presented in SI3. Equilibrium
diagrams, presented in Fig. 3 and SI3, plot the mole ratio of CO2 to inert
gas (mostly nitrogen in the absorber and steam in the desorber) in the
gas phase (Y) against the mole ratio of CO2 to liquid (sorbent) in the
liquid phase (X). Equilibrium curves, derived from concentration iso­
therms [18], define the relationship between X and Y at the three tem­
peratures of interest, 550 ◦ C, 600 ◦ C, and 650 ◦ C.
It is instructive to first consider the best possible thermodynamic
case under minimum operating conditions. This is presented for
isothermal operation at 600 ◦ C in Fig. 3(a) but other cases in SI3 follow
the same premise. With isothermal operation, only one equilibrium
curve needs to be considered, the 600 ◦ C curve in this case. Under the
assumption of infinite equilibrium stages in the absorber the CO2 rich
sorbent leaving the bottom is in equilibrium with the incoming CO2
(15.0 mol% CO2). This defines YA and therefore Point A (XA,YA), which
is located on the equilibrium curve, in Fig. 3(a). The sorbent leaving the
bottom of the absorber is the same as the sorbent entering the top of the
desorber, and therefore has the same composition, XA = XB. The steam
cycle defines the amount of LP steam available for the desorption, thus
fixes YB, and therefore Point B (XB,YB). The minimum operating line in
C. Halliday and T.A. Hatton
Fig. 3. Equilibrium diagrams describing operation, with absorber and desorber operating isothermally at 600 ◦ C (a) under minimum operating conditions (b) under
base operating conditions, operating near-isothermally (absorber at 600 ◦ C and desorber at 650 ◦ C) (c) under minimum operating conditions (d) under base
operating conditions (base case).
the desorber corresponds the line tangential to the equilibrium curve.
This defines Point C (XC,YC), since the incoming LP steam contains no
CO2 (YC = 0). The sorbent leaving the bottom of the desorber is the same
as the sorbent entering the top of the absorber, and therefore has the
same composition XC = XD. Again assuming infinite stages and equi­
librium between the CO2 lean sorbent entering the absorber and the CO2
lean flue gas exiting the absorber gives Point D (XD,YD).
The operating line in the absorber is the line that connects Point A
with Point D; the gradient of this line is the ratio of molar flowrates,
inert liquid to inert vapor (L’/V’), in the absorber. The operating line in
the desorber connects Point B with Point C; the gradient of this line is
the molar flowrate ratio, inert liquid to inert vapor (L’/V’), in the
desorber. The McCabe-Thiele method was then used to count off equi­
librium stages [39]. Fig. 3 (a) defines the best possible performance of
the system with infinite equilibrium stages in both the absorber and
desorber and therefore quickly identifies a pinch point (or multiple
pinch points). The working capacity of the sorbent in mmol/g can be
calculated from XB – XC (or XA – XD). The values of YA and YC are the
same in all cases though YB and YD may change. The ASPEN model was
solved iteratively to find YB, since the amount of LP steam available
depends on the CO2 capture efficiency (i.e. YD), and to a lesser extent the
working capacity of the sorbent (i.e. XB – XC). YD is the mole ratio at the
top of the absorber and hence defines the carbon capture efficiency.
Operating on the minimum operating line is unrealistic and requires
an infinite number of stages in both the absorber and desorber. There­
fore, a common assumption was used where the operating line in the
desorber (L’/V’) is 1.4(L’/V’)min [39]. This establishes the base condi­
tions and has a number of effects on the coupled system, which are
explained in SI3. This approach establishes a finite number of stages in
both the absorber and desorber. The result of this process is given in
7
Applied Energy 280 (2020) 116016
Fig. 3(b) for isothermal operation at 600 ◦ C. In short, the working ca­
pacity decreases, and the CO2 capture efficiency reduces, making more
steam available for desorption.
In the base case with capture scenario, near-isothermal operation at
600/650 ◦ C was considered. To understand non-isothermal operation
two equilibrium curves are required, one that defines equilibrium in the
absorber (600 ◦ C) and one that defines equilibrium in the desorber
(650 ◦ C). Fig. 3(c) shows this case under minimum operating conditions,
analogous to Fig. 3(a), where the operating line in the desorber is
tangential to the 650 ◦ C equilibrium curve and the pinch point(s) of the
absorber operating line occur on the 600 ◦ C operating line. The same
procedure used for the isothermal case was used to establish the base
operating conditions in the near-isothermal case; Fig. 3(d) represents
this base case with capture. Near-isothermal operation at 600/650 ◦ C
was taken as the base case because isothermal operation was severely
limited by the low capture efficiency. Better performance was observed
with 550/650 ◦ C, although capture at 550 ◦ C displayed imperfect per­
formance at the bench scale [20].
5. Simulation results
The material stream conditions for the without carbon capture case
and the base case with carbon capture (near-isothermal operation at
600/650 ◦ C) are presented in Table 3. The stream labels correspond to
those used in Fig. 2. The major energy flows and efficiencies of the two
plants are presented in Table 4. The simulation results for the case
without carbon capture are consistent with those of the ACS test case
presented by the DECARBit project [34]. This widely accepted bench­
marking study reproduced the actual performance of a large number of
existing state-of-the-art power plants. Hence the results are fully
C. Halliday and T.A. Hatton Applied Energy 280 (2020) 116016

Table 3
Material stream conditions for reference without carbon capture and base case with carbon capture, stream numbers correspond to labelling in Fig. 1.
Material stream conditions Reference without CO2 capture Base case with CO2 capture

Steam label & description Flowrate (kg/s) Temperature ( C)

◦
Pressure (kPa) Flowrate (kg/s) Temperature (◦ C) Pressure (kPa)

1 Air supply 706.0 15.0 101.3 706.0 15.0 101.3

2 Forced draft air supply 539.2 217.4 106.0 539.2 230.8 106.0
3 Primary air supply 131.5 217.4 111.0 131.5 230.8 111.0
4 Coal supply 65.8 15.0 101.3 65.8 15.0 101.3
5 Bottoms ash 1.9 400.0 101.3 1.9 400.0 101.3
6 Hot flue gas 734.6 294.4 101.3 592.8 294.3 101.3
7 Cooled flue gas 769.9 120.0 101.3 628.1 70.0 101.3
8 Fly ash 7.4 120.0 101.3 7.4 70.0 101.3
9 Final flue gas 761.8 85.0 101.3 620.7 84.4 101.3
10 Hot HP boiler feed water 600.0 284.4 27,840 600.0 284.3 27,840
11 HP steam 600.0 600.0 27,000 600.0 600.0 27,000
12 HP extract (various*) 113.2 N/A N/A 110.3 N/A N/A
13 Reheat steam 500.8 368.9 6400 532.9 368.9 6400
14 IP steam 500.8 620.0 6000 532.9 550.0 6000
15 IP extract (various*) 23.0 N/A N/A 17.0 N/A N/A
16 LP steam 463.8 377.8 1200 489.7 321.7 1200
17 LP extract (various*) 86.2 N/A N/A 117.9 N/A N/A
18 LP extract return 86.2 42.4 156.6 117.9 40.0 64.4
19 Condenser outlet 463.8 32.2 4.8 613.8 30.0 8.2
20 LP boiler feed water 463.8 32.4 2000 472.7 30.0 2000
21 HP extract return 113.2 200.2 1685 110.3 199.5 2970
22 HP boiler feed water 600.0 190.2 30,500 600.0 189.5 30,500
23 Cooling water supply 18,130 18.2 101.3 16,162 18.2 101.3
24 Cooling water return 18,130 29.2 101.3 16,162 29.2 101.3
25 Lean sorbent supply – – – 1680 605.0 101.3
26 Rich sorbent return – – – 1821 600.0 101.3
27 Rich sorbent supply – – – 1821 642.6 1080
28 Lean sorbent return – – – 1680 650.0 1080
29 Sweep steam supply – – – 472.7 630.0 1080
30 Sweep steam return – – – 613.8 650.0 1080
31 Low pressure wet CO2 – – – 199.9 30.0 8.2
32 Condensate (various*) – – – 58.7 28.0 N/A
33 Dry CO2 for Export – – – 141.2 28.0 15,000
* Indicates multiple streams at various conditions, see SI2 for details, total flowrates are given

temperature, enabled by high temperature acid gas removal, and the

Table 4 reduced amount of flue gas exiting the boiler, due to the removal of CO2.
Energy balance for reference without capture and base case with carbon capture.
On the steam side, modest changes in the flows of HP, IP, and LP steam
Energy balance Unit Reference Base case and the conditions of extraction points meet the constraints of the sys­
Fuel input (LHV) MWt 1655.0 1655.0 tem. The sorbent circulates at ~1 m3/s. Compression with intercooling
Steam output MWe 823.0 829.0 gradually reduces the water content of the wet CO2 from ~50%mol to
Auxiliaries (Total) MWe 60.6 169.1 ~3000 ppm with a glycol dehydration unit achieving <500 ppm.
Net electrical output MWe 762.4 659.9
Efficiency %LHV 46.06 39.87
Compression of CO2 was observed to consume over 100 MWe of the
Auxiliaries breakdown plant’s energy, Large quantities of water vapor compressed alongside
Fans Primary air MWe 1.6 1.6 CO2 contribute to the high energy demand.
Forced draft MWe 3.2 3.2 Beyond the overall efficiency, Table 5 presents the key results for the
Induced draft MWe 9.9 10.1
four with capture cases considered in Section 4. SI4 shows the same
Pumps LP BFW MWe 1.4 1.2
HP BFW MWe 29.6 29.6 results for the six sets of temperatures. The absorber and desorber
Cooling water MWe 5.4 4.8 operating conditions are presented alongside the number of theoretical
Condensate MWe – 0.2 equilibrium stages. The number of theoretical equilibrium stages pro­
Sorbent pumps MWe – 1.2 vides a rough guide to the height of packing required. Detailed design is
Other Coal handling MWe 3.3 3.3
Ash handling MWe 1.9 1.9
required to determine the exact height of the absorber and desorber
FGD auxiliaries MWe 3.4 3.7 sections, but as an order of magnitude guide to account for mass transfer
Balance of plant MWe 1.0 1.0 and kinetic limitations, ~1m per stage and an overall stage efficiency of
CO2 compression MWe – 107.3 25% may be considered [39]. The columns would need to be ~12 m in
height, well within the 20–40 m available inside the upper section of the
boiler [40]. This is believed to be a conservative estimate due to the
consistent with the major plant manufacturers. The same cannot be said
sorbent’s rapid kinetics at these high temperatures. The 1.9 mmol/g
for the with capture case, since no plants exist to validate the results.
working capacity of the sorbent is lower than that reported at the bench
Hence, the degree of confidence to be assumed in consideration of the
scale [20]. This is due to the limitations of staged processes and the finite
presented results varies significantly between the two cases. To mitigate
number of equilibrium stages. However, these working capacities
this uncertainty, as few changes as possible were made on implementing
remain high relative to most systems. In the amine system the working
the with capture case, and a sensitivity analysis is presented in Section 6.
capacity is 1.0 mmol/g [34], and the density is halved. Hence, a four-
An energy penalty of 6.2% points was observed in the base case with
fold reduction in sorbent flow is realized along with an associated
molten sorbents. This is primarily attributed to CO2 recompression and
reduction in absorber and desorber volume.
compression. Most material and energy flows were similar between the
In the base case a CO2 capture efficiency of 87.8% was observed,
two cases. On the boiler side the differences are due to the lower flue gas

8
C. Halliday and T.A. Hatton Applied Energy 280 (2020) 116016

Table 5
Key results for reference case without carbon capture and main cases with carbon capture as discussed in Section 4 (right-most column corresponds to base case with
capture).
Main case results Unit Reference Minimum operating conditions Base operating conditions

Absorber temperature ◦
C – 600 600 600 600
Desorber temperature ◦
C – 600 650 600 650
Absorber (L’/V’) mol/mol – 0.77 0.56 1.09 0.78
Desorber (L’/V’) mol/mol – 0.60 0.44 0.84 0.62
Absorber Eqm. stages – – 1.6 1.9 2.8 3.2
Desorber Eqm. stages – – 1.5 1.7 2.8 3.0
Working capacity mmol/g – 2.0 3.0 1.1 1.9
CO2 capture efficiency % 0 88.6 96.7 67.8 87.8
CO2 emissions rate kg/MWh 758.4 100.4 29.3 276.4 107.0
Plant efficiency %LHV 46.06 39.71 39.41 40.71 39.87
Energy penalty %pt – 6.35 6.65 5.35 6.19
SPECCA MJe/kgCO2 – 1.90 1.81 2.13 1.86

close to the 90% target commonly assumed for power plants looking to
implement carbon capture. CO2 capture efficiency was found to be the
output most sensitive to the operating temperature and conditions. For
the base operating conditions, isothermal operation reduced the CO2
capture efficiency to 67.8%, highlighting the benefit of even a modest
50 ◦ C increase in temperature between the absorber and desorber. The
plant efficiency in the isothermal case is higher primarily because less
CO2 needed to be compressed, reducing the electrical demand of the
compression train.
Fig. 4 shows the trade-off between CO2 emissions and plant effi­
ciency for the six sets of temperatures with minimum and base case
operating conditions to give a sense of the possible performance metrics.
For reference, the case without capture and the state-of-the-art tech­
nology that uses amines for low temperature capture are also plotted
[34]. It was observed that the molten sorbents reduce the energy penalty
by around half relative to the amine technology, and in the base case
achieved a comparable level of emissions reduction. The Specific Pri­
mary Energy Consumed for CO2 Avoided (SPECCA), expressed as MJe/
kgCO2 [34], combines emissions and efficiency in a single metric with
lower values representing the more efficient use of carbon based re­
sources, Table 5. The reported SPECCA for amines is over 4 [34], indi­
cating that molten sorbents, with a SPECCA value of around 2, hold
substantial potential for CO2 capture in power plants from a thermo­
dynamic perspective.
6. Sensitivity analysis
It is important to consider the sensitivity of the results to the as­
sumptions and parameters chosen in Section 3. The results in Section 5
reveal that the energy penalty can be largely attributed to the
compression train, in particular the compression from the outlet of the
Fig. 4. Comparison between reference without capture, the state-of-the-art
represented by amines, and various cases with molten sorbents.
condenser back up to atmospheric pressure. The operating pressure of
the condenser and first compressor were design decisions; here the aim
was to maximize the efficiency of the plant. Operating the condenser at
the lowest possible pressure maximizes the useful energy extracted from
the condensing steam. This is why the plant without carbon capture
operates at the low condenser pressures of 4.8 kPa. However, in the case
with capture, operating at this condenser pressure requires recom­
pressing CO2 from a very low initial pressure. It was observed doing so
requires an unreasonably large amount of electrical energy and signifi­
cantly reduces the plant efficiency. Furthermore, the condenser is
limited by the temperature of the available cooling water. Lower pres­
sures reduce the saturation temperature and result in more water vapor
in the wet CO2 stream. As a result, low pressures penalize the system by
sending a greater volume of wetter CO2 into the compression train. After
the first compressor a second compressor takes the stream up to 1 bar
and onto the standardized part of the compression train. The outlet
pressure of the first compressor is therefore unrestricted and was treated
as a parameter alongside the condenser pressure.
A two-dimensional optimization was carried out to maximize the
overall efficiency, balancing the electrical energy produced by the steam
turbines with that consumed by the CO2 compressors. Results are pre­
sented in Fig. 5(a). The optimal efficiency of 39.87% occurred at a
condenser pressure of 8.2 kPa and first compression of 19.0 kPa for the
base case conditions. However, this was sensitive to the CO2 capture
efficiency, which varies substantially across different cases. The less CO2
captured the less the compressors contribute to the plant’s energy pen­
alty and the greater the benefit of operating at a lower condenser
pressure. Therefore, the optimal operating pressures were calculated for
each set of temperatures considered in the cases with capture. These
values were found to lie between 7 and 9 kPa for the condenser pressure
and 15 to 20 kPa for the first compression, and are presented in SI4.
High operating pressures, for example a 30 kPa condenser pressure and
50 kPa first compression, still result in a reasonably high efficiency of
37.6%, but lower pressures substantially penalize the plant.
Sensitivity of the plant efficiency to other parameters, including flue
gas temperature, absorber/desorber pressure drop, and sorbent prop­
erties, is presented in Fig. 5(b). The CO2 capture efficiency remains
unchanged with the five parameters considered. It was assumed in
Section 3 that the upstream removal of SOx to 5 ppm would reduce the
sulfuric acid dew point and enable a flue gas temperature of ~70 ◦ C
without unmanageable corrosion in the air-preheater. Flue gas tem­
peratures of 55 ◦ C and 85 ◦ C, corresponding to SOx of 1 ppm and 30 ppm
respectively, were shown to have a modest effect on efficiency. The
minimum expected pressure drop across the absorber was taken as 10
kPa, the same as the pressure drop across the FGD system in place in the
plant without carbon capture. 12 kPa and 15 kPa were assumed in the
base case and low efficiency case to account for the additional packing
required in the absorber. Likewise, in the desorber a 7% pressure drop
(84 kPa) was assumed in the pipework between IP and LP turbines in the
case without carbon capture. In the base case and lower efficiency case

9
C. Halliday and T.A. Hatton Applied Energy 280 (2020) 116016

the SPECCA. However, neither the efficiency of the power plant nor the
SPECCA is an ideal metric to use in evaluating the potential of a con­
ceptual design. Ultimately, cost determines potential for implementa­
tion. Efficiency and SPECCA are convenient proxies for cost because
they are grounded in thermodynamic arguments and fixed with respect
to time and geography. But they are nonetheless proxies and susceptible
to distortion of the true potential of a conceptual design.

7. Techno-economic considerations

Unfortunately, determination the cost of a conceptual design is full of

uncertainty, particularly at the early stages of technology readiness
[41]. Three techniques can help to manage this uncertainty: technology
leveling, sensitivity analyses, and the clear transparent statement of
assumptions [42].
Technology leveling means that equivalent assumptions were made
for all cases considered. The assumptions made in this work closely
follow the common economic framework and ASC test case presented by
the DECARBit project [34]. The cost of CO2 avoided is the preferred
metric to assess carbon capture technologies. This evaluates the cost of
building a plant with carbon capture over the plant that would have
been built if carbon capture were not implemented, expressed in dollars
per tonne of CO2 [42]. Calculating the cost of CO2 avoided involves
calculating a number of other metrics that are important in their own
right, including the total capital cost (CAPEX), total operating cost
(OPEX), and the Levelized Cost of Electricity (LCOE).
The economic basis and baseline parameters are presented in
Table 6. All economic evaluations were adjusted to the same time (basis
year 2020) and currency (real constant dollars, $). Data that required
conversion were from 2008 and euros (€) to 2020 and dollars ($). A
Chemical Engineering Plant Cost Index (CEPCI) of 600% in 2020 was
assumed (576% in 2008) and an exchange rate of $1.12/€ (in 2020)
[43]. The analysis was done on a real basis (without inflation) with a
discounted cash flow rate of 8% to reflect the average cost of capital.
Techno-economic considerations are particularly sensitive to the dis­
counted cash flow rate, lower and upper values of 4% and 12% were
considered. Economics were carried out on a pre-taxation rate and the
plant salvage value was assumed to cover end-of-life costs.
A top-down-approach was used to estimate the Engineering Pro­
Fig. 5. (a) Overall plant efficiency for various operating pressures along the curement and Construction (EPC) cost of the plant without carbon
compression train (b) sensitivity analysis for parameters used in Table 2. capture based on supplier estimates carried out by the DECARBit project
[34]. Owners costs and contingencies amounting to 15% of the EPC cost
with capture, 10% and 14% (120 kPa and 168 kPa) were used respec­ were assumed in determining the Total Overnight Cost (TOC). Capital
tively to account for the pressure drop across the desorber packing. This allocation in the ratio 20:30:30:20 was assumed over the four-year plant
sensitivity analysis showed that pressure drops across the expected construction period to give the Total Capital Requirement (TCR). 40%
range have only a small effect on the plant efficiency, ~0.2% points. and 65% capacity factors were assumed in the first and second years of
Detailed design is required to understand the pressure drop across the operation followed by an 85% capacity factor for the remainder of the
two sections but this preliminary analysis suggests the effect will be plants 40-year lifetime. This gave a Fixed Charge Factor (FCF) of 8.39%
small.
The properties of the sorbent have no noticeable effect on the plant
efficiency according to the model. The specific heat capacity dictates the Table 6
Economic basis and baseline parameters with lower and upper values in
energy moved between absorber and desorber as sensible heat, which is
parentheses.
minimal for isothermal and near-isothermal designs. As discussed in
Section 1, the enthalpy of reaction has no impact because the energy Basics Absorber/desorber system costs
generated in the absorber matches that consumed in the desorber. In Basis year 2020 Purchased cost $40 M (20–80)
practice, detailed design would reveal that these properties are impor­ Currency Constant $ Direct costs +100% PE
Discount rate 8% (4–12) Indirect costs +14% PE
tant, particularly in designing and locating the absorber and desorber
CEPCI, 2020 600% Contingency +50%
inside the boiler to match the desired operating temperatures of these Exchange rate $1.12/€ Operating costs $2.5 M/year (0–5)
units. The effect of the sorbent properties was therefore lumped into the Plant life Capacity factors
broader uncertainty around the operating temperatures achievable in Construction 4 years Year 1 40%
the absorber and desorber. Only a modest ~1.5% point change in effi­ Capital split 20:30:30:20 Year 2 65%
Lifetime 40 years (30–50) Year t (t ∕
= 1,2) 85% (75–95)
ciency was observed among the various absorber/desorber temperature
FCF 8.39% Levelized 79.7%
pairs discussed in Section 5 and SI4. The ~30% point difference in CO2 Plant costs Fuel & Product Prices/Costs/Values
capture efficiency across the range of temperatures considered has a Owners costs +15% EPC Coal price $50/tonne (25–100)
substantially greater impact on the effectiveness of the capture plant, Maintenance +2.5% EPC/year CO2 handling $10/tonne (5–20)
however. This would be better represented by a sensitivity analysis on Labor +1% EPC/year CO2 value $0/tonne (0–30)

10
C. Halliday and T.A. Hatton Applied Energy 280 (2020) 116016

and an effective levelized Capacity Factor (CFL ) of 79.7%, calculated
through the following equations,
r(1 + r)T
FCF =
(1 + r)T − 1
∑ (CF)
CFL = (FCF) t
t
t (1 + r)
where r is the discounted cash flow rate, and CF is the Capacity Factor in
the year t for a total of T years of plant life. The Levelized Cost of
Electricity (LCOE) reflects the present value of all costs to build and
operate the power plant over its economic life normalized by the net
electricity generated and sold over the same period, expressed in con­
stant $/MWh and defined,
(TCR)(FCF) + (Fix.OPEX)
LCOE =
(MW)(CFL × 8766)
+ (TotalVar.OPEX)
where, MW is the nominal net electrical output of the power plant. The
denominator, (MW)(CFL × 8766), is the annual electrical output of the
plant. (TotalVar.OPEX) is the total variable operating cost, ‘total’ indi­
cating inclusive of fuel, CO2 handling, etc.
The LCOE is a useful guide to the cost of electricity, in particular its
relative change between cases. However, to account for the reduction in
CO2 emissions between the plant with capture (CCS) and without cap­
ture (Ref) the Cost of CO2 Avoided, as defined below, is the preferred
metric. Emissions refer to the CO2 emission rate in tonnes of CO2 per
MWh of electrical output.
LCOECCS − LCOERef
CostofCO2 Avoided =
EmissionsRef − EmissionsCCS
Coal prices can be volatile. Here a delivered price of $50/tonne was
assumed with lower and upper values of $25/tonne and $100/tonne,
respectively [44]. The cost of CO2 handling (transport and storage)
varies between the type of transport needed, distance required, and
ultimate storage location. Typical, transport costs vary from $0–7/tonne
and storage costs from $ 1–12/tonne [12]. As a baseline, CO2 handling
costs of $10/tonne were taken with lower and upper values of $5/tonne
and $20/tonne, respectively. The capital cost of the transport network
was not considered. Enhanced Oil Recovery (EOR) is often proposed as a
possible revenue stream for the CO2 produced on the scale of industrial
plants [45]. However, the baseline assigns no value to the CO2 product,
nor was any carbon credit or tax accounted for.
The first approach economic results are presented in Table 7 for a
number of cases with and without carbon capture. The reference case
without carbon capture has an annual electrical output of 6.68 million
MWh per annum (MMWh/a) and an EPC cost of €1265.7 million (2008)
[34], which gives a Total Overnight Cost (TOC) of $1698.2 million
(2020). The fixed and variable operating costs, $31.5 million/year and
$10.5 million/year respectively, are based on those provided by power
plant suppliers [34]. Fuel costs are $103.7 million per year, and are the
same across each case since all cases have the same fuel input.
In the case with molten sorbents, no FGD or SCR systems are
necessary because in the base case it was assumed that upstream high
temperature acid gas capture would meet emission standards. No credit
was taken for any associated reduction in operating costs, which are
expected to be similar. However, the elimination of the FGD and SCR
plants represents a substantial reduction in CAPEX for a green-field site.
To understand the significance of eliminating these units, and to provide
transparency in the case with molten sorbents, the reference plant was
considered without the capital expense of FGD and SCR. The equipment
cost was taken from ESMAP with FGD and SCR expenditures of $95.3
million and $57.1 million (2008 dollars), respectively [46]. The result
was a total overnight cost reduction of ~$180 million and a ~$3.5/
MWh reduction in the LCOE, Table 7.
The third case was the state-of-the-art technology. As described
previously, amines achieve a 90% reduction in CO2 emissions but at a
significant cost to the plant efficiency. The total overnight cost of the
amine based carbon capture and compression system was reported as
$232.1 million [34]. The fixed operating costs were taken as percentages
of the EPC cost of the capture system; 2.5% for maintenance and 1% for
labor [21], or $8.2 million/year. Variable operating costs in the form of
cooling water and chemicals come to $17.9 million/year [34], with CO2
handling costs of $13.0 million/year. These costs were applied on top of
the other costs of the power plant to give a 64.3% increase in the LCOE at
a value of $91.2/MWh. The DECARBit results differ from those pre­
sented in this work because different assumptions were made around the
base line price of coal and fixed operating costs.
With molten sorbents the capital and operating costs of the absorber/
desorber system are largely unknown because determining these costs
requires detailed design. The main line items with estimated Purchased
Equipment (PE) costs include absorber packing and distribution
(absorber, ~$10 m), additional steam tube bundle with packing for
(desorber, ~$10 m), steam heat exchanger (~$5m), sorbent/sulfur

Table 7
First approach economic results for various cases including the reference case without capture, reference without FGD/SCR, state-of-the-art capture technology
amines, and two cases with molten borates, one which maximizes efficiency and one that minimizes cost.
First order economic Unit Reference without Reference without Amines (state-of- Molten base case Molten base case (min.
results capture FGD/SCR the-art) (max. eff.) cost)

CO2 emissions rate kg/MWh 758.4 758.4 104.7 107.0 110.6

Plant efficiency %LHV 46.06 46.06 33.4 39.87 37.12
Annual electrical output MMWh/ 6.68 6.68 4.85 5.79 5.39
a
Total Overnight Cost (TOC) M$ 1698.1 1515.6 1930.3 2570.4 1816.6
Total Capital Requirement M$ 2064.8 1842.8 2347.1 3125.5 2208.9
(TCR)
Total Operating Cost M$/a 145.7 145.7 184.8 201.9 174.3
(OPEX)
Levelized Cost of Elec. $/MWh 55.5 52.0 91.2 94.5 77.4
(LCOE)
Capital costs (CAPEX) $/MWh 32.5 29.0 51.0 56.8 43.1
Fixed costs (Fix. OPEX) $/MWh 5.9 5.9 10.3 13.8 9.5
Variable costs (Var. OPEX) $/MWh 1.6 1.6 5.8 3.3 2.9
Variable fuel costs $/MWh 15.5 15.5 21.4 17.9 19.2
Variable CO2 handling costs $/MWh 0.0 0.0 2.7 2.7 2.6
Percentage change in LCOE % N/A N/A +64.3 +70.3 +39.5
Cost of CO2 avoided $/tonne N/A N/A 54.6 59.9 34.1

11
C. Halliday and T.A. Hatton Applied Energy 280 (2020) 116016

recovery system (~$5m), two high temperature sorbent pumps (~$1m/

each), sorbent heat exchanger (~$1m), high temperature storage tank
(~$1m) and high temperature cross flow filter (~$1m). Other items
including the superheat and reheat steam bundles and the boiler walls
may also need to be constructed differently to ensure compatibility with
the molten sorbent (~$5m). Accounting for direct costs (+100% of PE)
[34], indirect costs (+14%) [34], and process contingency for a new
concept (+50%) [42] gives an EPC cost for the absorber/desorber sys­
tem of ~$140 m. In the absence of detailed design, a factor of two is
considered in the sensitivity analysis to give lower and upper values of
$70 and $280 million respectively. The true cost of these components
also depends on the material of construction, discussed in Section 8.
Variable operating costs in the absorber/desorber part of the molten
sorbent plant are low and gypsum sales are assumed to cover limestone
costs. Unlike with amines, no cooling water is needed for the absorber
and the various sorbent losses in an amine plant are not present for
molten sorbents. To account for unrecovered sorbent and possible
contamination with fly ash it was assumed as a baseline that the molten
sorbent is replaced in full every 100 h of operation. The lithium–sodium
borate is expected to cost ~$17.5/kg, which brings the variable oper­
ating cost to $2.5 million/year. A range from no additional expense up to
$5 million/year was considered. As with the amines case, fixed oper­
ating costs amounting to 3.5% of the EPC cost were assumed.
The use of non-standard equipment in the absorber/desorber system
makes it difficult to cost at the stage of conceptual design. However,
these limitations are less of a limitation for the compression train, which
were approximated using the ASPEN Economics package. The installed
and variable operating costs of the compression train were determined
in this way. The total installed cost (taken as the EPC cost) was calcu­
lated from the sum of compressors, pumps, separators, and coolers in the
train. In cases where the maximum size of the compressor was exceeded,
the stage was split equally until the size was acceptable.
In the base case with capture using molten sorbents the pressures of
the condenser and first compression stage, 8.2 kPa and 19.0 kPa
respectively, were optimized to maximize the thermodynamic efficiency
of the plant (39.87%). However, operating under these conditions in­
volves an extremely large actual flow of CO2 through the early stages of
the train. Requiring 21 (staged 14-4-1-1-1) compressors to handle the
flow of wet low-pressure CO2. The total EPC cost came to $777.3 million,
which substantially penalized the plant and negated any benefit gained
from the high efficiency. The result of this case, shown in Table 7, was a
70% increase in the LCOE compared to the reference plant and a cost of
CO2 avoided of $60/tonne, 10% higher than the state-of-the-art amine
technology.
However, it is not necessary to maximize the plant efficiency by
Fig. 6. (a) Cost of CO2 avoided for base case with capture under various
operating at very low condenser pressures. Increasing the condenser operating conditions (b) results of technnomic sensitivity analysis.
pressure, even very slightly, results in a substantial drop in cost as far
fewer compressors are required and the associated capital and operating
costs come down. Fig. 6 (a) shows how the plant efficiency and cost of
CO2 avoided change with various operating pressure scenarios. As pre­
achieved a slightly lower overall cost of CO2 avoided than that with five
viously identified in Fig. 5 (a), there is a trade-off between operating
stages. The case with four compression stages and five compressors
pressure and efficiency which leads to a case that maximizes the effi­
(staged 2-1-1-1) that achieved a cost of CO2 avoided of $34.1/tonne was
ciency of the plant. Introduced in this Section is a trade-off between
taken as the base case with molten sorbents that minimizes cost, Table 6.
efficiency and the cost of the plant, which leads to a case that minimizes
This represents a 38% reduction in cost over the state-of-the-art amine
the cost of CO2 avoided. In orange circles Fig. 6 (a), these two extremes
technology. The condenser operates at 35 kPa to achieve a plant effi­
(black outline) are identified along with various other cases to empha­
ciency of 37.12% and a LCOE 42.6% higher than the case without
size the bidirectional nature of the trade-off. By opting to minimize cost
capture.
rather than maximize efficiency the cost of CO2 avoided could be
A large number of parameters were assumed in determining these
brought down substantially to $34.3/tonne as only 8 compressors
first approach economic results. To understand the importance of these
(staged 3-2-1-1-1) would be required.
parameters and the overall confidence in the results a deterministic and
In green circles Fig. 6 (a) the number of compression stages was
probabilistic sensitivity analysis was carried out. The results of the
reduced from five to four. The maximum efficiency that may be obtained
deterministic analysis, where values were changed from their base line
was reduced by ~ 1% point. The cost of CO2 avoided reduced by around
individually, are shown in Fig. 6 (b). Also shown are the expected, or
$0.1/tonne in this case, since 11 compressors (staged 8-1-1-1) are
baseline, values that have been discussed throughout this section along
required, 8 of which remained at a very large costing of ~$81 million
with the upper and lower values that have been applied.
each. However, minimizing cost with only four compression stages

12
C. Halliday and T.A. Hatton
A ± 50% range for CAPEX (applied to the EPC cost) and OPEX (fixed
and operating costs excluding fuel and CO2 handling) was considered.
This reflects the substantial geographic variation in such costs [47], as
well as their general uncertainty [34]. Thermodynamic uncertainty,
Section 5, in plant efficiency, and in CO2 emissions were lumped
together with broader ambiguity around the absorber and desorber
system by considering the extremes observed in the six cases of different
operating temperatures from Section 4. A capacity factor of between
75% and 95% and plant lifetime from 30 to 50 years was assumed [34].
Finally, the possible value of CO2 for Enhanced Oil Recovery (EOR) or
other similar utilization opportunities was considered with a represen­
tative value of $30/tonne [12]. Note, the base line includes $10/tonne
for CO2 transport and storage so the effective value of CO2 at the plant’s
perimeter is $20/tonne.
The results identify the most sensitive parameters. Note that this
assessment is conservative in the sense that, when costs deviate from
their base line values, the operating conditions of the plant could be re-
optimized to minimize cost. For example, if upfront costs were known to
be lower, the ~1% point gain in efficiency of operating five compression
stages may outweigh the cost saving of only designing for four stages.
As is common in the economic assessment of capital-intensive pro­
jects the discount rate was found to be particularly important. The large
uncertainty in CAPEX and OPEX is also represented, with CAPEX as the
more substantial of the two. The CAPEX of the absorber/desorber system
is particularly uncertain and this is reflected in the sensitivity analysis.
Conversely, the variable OPEX of this system is very low and therefore
not as significant. The relatively high confidence in the plant efficiency
(recall the modest sensitivity to various parameters in Section 6) results
in a reasonably low effect of this parameter. The CO2 emissions on the
other hand are highly influential in increasing the cost of CO2 avoided.
The large capital outlay of the plant with capture means that if the plant
is not effective in removing CO2 then the expense is squandered. Higher
capacity factors and longer lifetimes improve the economics of the
capital-intensive capture plant while lower coal prices benefit the lower
efficiency plant with capture. The impact of CO2 handling costs is
modest while the benefit of EOR, or other markets for CO2, could be
substantial.
Individually many parameters could bring the cost of CO2 avoided to
values less than $30/tonne or as high as that of the amine system. To
understand the combined effect of all ambiguous parameters, a proba­
bilistic sensitivity analysis was carried out. This assumed the upper and
lower values represent 95% confidence limits (2 standard deviations) of
normal, or log-normal, distributions around the expected baseline value
of each parameter. The results, presented in SI5, indicate that with 95%
confidence the cost of CO2 avoided in the base case with capture that
minimizes cost lies between $18/tonne and $56/tonne, having a mean
value of $34/tonne. The increase in LCOE ranged from 25% to 49% and
the cost saving relative to amines ranged from a 27% to 50%.
In this study technology leveling assumptions were used to maintain
uniformity of parameters. Therefore, absolute results are of less impor­
tance than differences between cases. For example the total capital cost
and absolute Levelized Cost of Electricity (LCOE) are of less use than the
cost of CO2 avoided and the relative increase in LCOE between cases
[42]. However, even relative changes should be compared to the work of
others with caution. As the sensitivity analysis highlights, the cost of CO2
avoided is highly dependent on the assumptions that were made. Across
the literature different technical and economic assumptions lead to
dramatically different cost estimations. Therefore, the degree of confi­
dence to be assumed in comparing results external to this work should be
low.
The results of the economic assessment determine $54/tonne
($33–89/tonne) for the cost of CO2 avoided with amines (MEA). One of
the first comprehensive analyses in the literature reported $59/tonne
($43–72/tonne) [21]. In 2005 the IPCC Special Report of Carbon Cap­
ture [13], reported $45–113/tonne and $17–77/tonne with EOR
(adjusted to 2013 dollars) [12]. These values were reassessed after a
13
Applied Energy 280 (2020) 116016
decade of progress to $46–99/tonne and between $-5–58/tonne with
EOR [12]. Therefore the results of this work are consistent with the
literature on amines.
The results for the molten metal oxides $34/tonne ($18–56/tonne)
compare favorably with other proposed systems. Advanced next gen­
eration amines (aminomethyl propanol & piperazine) are expected to
reduce the cost of CO2 avoided by ~$7/tonne (€6/tonne) [48] compared
to the $20/tonne reduction calculated with molten sorbents. The cost of
CO2 avoided for other reported sorbents include ammonia at $52/tonne
[49], molecularly imprinted polymers at ~$36/tonne (£29/tonne) [50],
and calcium looping at $11–56/tonne (€10-50/tonne) [51]. However, it
is important to note that these alternative technologies are at a greater
level of development with correspondingly more certainty around their
feasibility and cost. There are also challenges in implementing
adsorbent-based designs such as calcium looping, as described in Section
1. Molten sorbents display economic potential similar to calcium loop­
ing but without these challenges. Inevitably, other challenges arise, and
these are discussed in Section 8.
The cost of CO2 avoided may also be compared to the damage
resulting from unchecked climate change. This is represented by the
social cost of carbon, at $52/tonne, (in constant 2020 dollars) with 95%
confidence limits between $0/tonne and $153/tonne [52]. However,
this social cost assumes a discount rate of 3%. A fairer comparison would
see the same discount rate applied to the social benefit of mitigation
technologies. This gives a cost of CO2 avoided of $25/tonne for the base
line with molten sorbents. Implementation would therefore be justified
economically. At even lower long-term discount rates, for example
2.5%, the expected social cost of carbon increases substantially to $77/
tonne suggesting mitigation costing $24/tonne would be highly im­
pactful. However, higher discount rates quickly favor no action on
climate change, for example a rate of 5% prices the damage at $15/
tonne compared to mitigation at $28/tonne. Although this case would
point towards no action on climate change the irreversible damage to
societies and ecosystems around the world undermines these quantita­
tive arguments.
8. Context & limitations
The purpose of this study was not to advocate for, or against,
implementing a carbon capture design based on molten sorbents. The
purpose was to explore the potential of these concepts to justify, or
dismiss, the work required to implement such designs. This work would
involve developing a deeper understanding of these materials, repro­
ducing their performance at larger scales under more realistic condi­
tions, and carrying out detailed design. A number of simplifying
assumptions limit this study. A probing of these assumptions is critical to
validating the results of the study. In the authors’ judgement, the as­
sumptions that require most attention surround corrosion, contactor
design, solids handling, and transient operations.
Corrosion is a predictable issue under the harsh conditions in which
the sorbents must operate. At the bench scale with a tubular reactor
constructed of Nickel 200/201, over 100 h of operation have been
demonstrated with minimal impact on the performance of the sorbent
[20]. In estimating the variable operating cost of the capture system,
these data led to the assumption that the sorbent could be used for 100 h
before replacement. The use of Nickel 200/201 also contributed to the
estimates of absorber/desorber system cost. The trend in boiler con­
struction is towards greater Nickel contents that enable higher temper­
atures and hence more efficient power cycles [40]. However, the use of
Nickel 200/201, which contains > 99% nickel, substantially adds to
capital costs. Further work is required to understand the interaction
between molten sorbents and various high temperature materials of
construction. This would identify whether Nickel 200/201 is a suitable
material for long-term use or if other alloys would be more appropriate,
either to reduce cost or to minimize corrosion.
In this work the absorber was assumed to operate isothermally and
C. Halliday and T.A. Hatton
the desorber was assumed to operate at the same or slightly higher
temperature, but also isothermally. In practice a temperature gradient
exists throughout the boiler and therefore along the length of both the
absorber and desorber. Intelligent positioning of steam tube bundles
could help control these temperature gradients and maximize the
achievable degree of separation. The six sets of temperatures considered
in this work cover the range of expected values. Therefore, this vari­
ability is captured in the economic sensitivity analysis. Detailed design,
including computational fluid dynamic modelling of the boiler internals,
would reduce uncertainty by understanding the operating temperatures
with more accuracy. Additionally, the relationship between the number
of theoretical equilibrium stages and the actual height of packing needed
in the absorber/desorber must be calculated using mass transfer co­
efficients determined under realistic conditions. This requires demon­
strations of the packed bed absorber/desorber as well a better
understanding the molten sorbent fluidic properties.
The way sulfurous species, and fly ash, are handled in this conceptual
design may introduce issues, specifically with the generation of solids in
the capture system and need to recover the valuable molten metal ox­
ides. Further investigation is required to better understand the nature of
the solid products and to design in detail their separation from the
circulating liquid. Here it was assumed that solids only accumulate at
the cross-flow filter and the retentate forms a minor part of the mass/
energy flows. Solids may also accumulate in other sections of the system,
for example in the absorber/desorber packing, which may cause oper­
ational issues. The solubility of these products in water should enable
effective routine maintenance but steps may need to be taken to limit
solids accumulation. At the extreme, this may involve burning higher
quality lower sulfur content and lower ash content fuels.
Other operational issues and opportunities related to deviations from
normal operation also need to be addressed. These include start-up,
shut-down, and load balancing. Not shown explicitly in Fig. 2(b) are
sorbent storage tanks. These would need to be well insulated to keep the
sorbent liquified during short periods of thermal isolation. Typical
molten salt storage tanks retain high temperatures for many hours or
even days [53]. To handle longer periods, or during a cold start, hot
exhaust gasses could be diverted through pipes internal to the storage
tank to melt and reheat the sorbent. The desorber could also act as an
effective storage tank during start-up. Additionally, an opportunity ex­
ists in load balancing which may warrant further exploration. An
increasingly volatile supply side to the electrical grid restricts base load
plants that cannot easily ramp their power output. If carbon capture
systems are flexible they may benefit base load plants as during peak
demand the capture plant may be ramped down to maximize power
output. However, this comes at the cost of high CO2 emissions during
peak periods. Alternatively, dynamic levels of CO2 rich and CO2 lean
sorbent in separate storage tanks could enable continuous carbon cap­
ture with load balancing capabilities. For brief periods, the flow to the
desorber could be reduced to produce additional electrical output and
vice versa during low demand.
This work has focused on a standardized greenfield coal fired power
plant. The concepts discussed could be further optimized, applied to
brownfield sites, or other sources of CO2. In designing for molten sor­
bents minimal changes were made from the reference coal plant.
However, a supercritical two pass single reheat system may not be
optimal for carbon capture. Designs that produce a greater quantity of
LP steam may benefit the desorption step and thus lower the cost of
carbon capture. Additionally, no attempt has been made to heat-
integrate the compression train with the feed water heaters or other
parts of the plant. Heat integration has been shown to realize a ~ 1%
point gain in efficiency, at the expense of system complexity and
reduced operational flexibility [54]. Advanced power cycles are pre­
dicted to further reduce the energy penalty of high temperature carbon
capture facilities [55].
The feasibility of implementing molten sorbents as retrofits to
brownfield sties could be explored. Fewer new coal plants are being
14
Applied Energy 280 (2020) 116016
considered and with a lifetime of many decades the opportunity for
carbon capture is strongest when applied to existing plants. However, in
this regard molten sorbents may be less well suited. With the majority of
the plant in place, a retrofit for molten sorbents would require signifi­
cant modifications to the boiler and steam cycles. Additionally, no
saving would be achieved for negating the FGD and SCR plants. As a
result, the reduction in cost relative to amines, which are better suited to
an ad-hoc approach, may be lessened or even eliminated. A better op­
portunity is foreseen in applying molten sorbents to other sources of CO2
found in the energy, chemicals, and heavy industry sectors discussed in
Section 1. Of particular relevance to the conceptual design presented
here is biomass combustion, which uses similar steam cycles, has low
sulfur/ash contents, and would enable net-negative emissions through
bioenergy with carbon capture and storage (BECCS) [56].
9. Conclusions
This work explored the potential of molten sorbents to reduce the
cost of carbon capture. A conceptual design was proposed based on an
advanced super critical pulverized coal fired power plant. Emerging
concepts were integrated into the design including high temperature
operation, simultaneous acid gas capture, and regeneration using steam
as a sweep gas. The thermodynamic and first order economic results
show that these materials, and the concepts they enable, could reduce
CO2 emissions with a small energy penalty and at a low cost.
The efficiency of the plant with carbon capture can be as high as
~40% with a Specific Primary Energy Consumption for CO2 Avoided of
1.8–2.2 MJ/tonne. Optimization of operating conditions to minimize
cost rather than to maximize efficiency achieved a cost of CO2 avoided of
around $34/tonne. Sensitivity analyses revealed a range between $18/
tonne and $56/tonne. This is 38% (27%–50%) lower than with amines,
the state-of-the-art in carbon capture. The Levelized Cost of Electricity
increases 39% (25%–49%) relative to the plant without carbon capture.
Corrosion, contactor design, solids handling, and transient operation
were identified as key issues that require focused attention. Detailed
design cannot be carried out with confidence until these issues are better
understood. Design optimization and application to other sources of CO2
also warrant investigation as these may provide even greater opportu­
nities to reduce CO2 emissions and mitigate the effects of climate
change.
Associated Content
We would like to thank the MIT Energy Initiative (MITei) Seed Fund
Grant Program for funding and Prof. Takuya Harada now at Tokyo
Institute of Technology for his contributions to this project.
CRediT authorship contribution statement
Cameron Halliday: Conceptualization, Investigation, Writing -
original draft. T. Alan Hatton: Supervision, Writing - review & editing.
Declaration of Competing Interest
The authors declare that they have no known competing financial
interests or personal relationships that could have appeared to influence
the work reported in this paper.
Appendix A. Supplementary material
Supporting Information (SI): SI1 boiler internals SI2 ASPEN model­
ling assumptions, SI3 sorber/desorber design details, SI4 key results for
all cases, SI5 supporting first order economic results. Supplementary
data to this article can be found online at https://doi.org/10.1016/j.
apenergy.2020.116016.
C. Halliday and T.A. Hatton Applied Energy 280 (2020) 116016

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