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Energy Procedia 114 (2017) 201 210

13th International Conference on Greenhouse Gas Control Technologies, GHGT-13, 14-18

November 2016, Lausanne, Switzerland

Aspen Plus Process Simulation of Calcium Looping with Different

Indirect Calciner Heat Transfer Concepts
Chameera K. Jayarathnaa,b*, Anette Mathisenb, Lars Erik ia, Lars-Andr Tokheima
a
University College of Southeast Norway, Faculty of Technology, Porsgrunn, Norway
b
Tel-Tek, Research Institute, Porsgrunn, Norway

Abstract
CO2 reduction has become an urgent need due to the greenhouse effect. Scientists working on the topic agree that the major
cause of global warming is greenhouse gases emitted due to human activities. Burning of fossil fuels is one of the main reasons.
Using a solid sorbent to capture CO2 at high temperature is a concept which is now being widely considered to reduce CO 2
emissions. Capture from flue gas by calcium looping (CaL) may be an attractive alternative due to cheap and readily available
sorbent (limestone). CaL may reduce considerably the energy penalty represented by the capture system. A significant transfer of
thermal energy is required for the endothermic calcination process. In first generation CaL, the heat is transferred directly by oxy-
combustion in the calciner; pure oxygen is then required as the oxidizer to avoid mixing CO 2 with N2, and the energy required to
produce oxygen gives an unwanted energy penalty. CaL technology would be an even more attractive alternative for the thermal
power industry if the heat could be transferred indirectly to the calciner. By high-temperature integration between the CO2 capture
plant and the power plant, the energy penalty associated with oxy-combustion would be avoided. In this work, Aspen Plus is
used to simulate the CaL process with indirect heat transfer applying different indirect heat transfer concepts. Six different cases
are studied and the results are discussed. It has confirmed such a scheme could give an energy penalty lower than for example
amine scrubbing or oxy-combustion.
2017 The Authors. Published by Elsevier Ltd. This is an open access article under the CC BY-NC-ND license
2017 The Authors. Published by Elsevier Ltd.
(http://creativecommons.org/licenses/by-nc-nd/4.0/).
Peer-review under responsibility of the organizing committee of GHGT-13.
Peer-review under responsibility of the organizing committee of GHGT-13.

Keywords: Calsium looping, Aspen Plus, Indirect heat trasnfer, Carbon capture

*Chameera Jayarathna. Tel.: + 47 35574000

E-mail address: chameera.jayarathna@tel-tek.no

1876-6102 2017 The Authors. 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/).
Peer-review under responsibility of the organizing committee of GHGT-13.
doi:10.1016/j.egypro.2017.03.1162
202 Chameera K. Jayarathna et al. / Energy Procedia 114 (2017) 201 210

1. Introduction

Greenhouse gases (GHG) affect significantly the earths temperature, and carbon dioxide is the most harmful one
due to the vast generation of this gas from human activities. Since the 18th century the atmospheric carbon dioxide
(CO2) concentration has risen by some 40% [1]. The main reason for the increase of global CO2 emission is
increased burning of fossil fuels and deforestation after the industrial revolution. As reported in 2007, the total
industrial CO2 production, primarily from burning coal, oil and natural gas and the production of cement, is about 8
Gt carbon per year [2]. During the last 100 years, the average surface temperature of the earth has increased about
0.8 C and is continuously increasing [3]. During the last decade the scientific research and knowledge on climate
change have progressed considerably. As results of that, technological and political goals were set to reduce the CO2
emissions. A worldwide agreement was made through the Kyoto agreement, and has led to a focus on reduction and
prevention of GHG emissions in most of the countries which ratified the agreement [4]. As results of that, capture
technologies are being developed and could be applied on thermal power plants, such as coal fired power plants.

CO2 capturing is not a new concept as removal of CO2 from gas streams has been a crucial unit operation for
many decades to avoid corrosion and also to improve the calorific value of gas streams. Even though the post
combustion CO2 capture technology using amine-based CO2 solvents to absorb CO2 from the exhaust gas is
scientifically well-established, there are other methods that could be more attractive due to lower energy penalties.
Carbon capture based on a solid sorbent operating at higher temperature is one of them. CO2 capture from flue gas
by calcium looping (CaL) may be an attractive alternative as limestone as a readily available and relatively
inexpensive material.
CaL was first reported as a potential carbon capture technology in 1999 [5], and is also called carbonate looping
as calcium carbonate (CaCO3) is generated in the process [6]. In CaL, calcium oxide (CaO) reacts with CO2 to form
calcium carbonate (CaCO3) in a fluidized bed reactor (carbonator) at a temperature around 650C, in an exothermic
reaction[7], (see Eq. 1)

CaO(s) +CO2 (g) CaCO3(s) (1)

Ho = 178 kJ mol1

The CaCO3 is separated from the cleaned exhaust gas by a gas/solid separator and the cleaned flue gas exiting
from the carbonator can be released to the atmosphere. In a second reactor, the calciner, the reverse reaction
happens, i.e. CaCO3 decomposes into CaO and CO2 at a temperature close to 900 C. This is an endothermic
process, so a significant flow of thermal energy must be supplied to the calciner for the reaction to occur. The
regenerated CaO is separated from the CO2 in a gas/solid separator and recycled back to the carbonator.
Most of the CaL processes described in the literature consist of fluidized bed (FB) reactors and the calcination
heat is transferred directly by an internal oxy-fuel combustor placed inside the calciner [8-15]. This is known as first
generation CaL technology. Even though in CaL most of the heat supplied for the calcination can be recovered at the
carbonator, there is an unwanted energy penalty associated with the oxy-fuel combustion process, especially, from
the air separation unit (ASU) which provides oxygen for the oxy-fuel combustion.
In the second generation CaL technology, the heat is transferred indirectly from the external combustor to the
calciner, and this could reduce the efficiency loss considerably compared with the direct heat supply method by
avoiding the oxy-fuel combustion in the calciner [16]. The basic idea is illustrated in Fig.1. The fact that the heat
transfer takes place at a temperature higher than the typical operational temperature of a coal fired power plant
means that the energy penalty usually associated with CO 2 capture processes can be significantly reduced. Different
indirect heat transfer methods may be applied. Strelow et al. [16] applied steam as the heat transfer medium, but use
of heat pipes is also being considered [17-19].
In this work, CaL with indirect heat transfer applied to an 1890MWth coal fired power plant is simulated using
Aspen Plus V8.6 software. Six different indirect heat transfer concepts are studied, and the impact on the energy
balance of the system for each case is evaluated. This work is a continuation of previously published work [20], in
which three different indirect heat transfer cases were simulated and analyzed. As the concept involves a complete
integration between the power plant and the capture plant, it may call Fully Integrated Calcium Looping (FICaL).
 Chameera K. Jayarathna et al. / Energy Procedia 114 (2017) 201 210 203

Cleaned
exhaust gas CO2

Heat

Heat
Carbonator Calciner
CaCO3
650oC 900oC Heat Combustor
CaO

Fuel (CmHn) +Air

Exhaust gas

Fig.1: Calcium looping cycle with indirect heat transfer between combustor and calciner

2. The simulated process

The simulated process (see Fig.2) includes three main process components; the calciner, the carbonator and the
combustor (coal-fired boiler). In these simulations, complete combustion of coal is assumed and the combustor
generates CO2, H2O, SO2 and other combustion products.
Since the desulfurization reactions take place at relatively high temperature, SO2 and SO3 is removed from the
system by adding CaCO3 in the coal-fired boiler. The added CaCO3 is calcined in the combustor and create CaO
which reacts with SO2 and SO3 create CaSO3 and CaSO4, respectively, (see Eq. 2 and 3).

CaO(s) +SO2 (g) CaSO3(s) (2)

CaO(s) +SO3 (g) CaSO4(s) (3)

The exhaust gas is cooled by the combustion air (which is pre-heated at the same time) and dedusted by the
conventional filters.
Carbonation takes place in the carbonator as the next step of the process, whereby a high fraction of the CO2 in
the flue gas reacts with CaO and form CaCO3 and heat as products. The heat supplied for the calcination reaction in
the calciner is recovered through the exothermic carbonation reaction in the carbonator. CaCO3 rich sorbent is
separated by a cyclone and the clean exhaust gas is vented to the atmosphere (after recovering the heat) via the
Induced Draft (ID) fan. CO2 loaded sorbent is then transferred to the calciner. In the reference case, steam is used as
the transport medium.
Calcination is an endothermic process, and the required heat is taken from the main combustor in the plant. CO 2
and CaO are produced in the calciner, and 100% calcination efficiency is assumed. CaO is separated from the gas
mixture (steam and CO2) in a cyclone and is fed back to the carbonator for a new cycle. The CO 2 and steam are then
separated in a condenser and the water is preheated to produce steam again for reuse as a transport medium in the
calciner. Pure CO2 is pulled out of the condenser by an ID fan, and after this step CO2 is ready to be compressed
and/or used for other purposes.
There are sulfates and sulfites in the combustor. Some of these minerals may end up in the bottom ash, some in
the fly ash. The fly ash is separated from the exhaust gas in a filter designed for operation at high temperature.
Two main assumptions are made for the reactions in the carbonator; it is assumed that 85% of the CO 2 is
captured. It is also assumed that only 18% of the CaO in the lean sorbent reacts with CO 2 and is converted in to
CaCO3. This is because the reactions occur mainly on the surface of the sorbent particles, and the remaining 82 %
exists as an unreacted core not available for reactions due to diffusion limitations [21].
204 Chameera K. Jayarathna et al. / Energy Procedia 114 (2017) 201 210

Heat required for the calcination is transferred indirectly via tube walls separating the hot combustion gases and
the gas/particle suspension in the calciner. Material temperature constraints are not specifically discussed here, i.e.
the simulations are based on the assumption that the heat exchanger is capable of transferring heat to capture 85 % of
the CO2 produced in the plant. However, operational actions to prevent overheating are considered in some of the
calculation cases (explained in Chapter 4).

Q Q Q Q Q

N2, O2,
CO2, H2O
Cyclone ID fan
N2, O2, CO2,
H2O, CaO, CaCO3 Carbonator
CaO,
CaCO3

CaO N2, O2,

CO2, H2O
CO2
ID fan

Condenser Purge
H2O Mixer CaCO3 (CaO)
CaO,
CO2 ,H2O
Pump CaCO3,
H2O

CO2, CaO, H2O Coal fired

Cyclone boiler
N2, O2, CO2,
H2O, Ash, CaSO3 CaSO3, Ash
Calciner
CaO
Q
Make-up Air
CaCO3 preheater

CaCO3
for de-SOx Air
Hot air
Coal Fan
Coal-air
Q
mixer Coal-air mix Ash

Fig.2: Process flow diagram based on heat transfer concept

3. FICaL Aspen Plus model and model description

The FICaL process simulation model is implemented in Aspen Plus 8.6V . The flow sheet type for the simulation
is selected with solids and a user defined unit package. The solid package facilitates feed input with particles or
particle-fluid mixtures, and it gives output stream results in the same way. The setup of the flow sheet involved
assigning the MCINCPSD stream class to the simulation. This allowed fluid streams (MIXED), conventional solid
streams with Particle Size Distribution (CIPSD) and non-conventional solid streams with a certain Particle Size
Distribution (NCPSD) to be specified. The process type was chosen as COMMON. The IDEAL base calculation
method was selected, thus phase equilibrium calculations were conducted using Raoults Law, Henrys Law, ideal
gas law, etc.
Applying the ultimate and proximate analyses of a specific coal type (shown in Table 1), coal was modelled in
Aspen Plus as a nonconventional solid, and the DCOALIGT model was selected to calculate the coal particle
density. The DCOALIGT model in Aspen Plus uses IGT correlations to approximate the density value of coal [22].
The enthalpy of coal is specified as a user defined value. The Particle Size Distribution (PSD) of coal was specified
as a group of particles with size 25-350 m.
Conventional components embedded in the Aspen thermophysical database were used to model the fluid streams
and also the conventional solids in the system. The required chemical and physical properties were also available in
the database for the fluid components water (H2O), oxygen (O2), sulfur dioxide (SO2), sulfur trioxide (SO3),
hydrogen (H2), chlorine (Cl2), hydrochloric acid (HCl), carbon monoxide (CO) and carbon dioxide (CO 2). Input data
for the conventional solid components, calcium oxide (CaO), calcium carbonate (CaCO 3), calcium sulfite (CaSO3)
and calcium sulfate (CaSO4), were also available in the database. Input values for the Aspen Plus simulations are
shown in Table 1. The air preheating temperature was set to 650 C.
 Chameera K. Jayarathna et al. / Energy Procedia 114 (2017) 201 210 205

All the components in the FICaL Aspen model, and also its calculation sequence, follow the process flow
diagram shown in Fig. 2. There are two main mass inputs to the process: coal and air to the combustor. In addition to
that CaCO3 is added at the combustor to remove SOx from the exhaust gas. CaO is an input to the carbonator, but it
is removed from the calciner as and output, which represents the recycling of CaO in the process. Steam/water in the
system is also recycling in the system. Makeup and purge streams are not included in the model. The major outputs
from the system are the clean gas and the pure CO 2. In addition, the bottom ash and the fly ash exit from the system.

Table 1: Input values used in the Aspen Plus simulations Fuel sulfur:
Sulfate 0.15 wt%
Parameter Value Unit
Pyritic 0.9 wt%
Thermal power, full-scale 1890 MWth
Organic 0.15 wt%
Fuel Coal -
Fuel ultimate analysis:
Fuel heating value 27.7 MJ/kg
C 71.7 wt%
Feed rate of coal 68.2 kg/s
Excess air 15 % H 3.9 wt%
O 5.9 wt%
Maximum material temperature 1100 C
S 1.2 wt%
Calcination temperature 900/9201 C
N 1.7 wt%
Carbonation temperature 650 C
Cl 0.1 wt%
Fuel proximate analysis:
Ash 14.3 wt%
Moisture 1.2 wt%
Moisture 1.2 wt%
Volatiles 23.7 wt% 1
Used only in the case 6
Fixed carbon 60.8 wt%
Ash 14.3 wt%

A calculator block in Aspen Plus is used to calculate the required amount of CaO feed in to the carbonator. The
required mass flow of CaO is calculated based on the required CO 2 capture efficiency in the plant (85 %) and the
fraction of CaO (18 %) which can react with CO2 and create CaCO3. The calciner and the carbonator were modelled
as stoichiometric conversion reactors, however at temperatures not violating the thermodynamic constraints. Some
key assumptions were applied to the simulations as shown below.

x The calcination of CaCO3 in the calciner is 100 % efficient, leaving no uncalcined material in the lean sorbent
exiting the calciner.
x The gas-solid separators are 100% efficient, leaving no dust in the gas exit streams.
x The pressure drop over the carbonator, calciner, heat exchangers and gas-solid separators are set to 110, 150, 10
and 10 mbar, respectively.

4. Case studies

Six different indirect heat transfer concepts are discussed here, and the cases are explained below. The process
explained in chapter 2 uses steam as the fluidization medium in the calciner. However in case 1, only CO2 is used for
fluidization in the calcination process. This is simplifying the Aspen plus model as the equipment related to
separation of CO2 and steam is not needed. Case 1 is discussed also by Jayarathna et al. [20] and is used as the
reference for the other cases.
The energy balance, based on the Aspen Plus simulation results, is summarized in Table 2 for all the cases. There
is a relatively small balance error (f0.5 %), which is due to the iterative calculations. However, the error is
sufficiently small that the numbers can be used to evaluate the concept.
206 Chameera K. Jayarathna et al. / Energy Procedia 114 (2017) 201 210

4.1. Case 1-Self fluidization

Here in case 1 (Fig.3) it is assumed that the CO2 developed during calcination is sufficient for fluidization. Due to
that reason the steams loop is not added to the model and there is no need of the condenser, the pump or the
water/steam pipelines. Case 1 is considered as the reference case in this study.

Fig.3: Aspen Plus flow diagram for case 1

4.2. Case 2 and 3 (high excess air)

In these two cases, extra combustion air is fed to the combustor in order to avoid potential material overheating.
The exhaust gas temperature will then drop because there is more air to heat up. In case 2 (Fig.4) the exhaust gas
temperature is 1200 C, and in case 3 it is 1500 C.

4.3. Case 4 and 5 (reduced capture ratio)

As an alternative to increasing the excess air as a means to reduce the combustion gas temperature one can
reduce the amount of CO2 captured in the system. A reduction in capture efficiency down to 31 and 65 % for case 4
(Fig.5Fig.5) and 5, is required in order to obtain gas temperatures of 1200 and 1500 C, respectively.

4.4. Case 6: Heat transfer concept based on inert solid recycling

Case number 6 (Fig. 6) is quite different from the other cases in that inert Al 2O3 particles are used to transfer heat
from the combustor to the calciner. The inert particles are heated to approximately 1200 C in the combustion
chamber and are then mixed with the loaded sorbent. The sorbent is heated up to the calcination temperature and
calcined while the inert particles are cooled down to the calcination temperature. The mixing, the solids-solids heat
exchange and the calcination take place in a rotary calciner. Downstream of the calciner, the inert particles and the
sorbent are separated from each other in a classifier (not shown in the process flow diagram).
Chameera K. Jayarathna et al. / Energy Procedia 114 (2017) 201 210 207

Fig.4: Aspen Plus flow diagram for case 2

Fig.5: Aspen Plus flow diagram for case 4

208 Chameera K. Jayarathna et al. / Energy Procedia 114 (2017) 201 210

Fig.6: Aspen Plus flow diagram for case 6

5. Energy penalty calculation

The material balance is given in the form of specified material streams between the equipment units in the Aspen
Plus flowsheet. The energy balance is given in the form of energy streams (enthalpy streams of material streams,
heat duties or electrical duties) into and out of the equipment units.
The energy penalty of the FICaL system can be defined as the difference in efficiency
between the FICaL process and a reference process  (in this case a coal-fired power plant without
CO2 capture). This difference is calculated by Eq. 4, which was derived and explained in a previous paper [20]. The
total pressure drop that has to be overcome in the reference process and the FICaL process are and ,
respectively.  is the fan power of the FICaL plant and  is the thermal energy input, i.e. the coal
combustion energy released.



(4)


6. Results and discussion

Case 2 and 3 are simulated with increased air flow rate into the combustor. 220 and 350 % extra air is used to
reduce the maximum gas temperature to 1200 and 1500 C, respectively. This increases the fan power. Compared to
case 1 (the reference case), the air fan power increases to 44 and 27 MW for case 2 and 3, respectively, vs. 13 MW
in the reference case. The exhaust gas fan power increases to 6 and 5 MW for case 2 and 3, respectively, vs. 2 MW
in the reference case. The increased fan power increases the energy penalty to 2.4 and 1.5 %, respectively, compared
to 0.6 % in the reference case. The duty of the air preheater also increases considerably (1700 and 1047 MW for case
2 and 3, respectively, vs. 482 MW in the reference case), and the duty of the exhaust gas cooler increases
accordingly (1648 and 1007 MW for case 2 and 3, respectively, vs. 445 MW in the reference case). This means
bigger equipment and higher capital costs.
 Chameera K. Jayarathna et al. / Energy Procedia 114 (2017) 201 210 209

Case 4 and 5 are simulated with reduced CO2 capture ratio and the consequences of these schemes are much
higher heat transfer rates from the combustor to the boiler steam cycle system (1454 and 1133 MW for case 4 and 5,
respectively, vs. 934 MW in the reference case). Naturally, the transfer rate from the carbonator is reduced (293 and
601 MW for case 4 and 5, respectively, vs. 791 MW in the reference case), since there is much less CO 2 to capture
and hence less energy released by the carbonation. The energy remaining in the hot clean exhaust gas is slightly
higher due to the higher CO2 content (502 and 467 MW for case 4 and 5, respectively, vs. 445 MW in the reference
case). Finally, the CO2 cooler duty goes down (51 and 105 MW for case 4 and 5, respectively, vs. 137 MW in the
reference case) due to the reduced CO2 flow rate. The energy penalty values are 0.5 and 0.6 %, respectively. This is
similar to the reference case (0.6%) since the total fan power and the pressure drop is the same even if the capture
ratio is lower.
The results from case 6 are quite similar to the reference case. The slightly higher CO2 cooler duty and CaO heat
recovery is due to a slightly higher calcination temperature (920 C).

A reasonable value for the total efficiency (produced electrical power / heat input from the coal feed) for a
modern coal based power plant is 40 %. With a thermal duty of 1890 MW this gives a total electrical power of 756
MW. The estimated energy penalty means that the FICaL plant will, in comparison, have and efficiency in between
37.6-39.5 % depending on the indirect heat transfer method. Including makeup and purge in the system (not
accounted for above) will increase the energy penalty. Additional heat losses from the FICaL system are likely to
occur due to higher surface area as a result of the extra equipment units, and this will also increase the energy
penalty. This contribution is however not included here as its value is unknown. Also, auxiliary equipment
potentially requiring some extra electrical energy is not included, but is not likely to be significant.
The pressure drop value of each unit (in particular the calciner and the carbonator) may later be determined more
accurately, giving a more accurate energy penalty value.

Table 2: Energy balance (MW) for case 1 to 6

Inputs: Aspen Plus Case 1 Case 2 Case 3 Case 4 Case 5 Case 6

flowsheet reference
Air preheating B-10 482 1700 1047 482 482 482
Air fan B-12 13 44 27 13 13 13
Exhaust gas fan B-15 2 6 5 2 2 2
CO2 fan B-11 3 2 2 1 2 3
Sum inputs - 499 1752 1081 498 498 499

Generation:
Coal combustion - 1890 1890 1890 1890 1890 1890
SOx unit CASO4-R 2 2 2 2 2 2
Sum generation - 1892 1892 1892 1892 1892 1892

Outputs:
Cooling and condensation of H2O/CO2 CO2HX+ B-18 137 137 137 51 105 143
Boiler energy to steam cycle B-1 + B-13 934 958 960 1454 1133 929
Carbonator energy to steam cycle CARBONAT 791 791 791 293 601 791
Hot clean exhaust gas energy EXHAUST-Q 445 1648 1007 502 467 445
Ash waste heat B-19 7 7 7 7 7 7
Cold clean exhaust gas waste heat B-17 58 71 45 57 58 58
Dryer heat recovery B-16 5 5 5 5 5 0
CaO heat recovery - 0 0 0 0 0 19
Sum outputs - 2377 3617 2952 2370 2376 2395
Energy penalty - 0.6 % 2.4 % 1.5 % 0.5 % 0.6 % 0.6 %

7. Conclusions

Aspen Plus has been used to simulate a CO2 capture plant fully integrated with a coal-fired power plant. Six
different cases were studied, and a simplified method was used to estimate the energy penalty. The estimated energy
penalty varies from 0.5 to 2.4 % depending on the indirect heat transfer method. Operation with a higher amount of
210 Chameera K. Jayarathna et al. / Energy Procedia 114 (2017) 201 210

excess air (implemented in order to reduce the maximum gas temperature in the heat exchange process) gives
increased energy penalty values and will also require bigger equipment and higher capital costs for the
implementation. Operation with reduced CO2 capture efficiency (another way to limit the maximum temperature)
does not affect the energy penalty. Use of inert solid particles for indirect heat transfer gives the same energy penalty
as in the reference case, but the calciner design has to be changed from fluidized bed reactor to a rotary calciner.

With careful design considerations, the FICaL process is characterized by a very low energy penalty. Even if
additional energy consuming effects are included, the FICaL process will likely have a competitive advantage over
other technologies.

Acknowledgements
The authors acknowledge funding from GE and Gassnova via the FIRCC project [23] and would like to thank Mr.
Michael Balfe from GE Power, Germany, for his valuable discussions.

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