Chemical Engineering Science 56 (2001) 3101–3113

www.elsevier.nl/locate/ces

A uidized-bed combustion process with inherent CO2 separation;

application of chemical-looping combustion
Anders Lyngfelt ∗ , Bo Leckner, Tobias Mattisson
Department of Energy Conversion, Chalmers University of Technology, 412 96 Goteborg, Sweden

Received 28 April 2000; received in revised form 13 September 2000; accepted 2 December 2000

Abstract
For combustion with CO2 capture, chemical-looping combustion has the advantage that no energy is lost for the separation of
CO2 . In chemical-looping combustion oxygen is transferred from the combustion air to the gaseous fuel by means of an oxygen
carrier. The fuel and the combustion air are never mixed, and the gases from the oxidation of the fuel, CO2 and H2 O, leave the
system as a separate stream. The H2 O can easily be removed by condensation and pure CO2 is obtained without any loss of
energy for separation. This makes chemical-looping combustion a most interesting alternative to other CO2 separation schemes,
which have the drawback of a large energy consumption. A design of a boiler with chemical-looping combustion is proposed. The
system involves two interconnected uidized beds, a high-velocity riser and a low-velocity bed. Metal oxide particles are used
as oxygen carrier. The reactivities needed for oxygen carriers to be suitable for such a process are estimated and compared to
available experimental data for particles of Fe2 O3 and NiO. The data available on oxygen carriers, although limited, indicate that
the process outlined should be feasible. ? 2001 Elsevier Science Ltd. All rights reserved.

Keywords: CO2 capture; Chemical-looping combustion; Fluidization; Environment; Energy; Fuel

1. Introduction Storage in used oil and gas 'elds: On an average, about

It has been known for more than a 100 years that CO2
is a greenhouse gas and that the release of CO2 from fos-
sil fuel combustion may a8ect the climate of the earth
(Arrhenius, 1896). In the last years the concern over the
e8ects of an increased release of greenhouse gases has
been growing. The release of CO2 from fossil fuel com-
bustion is the most important of these emissions. In the
developing countries, the economic growth results in a
rapid increase in the demand for energy supplied by fossil
fuels, while the developed countries have not yet found
the means for substantially decreasing their use of these
fuels. In the future it is not unlikely that radical measures
to decrease CO2 emissions will be demanded. Therefore,
various options need to be investigated.
One strategy to decrease CO2 emissions is to separate
the CO2 from the fuel gas and to store it. Several possi-
bilities for such sequestration have been proposed:
∗ Corresponding author. Tel.: +46-31-772-1427; fax: +46-31-
772-3592.
E-mail address: anly@entek.chalmers.se (A. Lyngfelt).
twice as much CO2 can be stored in depleted gas @elds
as the CO2 obtained from burning the gas extracted from
the @eld (Blok, Williams, Katofsky, & Hendriks, 1997).
In the case of oil @elds, the CO2 can be used to extend
the production, the so-called enhanced oil recovery.
Storage in deep coal beds: The CO2 injected in a coal
seam is absorbed in the coal and stored in its pore matrix,
releasing methane trapped, which can be collected and
sold (Anon, 1999). The process is called enhanced gas
recovery.
Storage in aquifers: The potential storage capacity
is large (Riemer, 1998). This possibility is already in
use in Norway, where natural gas containing CO2 is
cleaned, with the resulting CO2 injected into an aquifer
800 –1000 m below the bottom of the sea (Lindeberg &
Holloway, 1998). In fact, one million tons of CO2 per
year or 3% of Norway’s total CO2 emissions are disposed
in this way (Herzog, Eliasson, & Kaarstad, 2000).
Deep sea storage: At pressures above approximately
50 bar , corresponding to a depth of 500 m; CO2 becomes
a liquid. The density of this liquid is somewhat lower
than that of the surrounding seawater and in its pure form

0009-2509/01/$ - see front matter ? 2001 Elsevier Science Ltd. All rights reserved.
PII: S 0 0 0 9 - 2 5 0 9 ( 0 1 ) 0 0 0 0 7 - 0
3102 A. Lyngfelt et al. / Chemical Engineering Science 56 (2001) 3101–3113

the liquid will rise slowly and ultimately reach the level needed, however, to compress CO2 into a liquid suitable
where gas bubbles are formed. However, if proper mea- for sequestration.
sures are taken to allow the CO2 liquid to mix with the The purpose of the present paper is to assess the poten-
seawater, the resulting mixture obtains a higher density tial of chemical-looping combustion — is it technically
than the seawater and instead sinks. The storage capacity and economically realistic? In order to do this, a tentative
is enormous, but local e8ects on the environment need to design of the process is made. Aspects of importance for
be investigated. judging the realism of the process are discussed.
Deep sea bottom storage: At high pressures, i.e.
3000 m below the sea level, the density of pure CO2 is
higher than that of seawater. Thus, CO2 released at these 2. Chemical-looping combustion
depths will form “lakes” on the ocean oor. The poten-
tial storage capacity is vast considering the fact that the Chemical-looping combustion has been discussed ear-
average depth of the sea is 3700 m and that more than lier in the literature as an alternative to normal combustion
50% of the earth’s surface is found at a depth of more (Richter & Knoche, 1983; Ishida & Jin, 1994; Anheden,
than 3000 m. However, local e8ects on the sea oor NPasholm, & Svedberg, 1995). The system is composed
environment are obviously inevitable. of two reactors, an air and a fuel reactor, as shown in
The estimated cost of CO2 disposal, e.g. 4 –8 US $= Fig. 1. The fuel needs to be in a gaseous form and is intro-
ton C (Riemer, 1998), is small compared to the costs duced to the fuel reactor, which contains a metal oxide,
for separation of CO2 , which is typically in the range MeO. The fuel and the metal oxide react according to
100 –200 US $=ton C (Freund, 1998). Consequently,
(2n + m)MeO + Cn H2m → (2n + m)Me
the major problem seems to be to extract the CO2
from the fuel conversion process. The available or + mH2 O + nCO2 : (1)
proposed technologies all have the disadvantage of
The exit gas stream from the fuel reactor contains CO2
consuming large amounts of energy. The major loss
and H2 O, and almost pure CO2 is obtained when H2 O is
in eLciency arises from the energy needed for sep-
condensed. The reduced metal oxide, Me, is transferred
aration of CO2 and for compression to liquid form.
to the air reactor where the metal is oxidized according to
Typically, the energy needed for compression is about
one-fourth of the total energy needed for separa- Me + 21 O2 → MeO: (2)
tion and compression. For a coal-@red power plant,
roughly one-@fth of the electricity produced will be A full conversion from MeO to Me and back to MeO,
lost for CO2 separation and compression (Lyngfelt & as indicated by reactions (1) and (2), is not necessarily
Leckner, 1999). This decrease in eLciency alone in- obtained in a real system. The air oxidizing the metal
creases the cost for electricity production with one-fourth, produces a ue gas containing only N2 and some un-
and in addition there are costs related to separation and used O2 . Depending upon the metal oxide used, reaction
handling of CO2 . If natural gas is used as a fuel, the (1) is often endothermic, while reaction (2) exothermic.
relative loss in eLciency is somewhat smaller, but still The total amount of heat evolved from reactions (1) and
substantial. (2) is the same as for normal combustion, where the
Today, power production contributes with one-third of
the CO2 released from fossil fuel combustion world-wide
(Herzog et al., 2000). Although the cost for separation
of CO2 is substantial, power plants using fossil fuel
and CO2 capture may well be the least costly alterna-
tive for CO2 -free power production (Keith & Parson,
2000).
Chemical-looping combustion (CLC) o8ers a solution
where no energy is needed for the separation. The pro-
cess uses a solid oxygen carrier to transfer the oxygen
from the air to the fuel. The oxygen carrier is recycled
between a fuel reactor, where it is reduced by the fuel,
and an air reactor, where it is oxidized by the air. Thus,
the air is never mixed with the fuel, and the CO2 does
not become diluted by the nitrogen of the ue gas. The
outgoing gas from the reduction step will contain water
vapour and CO2 . The water vapour can easily be sep-
arated by condensation, and the CO2 is delivered with- Fig. 1. Chemical-looping combustion. MeO=Me denote recirculated
out an energy penalty for the separation. Energy is still oxygen carrier solid material.
 A. Lyngfelt et al. / Chemical Engineering Science 56 (2001) 3101–3113
oxygen is in direct contact with the fuel. The advantage of
chemical-looping combustion compared to normal com-
bustion is that CO2 is not diluted with N2 but obtained
in a relatively pure form without any energy needed for
separation.
Originally, the process was proposed as a method to
enhance the thermal eLciency of fuel combustion. The
idea was to supply low-temperature heat to the endother-
mic reaction in the fuel reactor, thereby increasing the
amount of heat produced in the high-temperature air
reactor. This possibility is not considered in the present
application, since it would make the process more com-
plex and also involves extra demands on the properties
of the oxygen carrier.
3. Reactor design
The reactors in Fig. 1 could be designed in a variety
of ways, but two interconnected uidized beds have an
advantage over alternative designs, because the process
requires a good contact between gas and solids as well
as a ow of solid material between the two reactors.
The system proposed is a circulating system composed
of two connected uidized beds, a high-velocity riser
and a low-velocity bubbling uidized bed (Fig. 2). The
bed material circulating between the two uidized beds is
the oxygen carrier in the form of metal oxide particles. In
the air reactor, or the riser, oxygen is transferred from the
combustion air to the oxygen carrier. In the low-velocity
uidized bed, or the fuel reactor, oxygen is transferred
Fig. 2. Layout of chemical-looping combustion process, with two
interconnected uidized beds.
3103
from the oxygen carrier to the fuel. The volumetric gas
ow in the air reactor is approximately 10 times larger
than that of the gaseous fuel, and to keep a reasonable
size of the reactors a high velocity is chosen in the air
reactor.
The gas velocity in the riser provides the driving
force for the circulation of particles between the two
beds. Thus, the particles carried away from the riser
are recovered by a cyclone and led to the fuel reactor.
From the fuel reactor the particles are returned to the
air reactor by means of gravity; the fuel reactor is lo-
cated at a suLciently high level. After condensation of
the water, the remaining gas, containing mostly CO2 , is
compressed and cooled in stages to yield liquid CO2 .
Remaining non-condensable gas from this stream, such
as unreacted methane, is recycled to the fuel reactor. In
order to avoid accumulation of non-combustible gases,
such as N2 , in the recycling loop, a minor part of this
ow is bled to the air reactor. Small amounts of water left
in the liquid CO2 have to be removed by a regenerable
solvent to make the CO2 ow less corrosive.
4. Oxygen carriers
The metal oxide, used as an oxygen carrier in
chemical-looping combustion, must have suLcient rates
of reduction and oxidation, at the same time as it pos-
sesses enough strength to limit particle breakage and
attrition. It is also an advantage if the metal oxide is
cheap and environmentally sound. A number of metals
and their corresponding oxides have been mentioned in
the literature as possible candidates: Fe, Ni, Co, Cu, Mn
and Cd. At Tokyo Institute of Technology, Ishida and
co-workers have investigated the rate of oxidation and
reduction of Ni, Fe and Co (Nakano, Iwamoto, Maeda,
Ishida, & Akehata, 1986; Ishida & Jin, 1994, 1996;
Ishida, Jin, & Okamoto, 1996, 1998; Ishida, Yamamoto,
& Saito, 1999; Jin, Okamoto, & Ishida, 1998, 1999) in a
thermogravimetric analyzer (TGA) using either H2 , CO
or CH4 as fuel and air as the oxidizing gas.
In order to increase the reactivity and durability of
the oxides, the particles have often been doped with
Al2 O3 , yttria-stabilized zirconium (YSZ), TiO2 or MgO.
The particle size of the oxygen carriers has been rather
large in most of these investigations, around 2 mm in
diameter. The rates of reaction vary widely depending
upon the type of metal oxide, particle size, reduction gas
and temperature. Generally, Ni and Co and their oxides
show higher oxidation and reduction rates than Fe and a
greater durability after repeated oxidation and reduction
cycles.
Many of the reduction experiments were made at a
◦
rather low temperature, less than 900 C. The reason for
this is the desire to use the fuel reactor as a heat sink to
enhance the process eLciency, as mentioned above. Since
3104 A. Lyngfelt et al. / Chemical Engineering Science 56 (2001) 3101–3113

Table 1
Literature data on oxygen carriers in chemical looping combustion
◦ ◦
Carrier=support Carrier=support Red. gas Tred: ( C) Tox: ( C) Dp (mm)
(continued)
Nakano et al. (1986) Fe2 O3 , Fe2 O3 = Ni H2 700 –900 800 –1000 0.007
Fe2 O3 = Al2 O3 H2 = H 2 O
Ishida and Jin (1994)a NiO=YSZ, Fe2 O3 = YSZ H2 600,800,1000 700,900,1100 1–3
NiO Fe2 O3 = Al2 O3
Ishida et al. (1996) NiO=YSZ H2 600,800,1000 600,800,1000 1.8
Ishida and Jin (1996)b NiO NiO=YSZ H2 600 1000,1200 2
Jin et al. (1998) NiO=YSZ, Co3 O4 = YSZ, H2 ; CH4 600 1000 1.8
Fe2 O3 = YSZ CoO-NiO=YSZ
Ishida et al. (1998)c NiO=YSZ Fe2 O3 = YSZ H 2 = N2 550,600,700
NiO= Al2 O3 Fe2 O3 = Al2 O3 CO= N2 800,900
NiO= TiO2 Fe2 O3 = TiO2 CO= CO2
CO= N2 = CO2
CO= N2 = H2 O
Jin et al. (1999)d NiO= Al2 O3 , CoO= MgO H2 600 1000 2.1,1.8
NiO= TiO2 , Fe2 O3 = Al2 O3 , H2 O= CH4 700 1000
NiO=MgO, Fe2 O3 = TiO2 ,
CoO= Al2 O3 , Fe2 O3 = MgO
CoO= TiO2 ,
Ishida et al. (1999)e NiO= Al2 O3 H2 (TGA) 900 900 0.07
H2 = Ar (CR )
Hatanaka et al. (1997)f NiO CH4 400 –700 0.07
a E8ect of H2 O on oxidation, e8ect of particle size.
b ◦
No NOx formation at 1200 C.
c Study of carbon deposition.
d E8ect of pressure.
e Data from continuous CLC reactor.
f Gas measurement with gas chromatography.

Table 2
Selected literature data on conversion rates
◦
Oxidation Reduction Conversion Average Agent T ( C) dp Reference
range rate (mm)

Fe2 O3 → 1 → 0:4 60%=min H2 900 0.007 Nakano et al. (1986)

→ Fe2 O3 0:1 → 0:5 60%=min air 900 0.007 Nakano et al. (1986)
NiO= YSZ → 1 → 0:23 60%=min CH4 600 1.8 Jin et al. (1998)
→ NiO= YSZ 0:3 → 1:0 20%=min air 1000 1.8 Jin et al. (1998)
NiO= Al2 O3 → 1 → 0:2 16%=min 1=3CH4 700 2.1 Jin et al. (1999)
2=3H2 O
→ NiO= Al2 O3 0:05 → 1 20%=min air 1000 2.1 Jin et al. (1999)
NiO= Al2 O3 → 0:8 → 0:2 210%=min H2 900 0.07 Ishida et al. (1999)
→ NiO= Al2 O3 0:3 → 0:8 90%=min air 900 0.07 Ishida et al. (1999)

this possibility is not regarded in the present application,
there is no reason to consider a lower temperature in the
fuel reactor than in the air reactor.
Most of the studies were made with the Ni–NiO sys-
tem, but some data are available for Fe2 O3 and CoO.
The reduction studies were normally made with H2 as
fuel, but isolated data are available for CH4 and CO. An
overview of the work made is given in Table 1. Exam-
ples of conversion rates from these studies are shown in
Table 2. These rate data were obtained in TGA and they
are therefore probably associated with a low conversion
of the reactant gas. For this reason these conversion rates
cannot be immediately applied to conditions where a high
conversion of the reactant gas is necessary.
Hatanaka, Matsuda, and Hatano (1997) performed
cyclic reactivity investigations of NiO in a @xed-bed
reactor, using methane and air, where the conversion of
the gases was measured but not the conversion rate of
the oxygen carrier. Recently, the conversion rate of iron
oxide particles was determined as function of conversion
of the gas in a @xed-bed reactor with methane as fuel
(Mattisson, Lyngfelt, & Cho, 2000a,b).
The process of chemical-looping combustion has been
demonstrated in a laboratory set-up at a temperature of
 A. Lyngfelt et al. / Chemical Engineering Science 56 (2001) 3101–3113 3105

◦
1200 C, where particles of NiO with a diameter of about and the reducer are given by the pressure drops, Vpox
0:1 mm were used as oxygen carrier and the fuel was H2 and Vpred :
(Ishida et al., 1999). The question of how a CLC boiler is Vpox Aox
designed remains to be answered. First, the basic design mbed; ox = ; (8a)
g
relationships will be formulated.
Vpred Ared
mbed; red = ; (8b)
g
5. Theory where g is the acceleration of gravity. The bed heights
are obtained from the density of the solid material, , and
Assuming that the fuel is completely burnt, the fuel the voidage, 
consumption is given by the heating value of the fuel, Hi , mbed; ox
and the fuel power, Pfuel : hbed; ox = ; (9a)
(1 − )Aox
Pfuel mbed; red
ṁfuel = : (3) hbed; red = : (9b)
Hi (1 − )Ared
The amount of oxygen needed for oxidation of the fuel The oxygen ratio, Ro , is a property of the carrier and
is then signi@es the mass fraction of oxygen in the carrier (in its
ṁfuel fully oxidized state)
ṁo = MO2 Sr ; (4)
Mfuel Mf:ox − Mf:red
Ro = ; (10a)
where Sr is the stoichiometric ratio for the reaction be- Mf:ox
tween fuel and oxygen, and Mi denotes the molar mass of where Mf:red is the molar mass of the fully reduced carrier,
species i. The air ratio, , is given by the volume fraction and Mf:ox is the molar mass of the fully oxidized carrier.
of oxygen in the air from the oxidizer, xO2 ;ex The degree of oxidation, X , henceforth called conversion,
0:21(1 − xO2 ;ex ) is then the actual mass of oxygen divided by the mass of
= ; (5) oxygen when fully oxidized
0:21 − xO2 ;ex
Mactual − Mf:red
where 0.21 is the volume fraction of oxygen in air. (In X= ; (11a)
Mf:ox − Mf:red
contrast to normal combustion, the gas ow leaving the
oxidizer does not contain CO2 and water, which explains where Mactual is the actual molar mass of the carrier in
the presence of the xO2 ;ex in the numerator.) The air mass its partially oxidized state. The solids in the two reactors
ow is then are assumed to be well stirred, and the conversion of the
ṁo  solids is therefore equal to the conversion of the solid
ṁair = ; (6) ows leaving these reactors. Since oxygen is transferred
0:233
from oxidizer to the reducer, the average conversion is
where 0.233 is the mass fraction of oxygen in air. The higher in the oxidizer, Xox , than in the reducer, Xred , and
uidizing velocity in the oxidizer is the di8erence in conversion, VX , is
ṁair va; air Tox VX = Xox − Xred : (11b)
uox = ; (7a)
Aox Ta
The capacity of the carrier, C, de@ned as the ratio of a
where va; i is the speci@c volume of gas i at ambient tem- fractional mass increase to an increase in conversion, is
perature, Aox is the cross-section area of the oxidizer, Tox a measure of how much oxygen the carrier is able to
is the temperature in the oxidizer and Ta is the ambient transfer for a given change in conversion
temperature. Similarly the uidizing velocity in the re-
ducer is 1 dm
C= ; (12)
m dX
ṁfuel va; fuel Rr Tred
ured = ; (7b) where m is the mass. For a conversion, X , equal to unity
Ared Ta
the capacity, C, is equal to Ro , but the capacity increases at
where the subscript red denotes the conditions in the lower conversions. After some manipulation the capacity
reducer and Rr is the recirculation ratio, i.e. ratio of the can be expressed as a function of the conversion for the
total ow of gas supplied to reducer and the fuel ow. oxidizer and the reducer
The uidizing velocity is based on the unconverted fuel. Ro
If the fuel is methane each fuel molecule is converted Cox = ; (13a)
1 − (1 − Xox )Ro
to three molecules, and accordingly the actual uidizing
velocity increases with a factor of three as the reaction Ro
Cred = : (13b)
proceeds. The amounts of bed material in the oxidizer 1 − (1 − Xred )Ro
3106 A. Lyngfelt et al. / Chemical Engineering Science 56 (2001) 3101–3113

The required conversion rates in the oxidizer and the (ii) the amounts of H2 , hydrocarbons and non-com-
reducer then become bustible gases in the recirculated gas can be neglected

compared to CH4 and CO.
d X

ṁo
rox =
= ; (14a)
d t ox Cox mbed; ox The conversion of the gas in the oxidizer is simply


d X

ṁo 1
rred =
= : (14b) $ox = : (20b)
d t red Cred mbed; red 
The fan power, Pbed , necessary to overcome the pressure The present work discusses two oxygen carriers, Fe2 O3
drop, Vp, of the uidized beds is given by and NiO. In the case of Fe2 O3 , possible reduced forms
 (n−1)=n  include Fe3 O4 , FeO and Fe. The de@nition used for the
n p1 va ṁi p1 + Vp conversion of Fe2 O3 here is based on a full conversion to
Pbed = − 1 ; (15)
(n − 1) "fan p1 Fe, and the oxygen ratio is
MFe2 O3 − 2MFe
where n is the isentropic coeLcient, p1 is the inlet pres- Ro; Fe = ; (10b)
sure, here assumed to be ambient, ṁi is the mass ow of MFe2 O3
either air or fuel, and "fan is the eLciency of the fan. ’p , where Mi is the molar mass of species i. Similarly the
the fractional fan power to overcome the pressure drop carrier ratio of NiO is
is obtained as
MNiO − MNi
Pbed Ro; Ni = : (10c)
’p = : (16) MNiO
Pfuel
The power consumed by the fans is only partially lost,
since it is converted to thermal energy in the gas ows 6. Design criteria
entering the process. For this reason, the loss in eLciency
due to pressure drop, ’loss , depends on the overall eL- Design criteria were chosen for the layout of an at-
ciency of the power process, "tot : mospheric boiler with a power of 10 MW. Such a boiler
is suitable for the demonstration of the technology and
’loss = ’p (1 − "tot ): (17) for obtaining data and experience of the process in a
semi-commercial scale. The boiler could be used for heat
The mass ow of entrained solids from the oxidizer to production, for district heating or for industrial process
the reducer, ṁsol , is related to the di8erence in conversion steam. As seen in Fig. 2, the design resembles that of a
ṁo circulating uidized bed (CFB) boiler for combustion of
ṁsol = : (18a) solid fuels, thus using elements of proven technology. The
VXCox
boiler, when a demonstration=research programme is @n-
The mass ow of solids returned from the reducer to the ished, can therefore be converted to a conventional CFB
oxidizer is somewhat smaller, because of the oxygen used boiler, or conversely, an existing CFB boiler could be
in the reducer, converted to a CLC boiler. A full optimization is prema-
ture at this state of knowledge. Instead design data were
ṁsol; ret = ṁsol − ṁo : (18b)
chosen according to the following considerations, which
The conversion of the fuel, here CH4 , to CO2 , henceforth to some extent rely on experience from CFB boilers:
termed the gas yield, is
• The fuel is methane, since natural gas is a suitable fuel
xCO2
$red = ; (19) for a @rst application of the process.
xCO2 + xCH4 + xCO • The air ratio aims at keeping down the gas ow in the
where xi is the measured volume fraction of species i reactor, and yet have a suLcient oxygen concentration
in the product gas. The gas recirculation ratio, Rr , is the for high conversion rate of the solids.
actual amount of gas that has to be compressed after • The oxidizer cross-sectional area gives a similar
removal of the water divided by the CO2 produced. The gas velocity as in a CFB combustor, and the same
relation between gas yield and recirculation ratio is then cross-sectional area was chosen for the reducer, al-
though the gas velocity becomes smaller.
1
$red = (20a) • The temperatures reect the level where most of the
Rr experimental data are available at present. In the cal-
if the following assumptions are made: culations the choice of temperature only a8ects the gas
velocities. The temperature in the air reactor is some-
(i) gas losses from the recirculation loop can be ne- what higher because of the temperature fall in the fuel
glected except for the CO2 separated, reactor.
 A. Lyngfelt et al. / Chemical Engineering Science 56 (2001) 3101–3113 3107

Table 3 version rates of the oxygen carriers were 9%= min in the
Chosen or assumed parameter values oxidizer and 3%= min in the reducer and the required mass
Item Symbol Value Unit ow of solids between the two uidized beds is approx-
imately 50 kg= m2 s. These results are realistic judging
Power (fuel) Pfuel 10 MW
Flue gas oxygen xO2 ;ex 0.04 dimensionless
from the experimental data, as will be discussed below.
Oxidizer cross section Aox 2.5 m2 The reactivity of the carrier can be expressed in terms
Reducer cross section Ared 2.5 m2 of conversion rate. The conversion rates, rox and rred ,
Temperature oxidizer Tox 1243 K are in turn linked to the gas yields, $ox and $red , and to
Temperature reducer Tred 1223 K the conversion di8erence of the solids, VX . A lowered
Recirculation ratio Rr 1.05 dimensionless
Pressure drop, oxidizer Vpox 7 kPa
gas yield or conversion di8erence raises the conversion
Pressure drop, reducer Vpred 20 kPa rates. All three parameters are important input for design,
Voidage in bed  0.6 dimensionless as shown in Fig. 3, and the interdependence of these
Fan eLciency "fan 0.9 dimensionless parameters is important in the optimization of the process.
Ambient pressure p1 101 kPa Therefore, laboratory studies of oxygen carrier reactivity
Carrier properties
Density of oxygen carrier  5000 kg= m3
should not only show the conversion rate, but also how
Oxygen ratio Ro 0.3 dimensionless the rate depends on gas yield and conversion di8erence
Conversion in oxidizer Xox 0.98 dimensionless of solids.
Conversion di8erence VX 0.02 dimensionless
7.1. Comparison to experimental data on reactivity
Table 4
Constants Conversion rates of 200 m natural hematite particles
Item Symbol Value Unit were studied by Mattisson et al. (2000b). The particles
were cyclically exposed to air and methane in a @xed-bed
Lower heating value Hi 50 MJ=kg
Stoichiometric ratio Sr 2 dimensionless
reactor, thus simulating the environment of particles mov-
Ambient temperature Ta 293 K ing between the air and fuel reactor. The oxidation rates
Molar mass air Mair 29 kg=kmol were high, signi@cantly above the desired 9%= min. The
Molar mass fuel Mfuel 16 kg=kmol reduction rates were obtained as a function of gas con-
Molar mass oxygen M O2 32 kg=kmol version and conversion range, see Fig. 4. A 95% yield of
Speci@c volumea of air va; air 0.841 m3 = kg
Speci@c volumea of fuel va; fuel 1.50 m3 = kg
gas was obtained at a conversion rate of 3–4%= min and
Gravity acceleration g 9.81 m2 = s with a conversion di8erence of 2%. Consequently, the
Isentropic coeLcient n 1.4 dimensionless gas yield and conversion rates of Table 5 are ful@lled. In
a At
a later study much higher reduction rates were obtained
ambient temperature.
with synthetic particles of Fe2 O3 and Al2 O3 (Mattisson et
al., 2000a).
• The recirculation ratio is low to minimize the power The rate data in Table 5 were derived for Fe2 O3 , but
needed for compression of CO2 . most literature data are given on NiO, normally in com-
• The pressure drop in the oxidizer is similar to that bination with an inert binder material. For comparison,
of CFB combustors. The pressure drop in the reducer desired conversion rates were also determined for a car-
is higher than in the oxidizer, in view of the lower rier composed of 60% NiO, and 40% inert material. The
conversion rates of the reduction. assumptions and the results are given in Table 6. A higher
• The conversion di8erence is small, which will give a conversion rate is needed for the NiO=inert material than
large recirculation rate of solids. With a large recircu- for Fe2 O3 since the oxygen ratio is lower for NiO=Ni, and
lation rate the temperature di8erence between the re- this oxygen ratio is further reduced by the presence of
actors becomes small. inert material, cf. Eqs. (10); (13) and (14).
• The oxygen carrier is hematite, but a comparison is The reactivity data in Table 2 show approximate con-
made with data on NiO=YSZ. The particle size is version rates for di8erent VX , probably obtained at low
200 m, although this is not used in the calculations. gas conversions. Assuming a @rst-order reaction, the con-
version rate is proportional to the concentration of the
The design values are listed in Table 3. The constants reactant. The e8ective concentration of the reactant gas
used are given in Table 4. can be approximated by the logarithmic mean value
xin − xout
xave = ; (21)
ln(xin =xout )
7. Results and discussion
where xin and xout are the volume fractions of the reactant
Eqs. (3)–(20) together with the values of Tables 3 and gas entering and leaving the reactor. In the case of air,
4 give the results presented in Table 5. The required con- the assumed inlet and outlet volume fractions are 0.21
3108 A. Lyngfelt et al. / Chemical Engineering Science 56 (2001) 3101–3113

Table 5
Parameter values derived from the basic assumptions in Table 3

Item Symbol Value Unit Eq.

Fuel ow ṁfuel 0.2 kg=s (3)

Oxygen transferred ṁo 0.8 kg=s (4)
Air ratio  1.19 dimensionless (5)
Air ow ṁair 4.07 kg=s (6)
Fluidising velocity, oxidizer uox 5.7 m=s (7a)
Fluidising velocity, reducer ured 0.53 m=s (7b)
Bed mass, oxidizer mbed; ox 1529 kg (8a)
Bed mass, reducer mbed; red 5097 kg (8b)
Bed height, oxidizer hbed; ox 0.31 m (9a)
Bed height, reducer hbed; red 1.02 m (9b)
Carrier capacity, oxidizer Cox 0.30 dimensionless (13a)
Fractional conversion rate, oxidizer rox 9 %=min (14a)
Fractional conversion rate, reducer rred 3 %=min (14b)
Fan power for Vp in oxidizer Pbed; ox 26 kW (15)
Fractional fan power for Vp in oxidizer ’p; ox 0.26 % (16)
Fan power for Vp in reducer Pbed; red 6.3 kW (15)
Fractional fan power for Vp in reducer ’p; red 0.06 % (16)
Entrained solids mass ow from oxidizer ṁsol 133 kg=s (18a)
Return solids mass ow ṁsol; ret 132 kg=s (18b)
Gas yield in reducer $red 0.95 dimensionless (20a)

Fig. 3. The basic relations between carrier reactivity and design input data.

and 0.04, yielding a logarithmic mean of 0.1. This means
that the experimental conversion rates probably should
be reduced by a factor of two to allow a comparison with
the desired rates in Table 5. The oxidation rates of Jin et
al. (1998, 1999), about 20%= min, Table 2, therefore cor-
respond to approximately 10%= min, which is about half
of the desired 21%= min, see Table 6. These experimen-
tal values were, however, obtained for large particles and
smaller particles show much higher conversion rates, e.g.
90%= min, as seen in Table 2.
The concentration of the reactant gas leaving the fuel
reactor can be derived from the assumed recirculation
ratio, 1.05, yielding a logarithmic mean volume fraction
of methane of 0.24. The best data for comparison are
those with a 1:2 mixture of CH4 and H2 O, i.e. a volume
fraction of CH4 of 0.33 (Jin et al., 1999). Here the rate was
15%= min, Table 2, which, if corrected for partial pressure,
corresponds to about 10%= min, to be compared to the
desired 7%= min, Table 5. Again the laboratory data were
obtained for large particles and much higher conversion
rates were found for small particles, e.g. 210%= min, see
Table 2.
Thus, the literature data support the conclusion that
oxygen carriers can be found that ful@l the conversion
rates needed for the proposed design.
7.1.1. Bed mass and bed dimensions
The needed bed mass, i.e. the bed volume (cross-section
area × bed height), is determined by the conversion
rate, Eq. (14a) and (14b). A higher bed raises the power
 A. Lyngfelt et al. / Chemical Engineering Science 56 (2001) 3101–3113 3109

7.2. Conversion di7erence and solids exchange

An average conversion di8erence between the two re-

actors of 2% gives a recirculation of particles of 130 kg= s
(Eq. (18a)), or about 50 kg= s m2 . This value is simi-
lar to that measured in a CFB boiler of similar size at
a uidizing velocity of 5 m= s, a pressure drop over the
bed of 7 kPa and with silica sand particles of 0:32 mm
diameter (Johnsson & Leckner, 1995). The circulation
behaviour of the particles used corresponds to that of
0:2 mm hematite particles, because of the di8erence in
density. In conclusion, the required recirculation mass
ows are feasible. The recirculation mass ow depends
on uidizing velocity and particle size, and these must be
well matched to achieve a suitable solids ow.

7.2.1. Conversion of gas

Fig. 4. Conversion rate of reduction with methane as function of In many applications of chemical reactors it is diL-
conversion di8erence and gas yield (from Mattisson et al., 2000b). cult to obtain complete conversion. For instance, in nor-
mal combustion only a very small release of combustible
matter can be accepted because of environmental con-
Table 6 cern. In the present case there is no similar problem in
Oxygen ratio, assumed conversions and required reaction rates. (The the oxidizer or in the reducer:
values of VX were chosen to give similar recirculation solid ows)
(i) The air passing through the oxidizer does not
Oxygen carrier Ro Xox VX rred rox contain combustibles. (There is no need for a complete
(%=min) (%=min) conversion of the oxygen in this ow — an exit O2
Fe2 O3 0.30 0.98 0.02 3 9 concentration of 4% has been assumed.)
NiO 0.21 0.98 0.03 4 13 (ii) There is no gas emission from the fuel reactor.
NiO=inert 60=40 0.13 0.98 0.05 7 21 When water and CO2 have been condensed from the
reducer gas, the remaining combustible gases are recir-
culated to the fuel reactor. This gas loop is closed al-
though a minor fraction of this ow must be bled to the
consumption of the fan, Eq. (15). In Table 5 the frac- air reactor.
tional fan power consumptions are 0.26 and 0.06% for
the air reactor and the fuel reactor, respectively. A dou- Incomplete conversion of the gas from the fuel reactor
bled pressure drop in the air reactor therefore decreases increases the gas ow and the power consumption for
the overall eLciency with about 0.1%, cf. Eq. (17). Be- compression of CO2 to a liquid. Consequently, a high
cause of the much lower gas ow in the fuel reactor, conversion of the gas in the reducer is aimed at. Judging
the consequences of an increased pressure drop here are from the experimental data such a high conversion can
much smaller than in the air reactor. The cross-section be attained.
area a8ects the investment cost, and a small cross-section An important di8erence from normal combustion is the
area is desired. This leads to a high gas velocity; but the absence of homogeneous gas-phase reactions, at least in
gas velocity is limited by entrainment of bed material. the air reactor. Therefore, the gas residence time as such
is of little interest, and only the contact between gas and
solid phase is important. In the reducer, homogeneous
7.1.2. Reaction rates gas-phase reactions are possible, but it is not likely that
The conversion rates of the oxygen carriers are suL- they will improve the conversion, so again gas residence
cient. Nevertheless, higher rates are an advantage, since time is of little interest.
the bed masses can be reduced. The reaction rates can
probably be increased further by reducing the particle size 7.3. Leakage of gas between the two reactors
or by increasing the reaction temperature. Only a lim-
ited amount of work has been spent on @nding suitable The pressure in the two reactors should be approxi-
oxygen carriers and it is likely that these materials can mately equal in order to minimize gas leakage between
be improved, considering the many choices available for them. If gas leaks from reducer to oxidizer, combustible
making these particles. gases will be oxidized to CO2 and water in the oxidizer,
3110 A. Lyngfelt et al. / Chemical Engineering Science 56 (2001) 3101–3113

leading to a reduced capture of CO2 in the process. A Table 7

◦
leakage of gas into the reducer means that N2 enters the Reaction enthalpies at 1000 C. All reactions are normalized to 1 mole
of O2 . Based on data from Barin (1989, 1993), Barin, Knacke, and
gas recirculation loop. A minor amount of N2 , however, Kubuschewski (1973) and Knacke, Kubuschewski, and Hesselman
does not disturb the process, since it will be rejected with (1991)
the bleed. The leakage can be reduced by loop seals. If
these loop seals are uidized with steam there is no leak- Reaction VH (kJ= mol) VH=VHdir; comb
age of CO2 into the oxidizer and no leakage of N2 into O2 + 1=2CH4 → 1=2CO2 + H2 O −401:39 1.00
the reducer. O2 + 4=3Fe → 2=3Fe2 O3 −539:12 1.34
O2 + 4FeO → 2Fe2 O3 −554:29 1.38
O2 + 4Fe3 O4 → 6Fe2 O3 −481:04 1.20
7.4. Emissions of gas, liquid and solids O2 + 2Ni → 2NiO −467:96 1.17
O2 + 2Co → 2CoO −466:67 1.16
The air introduced to the oxidizer does not give any O2 + 3=2Co → 1=2Co3 O4 −446:65 1.11
harmful emissions. The temperature is too low for the O2 + 2Cu → 2CuO −296:25 0.74
O2 + 4Cu → 2Cu2 O −331:71 0.83
formation of thermal NOx , as veri@ed by Ishida et al. O2 + 2Mn → 2MnO −772:49 1.92
(1996). The bleed from the recirculation loop causes mi- O2 + 4MnO → 2Mn2 O3 −359:17 0.89
nor amounts of combustible gases to enter the oxidizer, O2 + 6MnO → 2Mn3 O4 −449:45 1.12
where they are oxidized to CO2 and water.
The condensed water from the reducer gas may contain
minor amounts of combustible gases. By leading an air-
ow through the condensate such gases could be brought 7.5. Temperature
to the oxidizer to be burnt. Formation of soluble organic
compounds is not expected, but if this should be the case, The choice of process temperature is important. There
the condensed water can be treated in a sewage plant. are three aspects to be considered:
Bed particles, or fragments of bed particles, may be
entrained with the gas ow, but @lters reduce such emis- • Higher temperature, in general, enhances the reaction
sions to a very low level. Bed material probably has to be rates (e.g. Ishida et al., 1996) and therefore reduces
exchanged in order to maintain the reactivity of the oxi- the amount of bed material.
dizer. The exit stream of oxygen carrier must be reacti- • Extremely high temperature may give technical prob-
vated, @nd alternative use or be disposed of. Thus, carrier lems, such as sintering of bed material.
material has to be handled outside the reactors and health • High temperature, in the case of a combined
and environment aspects of the carrier material have to gasturbine=steam cycle is essential for high eLciency,
be considered. but a high temperature in the turbine inlet can also be
achieved by burning fuel after the oxidation reactor.
The latter reduces the CO2 captured in proportion to
7.4.1. Fuel the fraction of fuel used, unless hydrogen is used as
Fossil gas can be used directly in CLC, but solid fuels fuel. (Other CO2 capture processes are often designed
@rst have to be gasi@ed. If used directly the solid fuel for capture of about 90% of the CO2 .)
particles would follow the particle recirculation loop and
burn in the oxidizer. The factors limiting bed temperature have to be further
analysed. They are probably connected to the choice of
7.4.2. Heat balance bed material.
By dividing the reaction enthalpy of oxidation with Because of the endothermic reactions in the fuel reac-
that for combustion of methane, the heat release in the tor, the recirculation mass ow must be suLcient to pre-
air reactor is obtained relative to that of conventional vent a large temperature drop in the fuel reactor. Fig. 5
combustion, see last column in Table 7. For instance, shows the temperature decrease in the fuel reactor versus
for oxidation of Ni the heat release is increased by 17%, the conversion di8erence. The latter is inversely propor-
and the corresponding amount of energy is absorbed by tional to the mass ow, Eq. (18a).
the endothermic reaction in the fuel reactor, since the
total heat of reaction is the same as for conventional 7.5.1. Pressure
combustion. This leads to a temperature fall in the fuel It is reasonable to operate a @rst application of this pro-
reactor. Most oxygen carriers give such a temperature cess at ambient pressure. However, the process should be
fall, and therefore the fuel reactor is normally not cooled developed for use under pressurized conditions because
(Table 7). The cooling of the system is similar to that of
a CFB boiler, and can take place in the air reactor or in a (i) The process should be included in a combined gas
particle cooler operating on the recirculating solids ow turbine=steam power cycle for a high overall eLciency
either in parallel to or after the fuel reactor. of electricity production.
 A. Lyngfelt et al. / Chemical Engineering Science 56 (2001) 3101–3113 3111

sion of the gas ows, the yield, is suLcient. Thirdly, the

capacity of the oxygen carrier is high enough to transfer
oxygen between the two reactors with a realistic mass
ow of solids.
The analysis is mainly concerned with the layout of
the combustion process. Yet, some important conclusions
can be made for the use of this process in a power cy-
cle. There are, so far, no evident obstacles for the use of
CLC in a high eLciency combined cycle for power pro-
duction. Before any @nal conclusions can be made in this
respect, however, more work is needed to assess the po-
tential of di8erent oxygen carriers at high temperatures
and elevated pressures. This @rst tentative design of a
chemical looping combustor shows the feasibility of the
process, and that such a combustor should involve an in-
vestment cost which is in the same order as for a uidized
bed boiler.

Fig. 5. Temperature di8erence between air and fuel reactor. Full

conversion to FeO and Fe3 O4 corresponds to a V X of 0.33 and 0.11,
respectively, which explains the ending of these lines. Notation

Aox oxidizer cross section, Table 3, m2

(ii) A higher pressure is expected to give higher reac- Ared reducer cross section, Table 3, m2
tion rates with the corresponding reduction of the amount C carrier capacity, Eq. (12), dimensionless
of bed material, and furthermore, a greater cross-sectional Cox carrier capacity, oxidizer, Eq. (13a), dimen-
mass ow of gas is possible because of higher density of sionless
the gas. As a consequence of these two e8ects the com- Cred carrier capacity, reducer, Eq. (13b), dimen-
bustion chambers can be reduced signi@cantly in size. sionless
g gravity acceleration, Table 4, m2 = s
The experience from developing pressurized uidized- hbed; ox bed height, oxidizer, Eq. (9a), m
bed combustion (PFBC) for solid fuels is useful, hbed; red bed height, reducer, Eq. (9b), m
although pressurized CLC is di8erent in many ways. In Hi lower heating value, Table 4, MJ= kg
a coal-@red PFBC there are large outgoing solid ows, mbed; ox bed mass, oxidizer, Eq. (8a), kg
i.e. fuel ash and sorbent for sulphur capture, to be sep- mbed; red bed mass, reducer, Eq. (8b), kg
arated and handled. In the pressurized CLC process the ṁair air ow, Eq. (6), kg= s
fuel is ash-free and the only outgoing ows of solids are ṁfuel fuel ow, Eq. (3), kg= s
oxygen carrier particles, leaving the system because of ṁo oxygen transferred, Eq. (4), kg= s
particle attrition=fragmentation or because the oxygen ṁsol; ret return solids mass ow, Eq. (18b), kg= s
carrier has to be substituted due to a loss in reactivity. ṁsol entrained solids mass ow from oxidizer, Eq.
In chemical-looping combustion the properties of the (18a), kg= s
oxygen carrier can be optimized to minimize these ows. Mfuel molar mass fuel, Table 4, kg= kmol
MO 2 molar mass oxygen, Table 4, kg= kmol
Mair molar mass air, Table 4, kg= kmol
8. Conclusions n isentropic coeLcient, Table 4, dimensionless
p1 ambient inlet pressure, Table 3, Pa
A design of a combustor based on chemical-looping Vpox pressure drop, oxidizer, Table 3, Pa
combustion with two interconnected uidized beds is pro- Vpred pressure drop, reducer, Table 3, Pa
posed. The required reactivities of oxygen carriers, suit- Pbed; ox fan power for Vp in oxidizer, Eq. (15), W
able for such a process, are estimated. It is concluded Pbed; red fan power for Vp in reducer, Eq. (15), W
from the limited experimental data on oxygen carriers Pfuel power (fuel), Table 3, MW
available in the literature that the process outlined is real- rox fractional conversion rate, oxidizer, Eq.
istic. Firstly, the reaction rates for both reduction and ox- (14a), %= s
idation are suLcient in terms of the bed masses needed. rred fractional conversion rate, reducer, Eq.
This means that the dimensions of the reactors, as well as (14b), %= s
the pressure drops, are reasonable. Secondly, the conver- Ro oxygen ratio, Eq. (10), dimensionless
3112 A. Lyngfelt et al. / Chemical Engineering Science 56 (2001) 3101–3113

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