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Chemical Looping Combustion: Status and Development Challenges

Anders Lyngfelt*

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ABSTRACT: Because the CO2 capture is inherent in chemical looping combustion (CLC), thus ideally avoiding costly gas
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separation, this process has potential for uniquely low costs of CO2 capture. The review reports on operational experiences with
different oxygen carriers in CLC pilot operation. Further, the application to solid fuels is discussed in terms of technology challenges,
routes for upscaling to commercial size, downstream gas treatment, options for achieving adequate circulation, and the use of
biofuels in CLC to reach negative emissions. It is concluded that the necessary elements for a scale-up are at hand. Oxygen carrier
materials of low cost have been tested in extended operation and found to have reasonable performance with respect to reactivity
and lifetime. Designs for large-scale units have been performed, indicating that the process is technically realistic and should have a
low cost of CO2 capture. A scale-up strategy to minimize risk and costs has been suggested.

1. INTRODUCTION with different oxygen carriers, different fuels, and in different

Chemical looping combustion (CLC) has emerged as an
attractive option for carbon dioxide capture because CO2 is
inherently separated from the other flue gas components.
Ideally, no gas separation equipment is needed, and no energy is
expended for gas separation. The CLC system is normally
composed of two interconnected fluidized bed reactors: an air
reactor and a fuel reactor (Figure 1). Oxygen carriers in the form
Figure 1. CLC principle. MexOy is the metal oxide circulated.
of metal oxide particles transfer oxygen between the two
reactors. Thus, the fuel reacts with the oxygen carrier in the fuel
reactor and forms CO2 and H2O, and after condensation of
H2O, the flow coming from the fuel reactor will consist of more
or less pure CO2. The oxygen carrier is then regenerated in the
air reactor.
pilots; oxygen carriers and laboratory examinations,10−13 and
material overviews in Ph.D. theses;14−17 solid fuels;18−24 pilot
designs;1,25,26 and process concepts,27 including one book on
chemical looping systems.28
Other important aspects are lifetime and material integ-
rity,29,30 thermodynamic properties of oxygen carriers,31,32 with
the latter focusing on combined manganese materials, and
chemical looping with oxygen uncoupling (CLOU), i.e., the
ability of some oxygen carriers to release gaseous oxygen.32−35
This paper will present operational experiences with oxygen
carriers in pilots and also discuss the future development of CLC
technology.
2.2. Applications of CLC. Chemical looping or CLC
normally refers to combustion or partial combustion using an
oxygen carrier to transfer oxygen from air to fuel. Although some
other schemes have been proposed, the normal approach is the
use of interconnected fluidized beds, where the oxygen carrier
constitutes the bed material. The oxygen carrier particles
circulate between the two beds, commonly called air and fuel
reactors, thus transferring oxygen from air to fuel.
An important aspect of the CLC process is the fuel used.
Gaseous fuels: Gas-CLC could include fuels, such as natural gas,
refinery gas, or off-gas from steam reforming. Further, gas
coming from gasification of solid fuels is, from a process point of
view, also a gaseous fuel, even if the primary fuel is solid. Solid
fuels: SF-CLC could be applied to fuels, such as coal, petroleum
coke, biomass, and waste. If biomass and biogenic waste are
used, CO2 captured could be used for negative emissions. SF-

2. BACKGROUND Received: May 7, 2020

2.1. Previous Work on Chemical Looping. A number of Revised: June 23, 2020
reviews of CLC research have been published, with different Published: June 25, 2020
focuses, including overall reviews,1−8 with the first two being the
most comprehensive and the last being the most recent;
operational experiences,9 involving 11 000 h of pilot operation

© 2020 American Chemical Society https://dx.doi.org/10.1021/acs.energyfuels.0c01454

9077 Energy Fuels 2020, 34, 9077−9093
Energy & Fuels
CLC adds some complications to the process compared to gas-
CLC. However, the application to solid fuels is facilitated by the
large experience of burning solid fuels in fluidized bed boilers.
Thus, a CLC boiler could have large similarities to a circulating
fluidized bed (CFB) boiler. Liquid fuels: LF-CLC could be used
for any liquid fuel, but the most likely interest would be the use
of cheaper and dirtier fuels, such as heavy oil.36
Another aspect of CLC is the reaction mechanism.
Heterogeneous CLC involves a gas−solid reaction mechanism,
where gaseous combustibles react directly with the oxygen
carrier. This is also the normal and most studied form of CLC.
Chemical looping with oxygen uncoupling or CLOU involves a
two-step reaction, where the oxygen carrier, when subject to the
low oxygen concentration in the fuel reactor spontaneously
releases gaseous oxygen that subsequently reacts with the
gaseous, liquid, or solid fuel. Heterogeneous CLC and CLOU
may occur in parallel and, in some cases, it could also be difficult
to safely distinguish between the two mechanisms.
CLOU is a reaction mechanism of CLC that may improve the
conversion of gaseous, liquid, and solid fuel. The material with
the strongest CLOU properties is the CuO−Cu2O system, but a
number of combined manganese oxides as well as natural
manganese ores have been shown to have more or less ability to
release oxygen. Also, ilmenite ore has been shown the ability to
release small amounts of oxygen.37 Thus, CLOU is not a
different process but rather a reaction mechanism that may take
place instead of or in parallel with heterogeneous CLC. The
contribution from each of these two reaction mechanisms could
be difficult to establish and would be dependent upon the fuel,
the temperature, the oxygen carrier, and the reactor design as
well as other operational conditions.
Often in situ gasification chemical looping combustion (iG-
CLC) is used with the same meaning as SF-CLC, but other
times it is used to indicate chemical looping of solid fuels in a
process where no CLOU takes place, i.e., heterogeneous CLC.
The name iG-CLC could be confusing, because it gives
associations to gasification processes, although heterogeneous
CLC is a combustion process where the gasification is not a
separate process step but rather a reaction step or part of a
reaction mechanism. Further, iG-CLC should not be confused
with integrated gasification chemical looping combustion
(IGCLC). Thus, the term iG-CLC is not used here.
Further, CLC can have different purposes, i.e., power/heat
production or fuel production (Table 1). In the latter case,
partial oxidation may be used.
Table 1. Purpose of CLC
oxidation
output full oxidation partial oxidation
power/heat CLC combustion
for heat/power
fuel CLR-S, chemical CLR-A, chemical CLG, chemical
looping with looping autother- looping gasifica-
steam reforming mal reforming tion of solid fuels
Fuel production can be devised in different schemes. For solid
fuels, chemical looping gasification (CLG) can be used to
convert solid fuel into combustible gases. There may be
advantages compared to thermal gasification in a dual fluidized
bed with respect to, e.g., gas composition, but an obvious
advantage is that CO2 will be in the concentrated product stream
from the fuel reactor and, thus, less costly to capture.
pubs.acs.org/EF Review
Moreover, for instance, natural gas could be partially oxidized
with the purpose to produce hydrogen, by autothermal chemical
looping reforming (CLR-A).38
CLR-S is an attractive scheme for converting methane to
hydrogen, which combines conventional steam methane
reforming (SMR) with CLC of the off-gas from the reforming.39
CLC would then provide the necessary heat for the endothermic
SMR and, at the same time, capture all carbon in the process,
CLR-S is close to conventional reforming, except that heat is
transferred from combustion to the reformer tubes using a
fluidized bed heat exchanger instead of gas burners. The more
efficient heat transfer makes the significantly lower temperature
outside of the reforming tubes possible, leading to lower heat
losses, i.e., higher reforming efficiency. Thus, the energy penalty
of capturing CO2 in this process could be negative, if the
necessary compression of captured CO2 is excluded.
2.3. CLC of Solid Fuels. With solid fuels, the reaction
between the char remaining after the release of the volatiles and
the oxygen carrier is not direct but involves an intermediate
gasification step, as outlined in Figure 2.
Figure 2. Solid fuel reactions in CLC.
Both release of volatiles and char gasification have
implications for the design of the fuel reactor. Ideally, the fuel
would be completely converted to CO2 and H2O in the fuel
reactor. In the case of solid fuels, a fully oxidized gas is normally
not attained, which can be remedied by, e.g., adding oxygen in a
post-oxidation chamber downstream of the fuel reactor, so-
called “oxy-polishing”. Figure 3 illustrates the three deviations
Figure 3. Inadequate performance of the fuel reactor.
from the ideal case: (i) loss of combustible gases, such as H2,
CO, and CH4, in the gas leaving the fuel reactor, (ii) loss of char
to the air reactor, and (iii) loss of char with the gas leaving the
fuel reactor. The corresponding performance indicators are as
follows: (i) Oxygen demand, ΩOD, is oxygen required to oxidize
unburnt gas leaving the fuel reactor to CO2 and H2O over total
oxygen needed to oxidize the gases released from the fuel in the
fuel reactor. 1 − ΩOD is the gas conversion. The oxygen demand
indicates oxygen needed for oxy-polishing. (ii) CO2 capture,
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Energy & Fuels
ηCO2, is the fraction of gaseous carbon leaving the fuel reactor
related to total carbon converted to gas in fuel and air reactors.
Thus, 1 − ηCO2 represents the ratio of carbon lost as CO2 from
the air reactor to total carbon in gaseous compounds leaving air
and fuel reactors. (iii) Fuel conversion, ηF, is used to indicate the
char conversion and is defined as the ratio of carbon converted
to gaseous compounds in the fuel and air reactors to total carbon
added. Consequently, 1 − ηF is the fraction of total carbon added
that is elutriated from the fuel reactor in the form of char.
2.4. Barriers for Chemical Looping Technology. There
are several barriers for implementing CLC technology to
consider. (1) Incentives missing: At present, the climate targets
decided at the Paris meeting in 2015 have not yet been translated
into adequate incentives to accomplish the needed reduction in
emissions. (2) Confined process understanding: The process is
not well-known and understood outside the CLC community.
The CLC concept is a fundamentally novel principle of
converting fuels. Although a full-scale CLC boiler could have a
design largely similar to a CFB boiler, the reactions happening
inside are not normal combustion. The present knowledge,
understanding, and experience of this process, however, mainly
reside with a limited number of research groups that have been
operating small CLC pilots. (3) Risk of investment: A related
barrier is the risk of investment in a new technology not proven
in large scale. Closely related to this are the inherent difficulties
in the scaling up of fluidized bed technologies. It is evident that
the results in small pilots are not directly translatable to the large
scale. Thus, extrapolation of performance in the small scale to
large scale is uncertain. This also means that there are
uncertainties regarding the adequate full-scale design. Tech-
noeconomic designs have been proposed, e.g., for a 1000 MWth
design,40 but a fully optimized design could look different. (4)
No clear evolution path: Development of a novel technology is
easiest if it could proceed in small steps, going successively from
smaller to larger sizes, and build on accumulated experiences.
However, to meet climate goals, CO2 capture technology is
needed soon, and moreover, CO2 capture normally only makes
sense in a large scale and in direct connection with the
possibilities to store CO2. (5) The right choices in full-scale
design: Although there is significant small pilot experience, this
is only partly relevant for the large scale where other aspects of
the design need careful consideration. Because the small pilot
results cannot safely be translated to full scale, the large size
needs to be designed to accommodate some uncertainty in
performance.
A few reflections on these barriers are as follows: (1) If there
should be any reasonable chance of meeting the climate targets,
strong incentives will be necessary, and it is therefore reasonable
to expect these will come. (2) It is important that the CLC
community communicates the good results and the applicability
of the results and develops a close cooperation with industry and
society. (3) It is necessary that mechanisms for financing this
development are in place, which will be dependent upon
adequate incentives in combination with relevant measures to
support the phase of up-scaling. (4) The need to have an
accelerated development with a reduced number of steps to
reach full scale is facilitated by the large experience with the
closely related CFB technology. Further, there may be
opportunities to facilitate the demonstrations, as will be
discussed in section 8. (5) The first design of a demonstration
plant at scale will likely not be optimal, but to ensure successful
operation, it needs to be flexible and able to accommodate for
pubs.acs.org/EF Review
the uncertainties in predicting the detailed behavior in large
scale. On the other hand, there should be a multitude of ways to
configure this process that works. There is really no good reason
that the technology should not work sufficiently well at scale,
except possibly mistakes in the design.
Although there are barriers to overcome, this technology also
comes with a unique possibility for dramatic reduction of costs
and energy penalties.
3. OXYGEN CARRIERS: OPERATING EXPERIENCE
Today, chemical looping operation in the literature involves
more than 11 000 h of operation with fuel in more than 49 pilots.
A majority of the operational experiences with chemical looping
combustors uses gaseous fuels and manufactured oxygen
carriers. The operational experience in pilots with manufactured
materials is more than 8000 h, of which materials based on Ni
has been mostly used (cf. Table 2). Other commonly tested
Table 2. Reported/Estimated Operational Experiences from
222 Publications
type oxygen carrier time of operation (h)
manufactured NiO 3291
CuO 1455
Mn3O4 91
Fe2O3 1842
CoO 178
combined oxides 1480
natural ore or waste material Fe ore 1075
ilmenite 1524
Mn ore 735
CaSO4 75
total manufactured 8337
total natural/waste 3409
total 11746
materials are based on Cu, Fe, and combined oxides. A number
of previous literature reviews have presented the advantages and
disadvantages with the various monometallic oxides.1,6,11 In
recent years, there has been an increased interest in combined
oxides usually based on manganese combined with, e.g., Ca, Fe,
and Si, because these may have partial CLOU properties.
In the case of chemical looping operation with solid fuels, low-
cost materials, such as ores or waste materials, are often used.
First, because most solid fuels contain ash, which is expected to
reduce the possible lifetime of the oxygen carrier, and second,
because the hydrocarbons of typical gaseous fuels, such as
natural gas, require more reactive oxygen carrier materials than
the gas released from solid fuels, which contains more of the
reactive gases, H2 and CO. Low-cost materials include iron ores
and iron-based waste materials, ilmenite, and manganese ores.
3.1. Manufactured Materials. Operational experiences
with nickel-based materials are shown in Table 3. The oxidized
and reduced forms are NiO and Ni. These materials dominated
the earlier phases of CLC development, which had focus on
natural gas because of their high reactivity toward methane.
Typically, nickel oxide is supported on Al2O3 or MgAl2O4. The
high reactivity toward methane is likely associated with the
reduced form, i.e., metallic nickel, being a reforming catalyst.
The drawback with nickel materials is the high cost and health,
safety, and environmental concerns. There is also a thermody-
namic constraint that prevents gas conversion to around 99%
depending upon the temperature.
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Table 3. Operation with Nickel-Based Oxidesa oxides (Table 5). The oxidized form is Mn3O4, and the reduced
location unit time (h) fuel reference
form is MnO.
Chalmers 10 kW 1265 NG 41−44
Table 5. Operation with Manufactured Manganese-Based
KIER 50 kW 3 NG 45
Oxides
Chalmers 0.3 kW 363 NG/SG 38 and
46−50 location unit time (h) fuel reference
CSIC 0.5 kW 693 CH4, LHC, 51−64
CH4 + H2S, SG, Chalmers 0.3 kW 70 NG, SG 118
H2, CO, SG, LHC, Chalmers 0.3 kW LF 17 kerosene 112
ethanol, diesel, oil,
bioethanol
KAIST 1 kW 6 CH4 65 Iron oxides generally have a lower reactivity toward methane
Vienna UT 140 kW 272 NG, CO, H2, 66−77 compared to the other monometallic oxygen carriers. Never-
NG + H2S theless, the reactivity toward syngas is reasonable. The oxidized
Alstom 15 kW 100 NG 78 and reduced forms are Fe2O3 and Fe3O4. Lower oxidation states,
Nanjing 10 kW SF 230 coal, sawdust 79−81 e.g., FeO and Fe, may occur under highly reducing conditions
KIER 50 kW new 100−200 NG, SG 82 but are not possible for full oxidation of the gas. Operational
Nanjing 1 kW SF 30 coal 83 and experiences with manufactured iron oxide materials are given in
84 Table 6.
IFP-Lyon 10 kW GSF 18 CH4 85
Chalmers 0.3 kW LF 54 kerosene 86
Table 6. Operation with Manufactured Iron-Based Oxides
Nanjing 25 kW G >7 rice straw 87
KIER 200 kW 100 NG, SG 88 time
a location unit (h) fuel reference
Abbreviations used in Tables 2−11: SF, solid fuel; LF, liquid fuel;
GSF, gaseous, liquid, and solid fuel; G, Gasification; Pr, pressurized; Chalmers 10 kW 17 NG 42
NG, natural gas; SG, syngas; PC, petroleum coke; LHC, lower Chalmers 0.3 kW 40 NG/SG 119
hydrocarbons, e.g., ethane and propane; and PSA-OG, pressure swing CSIC 0.5 kW 164 PSA-OG, CH4, 96, 97, and
adsorption off-gas. CH4/H2S, sour gas, 120−122
acid gas
CSIC 1 kW LF 77 ethanol, diesel, oil 60 and 123
KAIST 1 kW 2 CH4 65
Copper oxides have also been studied extensively, with the Vienna UT 140 kW 34 NG 103 and
oxidized and fully reduced form being CuO and Cu. However, 124
CuO is also an excellent CLOU material, with the reduced form Nanjing 10 kW SF 30 biomass 125
being Cu2O. Early laboratory studies or operation did not Ohio 25 kW >300 CH4 126−132
consider the CLOU mechanism, for several reasons, for Ohio 25 kW SF 680 coal
instance, CuO reacting with the support added in excess, Guangzhou 10 kW G 62 sawdust 133−135
Al2O3, forming CuAl2O4 with low CLOU ability. The discovery NCCC 250 kW 360 SG + propane 136
of the strong CLOU potential of CuO has caused an increased Babcock and 250 kW 62 coal 137
interest for copper oxide for both gaseous and solid fuels. The Wilcox
operational experiences are given in Table 4. Ohio 15 kW 11 CH4 138
Despite being less costly than nickel and copper oxides and ITRI 30 kW 3 CH4 139
generally more reactive than iron oxide, little operation has been
reported with manufactured materials based on manganese In addition to the four main monometallic oxides considered
for CLC, there has also been some operation using the cobalt
Table 4. Operation with Copper-Based Oxides oxide system, CoO/Co (Table 7). Cobalt is more toxic and

time Table 7. Operation with Cobalt-Based Oxides

location unit (h) fuel reference
location unit time (h) fuel reference
CSIC 10 kW 120 NG 89 and 90
KIER 50 kW 28 NG 140
Chalmers 0.3 kW 23 NG 91
KIER 50 kW new 100−200 natural gas, SG 82
CSIC 0.5 kW 589 SG, LHC, CH4, sour 92−100
gas, acid gas
CSIC 1 kW LF 27 ethanol 60 costly compared to nickel, and thermodynamics restrict the
CSIC 0.5/1 kW LF 50 diesel, oil 62 conversion of methane to carbon dioxide to 95−97%. On the
Vienna UT 140 kW 130 syn, NG, NG (with 101−104 other hand, there might be a potential for CLOU using the
H2S) system Co3O4/CoO.33
CSIC 0.5/1.5 kW SF 168 coal, lignite, biomass, 105−111 Combined oxides are oxides where more than one oxide is
lignite, olive stone,
sawdust, almond chemically combined, for example, calcium manganite,
shell CaMnO3−δ. Many of the combined oxides studied include
Chalmers 0.3 kW LF 45 kerosene 112 manganese. This is because the combination of manganese with
WKentuU 10 kW 24 NG, syn 113 many other oxides, such as Ca, Fe, Si, Mg, Cu, and Ni, raises the
IFP 10 kW 270 CH4 114 and oxidation level of manganese. This also gives these combined
115 oxides partial CLOU properties, which have been demonstrated
SINTEF 150 kW 4 CH4 116 in the laboratory and explained by thermodynamic studies.32
Hamburg 25 kW SF 5 hardwood, lignite 117 Other examples of combined materials are Fe−Cu oxides.
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Because some of the previously mentioned monometallic Table 9. Operation with Natural/Waste Iron Oxide Materials
oxygen carriers actually react partially or fully with their support
time
materials, forming new oxides, the dividing line between location unit (h) fuel reference
monometallic and combined oxides is difficult to set. Here,
Chalmers 0.3 kW 57 SG SG, CH4 171 and
the dividing line is the intention, i.e., metal oxides, which happen 172
to fully/partially combine with material with the purpose of CSIC 0.5 kW 161 CH4,SG, PSA off-gas 173 and
being a support, are still considered monometallic. Operation 174
with combined oxides is shown in Table 8. In operation with Nanjing 1 kW SF 165 coal, sawdust, 175−185
anthracite, sewage
sludge
Table 8. Operation with Manufactured Combined Oxides CSIC 0.5/1.5 kW SF 206 coal, biomass, 186−191
anthracite, lignite,
time sawdust, olive
location unit (h) fuel reference stone, almond shell
Chalmers 10 kW 288 NG 141, 143, Chalmers 100 kW SF 26 wood char, two coals 192
and 144 Huazhong 5 kW G/SF 200 CH4, coal 193 and
Chalmers 0.3 kW 496 NG, syn, CH4, 145−154 194
kerosene and 154 Nanjing 25 kW G >6 rice husk 195
Chalmers 10 kW SF 106 wood char, petcoke, 155−157 Nanjing 50 kW Pr SF 19 coal 196
coal, lignite
Nanjing 20 kW SF 70 coal 197
CSIC 0.5 kW 81 CH4/H2S, CH4, syn 158 and
159 Huazhong 50 kW SF 8 coal 198 and
199
Vienna UT 140 kW 64 NG, NG (+H2S) 103, 124,
and 160 Zabrze 10 kW 3 CH4 200
Xi’an 10 kW Pr 15 coke oven gas 161 NETL 50 kW 2 NG 201
Jiaotong CSIC 50 kW SF 35 olive stone, sawdust, 202 and
Darmstadt 1 MW 80 NG 162 and coal 203
163 Chalmers 10 kW SF 28 wood char, wood 172
NETL 50 kW 91 NG, CH4 164−167 pellets
Chalmers 10 kW LF 10 heavy fuel oil 36 Darmstadt 1 MW 42 coal, torrefied 204
biomass
CSIC 0.5/1.5 kW SF 160 lignite, olive stone, 110, 111,
sawdust, almond 159, and Nanjing 5 kW SF/s 16 sewage sludge, coal 205−207
shell, coal 168 Nanjing 5 kW SF/i 6 biomass, CO 208
IFP 10 kW 75 CH4 169 Nanjing 2 kW 12 SG, NG 209
Chalmers 100 kW SF 18 biomass 142 and Nanjing 25 kW SF 13 coal 210 and
170 211

natural gas, full conversion and oxygen excess have been possible
to reach with calcium manganite,141 and also, with solid fuels,
very high conversion has been shown.142
3.2. Natural Ores or Waste Materials. Reported use of
iron ores or iron-based waste materials are given in Table 9. The
obvious advantage of iron materials is the low cost and large
availability. A number of different iron ores have been
successfully used in operation as well as some iron-based
waste materials. Interestingly, the work also includes results
from a pressurized unit.
The first operation of solid fuels in CLC used ilmenite ore,
and ilmenite is also the most used low-cost material in operation
(Table 10). The mineral ilmenite, FeTiO3, is the reduced form,
whereas the oxidized form is Fe2TiO5 + TiO2.212 There is also
considerable operational experience with ilmenite as bed
material in fluidized bed combustion (FBC); more than
12 000 h of operation in a 75 MWth circulating fluidized bed
boiler has been reported.213 When used in FBC, the purpose is
to improve combustion, which is called oxygen-carrier-aided
combustion (OCAC).
The operational experience with manganese ores is smaller
than with ilmenite or iron ores (see Table 11). This is a bit
surprising because manganese ores generally appear to be more
reactive than both iron ores and ilmenite. A possible explanation
could be that the manganese ores are less easy to access.
Published results with calcium sulfate as the oxygen carrier are
available from Alstom’s 3 MW pilot (see Table 12), where
fluidized bed boiler ash containing sulfated limestone was used.
The oxidized and reduced forms are CaSO4 and CaS. A
challenge with using calcium sulfate is controlling the release of
9081
sulfur. This is because of a thermodynamic complication; the
shifts between oxidizing and reducing conditions, where CaSO4
and CaS are stable, pass through an intermediate region, where
CaO is stable and, thus, SO2 is released.262
The literature presented above indicates that a number of low-
cost materials have been shown to work in actual operation.
Because the reported work has been performed in a number of
different units at different conditions, general comparisons are
not so easy. However, comparisons can be made from different
materials operated in the same unit. In the case of ilmenite and
iron ores, which have been operated at the Spanish National
Research Council (CSIC) and Chalmers, there are contradicting
results.
Comparisons between results with ilmenite and manganese
ores have been made at the two units at Chalmers, clearly
indicating that manganese ores give a higher conversion of the
gas, which is also consistent with laboratory investigations
covering 25 materials.254,264,265 Moreover, the presence of
potassium in manganese ores may promote the steam
gasification of the char.266 On the other hand, manganese ores
show higher loss of fines compared to ilmenite, although the
attrition rates vary between different manganese ores.
3.3. Operating Experiences with Solid Fuels. In total,
3787 h of operation with solid fuels has been reported, half with
low cost oxygen carriers. Thus, operation with solid fuels also
involves work with manufactured materials, including nickel
materials, copper materials, and iron materials, as well as the
combined oxides, calcium manganite, Mn−Si−Ti oxide, and
Cu−Mn oxide. In the case of copper materials, very high
performance can be reached; i.e., complete gas and fuel
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Table 10. Operation with Ilmenite Ore

location unit time (h) fuel reference
Chalmers 0.3 kW 168 NG, SG 171 and 214
Chalmers 10 kW SF 114 coal, petcoke 215−220
Vienna UT 140 kW approximately 160 CH4, CO, H2 72, 73, and 221
Stuttgart 10 kW 1 SG 222
CSIC 0.5/1.5 kW SF 170 coal, lignite 223−227
Chalmers 0.3 kW LF 80 kerosene 228
Chalmers 100 kW SF 88 coal, wood char 229−235
Hamburg 25 kW SF 90 CH4, coal, lignite, biomass 236 and 237
Chalmers 10 kW LF 70 diesel, heavy fuel oil 36 and 238
CSIC 50 kW SF 62 coal 239−241
Darmstadt 1 MW 73 coal 204, 242, and 243
Tsinghua 0.2 kW 140 CO 244
Chalmers 1.4/10 MW 61 biomass 245
VTT 20 kW 16 biomass 246
SINTEF 150 kW 5 wood pellets 247
CSIRO 10 kW SF 35 brown coal 248
Tsinghua 30 kW SF 100 coal 249
JCOAL 100 kW GSF 71 NG, coal 250
Vienna UT 80 kW SF 20 wood pellets 251

Table 11. Operation with Manganese Ores

time
location unit (h) fuel reference
Chalmers 0.3 kW 134 NG, syn vol, syn, CH4, 152, 154,
kerosene and 252
Chalmers 10 kW SF 89 petcoke, wood char, pet 220 and
coke, wood pellets, coal 253−255
IFP-Lyon 10 kW GSF 90 CH4, SG 256
Tsinghua 1 kW 182 CO 257
Chalmers 100 kW SF 85 coal, petcoke, lignite, 255 and
wood char, wood pellets 258
VTT 20 kW 23 biomass 259
Chalmers 1.4/10 MW 32 biomass 260
CSIC 0.5 kW SF 100 coal 261

Table 12. Other Low-Cost Materials

place unit oxygen carrier time (h) fuel reference
Alstom 3 MW SF CaSO4 75 coal 263
Figure 4. Comparison of performance in three pilots using coal.

conversion can be reached because of the CLOU mechanism. A
drawback with copper materials is the higher cost. Further, the
melting temperature of Cu is relatively low, 1089 °C, and thus,
there could be issues with agglomeration at higher temperatures
if Cu is formed. Although Cu is not active in the oxygen
uncoupling reaction, Cu could be formed by reduction of CuO
or Cu2O with volatiles. Another CLOU material with potentially
lower cost is the combined calcium manganite, although the
release of oxygen is smaller and slower than with copper. As said,
operation with calcium manganite showed significantly
improved performance compared to low-cost materials, but
this material does not seem to be suitable for sulfur-containing
fuels.
4. PERFORMANCE IN LARGER PILOTS
Figure 4 shows a comparison of the operational performance in
the three pilots with coal and ilmenite or manganese ore: a 1
MW pilot in Darmstadt, a 100 kW pilot at Chalmers, and a 50
kW pilot at CSIC.
The 1 MW pilot used two quite different sizes of coal:
pulverized coal and larger coal particles of up to 8 mm in
9082
size.242,243 For pulverized coal, there is a very large loss of
elutriated carbon from the fuel reactor, 50%, in addition to the
loss to the air reactor, indicated by a carbon capture of 80%. For
the larger coal, there is instead a large loss of char to the air
reactor, indicated by a carbon capture of only 50%. Thus,
residence time is too short to convert the larger coal particles in
the fuel reactor.
The loss of carbon by elutriation from the 100 kW unit was
also high when using pulverized coal but lower than in the 1 MW
unit, around 35%.233 The difference is explained by the lower
operational temperature in the 1 MW pilot. Further, the loss of
carbon to the air reactor was low for the 100 kW unit, as
indicated by the high carbon capture. Moreover, the gas
conversion is slightly improved in the 100 kW unit. Adding
manganese ore improved the gas conversion but showed similar
results for carbon capture and loss of carbon by elutriation.235
Using intermediate size coal of 90−300 μm in the 100 kW
unit, the loss of elutriated carbon was significantly lowered but
without any measurable increase in the loss to the air reactor.258
In this operation, a manganese ore was used, which explains the
better gas conversion.
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Energy & Fuels
Figure 5. (a) 100 MWth chemical looping boiler design and (b) 1000 MWth chemical looping boiler design.
The 50 kW pilot, operated at 13.5 kW with another coal of
intermediate size, also showed a low loss from elutriation.240
Further, the 50 kW unit showed good gas conversion but higher
loss of carbon to air reactor compared to the 100 kW unit.
The above results clearly imply an important advantage of
using intermediate size fuel, which is logical. If the fuel particles
are too big, they will not have sufficient time to convert in the
fuel reactor before they follow the stream of circulation to the air
reactor. If fuel particles are too small, they may be rapidly
elutriated and lost with the gas stream.
However, the results in these pilots are only partly relevant for
the full scale. The 100 kW and 1 MW fuel reactors are 5 and 9 m
high, whereas a full-scale reactor could be 50 m, providing
additional residence time for char conversion. Also important
for char conversion is the cyclone performance, which can be
expected to be significantly better than in the pilots.
The higher gas conversion in the 100 kW pilot compared to
the 1 MW pilot is expected because the 1 MW pilot was operated
at a lower fuel reactor temperature with lower solids inventory,
and furthermore, the fuel entry point is high, 0.69 m above the
distributor plate. Lower char conversion, i.e., higher fraction of
volatiles, should also contribute to lower gas conversion in the 1
MW pilot. It is possible that these reasons should give an even
bigger difference but that the higher riser with a significant
pressure drop gives an important positive contribution to gas
conversion.
The following can be concluded from the comparison: The
fuel size is important, and significant improvement can be
reached by raising the average particle size compared to
pulverized coal. To reach good CO2 capture, sufficient
temperature and solids inventory are needed in the fuel reactor.
The fuel should be fed as low as possible in the fuel reactor bed
to achieve good contact between bed material and volatile
released. The results from the two smaller units indicate that
good or reasonable performance could be reached simulta-
neously for all three key performance criteria. Although this was
not the case for the 1 MW unit, reasons for inadequate
performance are well-understood as well as the measures needed
to improve performance.
pubs.acs.org/EF Review
5. PROPOSED DESIGNS FOR SCALE-UP
Presently, proposed designs of solid fuel chemical looping
boilers presented in the literature involve 100 MWth and 1000
MWth units (see panels a and b of Figure 5).40,267 The design of
the smaller unit is not linked to any existing CFB units but based
on more fundamental modeling, whereas the design of the 1000
MWth unit was performed with the purpose of showing that a
design can be made similar to large CFB boilers. Thus, this unit
has essentially similar gas velocities, cross sections, number of
cyclones, etc. as the 460 MWe Lagisza CFB plant. The important
difference compared to the Lagisza plant is the splitting of the
cross section in three parts to give a centrally placed fuel reactor
(see Figure 3b). Further, it was motivated to lower the heights of
the air reactors. The similarities of the CLC and CFB plants also
facilitated the estimation of the added costs of the CLC
compared to a CFB. Thus, the cost was estimated to around 20
€/tonne of CO 2 , where oxygen production and CO 2
purification/compression are the main costs.
In contrast to the 100 MWth design, the 1000 MWth design
does not include any carbon stripper. Also, the principle for
returning the circulating material from the fuel reactor to the air
reactor is different. Otherwise, the general principle of units is
similar. The smaller unit has lower riser heights and, despite the
smaller size, as many as eight cyclones. Moreover, velocities are
somewhat lower in the smaller unit, giving a higher cross-
sectional area per megawatt. The added gas flow from the carbon
stripper further increases the cross section of the fuel reactor.
As shown by the variety of designs of the 49 small CLC pilots,
there are many possibilities to arrange two or more fluidized
beds with circulation. Many of these would not be relevant for
the full scale, and it would also be an advantage to build on the
experiences from CFB technology.
6. IMPORTANT TECHNOLOGY CHALLENGES
Clearly, the experiences and know-how from CFB technology
are central for CLC. However, there are important differences
that have to be properly addressed to make the CLC technology
work. (1) Adequate circulation and control of circulation: For
the operation of a CLC unit, adequate circulation is an absolute
necessity. (2) Suitable oxygen carrier materials: The literature
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Energy Fuels 2020, 34, 9077−9093
Energy & Fuels
cited above shows that a number of low-cost materials have been
shown to work well in pilot operation. (3) Downstream
treatment: After the fuel reactor, an oxygen polishing step is
normally assumed, where the gas is fully oxidized to H2O and
CO2 and also reduced sulfur and nitrogen compounds are
oxidized. This step will produce a gas similar to that of oxy-
combustion, albeit with considerably less argon. Thus, the gas
from the oxy-polishing step can be treated in a similar way as
planned for the oxy-fuel process. This involves downstream
steps for making the CO2 stream pure enough for storage, which
would involve condensation and removal of moisture, removal
of acid gases and oxygen, and CO2 compression.
7. COST STRUCTURE
Cost estimations for solid fuel CLC range from 10 to 32 €/tonne
of CO2.40,268−270 An analysis of the cost structure indicates that
the major costs are downstream of the process, i.e., compression
and oxygen production for oxy-polishing.40 This analysis is
based on tangible differences between CLC and CFB
technologies, which makes the analysis transparent and possible
to update.
The expected costs of CLC are dramatically lower than those
of conventional CO2 capture, which makes sense because large
costs and energy penalties associated with gas separation are
avoided.
8. ROUTES FOR SCALE-UP AT REDUCED COSTS
The scaling-up of CLC to commercial size could proceed
through intermediate steps, which should verify the perform-
ance of the CLC process under conditions relevant for larger
scale. In these steps, CO2 capture would normally have little
relevance. This is an advantage and a simplification, avoiding
expensive process steps, which are not necessary without CO2
capture, such as CO2 purification and compression and oxygen
production. The latter is not needed if the fuel reactor gas is
oxidized with air.
However, a problem with scaling-up using an evolutionary
step-by-step development is of course that building and
operating these CLC would involve significant added costs
with no revenues. It would also delay a development that, given
the climate targets, needs to be rapid. Thus, options for more
rapid upscaling should be considered.
One option could be to investigate if any existing CFBs could
be equipped with a fuel reactors. This would, however, involve
significant challenges, for instance, to ensure that a sufficient
circulation and reactor temperature is achieved.
Another option could be to design a dual-purpose CLC/CFB.
The idea is to build a combined CFB/CLC boiler where the air
reactor would be fully operable as a CFB boiler but also have the
adequate design to demonstrate CLC technology when
connecting it to a fuel reactor. After a CLC demonstration
period, the unit can be used either as CFB or equipped with the
more expensive downstream gas conditioning steps needed to
achieve compressed CO2 of sufficient purity for transportation
and storage.
The rationale of such a two-step demonstration is that the
major added costs for CLC are downstream of the reactor.
The strategy in these approaches is to avoid or minimize the
costs of the air reactor and the peripheral systems. The fuel
reactor is necessary in CLC and has no use, except in CLC,
which means that the cost of the fuel reactor is not easily
avoided. The fuel reactor itself is expected to have moderate
pubs.acs.org/EF Review
costs because the walls are adiabatic. For example, the cost of the
fuel reactor walls of a 1000 MWth unit, including cyclones,
channels, etc., was estimated to 4 M€ or 0.2 €/tonne of CO2.40
This is in fact only a few percentages of the estimated boiler cost.
Other added costs to consider include systems for fuel reactor
fluidization, adequate control of the temperature and circu-
lation, fuel addition to both reactors, etc.
Nevertheless, it should be pointed out that the boiler cost is
around 30−40% of the power plant cost, and a large portion of
the boiler cost is associated with the heat extraction. Ideally,
costs for heat extraction would be similar if the thermal power of
CLC and CFB operation is the same.
9. DOWNSTREAM GAS TREATMENT
From the pilot operational experiences, it is clear that the gas
composition leaving the fuel reactor rarely contains only CO2
and H2O, which would be easy to separate, but also other
compounds. The needed purity of CO2 can vary depending
upon local conditions but may be determined by specifications
set to ensure that pipelines are not damaged. Such specifications
may simply be based on experiences with gas compositions that
have been shown to work. In particular, acid gases and oxygen
need to be in low concentrations, but specifications also indicate
the need for low concentrations of combustible gases.
Using gaseous fuels, together with oxygen carriers with CLOU
properties, it has been possible to reach low concentrations of
both combustible gas and oxygen. In the case of solid fuels, it is
possible to reach full conversion of combustibles using expensive
copper CLOU materials, but this would likely be in the presence
of some oxygen. Normally, inexpensive oxygen carriers are
preferred for solid fuels, in view of the likely losses associated
with separation of fuel ash. With these inexpensive materials, full
gas conversion is not expected.
Normally, it has been assumed that the gas coming from the
fuel reactor can be oxidized by oxygen, leading to a fully
converted gas, albeit with some oxygen present. Nevertheless,
removal of excess oxygen may be needed but also nitrogen
oxides and sulfur oxides. The fact that nitrogen and sulfur oxides
come in a concentrated stream should reduce costs and facilitate
removal.
Another possibility would be to separate CO2 from the
combustible gas and recycle the combustibles to the fuel reactor.
In industry, a common procedure for separating CO2 from
process gases similar to what is expected to come from the fuel
reactor, is the Benfield process (see Figure 6).
In the case of sulfur-containing fuels, the Benfield process
would capture a mixture of sour gases, such as CO2, SO2, and
Figure 6. Use of, e.g., the Benfield process for recovery of CO2 from
CLC.
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Energy & Fuels
H2S, and the latter two would need to be removed either before
or after the Benfield process. Advantages of using a Benfield
process are no need for oxygen production, no need for oxygen
removal from gas, and recycled gas that can be used instead of
steam to fluidize the fuel reactor, thus reducing the energy
penalty of steam addition to the fuel reactor.
The Benfield process would be less sensitive to the CLC
performance, whereas oxygen addition must follow the oxygen
demand of the gas. The Benfield process is likely most
advantageous for higher oxygen demands. Thus, the need for
oxygen is proportional to the oxygen demand, whereas the
compression energy for the Benfield process increases slowly
with oxygen demand.
10. CIRCULATION
One of the challenges when transferring the experiences from
CFB to CLC is to reach the adequate circulation. Normally, a
CLC process is assumed to use a CFB-type arrangement, where
the air reactor is the CFB and the fuel reactor receives the flow of
particles coming from the air reactor cyclone (cf. Figure 3).
Actual circulation in CFB boilers is not well-known, but there
are literature data indicating that circulation rates are lower than
what is needed in CLC, around 25 kg m−2 s−1.40 According to
Yue et al., circulation measured in large CFB boilers is around
6−10 kg m−2 s−1.271 There are several ways to design and
operate an air reactor to control the circulation,40 and increased
fluidizing velocity, reduced reactor height, and reduced oxygen
carrier particle size and density could be used to increase
circulation. However, the velocity used in CFB boilers might be
difficult to raise further with respect to attrition of boiler wall
tubes.
Another possibility could be a separate, dedicated high-
density riser. There is industrial experience of this in FCC units
with fluxes of 400−800 kg m−2 s−1 and even higher,272 albeit
with Geldart group A solids and not in the scale relevant for a
full-scale CLC boiler.
Another option could be to collect the downflow at the walls.
In a normal CFB, only a small fraction of the material that lifts
from the bed actually reaches the cyclone. This material falls
down along the walls, and the downflow may be 2 orders of
magnitude greater than the actual circulation flow. Part of this
flow could be collected and transferred to the fuel reactor. There
is some experience of collecting the wall downflow from the use
of external fluid bed heat exchangers of type INTREX. To
control circulation, a split loop seal could be used that controls
the amount of material led to the fuel reactor and the amount
being returned to the air reactor.
11. NEGATIVE CO2 EMISSIONS
The carbon budgets for meeting decided or desired climate
targets are rapidly being exhausted. Thus, the estimated budget
for having a 66% change of reaching the 1.5 °C goal is 420 Gt in
the period of 2018−2100.273 Thus, with present emissions, the
budget for limiting the global temperature increase to 1.5 °C is
exhausted around 2028. It is highly unlikely that this climate
target can be reached without significant negative CO 2
emissions removing overshooting CO2 from the atmosphere.
Also, for the targets of a maximum of 2 °C and well below 2 °C,
large future negative emissions can be expected to be necessary.
This could be accomplished by, e.g., combining combustion of
biomass or biogenic waste with carbon capture and storage.
pubs.acs.org/EF Review
11.1. Biomass in CLC. Although the majority of SF-CLC
work involves coal or other fossil fuels, more than 700 h of
operation with biogenic fuels has been reported.81,87,109,111,
117,125,133−135,142,155−157,170,172,176,182,187,190,191,195,202,204,205,208,
233−235,237,245−247,251,254,255,258−260
The work involves sawdust,
almond shells, olive stones, rice husks, wood char, wood pellets,
straw pellets, torrified biomass, and sewage sludge. Biomass
normally has a high volatile content, and comparisons of fuels of
different volatile content indicate lower gas conversion with an
increasing volatile content.24 Biomass pellets has been compared
in three CLC pilots, indicating oxygen demands of 25% or
higher.274 The gas conversion of the syngas released from char
has high conversion, likely because the char mixes well with the
bed material, whereas partial bypass likely reduces contact
between volatiles and bed material in the pilot testing. However,
the gas−solid contact is strongly dependent upon fluidization
conditions and could be greatly improved in a full-scale riser.
The application of CLC to biomass or waste, including
biogenic material, bio-CLC, comes with both challenges and
potential advantages. First, it can be noted that power
production using biomass typically has lower energy efficiency
than coal power. This also means that energy penalties of CO2
capture will have a greater relative impact on the process; i.e., a
greater fraction of the power will be lost. This further motivates
looking at concepts that reduce the energy penalty.
A reason for the lower energy efficiency is that biomass,
although generally having a low ash content, has aggressive ash
components, such as alkali. Potentially, CLC could reduce
problems with these ash components. First, it is known that
oxygen carriers may absorb alkali. Thus, ilmenite has been
shown to absorb potassium.275 Second, aggressive ash
components, such as potassium and chlorine, that are released
during devolatilization in the fuel reactor may leave the system in
the gas flow, leaving the fuel reactor. Low surface temperatures
of heat exchangers downstream of the fuel reactor could be
necessary to accommodate for this. However, most of the
process heat is extracted by downstream and inside the air
reactor, and if these surfaces would be significantly less exposed
to these ash components, surface temperatures could be raised.
Although this needs further study, the potential for reducing
problems with aggressive ash components in biomass could
mean both potential for raising steam temperatures, i.e., higher
efficiency, as well as reduced operational difficulties and costs. It
could also open up for use of difficult fuels with high alkali, such
as straw fuels.
Likewise, if fuel does not leak to the air reactor, the effluent
should be clean and free of any NO. NO formed from fuel
nitrogen should instead be concentrated in the CO2 stream,
where the costs for removal are lower.276
12. CONCLUSION
The necessary elements for a scale-up are at hand: Different
oxygen carrier materials of low cost have been tested in extended
operation and found to have reasonable performance with
respect to reactivity and lifetime. Operation with solid fuels in
pilots up to at least 100 kW has been shown to work. Operation
in a 1 MW pilot showed inadequate loss of char, but reasons for
this are understood and can be addressed. Designs for large-scale
units have been performed, indicating that the process is
technically realistic and should have low cost of CO2 capture. A
scale-up strategy to minimize risk and costs has been suggested.
To meet global climate targets, large future negative CO2
emissions will be needed and bio-CLC may provide significant
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Energy & Fuels
advantages with respect to energy efficiency and compatibility
with biomass ashes.
■
AUTHOR INFORMATION
Corresponding Author
Anders Lyngfelt − Chalmers University of Technology, 412 96
Göteborg, Sweden; orcid.org/0000-0002-9561-6574;
Email: anders.lyngfelt@chalmers.se
Complete contact information is available at:
https://pubs.acs.org/10.1021/acs.energyfuels.0c01454
Notes
The author declares no competing financial interest.
■ ACKNOWLEDGMENTS
This work was carried out within the Nordic Flagship Project
77732 “Negative CO2 Emissions in the Nordic Energy System”
funded by the Nordic Energy Research.
■
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