Solar Energy xxx (2017) xxx–xxx

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Solar Energy
journal homepage: www.elsevier.com/locate/solener

Particle reactors for solar thermochemical processes

Tatsuya Kodama a,c,⇑, Selvan Bellan b,c, Nobuyuki Gokon b,c, Hyun Seok Cho a,c
a
Department of Chemistry & Chemical Engineering, Faculty of Engineering, Niigata University, 8050 Ikarashi 2-nocho, Niigata 950-2181, Japan
b
Center for Transdisciplinary Research, Niigata University, 8050 Ikarashi 2-nocho, Niigata 950-2181, Japan
c
Pacific Rim Solar Fuel System Research Center, Niigata University, 8050 Ikarashi 2-nocho, Niigata 950-2181, Japan

a r t i c l e i n f o a b s t r a c t

Article history: Utilization of solar thermal power for high temperature fuel production has the potential to significantly
Received 10 April 2017 reduce the fossil fuel dependence of our current economy. Over the past two decades, remarkable pro-
Received in revised form 26 May 2017 gress has been made in the development of solar driven thermochemical reactors for the production of
Accepted 28 May 2017
hydrogen and syngas as they are promising energy carriers for transportation, domestic and industrial
Available online xxxx
applications. However, there are solar peculiarities in comparison to conventional thermochemical pro-
cesses – high thermal flux density and frequent thermal transients because of the fluctuating insolation-,
Keywords:
and conventional industrial thermochemical reactors are generally not suitable for solar driven reactors.
Particle reactors
Concentrated solar power
Therefore, solar-specific modifications of reactor design are necessary to realize efficient solar driven
Solar thermochemical processes thermochemical processes. In solar thermochemical reactors, the methods for solar-heating particulate
Solar gasification solid feedstock to high temperatures can be broadly classified as solar ‘‘directly” and ‘‘indirectly” absorb-
ing reactors. On solar thermochemical processes involving reacting solid particles at high temperatures,
such as ‘‘solar two-step water splitting with metal oxides” and ‘‘solar gasification”, various types of solar
directly and indirectly absorbing particle reactors have been developed. In this review, recent develop-
ment of solar particle reactors for the above solar thermochemical processes is described.
Ó 2017 Elsevier Ltd. All rights reserved.

1. Introduction with or geographically matching the incident solar radiation. In

The maximum direct insolation frequently reaches 1 kW m
2 in
the insolation rich ‘‘sunbelt” regions which include the Southwest-
ern United States, southern Europe, all of Australia, and broad
regions of the developing world (Kodama, 2003). The collection
and concentration of direct insolation can be achieved by sun-
tracking mirrors called collectors or heliostats. Some modern
solar-concentrating systems have maximum concentration factors
in the 1500–5000 range and can provide high-temperature solar
thermal heat (Kodama, 2003; Johnston et al., 2003; Mills, 2004;
Kalogirou, 2004; Yogev et al., 1998; Segal and Epstein, 2001;
Tamaura et al., 2006; Epstein et al., 2006). The concentrated solar
radiation is focused upon a solar receiver or reactor where maxi-
mum temperatures can exceed 1500 °C, depending upon the con-
figuration of the solar concentrating system.
The conversion of solar radiation into chemical fuels is an engi-
neering challenge. Chemical fuels offer the advantages of being
transportable as well as storable for extended periods of time. This
point is important because energy demand is rarely synchronous
⇑ Corresponding author.
E-mail address: tkodama@eng.niigagta-u.ac.jp (T. Kodama).
order to efficiently convert solar high temperature heat to chemical
fuels in the ‘‘sunbelt” regions, industrially efficient endothermic
processes are required which can be conducted at temperatures
ranging from 500 to 1500 °C (Kodama, 2003). Various important
industrial thermochemical processes exist, which may be con-
ducted utilizing solar high temperature heat as the process heat.
Some high temperature endothermic reactions for converting solar
energy to chemical fuels have been investigated as solar thermo-
chemical processes, such as two-step water splitting cycles with
metal oxides, natural gas reforming, and coal gasification. There
are, however, solar peculiarities in comparison to conventional
thermochemical processes: High thermal flux density (up to the
maximums of 1500 and 5000 kW m
2 for solar tower and dish type
concentrating systems respectively (Kodama and Gokon, 2007),
and frequent thermal transients because of the fluctuating insola-
tion. The latter is caused by astronomical but more drastically by
meteorological factors. Conventional industrial systems for ther-
mochemical reactions are generally not suitable for transient oper-
ation: e.g., increased energetic losses by heat transfer resistance
and catalysts designed for optimum activity in a narrow tempera-
ture range. Although insolation is intense and very stable at day-
time in the sunbelt (hence relatively stable reaction operation is
possible in solar driven chemical processes), still solar-specific

http://dx.doi.org/10.1016/j.solener.2017.05.084
0038-092X/Ó 2017 Elsevier Ltd. All rights reserved.

Please cite this article in press as: Kodama, T., et al. Particle reactors for solar thermochemical processes. Sol. Energy (2017), http://dx.doi.org/10.1016/j.
solener.2017.05.084
2 T. Kodama et al. / Solar Energy xxx (2017) xxx–xxx
Nomenclature
CIEMAT Centro de Investigaciones Energéticas, Medioambien-
tales y Tecnológicas, Spain
CNRS National Center for Scientific Research, France
ETHZ Swiss Federal Institute of Technology, Zurich, Switzer-
land
NREL National Renewable Energy Laboratory
modifications of conventionally used process technologies and
reactor design are necessary to realize efficient solar thermochem-
ical processes.
Thermochemical reforming of natural gas is a catalytic reaction
between methane with steam or CO2, and can proceed at temper-
atures above 850 °C. Solar reformer can be realized by solar indi-
rect heating of the catalyst and reactant gases. Two different
types of solar reformer using solar indirect heating have been
developed: one is a heat exchange type and another is directly irra-
diated reactor tube type (Kodama, 2003). In the former case, solar
radiant energy is collected by a conventional tube or volumetric
receiver, and the heat carrying medium heats the process gas in
the separate reformer. In the latter case of the directly irradiated
reactor tube type, the concentrated solar radiation is directly
absorbed by a metal wall of the reactor tube and then the catalyst
bed inside the tube is indirectly heated.
However, some of solar thermochemical processes, such as
solar gasification of coal and the thermal reduction of metal oxides
as part of a two-step water splitting cycle, require a high-
temperature solar chemical reactor being capable of operating at
1000–1500 °C. In these cases, it is not easy to retain such high tem-
peratures on coal or metal-oxide particles in conventional
externally-heated reactor systems if concentrated solar radiation
is used as its energy source, because of high heat resistance of
the exterior solar absorber wall. One effective way to reach and
retain such high temperatures in a solar chemical reactor is by
direct irradiation with high fluxes of concentrated solar radiation.
In solar chemical reactors with reacting particles, it is possible that
the particles are heated directly by concentrated solar radiation,
resulting in efficient and rapid heating rates. Radiation enters the
gas-particle mixture through a quartz window and due to the
low reflectivity of the particles, radiation is absorbed near the sur-
face; heat losses are thus minimized. Direct absorbing particle
receiver-reactors are candidates for conducting high-temperature
solar driven processes.
This paper reviews the recent developments of particle solar
reactors for thermochemical processes, which can convert solar
radiation into chemical fuels. The target processes of particle solar
reactors in this paper are ‘‘solar two-step water splitting cycles”
and ‘‘solar gasification”.
2. Solar two-step water-splitting cycles with metal-oxides
2.1. Introduction
Two-step reaction cycles are naturally the simplest multi-step
thermochemical water splitting methods. Funk and Reinstrom
(1966) investigated the potential for the first two cycle types at
temperatures up to 1100 °C, but feasible two-step cycles were
not found. This is in agreement with the thermodynamic analysis
made by Abraham and Schreiner (1974), which indicates that the
minimum number of reaction steps for thermochemical cycles
Please cite this article in press as: Kodama, T., et al. Particle reactors for solar thermochemical processes. Sol. Energy (2017), http://dx.doi.org/10.1016/j.
solener.2017.05.084
PREC Professorship of Renewable Energy Carriers, ETHZ,
Switzerland
PROMES Procédés, Matériaux et Énergie Solaire, Odeillo, France
PSI Paul Scherrer Institute, Switzerland
STL Solar Technology Laboratory, PSI, Switzerland
SSPS Small Solar Power Systems
operating between 298 and 1000 K is three, as inferred from the
required entropy change.
A two-step thermochemical water splitting cycle using a redox
system of non-volatile metal oxide is one of the promising pro-
cesses for converting concentrated solar high-temperature heat
into clean hydrogen in sun-belt regions. Nakamura (1977) first
proposed a two-step water-splitting cycle by a redox pair of
Fe3O4/FeO, and conducted a thermodynamic analysis. The two-
step cycle proceeds as follows:
Fe3 O4 ! 3FeO þ 1=2O2 ð1Þ
H2 O þ 3FeO ! Fe3 O4 þ H2 ð2Þ
The first high-temperature thermal reduction of Fe3O4 is highly
endothermic (DH°298K = 319.5 kJ/mol), and the second low-
temperature hydrolysis by FeO is slightly exothermic (DH
°298K =
33.6 kJ/mol). The two-step process eliminates the need
for high-temperature H2/O2 separation. The first solar high-
temperature step of the thermal reduction of magnetite (Fe3O4)
to wustite (FeO) proceeds at temperatures above 2500 K under
1 bar, while the second step of the hydrolysis reaction thermody-
namically proceeds at temperatures below 1000 K (Kodama and
Gokon, 2007). Because of the very high reduction temperatures
required for the Fe3O4/FeO redox pairs, mixed solid solutions
between the redox system Fe3O4/FeO and M3O4/MO have been
investigated to reduce the reduction temperature. Partial substitu-
tion of iron in Fe3O4 by Ni, Co, etc. is possible to form mixed metal
oxides (Fe1
xMx)3O4. The mixed oxide may be reducible at a lower
temperature than that required for the reduction of Fe3O4, while
the reduced phase (Fe1
xMx)1
yO is still capable of a hydrolysis
reaction. However, another essential problem of the water splitting
cycle with iron-based oxides or ferrites is the deactivation of ferrite
particles in the cyclic reaction. This is due to melting or sintering of
the ferrite particles at temperatures below 1400–1500 °C (Kodama
and Gokon, 2007). In order to solve the deactivation of ferrites in
cyclic reaction, ZrO2 supporting for ferrites has been investigated
(Kodama and Gokon, 2007; Kodama et al., 2005, 2008b). The sup-
porting ZrO2 alleviated the coagulation and/or sintering of the iron
oxides. Finally, Kodama et al. (2005) experimentally showed that
cobalt-doped and nickel-doped iron oxides (Co-ferrites and Ni-
ferrites) supported on monoclinic ZrO2 (m-ZrO2) are capable of
working below 1400 °C as the reactive redox metal oxide material
(Kodama et al., 2005, 2008b).
In recent years, non-stoichiometric cerium oxides have received
much more attention than ferrites as the working material because
of the high melting temperature of cerium oxides (Abanades and
Flamant, 2006; Chueh and Haille, 2009). Abanades and Flamant
(2006) first showed that CeO2/Ce2O3 two-step water splitting cycle
could produce hydrogen, but the thermal reduction temperature is
very high (2000 °C) (Abanades and Flamant, 2006). However, when
the thermal reduction temperature is performed at 1500 °C, cerium
oxide is still reactive as the redox material for two-step water split-
ting (Chueh and Haille, 2009; Siegel et al., 2010). In this case, CeO2
is thermally reduced to non-stoichiometric form in oxygen
 T. Kodama et al. / Solar Energy xxx (2017) xxx–xxx
(CeO2
d). In the second step of the hydrolysis step, the CeO2
d can
react with steam at lower temperatures to produce hydrogen.
Thus, the two-step reaction can be roughly written as follows:
CeO2 ¼ CeO2
d þ d=O2 T > 1500  C
CeO2
d þ dH2 O ¼ CeO2 þ dH2 T < 1000  C
The melting point data of CeO2 varies in the literature from
1950 to 2400 °C according to Abanades and Flamant (2006). But
in any case, the melting temperature of CeO2 is much higher than
those of ferrites.
As two-step water splitting cycle with volatile metal oxide,
ZnO/Zn cycle has been investigated the most (Palumbo et al.,
1998; Steinfeld and Palumbo, 2001; Steinfeld, 2002, 2005;
Wegner et al., 2006). The two-step water splitting cycle by a
ZnO/Zn redox pair is described below.
ZnO ! ZnðgÞ þ 1=2O2
Zn þ H2O ! ZnO þ H2
The thermal decomposition of ZnO to Zn vapor and O2 mole-
cules proceeds endothermically (DH0298K = 478 kJ), and the temper-
ature for which the DG0 equals zero is 2235 K (Steinfeld and
Palumbo, 2001). The hydrolysis by metallic zinc thermodynamically
proceeds at temperatures below 1400 K under 1 bar (Wegner et al.,
2006). The products, zinc vapor and oxygen, eventually must be sep-
arated or quenched to avoid recombination.
As mentioned above, the first solar endothermic step of thermal
reduction of metal oxide in the two-step water splitting requires a
high-temperature solar reactor that can be operated at temperatures
above 1400 °C. It is difficult to retain such high temperatures of metal
oxide particles in conventionally heated reactor systems. Thus, a
specific, novel solar reactor must be developed for this extremely
high-temperature gas-particle reaction (Steinfeld et al., 1999). Normal
designs of solar reactor for high temperature applications make use of
insulated cavity-type configurations in order to obtain isothermal
conditions and efficient solar energy absorption (Diver, 1987). How-
ever, for operating temperatures above 1300 °C under oxidizing atmo-
spheres, ceramic materials of construction are usually required for
lining the inner wall of the cavity. These massive refractory materials
are not resistant to the severe thermal shocks that often take place
under intermittent concentrated solar radiation. These problems pro-
mote the development of the direct absorbing receiver-reactors of
‘‘device” or ‘‘particles” types as a novel solar chemical reactor.
The direct absorbing ‘‘device” type receiver-reactors use honey-
comb or foam ceramic devices coated with or made of some active
redox materials such as ferrites or cerium oxide. In European
HYDROSOL projects, multi-channeled honeycomb ceramic sup-
ports coated with ferrite powder were used in a solar receiver-
reactor system, in a configuration similar to that encountered in
automobile exhaust catalytic converters (Agrafiotis et al., 2005,
2006; Roeb et al., 2016; Sattler et al., 2006). The ferrite-coated
SiC-based honeycombs were directly irradiated by concentrated
solar radiation through a quartz window and heated to 1200–
1300 °C in order to perform the thermal reduction step, while pass-
ing N2 gas through it. Steam was passed through the reactor to per-
form the hydrolysis step while decreasing the amount of solar
power input because of the lower temperature of the hydrolysis
step than that of the thermal reduction step. By other researchers
(Kodama et al., 2007; Chueh et al., 2010; Furler et al., 2012) cera-
mic foam devices coated with or made of the redox materials (fer-
rites or cerium oxide) were also used as the direct absorbing
devices and demonstrated on two-step water splitting in directly
solar-irradiated receiver-reactor systems (Kodama and Gokon,
2007; Kodama et al., 2007; Gokon et al., 2008a, 2008c, 2009b;
Cho et al., 2015; Petrasch et al., 2008; Chueh et al., 2010; Furler
Please cite this article in press as: Kodama, T., et al. Particle reactors for solar thermochemical processes. Sol. Energy (2017), http://dx.doi.org/10.1016/j.
solener.2017.05.084
3
et al., 2012; Haussener and Steinfeld, 2012). However, it must be
pointed out that such device type receiver-reactor concepts – the
monolithic or foam device type – have a disadvantage that the
mass of the redox materials to be loaded onto the support is very
ð3Þ
limited and therefore, only a small amount of the redox material,
coated on the restricted surface area of the support, can contribute
ð4Þ
to the chemical reactions. The active surface area of the redox
metal oxide is very limited due to the small loading of the material
in the reactor. Therefore, a small mass of hydrogen will be pro-
duced by ‘‘one run” of the cyclic reaction in the reactor. To realize
a large mass production of hydrogen by such reactor concepts, a
very large number of runs of the cyclic reaction are required. Dur-
ing the day, the sun availability is limited in time, thus, to realize
the very large number of runs for the limited period of time, very
fast kinetics of the reactions is required for the limited surface area
of the meal oxide in the reactor. In other words, the metal oxide
must realize a very high ‘‘turnover number”. However, the kinetics
ð5Þ
of hydrolysis step strongly depends on the active surface area of
the redox materials such as ferrites (Kodama and Gokon, 2007),
ð6Þ
thus, the large surface area will be required to realize the high
reaction kinetics. As a result, in order to allow the reactor concept
to be scaled up to multi-megawatt size, a cluster of the reactors
must be constructed at the top of a solar tower (Roeb et al., 2016).
On the other hand, the idea of direct absorbing ‘‘particles” type
receiver-reactors has been examined for more than three decades
(Rightley et al., 1992; Meier et al., 1996; Steinfeld et al., 1998). The
reactor concept is based on direct solar irradiation of ‘‘suspension
of reacting particles in a gas stream” or ‘‘falling particles”, providing
efficient heat transfer directly to a large mass of reacting particles.
For solar two-step water splitting with metal oxides, the concept
using a ‘‘suspension of reacting particles” has been well developed,
and several reactors have been demonstrated as mentioned below.
The difficulty in this concept is how to prevent the solar-heated par-
ticle suspension from contacting the transparent quartz window.
Provided that the reactor is combined with a conventional solar con-
centrating system such as a solar tower (Kodama, 2003; Kodama and
Gokon, 2007), solar high flux must enter horizontally into the reactor
housing through a side window as illustrated in Fig. 1a. In this case,
conventional fluidized beds of reacting particles cannot be utilized in
the solar reactor, but rather, a ‘‘cloud” of the reacting particles need
to be created by more swirling gas streams in the reactor to avoid
contact between the particle suspension and the window (Steinfeld
et al., 1998), as shown in Fig. 1a. Several reactors using a gas-
particle vortex flow confined in a solar cavity receiver with a window
have been demonstrated (Steinfeld et al., 1998).
On the other hand, it has been proposed that a solar chemical
reactor can be combined with the newly-developed solar reflective
tower with beam-down optics (Epstein et al., 2006; Kodama et al.,
2008a, 2014, 2016a, 2016b; Gokon et al., 2008b, 2009a, 2010,
2011; Matsubara et al., 2015). The optical path of the beam-
down is comprised of a heliostat field illuminating a hyperbolic
reflector that is placed on a tower and directs the beams down-
wards (Yogev et al., 1998; Segal and Epstein, 2001; Tamaura
et al., 2006; Epstein et al., 2006). This beam-down setup has an
advantage over normal tower top arrangements of reactor in that
it allows a large-scale reactor to be built on the ground, with the
solar radiation entering the reactor housing through a window in
the ceiling. In such a reactor design, conventional fluidized beds
of the reacting particles can be applied because an interspacing
gap can easily be produced between the fluidized particle bed
and the window to prevent their contact, as shown in Fig. 1b. With
this in mind, Kodama et al. (2008a) proposed and developed a
novel design concept for chemical receiver-reactors using an inter-
nally circulating fluidized bed of reacting particles (Kodama et al.,
2008a, 2014; Gokon et al., 2009a, 2011; Matsubara et al., 2015). In
this receiver-reactor concept, the cylindrical reactor body is made
4 T. Kodama et al. / Solar Energy xxx (2017) xxx–xxx
Fig. 1. Schematics of solar reactor concepts using (a) a particle cloud and (b) an internally-circulating fluidized bed of reacting particles.
of steel, but a transparent quartz window is installed in the ceiling
of the reactor. A draft tube is centrally inserted into the fluidized
bed region. Gases are introduced into the draft tube and annulus
regions of the bed separately. The concentrated solar radiation
passes downwards through the window and directly heats the
internally circulating fluidized bed of reacting particles. In this sys-
tem, the particles are always transported upwards in the draft tube
and move downwards in the annulus sections. This solid circula-
tion within the reactor provides solar energy transfer from the
top of the fluidized bed to the bottom since directly solar-heated
particles in the top region always move to the bottom region. This
creates a more uniform temperature distribution throughout the
solar-irradiated fluidized bed when compared with a normal
solar-irradiated fluidized bed. Another advantage is that the inter-
nally circulating bed reactor requires a rapid gas flow only in a
small region (solely in the draft tube), reducing the total gas flow
compared to a traditional fluidized bed reactor. This reduces the
energy required for gas flowing to the reactor extensively.
In this section, recent R&D on particle ‘‘cloud” and ‘‘fluidized”
receiver-reactors for solar two-step water splitting cycles are
described. In addition, indirect particle receiver-reactors and other
conceptual reactors are also presented.
2.2. Particle cloud vortex flow reactors for volatile ZnO process
Solar reactors for the thermal reduction of ZnO have been under
development and significant progress has been made for over two
Please cite this article in press as: Kodama, T., et al. Particle reactors for solar thermochemical processes. Sol. Energy (2017), http://dx.doi.org/10.1016/j.
solener.2017.05.084
decades (Steinfeld, 2005; Agrafiotis et al., 2015; Alonso and
Romero, 2015). Many reactor concepts, from packed bed to
quasi-batch arrangements (Schunk et al., 2008; Abanades et al.,
2007; Haueter et al., 1999; Chambon et al., 2010; Muller et al.,
2006), have been considered by various researchers worldwide.
Heat transfer in a direct absorbing receiver-reactor is predomi-
nantly transferred to particles by radiative heat transfer and to
the gas by particle–gas convective heat transfer. Hence, the radia-
tive heat transfer in a solar thermochemical reactor containing ZnO
particles, O2, and Ar was investigated by Dombrovsky et al. (2009).
Using the optical constants of ZnO, the local particle volume frac-
tion, the particle size distribution and the spectral radiative prop-
erties of ZnO particles were calculated using approximation and
Mie theory. Fig. 2 shows the absorption and transport scattering
efficiency factors of ZnO particles for different sizes (10, 100 and
500 mm) Dombrovsky et al. (2009). For the development of solar
reactors for the Zn/ZnO thermochemical cycle, The STL in collabo-
ration with PREC at ETHZ has contributed significantly. In 1998,
started at the fundamental and laboratory scale reactor (Palumbo
et al., 1998), which culminated with the 100 kW pilot scale of
demonstration process in 2014 (Koepf et al., 2016b). Hydrogen
production in zinc based thermochemical cycle has been exten-
sively studied at PSI. A rotary-cavity reactor called ROCA was the
first fully functional ZnO dissociation reactor introduced at PSI
(Haueter et al., 1999), which is shown in Fig. 3. The main aim of
the reactor was to improve the design principles of the SLOP reac-
tor, which was initially developed with an inclined surface to
 T. Kodama et al. / Solar Energy xxx (2017) xxx–xxx
Fig. 2. Radiative characteristics of ZnO particles using approximation and Mie theory (Dombrovsky et al., 2009).
which particulate ZnO could be fed to investigate kinetics and
extract practical operation parameters.
The ROCA reactor featured a windowed rotating cavity-receiver
and the zinc oxide particles fed through a screw conveyor located
at the rear end of the cavity. The zinc oxide powder was pushed
towards the reactor wall due to centrifugal force and a ZnO layer
was formed which served simultaneously as chemical reactant
and thermal insulator of the cavity. In order to decrease the cavity
aperture diameter and enhance the concentration of the incoming
radiation, compound parabolic concentrator (CPC) was used. The
particle-laden product stream was collected by a quench device
mounted at the rear end of the cavity. To reduce deposition, the
quartz window placed well in front of the cavity aperture and
flushed with an inert gas stream. With this setup, solar tests were
carried out on the high flux solar furnace with the nominal 10 kW
reactor prototype. ZnO surface temperatures of 2000 K were
reached in 2 s and the reaction rates as high as 6 g/min were
reported. However, this reactor was suffered from some problems
such as uneven distribution of zinc oxide in the reactor, thermal
loss due to water cooled front end, recombination of zinc and oxy-
gen to produce zinc oxide, inability to recover large percentage of
products from the reactor (Muller et al., 2006). These issues were
Fig. 3. Schematic of the ‘‘rotating-cavity” solar reactor concept for the thermal
dissociation of ZnO called ROCA (Haueter et al., 1999): (1) rotating cavity receiver,
(2) cavity aperture, (3) quartz window, (4) CPC, (5) outside conical shell, (6)
reactant feeder, (7) ZnO layer, (8) purge gas inlet, (9) product outlet, (10) quench
device.
Please cite this article in press as: Kodama, T., et al. Particle reactors for solar thermochemical processes. Sol. Energy (2017), http://dx.doi.org/10.1016/j.
solener.2017.05.084
5
addressed in the next generation solar reactor ZIRRUS, which was
developed by PSI following the ROCA.
The ZIRRUS reactor was successfully tested on the high flux
solar furnace for dissociation of zinc oxide at 2000 K (Muller
et al., 2006; Müller and Steinfeld, 2007). However, the Hf/HfO2 cav-
ity of the reactor showed mechanical stability problems due to
heating–cooling cycles and operation in oxidizing atmosphere
(Schunk et al., 2008, 2009a). Thus an improved ZIRRUS reactor
was designed and developed to operate at a power input of
10 kW as shown in Fig. 4. This reactor was also implemented a
rotating cavity. The inner walls of the cylindrical cavity were made
of sintered Al2O3 composite bricks. A layer of ZnO of a desired
thickness was spread over the surface using a screw feeder. The
inert gas was used to sweep across the reactor window and carry
the products to the quench device as ROCA reactor. Continuous
operation, about 4 h, was demonstrated for the ZIRRUS solar reac-
tor with 9.6 kW solar power input and the Zinc content of the
quenched product was reported as 25.4 ± 7% (Schunk et al.,
2008). Experimental tests around 1807–1907 K were carried out
and no cracks or any mechanical stability problems were found.
The reactor was able to operate with much less water cooling. In
further research, numerical models were developed to simulate
Fig. 4. Schematic of the improved reactor design (Schunk et al., 2008, 2009a,
2009b); (1) rotating cavity; (2) Al2O3–SiO2 insulation; (3) Al2O3–Y2O3 insulation; (4)
alumina fibers; (5) Al reactor shell; (6) aperture; (7) quartz window; (8) dynamic
feeder; (9) conical frustum; and (10) rotary joint.
6 T. Kodama et al. / Solar Energy xxx (2017) xxx–xxx
flow fields, heat and mass transfer (Schunk et al., 2009a, 2009b;
Villasmil et al., 2014; Müller and Steinfeld, 2007; Müller et al.,
2008; Dombrovsky et al., 2009, 2007; Coray et al., 2010; Lipinski
et al., 2006). The pre-exponential factor in the Arrhenius rate law
was used as a fitting parameter to match the experimental results.
A dynamic heat transfer models were developed for the zinc oxide
dissociation reactors (Villasmil et al., 2013b; Dombrovsky et al.,
2009). However, the dissociation kinetics of ZnO exposed to con-
centrated solar radiation is still lacking due to; size of the exposed
surface and temperature at the reaction surface. The development
work focused on optimizing the reactor’s operational parameters
for maximum exergy efficiency and improving the features of the
previous concepts. Challenging tasks to be addressed are design,
fabrication and incorporation of a Zn/O2 separation device, mini-
mization of back-flow of products through the aperture and
towards the quartz window.
After laboratory scale operation, the 10 kW ZIRRUS solar reactor
was up scaled at PROMES-CNRS to demonstrate zinc dissociation in
a 100 kW pilot plant (Hutter et al., 2011; Villasmil et al., 2013a). On
sun testing experiments were carried out for more than 60 h
(Villasmil et al., 2013a). In-situ flow visualization technique was
demonstrated by directly visualizing reactant and product parti-
cles illuminated by sunlight. Results reported that the successful
and long term operation of the reactor was acute due to the pro-
duct particle deposition over the quartz window (Koepf et al.,
2015b). After a series of proofing experiments conducted, the
100 kW reactor was first commissioned in 2011. In the initial
design, alumina tiles and porous ceramic insulation materials were
used to fabricate the cavity but it did not survive due to thermal
shock and rotation. A cavity design, utilized alumina bricks
arranged in an interlocking pattern, was demonstrated in 2012
(Villasmil et al., 2013a). Subsequently in 2014, the 100 kW reactor
was successfully demonstrated using the solar furnace of CNRS-
PROMES after successfully addressing the protection of the quartz
window and the occasional clogging of the reactor’s outlet (Koepf
et al., 2016b). Experiments were carried out over 13 days and
28 kg of ZnO was dissociated. Fig. 5 shows the 100 kW ZnO solar
reactor pilot plant developed at PSI (Koepf et al., 2016a). The pilot
plant reaction temperature was above 2000 K and sustained for
over 97 h operation. The flow pattern to protect the quartz window
was optimized by in-situ high temperature flow visualization
experiments (Koepf et al., 2015b). Thus, an uninterrupted opera-
tion for three consecutive full days was achieved without cleaning
Fig. 5. Schematic of the 100 kW ZnO solar pilot plant: (1) quartz window mount, (2) cavity aperture, (3) aluminum shell, (4) hopper containing ZnO, (5) retractable screw
feeder, (6) product hoses, (7) product filters, (8) movable carriage (Koepf et al., 2016b).
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solener.2017.05.084
the window (Koepf et al., 2016a). Due to an excessive use of
quench gas (nearly 2000 l/min), the solar-to-fuel efficiency of the
pilot-scale solar reactor was limited. A maximum solar-to-
chemical efficiency based on the collected products from the disso-
ciation reaction was reported at 3%, but the 100 kW reactor has the
potential to achieve as high as 16% when the reaction kinetics is
improved (Villasmil et al., 2016). Apart from PSI’s thermochemical
reactors for dissociation of ZnO, other researchers across the world
have been developing various solar reactor concepts for ZnO reduc-
tion (Abanades et al., 2007; Melchior et al., 2008; Perkins et al.,
2008; Haussener et al., 2009; Chambon et al., 2010, 2011; Koepf
et al., 2012, 2015a; Brkic et al., 2016).
2.3. Particle fluidized bed reactors for non-volatile meatal oxide
processes
Particle ‘‘fluidized bed” receiver-rector concept has been pro-
posed and developed for water splitting cycles with non-volatile
metal oxides such as ferrites and cerium oxide. This type of
water-splitting receiver-reactor concept was first experimentally
demonstrated using two kinds of laboratory-scale reactors.
Schematics of quartz tube and windowed stainless-steel tube reac-
tors are shown in Fig. 6 for the thermal reduction of a ferrite/zirco-
nia particles (Kodama et al., 2008a; Gokon et al., 2008b, 2009a,
2010, 2011). The monoclinic ZrO2 supported NiFe2O4 (NiFe2O4/m-
ZrO2) particle bed was internally fluidized by passing N2 gas
through from the bottom of the reactor. Then, the particle bed
was irradiated by about 1–3 kWth of concentrated visible light
from a sun-simulator to carry out the thermal reduction step of
the ferrite. In the case of the windowed stainless tube reactor,
the bed surface temperature on the top of the fluidized bed
reached in the range 1200–1600 °C while the bed bottom temper-
ature was in the range 1000–1200 °C, depending on the flow rate of
N2. After the irradiation, the thermally-reduced ferrite particles
were transferred to another fixed bed reactor and were reacted
with steam at 1000 °C. About 24–44% of the NiFe2O4 on the m-
ZrO2 support was converted to the reduced phase which was com-
pletely re-oxidized with steam at 1000 °C to produce hydrogen
(Gokon et al., 2008b, 2009a, 2010). With this system, pulverization
of the NiFe2O4/m-ZrO2 particles is not needed following thermal
reduction – similar levels of hydrolysis reactivity were obtained
either with or without pulverizing the particles. This implies that
the thermal reduction and hydrolysis steps can be conducted in a
 T. Kodama et al. / Solar Energy xxx (2017) xxx–xxx 7

Fig. 6. Schematics of experimental set-ups for an internally circulating fluidized bed laboratory-scale reactors; (a) a ‘‘quartz tube” reactor and (b) a ‘‘windowed stainless steel
tube” reactor.

‘‘single” reactor of this type by switching the feed gas between

inert gas (nitrogen) and steam. Successive two-step water splitting
with NiFe2O4/m-ZrO2 particles in a ‘‘single” fluidized bed receiver-
reactor was also demonstrated using the windowed stainless tube
(Gokon et al., 2011). The internally circulating fluidized bed of
about 140 g of NiFe2O4/m-ZrO2 particles was exposed to concen-
trated visible light from a sun-simulator with an input power of
2.4–2.6 kWth for the thermal reduction step and 1.6–1.7 kWth for
subsequent hydrolysis step. The feed gas was switched from N2
gas in the thermal reduction step to a gas mixture of N2 and steam
in the hydrolysis step. The hydrogen productivity was 951 N cm3
per cycle and the ferrite conversion was about 35% in the succes-
sive two-step water splitting by the windowed stainless tube.
Also for CeO2 process, two-step water splitting in a ‘‘single” flu-
idized bed receiver-reactor was successfully demonstrated in a
large reactor (Omori et al., 2012). A new reactor was fabricated
for 5 kWth input power of concentrated visible light from a sun
simulator. The configuration of the reactor is shown in Fig. 7. It
consists of an internally circulating bed reactor tube (420 mm
length and 85 mm inner diameter with a 7 mm thickness). The
body of the reactor tube was made of Inconel and stainless steel.
A metal foam distributor of porous stainless steel frits was fixed
at the bottom of the fluidized bed region of the reactor tube. The
draft tube was centrally located in the fluidized bed region. The
inner diameter of the draft tube is 28 mm with 3 mm thickness Fig. 7. Schematic of 5 kW internally circulating fluidized bed reactor.
and the tube length was 48 mm. The bottom of the draft tube is
positioned at 18 mm height from the metal foam distributor. The
top of the reactor tube is equipped with a diverging conical funnel for the hydrolysis step. The O2 and H2 productivities reached 2.7
for mounting a quartz window. About 1 kg of CeO2 particle was and 5.0 N dm3 per cycle respectively. The molar ratio of H2/O2
loaded in the reactor. A successive reaction of thermal reduction was about 1.9 which was close to stoichiometric one of water split-
step (Eq. (3)) and hydrolysis step (Eq. (4)) in the single reactor ting. In order to control the fluidization of CeO2 particles, a basic
was performed by switching the feed gas between N2 gas and relationship between pressure drop of the passing gas through
H2O/N2 gas mixture. Simultaneously, the input power of concen- the fluidized bed and the gas flow velocity was experimentally
trated visible light into the reactor from a sun-simulator was also investigated using the CeO2 particles with different particle size
changed from 5.1 kW for the thermal reduction step to 0.4 kW by a small-scale quartz tube (Etori et al., 2015). Particle sizes smal-

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8 T. Kodama et al. / Solar Energy xxx (2017) xxx–xxx

Fig. 8. (a) 30 kWth beam-down sun-simulator and (b) a bottom view of 19 xenon lamps in the simulator house.

ler than 300 lm were found to be desirable for the stable control of
fluidization of CeO2 particles. Then, the thermal reduction step of
the fluidized bed of CeO2 particles was investigated in more detail
using this 5 kWth windowed receiver-reactor with the sun-
simulator (Etori et al., 2015). CeO2 particles with a particle size
range of 50–100 lm were used as the fluidized reacting particles
in the receiver-reactor, and the relation between O2 productivity
during the thermal reduction step and the N2 gas flow velocity
was examined. A numerical computation for this windowed parti-
cles fluidized bed receiver-reactor was developed and studied by
Matsubara et al. (2014).
In order to carry out laboratory performance tests of the solar
particles fluidized bed receiver-reactor concept in a much larger
scale, a 30–40 kWth big ‘‘beam-down” sun-simulator was installed
at Niigata University (Kodama et al., 2016b) as shown in Fig. 8. The
big ‘‘beam-down” sun-simulator has 19  7-kW xenon-arc lamps
with elliptical reflective mirrors. The lamps are fixed on the top
dome of the simulator house to focus towards downwards
(beam-down orientation). The lamps emit visible light beam
downwards and irradiate the focal spot with about 20-cm diame-
ter. The total beam power on the focal spot is about 30–40 kWth.
The average light flux density within the focal circle area with a
20-cm diameter is about 950 kW/m2. The 30-kWth fluidized bed
receiver-reactor was newly fabricated. The basic structure of the
receiver-reactor is similar to the previous 5 kWth receiver-reactor
for CeO2 process (Fig. 7) but the draft tube was removed from this
receiver-reactor. The gas distributor at the bottom of the fluidized
bed region was changed from metal foam to an Inconel perforated
flat plate. The perforated plate at the bottom of the bed was made
by many holes with 0.5 mm diameter. In order to provide the jet
flow along the central axial region at the bottom-inlet, the density
of holes in the central axial region of the perforated plate was
increased than the near wall region to create an internally-
circulating fluidization. The diameter and length of the static par-
ticles bed were 16 cm  16 cm. The body of the reactor was made
of Inconel and stainless steel. The reactor has a quartz window
with a diameter of 42 cm at the top. In the first test campaign,
quartz sand particles were used as the fluidized particles. The
quartz sand fluidized bed was created by passing air from the bot-
tom distributor of the receiver, and about 30 kWth of high flux vis-
ible light from 19 xenon-arc lamps of the sun-simulator was
directly irradiated on the top of the fluidized bed in the receiver
through a quartz window. The particle bed temperature at the cen-
ter position of the fluidized bed went up to a temperature range
from 1050 to 1200 °C by the visible light irradiation with the aver-
age heat flux of about 950 kW/m2, depending on the air flow rate.
The output air temperature from the receiver reached 1000–
1060 °C (Kodama et al., 2016b). In the second test campaign,
two-step water splitting with CeO2 particles has been performed
using this 30 kWth reactor. About 8 kg of CeO2 particles was loaded
in the reactor. The fluidized bed temperature of CeO2 particles
reached above 1400 °C during the thermal reduction step while
passing N2 gas into the reactor. In subsequent hydrolysis step by
passing an H2O/N2 gas mixture at around 800 °C, about 10–
20 N dm3 of hydrogen per cycle were successfully produced. The
detailed results will be presented in upcoming solarPACES confer-
ence 2017 (September 26–29, 2017 in Santiago, Chile).
This fluidized particle receiver-reactor concept needs to be
combined with a beam-down type solar concentrator. Niigata
University, University of Miyazaki and Miyazaki prefecture have
started an R&D joint project since 2011, to demonstrate the up-
scaled fluidized bed receiver-reactor on solar. A new type of
100 kWth beam-down solar concentrating system with a secondly
elliptical reflector was built in August 2012 at the campus of
University of Miyazaki for solar demonstration of the receiver-
reactor. A snapshot of the demonstration plant is shown in Fig. 9
(Kodama et al., 2014). The new beam-down system consists of an
elliptical mirror with 4.6 m diameter, a central tower with 16 m
height, and 88 heliostats. Each heliostat consists of 10 small mir-
rors with 50 cm diameter. The heliostat field is 60  60 square
meters, and the total area of mirrors is 176 m2. The beam-down
Fig. 9. 100-kWth beam-down solar concentrating system at Miyazaki.

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 T. Kodama et al. / Solar Energy xxx (2017) xxx–xxx
Fig. 10. Principle of a novel beam-down system with an elliptical secondary
reflector.
Fig. 11. Photo of the 100-kWth solar particles fluidized bed receiver-reactor.
system has the first focal point at 14 m height and the second focal
point at 10 m above ground level. The heliostat mirrors reflect the
sunlight towards the first focal point of the elliptic mirror placed
on the central tower, and then the elliptical mirror concentrates
Fig. 12. Illustration of the experimental system.
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solener.2017.05.084
9
the radiation at the second focal point, as illustrated in Fig. 10. In
order to increase the concentration of solar fluxes coming through
the inlet of the reactor, a CPC was designed and fabricated for this
new beam-down system, which is a conical frustum shape tunnel
(150 cm height, 75 cm inlet diameter, 45 cm exit diameter) of
reflecting mirrors. The CPC was located at the second focal spot
of the Miyazaki beam-down system. The performance test of con-
centrating solar fluxes of this beam-down system with and with-
out the CPC was done in 2012–2014 (Kodama et al., 2014). The
solar receiver-reactor was newly fabricated as shown in Fig. 11
for solar on-site performance test using the Miyazaki beam-down
system (Kodama et al., 2016a). The receiver has a quartz window
with a diameter of 75 cm at the top. In the first campaign of the
solar performance test, a fluidized bed of quartz sand particles with
air was used for the solar receiver-reactor. About 17 kg of quartz
sand with particle size of 100–500 lm was filled in the receiver-
reactor. The diameter and the height of the static bed was 25 cm.
The experimental system is illustrated in Fig. 12. The first solar test
campaign was carried out in the middle of December 2015. The
central bed temperature of the sand particles in the fluidized bed
solar receiver-reactor attained 1100 °C, when the direct normal
insolation or DNI was over 950 W/m2 at the peak time, using the
beam-down solar concentrating system. The outlet air temperature
of the receiver-reactor reached 1120 °C. It was predicted that the
central bed temperature could have been higher than 1100 °C if
solar receiver-reactor test had been conducted in other seasons
than winter. The second solar campaign of the particles fluidized
bed receiver-reactor using ‘‘CeO2 particles” for two-step water
splitting is currently going on.
2.4. Indirect particle reactors for metal oxide process
In indirectly heated reactors, the concentrated solar radiation is
first absorbed by a non-transparent wall and then transferred to
the reactants and catalysts by conductive and convective coupled
heat transfer. The flow region of indirect reactor contains the reac-
tants in the form of either packed bed or fluidized bed. The use of
indirectly irradiated solar reactors avoids the use of windows.
However, heat transfer is strongly influenced by several factors
such as packing density of the particles, size of the particles, their
ability to move through the bed and physical properties of the
reactants (Adinberg et al., 2004). Absorber material properties play
a vital role and the following characteristics are required; chemi-
cally inert and sustainable at high temperature, high at radiative
10 T. Kodama et al. / Solar Energy xxx (2017) xxx–xxx

Fig. 13. Multi-tube reflective cavity solar-thermal reactor (Lichty et al., 2012, 2013).

absorbance and thermal conduction, and resistive to thermal
shocks (Piatkowski et al., 2011). In order to enhance the heat trans-
fer between the wall and the reactants, the use of intermediate
working fluids, such as gases or liquids have been used (Adinberg
et al., 2004).
A lab-scale indirect 5 kW cylindrical cavity reactor containing a
tubular ceramic absorber, subjected to high-flux solar irradiation
in the range 448–2125 kW/m2, was fabricated at ETH. The selected
chemical reaction was the thermal dissociation of ZnO into its ele-
ments, which proceeds endothermically at above 1800 K. A heat
transfer reactor model coupled with Monte Carlo ray-tracing was
developed and validated with the experimentally measured tem-
peratures and reaction rates in the range of 1780–1975 K
(Melchior et al., 2008). A research group at University of Colorado
tested a multi-tube reflective indirectly irradiated packed bed reac-
tor for water and carbon dioxide splitting (Lichty et al., 2012,
2013). Fig. 13 shows the multi-tube reflective cavity solar-
thermal reactor, which composed of a cooled reflective cavity with
5 reaction tubes. Cycling and robustness of the mixed metal oxide
particles were tested at National Renewable Energy Laboratory’s
(NREL) High Flux Solar Furnace (HFSF). Reaction rates as high as
15.2 and 9.8 lmol/s/g were observed for H2O and CO2 splitting
respectively.

Fig. 14. The GRAFSTRR beam-down solar thermochemical reactor: (1) water-cooled window mount and vortex-flow generation, (2) water-cooled cavity aperture, (3) data-
acquisition cavity access ports, (4) alumina-tile reaction surface, (5) annular solid ZnO exit, (6) bulk insulation and cavity-shape support, (7) central product-vapor and gas
exit (Koepf et al., 2012).

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 T. Kodama et al. / Solar Energy xxx (2017) xxx–xxx 11

Fig. 15. Schematic of solar reactor for continuous metal oxide processing (Abanades et al., 2007).

2.5. Other concepts of particle reactors for metal oxide processes
A thermochemical reactor GRAFSTRR (Gravity-Fed Solar-
Thermochemical Receiver/Reactor) was developed and tested for
the reduction of ZnO as shown in Fig. 14 (Koepf et al., 2012). The
reactor features an inverted conical-shaped reaction surface along
which reactant powder descends continuously as a moving bed,
undergoing a thermochemical reaction at high temperature. The
design objective of the GRAFSTRR concept was to simultaneously
achieve three goals: (1) create a cavity-type reaction environment
to achieve high and uniform temperature, (2) disperse reactants
along the cavity walls as evenly and uniformly as possible, and
(3) provide sufficient residence time for adequate reaction comple-
tion. Initial experiments using a high-flux solar simulator success-
fully demonstrated the mechanical stability of the reactor and
primary systems. Carbothermal reduction of ZnO with beech char-
coal was also performed in a directly irradiated 10 kW solar ther-
mochemical reactor using a high-flux solar simulator. Solar
thermochemical energy conversion efficiencies of up to 12.4% were
recorded, with reactant conversion as high as 14% (Koepf et al.,
2015a).
CNRS-PROMES designed a solar reactor for the continuous
metal oxide reduction up to 2300 K under controlled atmosphere
as shown in Fig. 15 (Abanades et al., 2007). A computational model
was developed by coupling the fluid flow, heat and mass transfer,
and the chemical reaction. The model predicted that the initial par-
ticle size plays a vital role on the conversion rate as shown in
Fig. 16. The maximum yield of particles recovery in the filter was
21% and the dissociation yield was up to 87% (Zn weight content
in the final powder) for a 5 NL/min gas flow-rate (Chambon
et al., 2010). A 1 kW lab-scale solar reactor was designed, built,
and operated for continuous dissociation of volatile oxides, ZnO
and SnO2 under reduced pressure (Chambon et al., 2011). The
kinetics of ZnO dissociation and activation energy was reported
by the O2 measurements.
approaches. The energy necessary to drive gasification reactions is
usually supplied by partial combustion of carbonaceous materials
with oxygen or air, but this releases large amounts of CO2 to the
atmosphere (Tart, 1990; McMullan et al., 1997). The clean high tem-
perature energy from concentrated solar radiation in the sunbelt may
be used to supply the process heat of gasification reactions. The use
of high temperature solar heat to drive the endothermic reactions
associated with gasification has been suggested and investigated
since the 1980s (Gregg et al., 1980a, 1980b; Aiman et al., 1981;
Taylor et al., 1983; Beattie et al., 1983; Epstein et al., 1994; Marray
and Fletcher, 1994; Kodama et al., 1998, 2001; Matunami et al.,
2000). This process, called ‘‘solar gasification”, produces not only a
highly useful and transportable end product, but also results in the
storage of a significant fraction of solar energy in the chemical bonds
of the fuel molecules. Thus, solar energy may be transformed into a
form that is both storable and transportable, and which can be used
in existing equipment.
The chemistry of gasification of coal and biomass involves the
two basic steps: pyrolysis and char gasification. The pyrolysis pro-
cess can be roughly represented as follows:
Coal or biomass ! charðcarbonÞ þ CO þ CO2 þ H2 þ CH4 þ tars
ð7Þ
This process is slightly endothermic and the energy required for
this reaction is relatively small. The pyrolysis process is essentially
complete by the time the coal reaches 1200 K (Gregg et al., 1980b).

3. Solar gasification

3.1. Introduction

Steam or CO2 gasification of carbonaceous materials, such as

coal, coke, biomass, etc., is highly endothermic, being a process
which is greatly dependent upon energy and high temperature
although the utilization of carbonaceous materials through conver-
sion to gaseous fuels embodies a number of different technical Fig. 16. Conversion rate vs. initial particle diameter (Abanades et al., 2007).

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12 T. Kodama et al. / Solar Energy xxx (2017) xxx–xxx
The primary reaction for chemically storing solar energy in pro-
duct gas is char gasification with steam, or CO2 in the next step.
The basic reaction of steam or CO2 gasification is the water gas
reaction (Eq. (8)), or the Boudouard reaction (Eq. (9)), which pro-
duces syngas:
C þ H2 OðlÞ ! CO þ H2 DH 298K ¼ 175 kJ
C þ CO2 ! 2CO DH 298K ¼ 172 kJ
Because of these highly endothermic reactions, the product syn-
gas has greater calorific value, ideally higher than initial coal by
44–45%. Equilibrium gas compositions of carbon-steam and
carbon-CO2 systems, as a function of temperature, shows that, car-
bon conversion is completed above 1200–1300 K and at 1 bar, and
that only CO and H2 are produced in both systems (Kodama, 2003).
Gregg et al. (1980b) presented a number of designs for solar
gasification reactors, such as moving-bed and fluidized-bed solar
gasifiers, solar gasifiers using direct heat exchange between coal
and solar-heated molten salt, and a gasifier using a closed fluid
(He) loop for heat transfer to the coal gasifier. It was anticipated
that each reactor design would have its own specific advantages
and technical problems. As mentioned above, in windowed solar
gasifiers, coal particles can be heated directly by concentrated solar
radiation, resulting in efficient and rapid heating rates. Radiation
enters the gas-particle mixture through a quartz window and
due to the low reflectivity of the particles, radiation is absorbed
on the surface, heat losses are thus minimized. Therefore, direct
absorbing particle receiver-reactors are also promising candidates
for solar gasification.
Gregg et al. (1980a) first demonstrated a fixed, packed-bed coal
gasification with steam or CO2 using direct solar irradiation in a
23-kW solar furnace. The solar radiation was focused directly onto
a fixed coal bed, through a quartz window, in an L-shaped gasifica-
tion reactor. The illustration of the L-shaped reactor is given in
Fig. 17a. The coal bed was contained in the 30-cm diameter vertical
section of the L, and a solar beam was admitted at the far end of the
horizontal member through a 20 cm-diameter quartz window.
Steam or CO2 was passed through the heated coal bed in the gasi-
fier. The coal bed temperature was measured at the positions about
2 cm behind the reaction front of the coal bed, which varied from
1175 to 1425 K. The product gases from the reactor were mainly
CO and H2. There was a considerable range of scatter of the chem-
ical storage efficiencies from 19% to 48% in the solar power range of
4–23 kW. They indicated that ash buildup in the reaction zone
caused less efficient operation by increasing the fraction of sun-
light reflected and by reducing coal concentration in the solar-
Fig. 17. Illustrations of (a) L-shaped, packed bed solar gasifier and (b) packed bed solar gasifiers with a plunger.
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solener.2017.05.084
heated reaction zone. Scatter of the data was believed to result
mainly from ash buildup and ash fusing, and from the different
positions of the reactor in the focal plane. For the CO2 gasification,
a solar power level of 10.7 kW was used, and 27% of this solar
power was chemically stored in the product gas. Taylor et al.
(1983) demonstrated charcoal gasification with steam, or CO2 in
ð8Þ a packed bed solar gasifier with a plunger for using a 2-kW solar
furnace. The structure is illustrated in Fig. 17b. The packed bed
ð9Þ was pushed up by the plunger. The steam was generated by spray-
ing water directly onto the surface of the charcoal and at the same
time, heating the charcoal at the focus of a solar furnace. At an
optimum rate of water injection, half of the steam reacted with
carbon and 30% of the incident solar energy was stored as chemical
enthalpy at solar power of 1.2 kW. In the charcoal gasification with
CO2, the fraction of incident solar energy utilized to produce CO
ranged in 31–42% with the solar power of 670–1270 W. The chem-
ical storage efficiency range was 35 ± 5%, about the same as that
observed previously by Gregg et al. (1980a). Chemical storage effi-
ciencies of around 30–40% were obtained in the fixed-bed solar
coal gasifiers.
However, in an industrial scale up, packed bed coal gasifiers
involve some technical drawbacks, such as limitations of mass
and heat transfer, long solid residence time and ash buildup to pre-
vent the reaction. From this point of view, other concepts of solar
gasifiers must be developed for industrial scale applications. In
Sections 3.2 and 3.3, the recent R&D on particle ‘‘cloud” and ‘‘flu-
idized” solar gasifiers are reviewed. Indirect particle gasifiers are
reviewed in Section 3.4.
3.2. Particle cloud vortex flow gasifiers
SYNPET (Hydrogen Production by Steam Gasification of Pet-
coke) is a collaborative project between CIEMAT, ETHZ and the
industrial partner PDVSA (Venezuela). The main purpose of this
project was to demonstrate the technical feasibility of solar gasifi-
cation of waste from extra-heavy oil in the Fajadel Orinoco. It
involves H2 production by solar gasification of petcoke and vacuum
residue from heavy oil refining. In the initial phase of this project, a
5 kW prototype was developed and tested at PSI. From the
obtained results, the design of a solar reactor with quartz window
was scaled up for an evaluation of a 500 kW installation at the PSA
CRS tower.
Using concentrated solar energy and petroleum coke, the ther-
modynamics and kinetics of the pertinent reactions were analyzed
for two types of petroleum coke: Flexicoke and Petrozuata delayed
coke (Trommer et al., 2005). Based on reaction mechanisms
 T. Kodama et al. / Solar Energy xxx (2017) xxx–xxx 13

(describing reversible adsorption/desorption processes) and irre-
versible surface chemistry, kinetic rate laws were formulated. An
experimental quartz tubular reactor containing a fluidized bed of
petroleum coke in steam was directly exposed to concentrated
radiation to determine the kinetic parameters and their
Arrhenius-type temperature dependence. Syngas containing
approximately an equimolar mixture of H2 and CO and with a rel-
ative CO2 content of less than 5% was produced at above 1350 and
1550 K for Flexicoke and Petrozuata delayed coke respectively. Fol-
lowing this study, design of a 5 kW prototype solar reactor was
presented with modeling and testing results (Z’Graggen et al.,
2006). As shown in Fig. 18, the reactor features a continuous vortex
flow of steam laden with petcoke particles confined to a cavity
receiver and directly exposed to concentrated solar radiation. The
reactor was tested in a high-flux solar furnace at PSI in the range
of 1300–1800 K, and up to 87% petcoke conversion was obtained
in a single pass of 1 s residence time. The reactant mass flow rate
was in the range of 1.85–4.45 g petcoke/min and 3.68–9.04 g
steam/min. In order to prevent the steam condensation and protect
it from radiation spillage, the window was oil cooled and kept in
the range 393–453 K. The window was kept clean by an aerody-
namic protection created by a tangential flow through four tangen-
tial nozzles (Z’Graggen et al., 2006).
A petcoke–water slurry was continuously injected into a solar
cavity-receiver, to create a vortex flow directly exposed to concen-
trated radiation, and the effect of particle size (range 8.5–200 mm)
and slurry stoichiometry (range 2.1–6.3) on the degree of chemical
conversion and energy conversion efficiency was examined
(Z’Graggen et al., 2007). The solar energy conversion efficiency,
defined as the portion of solar energy absorbed as chemical energy
and sensible heat, was about 17%. For solar inputs between 3.3 and
5.1 kW, the energy conversion efficiency was between 0.5% and
4.7%. The average composition of the syngas production was: 62%
H2, 25% CO, 12% CO2 and 1% CH4. The maximum degree of carbon
conversion obtained was 87% at 1500 K, with water-petcoke molar
ratio of 4.8 and 2.4 s of residence time. Subsequently, the combined
pyrolysis and steam-gasification of petroleum vacuum residue was
performed using a 5 kW aerosol-flow solar chemical reactor in the
temperature range 1420–1567 K (Z’Graggen et al., 2008). The feed-
stock was continuously injected as a liquid spray at 423 K into the
reactor’s cavity along with a coaxial steam flow. This reactor was
further used for upscaling the 5 kW prototype to a 300 kW and
solar gasification with petroleum vacuum residue and steam
(Z’Graggen and Steinfeld, 2008). A two-phase reactor model that
couples radiative, convective, and conductive heat transfer to the
chemical kinetics was developed to optimize the reactor geometri-
cal configuration and operational parameters such as particle size,
feeding rates, and solar power input. For the 300 kW reactor, com-
plete reaction extent was predicted for an initial feedstock particle
size up to 35 lm at residence time of less than 10 s and peak tem-
peratures of 1818 K. The upscaling of this reactor concept to a
500 kW at the SSPS-tower (PSA, Spain) was presented (Vidal
et al., 2010). The reactor was designed to produce about 100–
180 kg/h of syngas from 50 kg/h of petcoke.
3.3. Particle fluidized bed gasifiers
Because of some technical drawbacks of a fixed-bed coal gasi-
fier, such as limitations of mass and heat transfer, long solid resi-
dence time and ash buildup to prevent the reaction, Epstein
suggested in 1994 that the circulating, or spouted fluidized-bed
reactors are desirable (Epstein et al., 1994). The solid residence
time must be accomplished in minutes, depending on the chemical
reactivity and temperature level. Earlier, Taylor et al. (1983)
demonstrated the fluidized-bed coal gasifier with CO2 under direct
solar irradiation in their 2-kW solar furnace. The reactor was
essentially a vertical silica-glass tube (5-cm diameter) located at
the focus of the solar furnace. The downward high-flux solar beam
illuminated the upper surface of the fluidized bed in the silica-glass
tube. At a solar power of about 1.1 kW, the maximum chemical
storage efficiency was 10% with 30% CO2 conversion. Marray and
Fletcher (1994) also investigated the steam gasification in a flu-
idized bed of cellulose using a quartz reactor and a solar furnace.
The present author (Kodama et al., 2002) also tested a quartz tube
reactor for CO2 gasification of bituminous coal under direct irradi-
ation of the fluidized coal bed with 0.3 kWth of concentrated visible

Fig. 18. Scheme of a vortex-flow solar thermochemical reactor for the steam-gasification of petcoke (Z’Graggen et al., 2006).

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solener.2017.05.084
14 T. Kodama et al. / Solar Energy xxx (2017) xxx–xxx
light from a sun-simulator. Von Zedtwitz and Steinfeld (2005)
modeled and investigated a quartz tube reactor containing a flu-
idized bed of coal particles for steam generation. Muller et al.
(2003) studied the reaction kinetics for steam gasification of a flu-
idized bed of coal using a quartz tube reactor.
For about a decade, the present author (Kodama et al., 2008a)
has developed a ‘‘window-type” solar gasifier containing a flu-
idized bed of coal particles exposed to concentrated visible light
(Kodama et al., 2008a, 2010; Gokon et al., 2012, 2014, 2015).
Laboratory-scale prototype windowed gasifiers were fabricated
for 1–3 kWth input power scales of concentrated visible light from
sun-simulators in order to test their reactor performances on
steam or CO2 gasification of coal or coke particles. The structures
of the prototype windowed gasifiers are similar to the particle flu-
idized receiver-reactor for CeO2 process of water splitting (Fig. 7).
In the typical design of the prototype windowed gasifier for 3 kWth
input power of concentrated visible light, the fluidized bed reactor
tube has a 420 mm length, and 62 mm inner diameter and 7 mm
thickness. The reactor tube was made of a stainless steel
(SUS310S). A metal foam distributor of porous stainless steel frits
was fixed at the bottom of the fluidized bed region in the reactor
tube. The internal centrally located draft tube has an inner diame-
ter of 20 mm and is 3 mm thick and 44 mm long. The bottom of the
draft tube was positioned 28 mm above the distributor. The top of
the reactor tube was equipped with a diverging conical funnel for
mounting a quartz window.
In the first concept of gasification by this prototype windowed
gasifier, coal or coke particles were solely loaded (without other
fluidizing media such as sand particles) in the fluidized bed region,
and the fluidized bed of the particles was directly exposed to con-
centrated visible light. Two designs of the fluidized bed reactor –
internally circulating type with a draft tube and normal type with-
out a draft tube – were compared on steam and CO2 gasification
performances of coal coke (Kodama et al., 2008a, 2010; Gokon
et al., 2012, 2014, 2015). The design with the draft tube, that
enhances an internally circulation of the particles within the flu-
idized bed, showed a much more uniform temperature distribution
within the fluidized bed along with the depth direction of the bed,
superior gasification rates, coke conversion, and light-to-chemical
energy conversion (chemical storage efficiency) compared with
the normal fluidized gasifier design without a draft tube. For steam
gasification of coal coke particles, the windowed, internally circu-
lating fluidized bed gasifier with a draft tube for 3 kWth input
power of light irradiation showed 10% of the peak light-to-
chemical energy conversion (Gokon et al., 2015). The coke conver-
sion was about 60% in 120 min of light irradiation. For CO2 gasifi-
cation of coal coke, a peak light-to-chemical energy conversion of
12% was obtained by the same windowed gasifier with a draft tube
for 3 kWth input power of light irradiation (Gokon et al., 2012). The
coal coke conversion reached 73% in 120 min of light irradiation. A
kinetics analysis based on homogeneous and shrinking core mod-
els was also done for CO2 gasification for the windowed, fluidized
bed gasifier (Gokon et al., 2012).
In the second concept for the gasification by this windowed
gasifier, in order to enhance the gasification rate in the fluidized
bed, quartz sand particles were investigated as a chemically inert
fluidized bed material which improves heat transfer within the
bed and thermal storage of the bed during direct light irradiation
of the bed (Gokon et al., 2014). The mixture of coal coke and quartz
sand particles was loaded in the windowed gasifier and the steam
gasification of coke particles was performed by irradiating the top
surface of the fluidized bed of the mixture with about 3 kWth input
power from a sun-simulator. 96–320 g of quartz sand and 32–
112 g of coke particles were used for the fluidized bed. The static
bed height was about 110 mm. The bed temperature distribution
during irradiating the top surface of the fluidized bed with concen-
Please cite this article in press as: Kodama, T., et al. Particle reactors for solar thermochemical processes. Sol. Energy (2017), http://dx.doi.org/10.1016/j.
solener.2017.05.084
trated visible light could be reduced by optimizing the passing gas
velocities of steam, and the almost uniform temperature distribu-
tion within the bed was created at around a temperature between
1000 and 1200 °C depending on the gas velocities. The test cam-
paign for coal coke gasification was performed by two operation
modes of the windowed gasifier. The first operation mode was a
batch-type reaction mode. Steam was passed through the bed of
the mixture of coal coke and quartz sand to prepare a fluidized
bed and simultaneously gasify the fluidizing coal coke particles
by heating with direct light irradiation. The coke conversion after
120 min of irradiation reached 60–88%. The peak light-to-
chemical energy conversion was 5–13%. The second operation
mode involved a series of processes. This mode was essentially a
batch-type reaction mode but carried out for future application
to an operation mode in which coal coke particles are continuously
fed to the fluidized sand bed (by using screw feeder with hopper)
at a high temperature above 1000 °C in the solar windowed gasi-
fier. A mixture of coal coke and quartz sand was initially fluidized
by passing N2 gas while irradiating the bed top surface with con-
centrated light in order to create a stable particle fluidization
before gasification reaction. After reaching the steady state of flu-
idization at around 1000 °C, passing gas was switched from N2 to
steam to start the gasification reaction at the high temperature.
Immediately after switching the passing gas from N2 to steam,
the strong peaks of CO and H2 evolution appeared. The gasification
of coal coke was completed in 10–30 min after switching gas to
steam. The coke conversion was about 93% and the light-to-
chemical energy conversion was 13% at the peak.
As mentioned above, at the new beam-down solar concentrat-
ing system at Miyazaki, Japan, 17 kg of quart sand particles was
fluidized in the 100-kWth windowed receiver-reactor and the top
surface of the fluidized bed was exposed to concentrated solar
radiation from the beam down system through the quartz window
at the top of the receiver-reactor (Kodama et al., 2016a). The cen-
tral bed temperature of the sand particles in the fluidized bed
exceeded 1100 °C even in the middle of December in Miyazaki,
Japan. The fluidized bed temperature above 1000 °C is sufficient
for operating gasification reaction. This implies that by combining
the new beam-down system and the new windowed solar gasifier,
solar gasification can be probably operated if coal particles are fed
to solar-heated fluidized bed of sand particles.
3.4. Indirect particle gasifiers
An indirectly heated 5 kW packed-bed reactor prototype was
designed as shown in Fig. 19 for a beam-down system
(Piatkowski and Steinfeld, 2008). In which, the sunlight collected
by the heliostat field was redirected, by a hyperbolic reflector, to
the receiver at ground level. The reactor consisted of two cavities
in series separated by SiC-coated graphite plate as a radiant emit-
ter plate. A CPC (compound parabolic concentrator) was incorpo-
rated in the reactor’s aperture to increase the incident solar flux.
The upper cavity contained a small windowed aperture served as
the solar absorber. The lower one was the reaction chamber and
contained the reacting packed-bed. The reactor was tested with
beech charcoal up to 1440 K packed-bed temperature. A quasi-1D
transient thermal model was developed by coupling combined
radiative–conductive heat transfer with chemical reaction kinetics
for steam gasification of coal. Model validation was accomplished
by experimental measurements of bed temperatures, gasified mass
and bed shrink rates for beech charcoal. The overall reaction rate
was determined experimentally by thermogravimetry, while the
effective thermal conductivity was determined experimentally in
a radial heat flow oven. The authors concluded that above
1300 K, radiative transfer was the predominant mode of heat
transport within the bed, consequently the effective thermal con-
 T. Kodama et al. / Solar Energy xxx (2017) xxx–xxx
Fig. 19. Indirectly irradiated solar packed-bed reactor for steam gasification of coal (Piatkowski and Steinfeld, 2008).
ductivity was significantly increased. This prototype reactor was
further used to test solar steam gasification of industrial and sew-
age sludge, scrap tire powder, fluff, south african coal and beech
charcoal (Piatkowski et al., 2009). It was reported that the reactor
was operated up to 1490 K and yielded high-quality syngas with
typical molar ratios of H2/CO = 1.5 and CO2/CO = 0.2. The calorific
content was upgraded up to 30%. Solar-to-chemical energy conver-
sion efficiencies varied between 17.3% and 29%. A multiple pseudo-
component first-order reaction model was formulated to describe
the rates of the combined pyrolysis and gasification processes by
Piatkowski and Steinfeld (2010). Arrhenius-type kinetic parame-
ters were determined by dynamic thermogravimetric experimen-
tal runs conducted in the temperature range of 473–1476 K.
Further efforts were made by the same group (Piatkowski and
Steinfeld, 2011) to develop a more complex dynamic model for
the solar-driven packed-bed reactor for the steam gasification of
heterogeneous, high-volatile content, carbonaceous waste feed-
stocks. Model validation was accomplished in terms of converted
mass, reactor temperatures and efficiency based on experiments
with an 8-kW reactor (packed bed temperature up to 1490 K).
The model was further applied to analyze a 200 kW upscaled solar
gasifier of sludge operating under a simulated solar day; for a reac-
tor having a 4 m diameter packed bed, energy conversion efficiency
was up to 89.4%.
A two-phase biomass char (biochar) steam gasification fluidized
bed model was developed, as shown in Fig. 20, with concentrated
solar heat as source of energy (Gordillo and Belghit, 2011). The
Rosseland approximation was used to calculate the radiative trans-
fer within the bed (Gordillo and Belghit, 2011; Bardos et al., 1987).
Their trends and predictions were in good agreement with the
reported results (Piatkowski et al., 2009). The steam-gasification
of biochar with concentrated solar radiation was experimentally
investigated using a 3 kW solar reactor consisting of a cylindrical
cavity-receiver containing an opaque tubular absorber (Melchior
et al., 2009). Fig. 21 shows the scheme of the indirectly irradiated
Please cite this article in press as: Kodama, T., et al. Particle reactors for solar thermochemical processes. Sol. Energy (2017), http://dx.doi.org/10.1016/j.
solener.2017.05.084
15
entrained-flow solar reactor, which consisted of a 5 cm diameter
cylindrical cavity receiver and a single 2.5 cm diameter SiC concen-
tric tubular absorber. The cavity receiver made of 10 wt% YO2-
stabilized ZrO2 lined with Al2O3 insulation. The maximum thermal
energy conversion efficiency was 1.53%. A maximum carbon con-
version was 26% at 1425 K. A reactor model that couples radiative,
convective and conductive heat transfer to the chemical kinetics
was formulated and validated by comparing with experimentally
measured temperatures and carbon conversions. The developed
model was further applied to examine the thermal performance
of 100 kW and 1 MW scaled-up solar reactor containing multiple
tubular absorbers. The predicted results showed that a maximum
solar-to-chemical energy conversion efficiency was about 39%
and 50% for 100 kW and 1 MW respectively. The same model
was further improved and applied to estimate the performance
of a 10 MW scaled-up reactor for a solar tower system (Maag
et al., 2010; Maag and Steinfeld, 2010). It was solved numerically
by Monte Carlo and finite volume techniques. For an optimized
reactor geometry and a desired outlet temperature of 1500 K, a
solar-to-chemical energy conversion was 37%.
High temperature biomass gasification was performed in a pro-
totype concentrated solar reactor (Lichty et al., 2010). Fig. 22
shows the schematic of the indirectly irradiated entrained-flow
solar reactor which consisted of a cylindrical cavity receiver
(18 cm diameter) with specular reflective inner surfaces containing
5 absorbing tubes. It was installed and tested at NREL’s high flux
solar furnace. For 7.5 kW solar power with an interchangeable
cooling plate, the central tube temperature was 1660 K for alumina
tubes. The highest temperature was achieved at the central tube
while the front and rear tubes were 350 and 250 K respectively.
Experiments were conducted to determine the effects of tempera-
ture, gas flow rate, and feed type on the gasification performance. A
tubular reactor was constructed and tested for hydrogen produc-
tion by biomass gasification in supercritical water using concen-
trated solar energy Chen et al. (2010). Fig. 23 shows the scheme
16 T. Kodama et al. / Solar Energy xxx (2017) xxx–xxx

Fig. 20. (a) Packed bed gasifier (Piatkowski et al., 2009) converted into (b) bubbling fluidized bed gasifier (b) (Gordillo and Belghit, 2011).

of the tubular reactor which was made of SS 316 stainless steel
with 10 mm outer diameter, 6 mm internal diameter and 18 m
length. 6 kW experimental setup was fabricated. Glucose and bio-
mass (corn meal and wheat stalk) were gasified. The reactor was
exposed to concentrated solar irradiation entering through the
aperture of cavity. The complete gasification was achieved with
0.2 M glucose as substrate, and the maximum yield ratio (the mass
of product gas/the mass of feedstock) reached up to 110%. This
study was further continued by a technical and economic analysis
and the cost for hydrogen production was estimated (Lu et al.,
2011).
4. Summary
In solar thermochemical particle reactors, directly irradiated
reactor is more efficient than the indirectly irradiated reactor.
However, one of the challenging tasks is to keep the window clean
and transparent. Thus, it has been considered as a critical and trou-
blesome component under high-pressure environments and large-
scale designs. Moreover, for operating temperatures above 1300 °C
under oxidizing atmospheres, ceramic materials are usually
required for lining the inner wall of the cavity. These refractory
materials are not resistant to the severe thermal shocks that often
take place under intermittent concentrated solar radiation. These
problems promote the R&D on the ‘‘direct solar absorbing parti-
cles” reactor. Particles cloud vortex flow, windowed reactors have
been developed for volatile ZnO process of two-step water split-
ting. In recent years, fluidized bed windowed reactor has been
developed for non-volatile ferrite or CeO2 process. These reactor
concepts have also been applied for solar gasification of carbona-
ceous materials such as coal, coke, biomass, etc. and demonstrated
for the solar power input scales above 100 kWth.
In solar indirectly absorbing or irradiated reactors, the main
advantage is to avoid the use of window. However, heat transfer
rate is less due to high thermal resistance of non-transparent wall.

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solener.2017.05.084
 T. Kodama et al. / Solar Energy xxx (2017) xxx–xxx 17

Fig. 22. Indirectly irradiated entrained-flow solar reactor for gasification of biomass
at high temperatures (Lichty et al., 2010).

in the field of directly irradiated reactors. As far as the indirectly

Fig. 21. Indirectly irradiated entrained-flow solar reactor for steam-gasification of
biochar (Melchior et al., 2009).
In addition, heat transfer is also affected by several other factors
such as packing density of the particles and physical properties
of the reactants. To enhance the heat transfer between the wall
and the reactants, appropriate intermediate working fluids should
be used. According to the literature, more research has been done
irradiated reactors is concerned, some examples of packed-bed
and entrained-flow reactors can be found; a few reactors have been
developed for thermal reduction of metal oxides; most of the indi-
rectly heated reactors have been designed and tested for solar gasi-
fication of biomass and other carbonaceous materials like coke,
coal and petroleum residues.
From this review, it can be concluded that these studies on solar
particle reactors have been mostly done at laboratory or pilot plant
scale levels. Further research has to be conducted to scale up theses
reactors towards the commercial scale level.

Fig. 23. Serpentine tubular reactor configuration for biomass gasification in supercritical water (Chen et al., 2010).

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solener.2017.05.084
18 T. Kodama et al. / Solar Energy xxx (2017) xxx–xxx

Conflict of interest Gokon, N., Mizuno, T., Nakamuro, Y., Kodama, T., 2008c. Iron-containing yttria-
stabilized zirconia system for two-step thermochemical water splitting. J. Sol.
Energy Eng. 130, 011018.
The authors declared that there is no conflict of interest. Gokon, N., Hasegawa, T., Takahashi, S., Kodama, T., 2008a. Thermochemical two-
step water-splitting for hydrogen production using Fe-YSZ particles and a
ceramic foam device. Energy 33, 1407–1416.
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