Energy Fuels 2010, 24, 65406547 : DOI:10.

1021/ef100936j
Published on Web 11/10/2010

Design of a 10 MW Particle-Flow Reactor for Syngas Production by Steam-Gasification

of Carbonaceous Feedstock Using Concentrated Solar Energy
Gilles Maag and Aldo Steinfeld*,,

Department of Mechanical and Process Engineering, ETH Zurich, 8092 Zurich, Switzerland, and

Solar Technology Laboratory, Paul Scherrer Institute, 5232 Villigen, Switzerland

Received July 22, 2010. Revised Manuscript Received October 4, 2010

Steam-gasification of carbonaceous feedstock is carried out in a solar reactor consisting of a cavity-receiver

containing an array of tubular absorbers, through which a two-phase flow of water vapor laden with m-
sized carbonaceous particles reacts to form H2 and CO (syngas). Concentrated solar radiation, entering
through the cavitys aperture, is supplied as the source of high-temperature process heat to the endothermic
reaction. A heat transfer model is formulated by coupling radiation/convection/conduction heat transfer
to the chemical kinetics for a solid-gas reacting flow. It is solved numerically by Monte Carlo and finite
volume techniques. Experimental validation is accomplished for biochar gasification with a 3 kW
prototype reactor subjected to high-flux thermal irradiation. The model is applied to analyze the
performance of a 10 MW industrial-scale reactor mounted on a solar tower configuration. For an
optimized reactor geometry and a desired outlet temperature of 1500 K, a solar-to-chemical energy
conversion of 37% is predicted for 1500 suns solar concentration.

1. Introduction amount equal to the enthalpy change of reaction;theoretically,

The thermal steam-gasification of carbonaceous materials
yields synthesis gas (syngas), a mixture of mainly H2 and CO
that can be use for power generation in efficient combined
cycles and fuel cells,1,2 or further processed to liquid fuels via
Fischer-Tropsch or other catalytic reforming processes.3,4
The simplified net reaction can be represented by


z ventional coal-fired generation plants.7 CO2 neutrality can be
CHz Oy s 1 - yH2 Og f 1 - y H2 g COg
2
Mineral matter, intrinsic water content, and other impurities
contained in the feedstock are omitted from consideration in
eq 1. Their presence may have an effect on the kinetics and
final product composition, but their exclusion does not affect
the main conclusions of the present analysis. Autothermal
gasification requires approximately 35% of the injected feed-
stock to be combusted to supply the high-temperature process
heat required to drive the endothermic reaction (eq 1),5 which
results inherently in low feedstock utilization, the necessity of
an air-separation unit for pure O2 stream, and the contamina-
tion of the off-gas with combustion byproducts. The use of
concentrated solar energy as the source of high-temperature
process heat can eliminate these drawbacks.5 It produces high-
quality syngas with higher output per unit of feedstock. It
further upgrades the calorific value of the feedstock by an
*To whom correspondence should be addressed. Telephone: 41 44
6327929. Fax: 41 44 6321065. E-mail: aldo.steinfeld@ethz.ch.
(1) Wright, I. G.; Gibbons, T. B. Int. J. Hydrogen Energy 2007, 32,
36103621.
(2) Steele, B. C. H.; Heinzel, A. Nature 2001, 414, 345352.
(3) Rostrup-Nielsen, J. R. Catal. Today 2000, 63, 159164.
(4) Wilhelm, D. J.; Simbeck, D. R.; Karp, A. D.; Dickenson, R. L.
Fuel Process. Technol. 2001, 71, 139.
(5) Piatkowski, N.; Wieckert, C.; Weimer, A. W.; Steinfeld A. Energy
Environ. Sci. 2010, DOI: 10.1039/C0EE00312C.
by up to 33%;resulting in a significant reduction of CO2
emissions vis-a-vis conventional autothermal gasifiers.5,6 A
second-Law (exergy) analysis indicates that combined Bray-
ton-Rankine power cycles running on solar-made syngas
from coal can double the specific electric output per unit mass
of coal, and consequently achieve specific CO2 intensities of
0.49-0.56 kg CO2/kWhe;approximately half that of con-
achieved if biomass is used as feedstock. Ultimately, solar-
driven gasification is a means of storing intermittent solar
1 energy in a transportable and dispatchable chemical form.
Solar-driven pyrolysis and gasification was investigated in
early studies.8-11 More recently, solar thermal gasification was
successfully applied to various carbonaceous materials
(e.g., coal, petroleum coke, vacuum residue, charcoal) using
directly irradiated fluidized-bed,12,13 molten-salt pool,14 and
vortex-flow reactors15 with reactants directly exposed to con-
centrated solar radiation, as well as indirectly irradiated packed-
bed6,16 and particle-flow17 reactors with graphite/ceramic tubes
(6) Piatkowski, N.; Steinfeld, A. Energy Fuels 2008, 22, 20432052.
(7) v. Zedtwitz, P.; Steinfeld, A. Energy 2003, 28, 441456.
(8) Murray, J. P.; Fletcher, E. A. Energy 1994, 19, 10831098.
(9) L
ed
e, J. Sol. Energy 1999, 65, 313.
(10) Gregg, D. W.; Taylor, R. W.; Campbell, J. H.; Taylor, J. R.;
Cotton, A. Sol. Energy 1980, 25, 353364.
(11) Beattie, W.; Berjoan, R.; Coutures, J. P. Sol. Energy 1983, 31,
137143.
(12) Kodama, T.; Kondoh, Y.; Tamagawa, T.; Funatoh, A.; Shimizu,
K.-I.; Kitayama, Y. Energy Fuels 2002, 16, 12641270.
(13) v. Zedtwitz, P.; Lipi
nski, W.; Steinfeld, A. Chem. Eng. Sci. 2007,
62, 599607.
(14) Adinberg, R.; Epstein, M.; Karni, J. J. Sol. Energy Eng. 2004,
126, 850857.
(15) ZGraggen, A.; Haueter, P.; Maag, G.; Vidal, A.; Romero, M.;
Steinfeld, A. Int. J. Hydrogen Energy 2007, 32, 992996.
(16) Piatkowski, N.; Wieckert, C.; Steinfeld, A. Fuel Process. Technol.
2009, 90, 360366.
(17) Melchior, T.; Perkins, C.; Lichty, P.; Weimer, A. W.; Steinfeld,
A. Chem. Eng. Process. 2009, 48, 12791287.

r 2010 American Chemical Society 6540 pubs.acs.org/EF

Energy Fuels 2010, 24, 65406547 : DOI:10.1021/ef100936j
Figure 1. Solar reactor configuration consisting of a cavity-receiver
with a windowless slab aperture containing an array of tubular
absorbers, through which a reacting mixture of steam and carbo-
naceous particles flow. A CPC is incorporated at the aperture.
or other opaque surfaces serving as absorbers and heat
conductors. Of special interest is the latter reactor concept,
schematically shown in Figure 1. It consists of a cylindrical
solar cavity-receiver with a windowless slab (rectangular)
aperture containing an array of tubular absorbers, through
which a reacting mixture of steam and carbonaceous particles
flow. A trough compound parabolic concentrator (CPC)18 is
incorporated at the aperture to further augment the
incident solar flux, reduce the aperture size, and minimize
reradiation losses. Concentrated solar energy entering
through the aperture is transferred by combined radiation/
conduction/convection to the reacting flow. In the present
study, a numerical reactor model that couples heat transfer,
fluid flow, and chemical kinetics is developed. Its exper-
imental validation is accomplished with a 3 kW reactor
prototype tested for the steam-gasification of biochar. The
reactor model is then applied to optimize the design and
simulate the performance of a 10 MW reactor for a solar tower
system.
2. Solar Reactor Model
The solar reactor prototype for 3 kW solar thermal power
input with a single tubular absorber has been previously
described.17 The radiative exchange between the cavity and
absorber tube has been modeled in a previous study.19 Thus,
the outer absorber tube surface is taken as domain boundary.
The model domain is shown schematically in Figure 2. It
consists of an absorber tube made of reaction-bonded silicon-
infiltrated silicon carbide (SiSiC, HALSIC-I: 88-92 vol% SiC,
12-8 vol% metallic Si)20 of outer diameter dabsorber,o = 2.5 cm,
inner diameter dabsorber,i = 1.8 cm, and length Labsorber = 15 cm.
Water vapor at a mass flow rate m_ H2 O, in 0:79 g 3 min - 1 and
Ar at a volumetric flow rate V_ Ar, in 4:5 LN 3 min - 1
(18) Welford, W. T.; Winston, R. High Collection Nonimaging Optics;
Academic Press: San Diego, CA, 1989.
(19) Maag, G.; Rodat, S.; Flamant, G.; Steinfeld, A. Int. J. Hydrogen
Energy 2010, 35, 13232-13241.
(20) Haldenwanger, W. Technische Keramik GmbH & Co. KG.
HALSIC-R/-RX/-I/-S/ Silicon Carbide Special Materials Catalogue.
http://www.haldenwanger.de (accessed 2007).
6541
Maag and Steinfeld
Figure 2. Longitudinal section view of an absorber tube.
Figure 3. Particle number and volume density distribution of the
beech charcoal feedstock and the 11 discrete size intervals used for
computation of the radiative properties of the particle suspension.
(LN means liters under normal conditions at 273 K and 1 atm),
which results in an inlet gas H2O molar fraction xH2 O, in 0:18,
are injected into the tube at Tin = 473 K and pin = 101 325 Pa.
Beech charcoal particles (biochar, Fluka 03866, Fbiochar =
450 kg 3 m-3,21 ash content 5%) are used as the carbonaceous
feedstock. The BET specific surface area of 180 m2g-1 was
determined by N2 adsorption at 77 K (Micromeritics TriStar
3000). The particle size distribution functions, mea-
sured by laser scattering (HORIBA LA-950), are shown in
Figure 3. Plotted are the number density and the respective
volume density of the beech charcoal feedstock, which has a
mean particle size of 7.2 m. The elemental composition,
C1H0.418O0.117S0.0003N0.006, was determined with Leco CHN-
900 (C-, H-, N-detection), Leco RO-478 (O-detection), and
Leco CHNS-932 (S-detection) instruments.
Biochar particles are fed into the gas stream using a rotating
brush feeder at a rate of 0.35 g 3 min-1, resulting in a particle
volume fraction fV = 8.2  10-5 at inlet. Heat is transferred by
conduction through the tube wall and by combined radiation,
convection, and conduction into the axially flowing, reacting
medium. For conduction,
 
2kSiC Tabsorber, o - Tabsorber, i z
qconduction z   2
ln dabsorber, o =dabsorber, i
A value of kSiC = 45.2 W 3 m-1 3 K-1 at 1073 K is given by
the manufacturer,20 which results in a difference between
inner and outer surface temperature lower than 10 K. A
constant outer absorber temperature Tabsorber,o is assumed
(21) Brocksiepe, H.-G. Charcoal. In Ullmanns Encyclopedia of In-
dustrial Chemistry; Wiley-VCH: Weinheim, Germany, 2005.
Energy Fuels 2010, 24, 65406547 : DOI:10.1021/ef100936j Maag and Steinfeld

over the reaction zone. Convective heat transfer in the inner Table 1. Coefficients a, b, and c Determined by Least-Square Fitting
tube is given by22 of a Second-Order Polynomial Function to Radiative Heat Transfer
Rates Obtained by MC for the 3 kW and the 10 MW Reactor Designs
for laminar flow : Nuz 3:66 3
Qnominal dabsorber,i a b c
(kW) (m) (W 3 m-2 3 K-4) (W 3 m-2 3 K-4) (W 3 m-2 3 K-4)
for turbulent flow : Nuz 0:023Rez0:8 Prz0:4 4
  3 0.018 -3.56 1.88  10-4 0
with Re (z) = [F(z) w(z) dtube,i]/(z), Prz cp zz =kz, 10,000 0.08 -3.37 7.02  10-4 0
and Nu (z) = [R (z) d (z)]/k(z). For transitional flow (2300 e
Re e 10 000), Nu is obtained by linear interpolation between intervals of the particle size distribution of Figure 3, based on
the two cases. The heat conductivity and dynamic viscosity the particle size parameter = dp/ in the range 10-1 to 102
of the gas mixture (Ar, H2O, H2, CO) is calculated from the and the complex refractive index of the particle approximated
kinetic gas theory,23 whereas polynomial approximations are by that of propane soot.31,32 For a given particle size distribu-
used for specific heat cp .24 Properties are computed by a tion, the radiative heat flux between the inner tube wall and
weighted sum for all gas species, using their molar concentra- the medium can be reasonably well approximated in the range
tion as weight function. of interest by19
Radiative heat exchange between the tube walls and the qradiation z
carbon particles in the reacting flow is treated by a collision-  
based Monte Carlo (MC) ray-tracing model.25 Application of afV2 z bfV z c Tabsorber
4
, i z - Tbulk z
4
7
the line-by-line model to the molecular spectroscopic database
HITRAN-200426 for similar fV of particles indicated that the where the parameters (a, b, c) are obtained by least-squares
contribution of the gas phase is less than 5% of the total fitting to the data points generated by MC. The parameters
radiative flux, and therefore negligible.27 The radiative flux are listed in Table 1 for the 3 kW and the 10 MW reactor
divergence is given by28 design. The steady-state 1D mass conservation equation is
P formulated for each gas component i
Qray, k K, p dsk
DQr,
d r 3 qr, d  4KP T 4 - k 5 DFi z D 
DV 2rdrdz 0 - F zwz r 000 i z 8
Dt Dz i
where k designates a generic stochastic ray traversing
with w being the flow velocity in the axial direction for both
in 3D the path length dsk within subelement of volume
particles and gas. The boundary condition at inlet is
 and carrying
dV R L R rabsorber,ai portion
of radiative flux Qray, k
-1 Fi z 0 xi, in pin =RTin for each inlet gaseous component
Qe 4 0 0 KP T 4 2rdrdz Nrays . The path length
hi = (H 2O, Ar), and Fj z 0 xj, 0 fV , 0 Fbiochar =
to a scattering event s is calculated from  i

Z s  M biochar 1 fV , 0 for each solid component of biochar j =
R s exp - sca, sds 6 C, H, and O (N and S are neglected), with fV , in
V_ p, in = V_ p, in V_ g, in .
0

where Rs is a random number chosen from a uniform The reaction kinetics was determined by thermo-
distribution set between 0 and 1 that represents the prob- gravimetry.5 Application of the shrinking spherical particle
abilistic cumulative distribution function for scattering by model for an unreacted spherical core33 yields the reaction rate
particles. Similarly, the wavelength and direction of emis- of each component i
sion and direction of scattering can be calculated using the dFi z
ri 000 z i FC, in 1=3k 0 zFC 2=3z 9
corresponding cumulative distribution functions. Radia- dt
tive properties of the biochar particles are calculated by
assuming independent scattering and the refractive index where is the stoichiometric coefficient of each species of
of the gas phase to be equal to unity.29 The absorption, eq 1. The rate constant
 is assumed to obey the Arrhenius law,
0
scattering, and extinction coefficients and the scattering phase k z k0 exp - Ea =RTbulk z , with an apparent activa-
function are obtained by applying the Mie theory30 for 11 size tion energy Ea =43,154 J 3 mol-1 and a pre-exponential factor
k0 = 120.6 s-1, the latter being adjusted for the experimental
(22) Incropera, F. P.; DeWitt, D. P. Fundamentals of Heat and Mass validation and in good agreement with the one obtained by
Transfer, 4th Ed.; John Wiley & Sons: New York, 1996. applying a 2D steady-state reactor model with uniform reac-
(23) Silbey, R. J.; Alberty, R. A.; Bawendi, M. G. Physical Chemistry,
4th Ed.; John Wiley & Sons: Hoboken, NJ, 2005. tion zone temperature (k0 = 124.6 s-1).17 Assuming plug flow
(24) Binnewies, M.; Milke, E. Thermochemical Data of Elements and and ideal gas while neglecting the volume of the solid phase
Compounds, 2nd Ed.; Wiley-VCH: Weinheim, Germany, 2002. ( fV < 10-4) and the pressure drop (below 1% across the
entire system), V_ gas z n_ gas zRTbulk z=pin . Deriving with
(25) Yang, W.-J.; Taniguchi, H.; Kudo, K. Radiative Heat Transfer
by the Monte Carlo Method. In Advances in Heat Transfer; Harnett, J. P.,
Irvine, T. F., Eds.; Academic Press: San Diego, CA, 1995; Vol. 27, pp 3-215. respect to axial distance z yields the infinitesimal flow velocity
(26) Rothman, L. S.; et al. J. Quant. Spectrosc. Radiat. Transfer 2005, change
96, 139204.
(27) Maag, G.; Lipi
nski, W.; Steinfeld, A. Int. J. Heat Mass Transfer dwz RTbulk z X 000 wz dTbulk z
2009, 52, 49975004. ri z 10
(28) Farmer, J. T.; Howell, J. R. Comparison of Monte Carlo dz p i
T bulk z dz
strategies for radiative transfer in participating media. In Advances in
Heat Transfer; Harnett, J. P., Irvine, T. F., Eds.; Academic Press: San Diego,
CA, 1998; Vol. 31, pp 333-429; (31) Dalzell, W. H.; Sarofim, A. F. J. Heat Transfer 1969, 91, 614618.
(29) Tien, C. L.; Drohlen, B. L. Annu. Rev. Numer. Fluid Mech. Heat (32) Bond, T. C.; Bergstrom, R. W. Aerosol Sci. Technol. 2006, 40,
Transfer 1987, 1, 132. 2767.
(30) Bohren, C. F.; Huffmann, D. R. Absorption and Scattering of (33) Levenspiel, O. Chemical Reaction Engineering; John Wiley &
Light by Small Particles; Wiley: New York, 1983. Sons: New York, 1999.
6542
Energy Fuels 2010, 24, 65406547 : DOI:10.1021/ef100936j Maag and Steinfeld

The first right-hand term accounts for gas moles being

produced by the chemical reaction while the second term
considers thermal gas expansion. Boundary condition at inlet
is wz 0 win V_ gas, in =Atube, i . Atube,i is the inner cross-
section area of the tube.
The steady-state 1D energy conservation equation is for-
mulated assuming infinitely fast thermal exchange between
the particle suspension and the gas


D X
Fi zhi z 0
Dt
D X Dq
conduction z
Fi zwzhi z - rC 000 zhR z 11
Dz i Dz

with the initial condition T(z = 0) = Tin = 473 K, where

P  
hR z i hi Tbulk z is the enthalpy change over the Figure 4. Averaged experimentally measured (18 runs at 9 Tabsorber,o)
i
reaction per reacted number of C moles. Since charcoal has no and theoretically calculated reaction extent as a function of Tabsorber,o
for the 3 kW reactor prototype.
reference enthalpy, all enthalpy changes were calculated by
assigning to charcoal the reference enthalpy of its elemental
composition at 300 K, and further adjusting for the small
offset between the heating value of charcoal (473.9 kJ 3 mol,
calculated from elemental composition34) and the enthalpy
change of the combustion reaction at 300 K given by



z y z z
C H2 O2 1 O2 f H2 O CO2 12
2 2 4 2

Equations 6, 8, and 9 are discretized in space and solved using

the finite volume (FV) method.35
The reactor model is validated by comparing its results to
those obtained experimentally using a 3 kW solar reactor
prototype tested at ETHs high-flux solar simulator.17,36 The
extent of chemical reaction is obtained through C-balance:
n_ CO, out n_ CO2 , out n_ CH4 , out
XC 13
n_ C, in

Inlet biochar mass flow was determined by experimental

calibration of the brush feeder. Outlet gas composition was
measured online by gas chromatography. A shielded thermo-
couple was employed for the temperature measurement on the
outer absorber tube wall. Measurement of the temperature
profile along the tube was not technically possible in the present
experimental setup. Error bars resulted from inaccuracies in the
measurement and feeding devices (temperature (2% of read-
ing, gas flow controllers (0.8% of reading plus (0.2% of
scale, water flow controller (1% of reading, outlet gas concen-
trations (0.005 vol%, biochar feeding rate (0.05 g 3 min-1).17
Figure 4 shows the numerically calculated (curve) and averaged
experimentally measured (data points) reaction extent as a
function of Tabsorber,o. The agreement between calculated and
the averages of 18 experimentally obtained values at 9 differ-
ent Tabsorber,o lies within 18.8% ( 23.7% (mean difference (
standard deviation). The very efficient heat transfer from the
inner wall to the reacting flow is mainly due to the thermal
radiation absorbed by the particles (30-50% of total absorber-
to-bulk heat transfer rate), leading to a fast (0.030 s, 0.077s,
(34) Netz, H. Verbrennung und Gasgewinnung bei Festbrennstoffen;
Resch: Grafeling/M
unchen, Germany, 1982.
(35) Ferziger, J. H.; Peri
c, M. Computational Methods for Fluid
Dynamics, 3rd Ed.; Springer: Berlin, Germany, 2002.
(36) Hirsch, D.; v. Zedtwitz, P.; Osinga, T.; Kinamore, J.; Steinfeld,
A. J. Sol. Energy Eng. 2003, 125, 117120.
(37) ZGraggen, A.; Steinfeld, A. J. Sol. Energy Eng. 2004, 126,
819822.
6543
Figure 5. Front and top view of the 10 MW solar reactor, consisting of a
cavity-receiver with seven apertures-each having a hexagonal CPC-
and containing an array of tubular absorbers (dimensions in mm).
for Tabsorber,o = 1600 K) convergence of the medium tem-
perature Tbulk(z) within 95% of Tabsorber,i(z).
Main product gases were H2, CO, and CO2. Relatively
small amounts of CH4 were detected, produced from pyrolysis
reactions. The meas-red molar ratios H2:CO and CO2:CO
were higher than the corresponding equilibrium molar ratios
calculated for the fed molar ratio H2O:C = 1.88 for the same
Tabsorber,o, most likely due to the water-gas shift reaction
occurring as the products cool at the exit of the reactor.
3. Scale-Up to 10 MW Solar Power Input
An industrial-scale solar reactor mounted on a solar tower
system is considered. A schematic of the optimized cavity-
receiver configuration is shown in Figure 5. It has seven
apertures and contains an array of tubular absorbers. Viewed
from the top, the cavity has the shape of a circular section
having chord length W and height D. Each absorber tube of
Energy Fuels 2010, 24, 65406547 : DOI:10.1021/ef100936j Maag and Steinfeld

Table 3. Band-Approximated Overall Spectral Emittance E,

Reflectance R, and Transmittance V of the Quartz Window37
spectral band E R V

0-0.1 m 0.90 0.10 0.00

0.1-5 m 0.00 0.06 0.94
5- m 0.90 0.10 0.00

enclosures39 is applied to obtain a spectral-dependent system

of equations in terms of the steady-state temperatures and net
radiative fluxes on each surface
X

2
1   dqj  
kj - Rj, i Fk - j - Ej, o eb Tj
E
j 1 j , i
d

 dqe, j
1 - Rj, o
d
!
Figure 6. Top view of three cavity-receivers, each one facing its
X2   Vj, o dqe, j    
eb Tj kj - 1 - Vj, i Fk - j 14
dedicated portion of the heliostat field (North, East, and West), E j , i d
j1
positioned at an angle of 60 from each other to allow efficient
capturing of the incoming concentrated solar radiation by the CPCs. for 1 e k e (Nabsorbers 8), (1-7 = windows, 8 = cavity, 9 -
(Nabsorbers 8) = absorber tubes, where qe,i = Qsolar/Awindow
Table 2. Dimensions of the Scaled-Up Cavity-Receivers
(for 1 e i e 7), qe,i = 0 (for 8 e i e (Nabsorbers 8)), and
cavity qj = -Qabsorber, j/Aabsorber, j, for 9 e j e (Nabsorbers 8).
dimension symbol unit North East/West Subscripts i and o denote inner and outer properties of the
boundary walls, respectively. Neglecting external emission at
depth D m 2.0 1.2
height H m 4.0 4.0 the walls and absorber tubes, {Ej,o;Rj,o;Vj,o} = {Ej,i;Rj,i;Vj,i},
width W m 4.0 3.0 for 1 e j e 7, and Ej,o = Rj,o = Vj,i = Vj,o = 0, for 8 e j e
number of absorbers Nabs 26 20 (Nabsorbers 8). The view factor matrix F between the faces is
absorber outer diameter dabs,out m 0.14 0.14 obtained by Monte Carlo ray-tracing code. The system of
absorber inner diameter dabs,in m 0.08 0.08
distance between absorbers m 0.15 0.15
eqs 14 is integrated over the windows three spectral bands l to
yield a system of (Nabsorbers 8)  3 spectrally independent
diameter dabsorber is positioned at a 1 cm gap to the adjacent equations for totally (Nabsorbers 8)  (3 1) unknowns (qj,l,Tj).
one and to the wall. Secondary concentrators (CPC18) are The remaining equations are obtained from the relationship
incorporated at the apertures to obtain radiative flux intensities P3
qj qj , l , for 1 e j e (Nabsorbers 8). The incoming
above 3 MW 3 m-2 (3000 suns). Due to the limited acceptance l1
angle of the CPCs, a system of three cavity-receivers is con- radiation heat flux per spectral band l for each face is
R 2, l
qe, j, l Te,4j 1, l eb , Tsun d. Since the total (spectrally
q
sidered, each one facing a dedicated part of the heliostat field as
sun
shown in Figure 6. The central cavity-receiver has 26 tubular
integrated) optical properties of the window and the walls
absorbers, and the two lateral cavity-receivers have 20 tubular
are influenced by their temperatures Tj, their value has to be
absorbers each. The diameter and thickness of the absorber
determined iteratively.
tubes are limited by mechanical/thermal stability requirements,
The coupling between the cavity-receiver model19 and the
as heat transfer and fluid mechanics aspects (e.g., friction losses)
absorber tube model (presented in Section 3) is shown in the
play lesser roles in the range of dimensions considered. Dimen-
flow sheet of Figure 7. The cavity-receiver model considers the
sions resulting from previous cavity optimization for solar
incoming solar power Qsolar and the net heat sink Qabsorber,j on
thermal cracking of methane19 for a total Qsolar = 10 MW are
each absorber tube, and computes the outer surface tempera-
listed in Table 2 and differ for the central (North) and the two
tures Tabsorber,j of each absorber tube. These serve as input
lateral (East/West) solar cavity-receivers due to the different
for the absorber-reactor model which, given the inlet condi-
incident solar heat fluxes.
tions (Tin, pin), the composition (xi, in ) of the gas mixture, and
Band-approximated spectral optical properties for the
the inlet particle volume fraction (fV,in), is used to compute
quartz window are listed in Table 3. For the absorbers and
the net absorbed process heat by the flow in each tube,
cavity walls, a constant value for SiC of E = 0.9 is chosen.38
*
Qabsorber,j . The matching combinations of Qabsorber, j and
Qsolar is assumed to have Plancks spectral distribution of a
Tabsorber,o, j are obtained by iteration with convergence criterion
blackbody source at Tsource = 5780 K. Net absorbed process 
j1 - Qabsorber, j Tabsorber, o, j , Tin , pin , xi, in =Qabsorber, j j e0:001,
heat is modeled as a heat sink on the absorber surface. Further
for each surface j.
assumptions are the following: diffuse window, opaque-
Two energetic performance indicators of the system are
diffuse cavity walls, uniform radiative heat flux, temperature,
considered. The thermal energy conversion efficiency is defined as
and properties on both surfaces, as well as no conductive or
convective heat transfer between window, cavity, and absorbers. Qthermal Qchemical
thermal 15
The radiosity method (enclosure theory) for semitransparent Qsolar
The solar-to-chemical energy conversion efficiency is de-
(38) Touloukian, Y. S.; DeWitt, D. P. Thermophysical Properties of fined as
Matter, Thermal Radiative Properties: Nonmetallic Solids, Vol. 8; IFI/
Plenum: New York/Washington, DC, 1972. Qchemical
(39) Siegel, R.; Howell, J. R. Thermal Radiation Heat Transfer, 4th chemical 16
Ed.; Taylor & Francis: New York, 2002. Qsolar
6544
Energy Fuels 2010, 24, 65406547 : DOI:10.1021/ef100936j
Figure 7. Flow sheet of the solar reactor model.
Figure 8. Variation of the outlet gas temperatures Tout with inlet
H2O mass flow ratefor the North (a) and East/West (b) scale-up
cavity-receivers. The parameter is the solar radiative flux through
the reactor aperture qsolar = 1.5, 2.0, 2.5, 3.0, 3.5, and 4.0 MW 3 m-2
and the inlet H2O:C molar ratio is 2.0.
P R Tout
with Qthermal _
Tin nin, i cp, i TdT being the power sup-
plied for
R Labsorber 000 heating i up the injected gases i and Q
chemical
0 r C zhR T bulk A absorber , i dz the enthalpy difference
between reactants and products at reaction temperature. The
performance of the three cavity-receivers is simulated over the
relevant range of operational conditions, assuming pure H2O
inlet flow laden with particles at a H2O:C ratio of 2.0 and
preheated to 473 K. Figure 8 shows the outlet gas temperature
Tout as a function of inlet H2O mass flow rate m_ H2 O, in and the
incoming solar radiative flux through the apertures qsolar
for the North (Figure 8a) and the East/West (Figure 8b)
(40) M uller, R.; v. Zedtwitz, P.; Wokaun, A.; Steinfeld, A. Chem. Eng.
Sci. 2003, 58, 51115119.
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Maag and Steinfeld
Figure 9. Variation of the extent of chemical reaction XC as a
function of the inlet H2O mass flow ratem _ H2 O, in for the North
(a) and East/West (b) scale-up cavity-receivers. The parameter is the
solar radiative flux through the reactor aperture qsolar = 1.5, 2.0,
2.5, 3.0, 3.5, and 4.0 MW 3 m-2 and the inlet H2O:C molar ratio
is 2.0.
Figure 10. Variation of the thermal energy conversion efficiency
thermal as a function of the inlet H2O mass flow ratem _ H2 O, in for the
North (a) and East/West (b) scale-up cavity-receivers. The para-
meter is the solar radiative flux through the reactor aperture qsolar =
1.5, 2.0, 2.5, 3.0, 3.5, and 4.0 MW 3 m-2 and the inlet H2O:C molar
ratio is 2.0.
cavity-receivers. Since Tout > 1400 K is required for mini-
mizing the CO2:CO ratio in the outlet gas,40 Tout = 1500 K is
set for the present analysis. For qsolar = 3.5 MW 3 m-2, such an
outlet temperature is obtained with m_ H2 O, in 2:21 kg 3 s - 1 ,
while for lower qsolar = 1.5 MW 3 m-2, only 0.61 kg 3 s-1 can be
processed. Figure 9 shows the extent of the chemical reaction
XC as a function of m_ H2 O, in and qsolar for the North (Figure 9a)
and the East/West (Figure 9b) cavity-receivers. XC drops
rapidly with increasing m_ H2 O, in due to insufficient residence
times. For example, XC = 31% for qsolar = 3.5 MW 3 m-2
at higher mass flow rate, but XC = 67% for q solar =
1.5 MW 3 m-2 at lower mass flow rate. Also, the bigger
quantity of processed mass barely compensates for the higher
solar concentrations necessary for heating it up and reaching
the desired Tout. This is corroborated in Figure 10, which
shows the thermal energy conversion efficiency thermal as a
function of m_ H2 O, in and qsolar for the North (Figure 10a) and
the East/West (Figure 10b) cavity-receivers. In fact, for the
envisaged inlet mass flow rates, the gain in thermal;from
75% for q solar = 1.5 MW 3 m -2 to 83% for q solar =
3.5 MW 3 m-2;is relatively modest in comparison to the
Energy Fuels 2010, 24, 65406547 : DOI:10.1021/ef100936j Maag and Steinfeld

the execution of the experimental runs at ETHs high-flux solar

simulator.

Nomenclature
2
A = area, m
a,b,c = polynomial coefficients, W 3 m-2 3 K-4
cp = specific heat, J 3 mol-1 3 K-1
D = depth, m
d = diameter, m
E = emittance
Ea = activation energy, J 3 mol-1
e = Plancks spectral emissive power distribution,
W 3 m-2 3 m-1
F = view factor matrix
Figure 11. Variation of the chemical energy conversion efficiency Fk-j = view factor between surfaces k and j
chemical as a function of the inlet H2O mass flow ratem
_ H2 O, in for the fd = particle size distribution probability density, % 3 m-1
North (a) and East/West (b) scale-up cavity-receivers. The param- fV = solid phase volume fraction
eter is the solar radiative flux through the reactor aperture qsolar = H = height, m
1.5, 2.0, 2.5, 3.0, 3.5, and 4.0 MW 3 m-2 and the inlet H2O:C molar hh = specific enthalpy, J 3 mol-1
ratio is 2.0.
hR = specific enthalpy of reaction, J 3 mol-1
variation of chemical in the same range. Figure 11 shows the k = thermal conductivity, W 3 m-1 3 K-1
solar-to-chemical energy conversion efficiency chemical as a k0 = rate constant, s-1
function of m_ H2 O, in and qsolar for the North (Figure 11a) and k0 = pre-exponential factor, s-1
the East/West (Figure 11b) cavity-receivers. An optimum L = length, m
qsolar = 1.5 MW 3 m-2 results in maximum chemical = 32%, Mh = molar mass, kg 3 mol-1

while for qsolar = 3.5 MW 3 m-2 a relatively low chemical = m = mass flow rate, kg 3 s-1
18% is reached. Since XC decreases with increasing m_ H2 O, in , Nabsorbers = number of absorber tubes

the maximal attainable values for chemical decrease with n = molar flow rate, mol 3 s-1
higher qsolar. Assuming XC = 1 (complete gasification), Nu = Nusselt number
chemical = 37% for qsolar = 1.5 MW 3 m-2 and chemical = p = pressure, Pa
41% for qsolar = 3.5 MW 3 m-2, thus pointing out the sig- Pr = Prandtl number
nificant solar-to-chemical efficiency gain potential through Q = power, W
cavity shape and absorber tube size optimization at highly q = heat flux, W 3 m-2
concentrated solar flux. R = reflectance
Rh = universal gas constant, 8.314 J 3 mol-1 3 K-1
Rs = random number
Summary and Conclusions
r = radius, Cartesian coordinate, m
We have developed a heat transfer model to simulate a solar r000 = reaction rate, mol 3 s-1 3 m-3
chemical reactor for steam-gasification of carbonaceous par- Re = Reynolds number
ticles. The model couples radiative heat transfer within the s = path length, m
cavity-receiver with radiation/convection/conduction heat T = temperature, K
transfer for a reacting flow inside the absorber tubes. Experi- V = transmittance; volume, m3

mental validation of the absorber tube model was carried out V = volume flow rate, m3 3 s-1
with a 3 kW solar reactor prototype. The agreement between W = width, m
the calculated curve for XC in function of Tabsorber,o and the 19 w = flow velocity in z-direction, m 3 s-1
experimentally obtained values lies within 18.8% ( 23.7% XC = extent of chemical reaction
(mean difference ( standard deviation). The validated model xh = mole fraction
was applied to estimate the performance of a 10 MW scale-up z = Cartesian coordinate, m
reactor for a solar tower system. For a desired outlet tem- Greek Letters
perature of 1500 K, relatively low solar flux concentrations of
1500 suns result in a higher solar-to-chemical energy conver- R = convective heat transfer coefficient, W 3 m-2 3 K-1
sion efficiency (32%) than that obtained with a solar flux ij = Kronecker delta function (ij = 1 for i = j, ij = 0 for i
concentrations of 3000 suns (18%) due to the higher mass flow
6 j)
and consequently lower residence times and extents of chemi- = energy conversion efficiency
cal reaction of the latter case. An estimation of the improve- = absorption coefficient, m-1
ment potential for the solar-to-chemical energy conversion = wavelength, m
efficiency shows values up to 41% at 3500 suns to be achiev- = dynamic viscosity, Pa 3 s
able by optimization of the cavity and absorber tube sizes for = stoichiometric factor
complete reaction extent of the fed biochar. = particle size parameter
F = density, kg 3 m-3
Acknowledgment. This work has been financially supported F = molar concentration, mol 3 m-3
by the Swiss National Science Foundation under contract = Stefan-Boltzmann constant ( = 5.6705  10-8
200021-115888. We thank T. Melchior and E. Guglielmini for W 3 m-2 3 K-4)
6546
Energy Fuels 2010, 24, 65406547 : DOI:10.1021/ef100936j Maag and Steinfeld
-1
sca = scattering coefficient, m o = outer
= residence time, s out = at outlet
P = Planck mean
Symbols p = particle phase
r = radiative
r = Nabla operator (cylindrical coordinates)
= spectral
Subscripts Abbreviations
e = entering through window CPC = compound parabolic concentrator
g = gas phase MC = Monte Carlo
i = inner FV = finite volume
in = at inlet XRD = X-ray diffraction

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