pubs.acs.

org/EF Article

Design of a Self-Management Solar Pyrolysis Packed-Bed Reactor by

Coupling Thermal Energy Storage
Hongyang Zuo, Kuo Zeng,* Dian zhong, Jun Li, Huaqian Xu, Yongwen Lu, Wang Lu, Hongyu Zhou,
Gilles Flamant, Haiping Yang, and Hanping Chen
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ABSTRACT: A new packed-bed reactor coupled with thermal

energy storage (TES) for solar pyrolysis of biomass is developed to
Downloaded via MINES PARISTECH on September 23, 2023 at 09:50:11 (UTC).

overcome the shortcomings of solar energy. The numerical model of

a 3.5 kW reactor is formulated by coupling heat and mass transfer
balances to chemical kinetics for biomass pyrolysis. It is solved
numerically by finite element techniques. The model is applied to
analyze the influence of the storage component on the thermal and
chemical performance of the pyrolysis process. A new criterion Y
defined as the ratio of the char yield and the effective solar power
input is proposed to evaluate the effectiveness of solar power input.
Under different solar radiation conditions, the coupled TES reduces
the solar energy consumption for the char production by over 16%.
The storage component can alleviate the overheating and thermal
cyclic stresses on the absorption surface. As compared to the non-TES design, the new design can decrease the temperature
fluctuation on the absorption surface for over 300 K during solar intermittencies. Moreover, the latent heat in the storage component
makes the pyrolysis process stable. Under short-term interruptions, the variation of char yield in the terminal temperature range of
623−673 K is as large as 34.9% in the non-TES design, and it can be decreased to 16.5% after coupling TES. This value can also be
decreased from 66.8% to 17.0% under long-term interruptions by coupling the storage.

1. INTRODUCTION a concentrated solar heating system is recognized as an

Global warming and fossil fuel depletion promote the rapid
development of renewable energy. Biomass, the fourth most
available energy source, is considered to have the potential to
be a major source of sustainable energy in the future.1
However, the low energy density as well as the remote
distribution of the raw biomass lead to a high cost of
transportation and storage. Therefore, the development of
more economic ways to utilize and upgrade the biomass energy
is urgently needed.2,3
Among the various biomass utilization technologies,
pyrolysis is recognized as one of the promising thermochemical
processes to convert biomass into biofuels. The product of
biomass pyrolysis has a significant economic potential,
especially the char produced by slow pyrolysis.4 For conven-
tional pyrolysis, the combustion of feedstock is required to
provide the thermal energy, which significantly reduces the
amount of biochar production.5,6 To improve the combustion
efficiency and avoid contamination by NOx during the
autothermal pyrolysis process, purification of air to produce
O2 must lead to an extra cost.7 Consequently, in this context,
the combination of biomass pyrolysis and concentrated solar
energy is of interest.8−10 Because of advantages of achieving
extensive heat input without combustion, the incorporation of
effective way to decrease the environmental pollution and
heating cost, and to increase feedstock valorization of biomass
pyrolysis.11
The solar reactor serves as the vital component of the solar-
driven pyrolysis system. Therefore, extensive studies focus on
the reactor design, and many different types of reactors have
been developed, including the fluidized bed,12,13 molten-salt
pool,14,15 vortex-flow cavity,16,17 and packed-bed.18 The
packed-bed reactor is characterized by its reliability, simplicity
of operation, and an outstanding adaptability to the moist
feedstock of any shape and size.5,19 Ayala-Cortés et al.20 carried
out pyrolysis experiments of 25 g bagasse fibers in the 25 kW
IER-UNAM solar furnace to investigate the impact of the
temperature and heating rate on the carbon composition,
structure, surface area, and electrochemical response. Sobek et
al.21 conducted a comparative study of the products’
Received: November 16, 2022
Revised: January 4, 2023
Published: January 19, 2023

© 2023 American Chemical Society https://doi.org/10.1021/acs.energyfuels.2c03884

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Energy & Fuels
Figure 1. Scheme of the packed-bed reactor and computational domain.
distribution and the in situ heating behavior of waste biomass
pyrolysis (fixed pellets with 18 mm diameter) driven by a 1.6
kW xenon lamp, revealing the gaseous species evolution of the
solar pyrolysis process. Zhong et al.22 investigated the unique
structural characteristics of solar pyrolysis char with 10 mm-
diameter wood pellets in a fixed-bed reactor heated under 1.1
MW/m2 radiation heat flux. Weldekidan et al.23 pyrolyzed
biomass waste particles with different sizes (280 and 500 μm)
with a 1.5 kW lab-scale solar furnace. The influence of the high
heating rate (from 10 to 500 °C/s) and temperature (from 800
to 1600 °C) on the pyrolysis products was analyzed. Currently,
studies on packed-bed (also known as fixed-bed) solar
pyrolysis were mainly conducted at the lab-scale, and
researchers paid more attention to the operation parameters
of the pyrolysis process.
Thus, the scale-up of solar pyrolysis reactors is urgently
needed to achieve commercial status. The development of a
large-scale solar pyrolysis reactor faces some crucial challenges:
(1) The first is the thermal management of the solar power
input. On the one hand, the uneven solar thermal power will
cause incomplete pyrolysis of the feedstock and non-negligible
thermal cyclic stresses.24,25 On the other hand, the directivity
and large power density of the concentrated solar radiation can
lead to the overheating of the absorption component.
Consequently, these particularities result in increasing the
difficulty in controlling the product quality.20,26
(2) The second is heat transfer enhancements inside the
reaction chamber. Increasing the size of the packed-bed causes
overlying thermal resistance and, therefore, makes a large part
of the feedstock react under an unexpected heating rate or
terminal temperature.7,27
To overcome the intermittency of solar radiation and
develop the self-management capacity of the pyrolysis process,
a novel solar pyrolysis packed-bed reactor coupled with the
high-conductive phase change material (PCM) is developed in
the current study. A two-dimensional transient model of the
developed reactor is established and further validated with
experimental data from the literature. The thermal and
chemical performances of the solar pyrolysis reactor under
constant and intermittent heating conditions are analyzed. On
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the basis of the terminal temperature of the pyrolysis process,
new performance indicators are proposed to quantitatively
assess the effectiveness of solar power utilization and the
quality of pyrolysis product in the packed-bed reactor,
respectively. The current study establishes the correlation
between TES and the pyrolysis process, which can provide
guidance in the optimization and regulation of the solar
pyrolysis process.
2. MODEL DESCRIPTION
2.1. Reactor Design and Computational Domain. The
concept of the packed-bed reactor coupled with a TES storage
component for solar pyrolysis is illustrated in Figure 1. This
reactor that consisted of three cavities is specifically designed
for a “beam-down” optical configuration of solar towers.7,27 An
aperture, which is covered by a quartz window, at the top of
the inner cavity enables the access of concentrated solar
radiation. SiC is employed to construct the encapsulation as
well as the absorption component of the inner cavity with
advantages of a high thermal conductivity and absorptivity.27,28
The chlorine salt composite with a molar ratio of NaCl:KCl =
6:4 used for high temperature thermal energy storage is
encapsulated in the middle cavity. Because of the low thermal
conductivity of the salt-mixture (0.84 W/mK), a SiC foam30,31
is immersed into the middle cavity to improve the heat transfer
performance. The salt-mixture is supposed to be fully
infiltrated in the pores of the foam. The outer cavity is packed
with the feedstock (beech wood) and acts as the reaction
chamber. The properties of the aforementioned materials,
pyrolysis products, the feedstock, and packed-bed applied in
the numerical simulation are summarized in Tables S1 and S2.
Because of the axial symmetry of these cavities, an axial-
symmetrical 2D domain is employed for the numerical
simulation. Similar to the emitter plate designed for indirect
solar heating, the high-conductive SiC foam can significantly
improve the uniformity of radiation absorption. Thus, the
irregularity of the radiation distribution on the wall of inner
cavity is neglected.7 As shown in Figure 1, only the middle
cavity and outer cavity are considered in the current numerical
model. The symbols rin and rmid indicate the radii of the inner
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Energy & Fuels
Figure 2. (a) The transition region of heat flux at the beginning of the pyrolysis process, (b) short-term interruptions, and (c) long-term
interruptions.
and outer boundaries of the PCM/skeleton domain (the
middle cavity); rout is the radius of the packed-bed domain (the
outer cavity); and a 5 mm SiC wall locates between these two
domains and separates them. The heights (H) of all domains
are set identically. On the basis of the prestudy, the geometry
parameters, rin, rmid, rout, and H, are designed as 5, 12, 17, and
20 cm, respectively. These parameters ensure a sufficient
storage capacity as well as satisfactory heat transfer perform-
ance in the reaction chamber.
To better analyze the effect of the storage component, a
series of non-TES cases, which have the same size of the
packed-bed domain as the main design, are also simulated in
the current study.
In the current reactor, five thermocouples (TC) are
numerically settled. These temperature probes are marked as
TC1−5 and horizontally distributed at the middle of the
reactor as shown in Figure 1. They enable one to analyze the
temperature of the absorption surface, the inner side of the
PCM, and the horizontal packed-bed layers.
For the initial conditions, the initial temperature of the
computational domain is 298.15 K, the initial pressure is 1 atm,
and the initial gas-phase density and feedstock density are 1.25
and 441 kg/m3, respectively. For the boundary conditions,
considering that the reactor may involve a multiunit
design,37,38 the side and the bottom boundaries of the
computational domain are considered adiabatic. The top
boundary of the packed-bed is set as the outflow condition.
Because of the high conductivity of the PCM/skeleton
assembly, the temperature in the inner cavity is considered
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uniform.7 Thus, the heat flux on the inner boundary of the
PCM/skeleton domain is determined as follows:
4 4
Q inlet = Q solar(t ) + eSiCA(Tenv Tcavity ) (1)
where eSiC is the emissivity of SiC, A is the area of the aperture,
and σ is the Stefan−Boltzmann constant. The current study
accounts for different types of radiation heating conditions,
and the solar power input Qsolar(t) will be introduced in the
following section.
2.2. Heating Conditions and Simulated Cases. Three
types of radiation heating conditions (total solar power input
on the wall of the inner cavity) are investigated, the constant,
short-term interrupted, and long-term interrupted radiation. As
shown in Figure 2a, all radiation heating conditions experience
a transition region in which the solar power input rises from 0
to 3.5 kW linearly within 1000 s. For the constant radiation
(Figure 2a), the solar power input remains at 3.5 kW after
1000 s. Figure 2b and c presents the interruptions and
durations for the short-term interrupted radiation and long-
term interrupted radiation. The short-term interrupted
radiation includes intermittencies of 5, 10, and 20 min.
These durations can be commonly found in previous
experimental studies on solar-driven reactors.7,24,27 After each
intermittence, the solar power input is set again to 3.5 kW and
remains for the same duration to investigate the energy
recovery of the PCM/skeleton composite. The long-term
interrupted radiation employs an intermittence of 40 min to
test the performance of the current design. The solar power
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input then is stopped to investigate the discharging perform-

ance of the PCM/skeleton composite.
Cases simulated in the current study are summarized in
Table 1. As shown in the table, cases related to the main design
Figure 3. Beech wood pyrolysis scheme.34
Table 1. Case Design in the Current Study
case mark heating conditions TES coupling Table 2. Kinetic Parameters for Beech Wood Pyrolysis34
C constant radiation PCM/skeleton reaction Ai (s−1) Ei (kg/mol) Δh (kJ/kg)
C′ constant radiation non-PCM 10
wood → tar 2.0 × 10 148.0 110
S short-term interruptions PCM/skeleton
wood → intermediate solid 2.51 × 107 117.0 0
S′ short-term interruptions non-PCM
intermediate → char and gas 1.38 × 1010 161.0 −210
L long-term interruptions PCM/skeleton
L′ long-term interruptions non-PCM

The effective thermal conductivity λbed,eff at any instant is

(base cases) and the aforementioned radiation heating calculated as the weighted sum of the feedstock particle,
conditions are marked as case C (constant), case S (short- volatiles’ conductivity, and accounting for radiation heat
term), and case L (long-term), respectively. The non-TES transferring through the packed-bed.
cases are named as case C′, case S′, and case L′,
correspondingly. Considering that the PCM/skeleton compo- 16 Tbed 3
bed,eff = p(1 bed) + bed v +
site causes a delay in the pyrolysis process, interruptions in 3 bed (6)
non-TES cases should also be modified to improve the
comparability. On the basis of the presimulation, the 3(1 bed)
interruption is set at 3000 s, which ensures a similar feedstock bed =
dp (7)
mass fraction between the main design and the non-TES
design at the beginning of the first radiation interruption. where κbed is the extinction coefficient, εbed is the porosity 32,33
2.3. Governing Equations. 2.3.1. Reaction Chamber. of the packed-bed, and dp is the average particle diameter of
Several assumptions are employed in the reaction chamber the feedstock. The particle thermal conductivity λp is
model. calculated as the weighted sum of virgin beech wood and
(1) Pyrolysis reactions are modeled using first-order kinetics char accounting for radiation heat transfer through the pore
and Arrhenius laws.21,34 inside the feedstock particle.34−36
(2) A unique temperature is used to describe fluid and solid
temperatures at a given element.39,40 13.5 Tbed 3d p,pore
(3) The volatile inside the feedstock particle is supposed to p = (1 ) w,p + c,p +
ec (8)
be released from the particle in a very short time.41,42
(4) Particle shrinkage will not be taken into account.34,43
d p,pore = dw,pore(1 ) + dc,pore (9)
(5) Radiation heat transfer in the packed-bed is simplified by
using the Rosseland approximation.32−34
where ηρ is the degree of pyrolysis, which can be calculated by
On the basis of the aforementioned assumptions, governing
the following equation:
equations of the heat and mass transfer in the reaction
chamber are given as follows. w
+ is
=1
Energy balance: w,in (10)
Tbed Mass balance:
( Cp)bed,eff + v Cp ,v (uTbed) = ( bed,eff Tbed)
t The different species are simulated with density fields. The
+Q (2) mass change per unit volume of each solid-phase species is
presented as follows.
( Cp)bed,eff = w
Cp,w + C
is p ,is
+ t Cp ,t + C
g p ,g
+ c Cp ,c Wood:
(3)
w
where Q is the heat source term; Cp is the specific heat; ρ is the = Sw = (k t + k is) w
t (11)
density; T is the temperature; t is the time; and u⃗ is the flow
velocity of gaseous species. The reaction rate ki obeys Intermediate solid:
Arrhenius laws, and the reaction heat is calculated as follows:
is
Q= (k t ht + k is his) w kc,g hc,g is (4) = Sis = k is w kc,g is
t (12)
Ei / RTbed
k i = Ai e (5) Char:
where Ai is the pre-exponential constant, Δh is the enthalpy of c
pyrolysis, and E is the activation energy. The wood pyrolysis = Sc = kc,g is
t (13)
kinetic and correlated parameters are presented in Figure 3 and
Table 2, respectively. For gaseous species:
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Tar: 1.75
F = 3/2
( 150 bed (19)
bed t )
+ (u t ) + ( D t) = St = k t w
dt (14)
The pressure P is the sum of the partial pressures of the tar
Gas: and gas that are assumed to behave as ideal gases.
( bed g )
+ (u g ) + ( D g) = Sg = (1 )k g v RTbed
dt w P= = Pt + Pg
(15) Mv (20)
where D is the gas diffusion tensor typical value.
2.3.2. PCM/Skeleton Composite. Several assumptions are
Momentum balance:
The reaction chamber in the computation domain is filled employed in the model of the PCM/skeleton composite:
with the feedstock in the form of a packed-bed. Thus, the flow (1) A unique temperature is used to describe the fluid and
velocity u⃗ can be calculated as follows: solid temperatures in a given element.29,38,46
( g
+ t) u ( g
+ t) P (2) The variation of PCM thermophysical properties is
x 2
+ 2
(u · )ux = + ux considered negligible.47,48
t bed x bed
(3) The natural convection of PCM is neglected.49,50
ij a S + agSc yz
jj + F |u | + t c zzu (4) The equivalent heat capacity method is applied to
jj 2 zz x
kK K bed { (16) simulate the phase change process of PCM.29,38,46
( + t) u ( + t) On the basis of the aforementioned assumptions, the
g x g P 2
+ 2
(u · )u y = + uy governing equations for the heat transfer in the storage
t bed x bed
component are given as follows:
ij a S + agSc yz
jj + F |u | + t c zzu
jj zz y ij
k K K 2
{ jjC f yzz Tavg
bed (17)
j + L zz
composite j j Tavg zz t
p ,composite composite
where μ is the viscosity, which is calculated as the weighted k {
sum of the gaseous species. K is the permeability of the packed-
= ( composite Tavg ) (21)
bed, and Fε is the structure function, which can be calculated
by the following equations:44,45
3 2
where L is the latent heat of fusion and Tavg is the temperature
bedd p of the PCM/skeleton composite. f is the melting fraction,
K= 2
150(1 bed) (18) which is described by the following equation:

l0
o Tavg < Tm,PCM TPCM /2
o
o
o
o
oT
o
o
o avg Tm,PCM + TPCM /2
f=m
o Tm,PCM TPCM /2 Tavg Tm,PCM + TPCM/2
o
o TPCM
o
o
o
o
o
o1 Tavg > Tm,PCM + TPCM /2
n (22)

The effective latent heat of fusion, specific heat, and density In the applied equivalent heat capacity method, f
is
of the PCM/skeleton composite are calculated on the basis of Tavg
the skeleton porosity and mass percentage ω. simplified by the Gaussian function.
ÄÅ É
Å (Tavg Tm,PCM)2 ÑÑÑ
Lcomposite = L PCM (23) expÅÅÅÅ ÑÑ
f ÅÅÇ ( TPCM / 2)2 ÑÑÑÖ
=
Cp,composite = Cp ,PCM + Cp,SiC(1 ) Tavg ( T /2)2 (28)
(24) PCM

where Tm,PCM is the melting point of the PCM and ΔTPCM

composite
= PCM core
+ SiC
(1 core) (25) describes its melting range.
2.4. Simulation Setup. The finite element method is
applied to solve the governing equations, and a rectangular
PCM = PCM,s +( PCM,l PCM,s )f (26) mapping grid is adopted for the computational domain. The
maximum relative error is less than 10−4 with the PARDISO
The effective thermal conductivity of the PCM/skeleton solver. Three sets of grids with 3.50 × 105, 5.76 × 105, and 7.85
composite is calculated as the volume-weighted sum of the × 105 elements are tested to ensure the independence of the
skeleton and PCM: grid size. The adaptive time step is employed in the simulation.
Three maximum time step restrictions of 10, 5, and 1 s are
core,eff = SiC(1 core) + core PCM (27) tested to ensure the time step independence. The deviation is
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Figure 4. Validation of the current numerical model: (a) compared to the beech wood pyrolysis process measured by Park et al.;34 and (b)
compared to the PCM/skeleton charging process measured by Liu et al.31

Figure 5. (a) Temperature response of non-TES case C′; (b) temperature response of base case C; (c) power partitioning and applied solar power
input of non-TES case C′; and (d) power partitioning and applied solar power input of base case C.

less than 0.1% for different meshes (5.76 × 105 and 7.85 ×
105) and different time step restrictions (5 and 1 s),
respectively. The grid with 5.76 × 105 elements and the
maximum time step restriction of 5 s are chosen for the current
models to reduce the computation cost.
3. MODEL VALIDATION
The simulation of the current reactor mainly involves the
beech wood pyrolysis model in the reaction chamber
2139
combined with the TES composed of a PCM/skeleton
composite. On the one hand, Park et al.34 numerically
investigated a series of beech wood pyrolysis models and
conducted experiments with a lab-scale fixed-bed reactor to
validate the proposed pyrolysis models. The current study
applies the same feedstock and a similar geometry of feedstock
particles as that of Park et al.34 Therefore, the numerical
predictions of the previously introduced pyrolysis model in a
2D computational domain are compared to the results of Park
et al.34 As shown in Figure 4a, the temperature as a function of
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Energy & Fuels
Figure 6. (a) Reaction front and heating rate distribution of case C′; and (b) reaction front and heating rate distribution of case C.
the time and the char yield is in good agreement with the
experimental and numerical results reported in this previous
study. The error between the current numerical results and the
experimental data is about 5%, which is mainly caused by
neglecting the particle shrinkage.
On the other hand, Liu et al.31 developed SiC-based phase
change composites and carried out detailed experiments on
their melting process. The current study applied skeleton
material with the same physical properties as in Liu et al.31
Therefore, numerical prediction applying the current TES
model is compared to the experiment conducted by Liu et
al.31Figure 4b shows that the temperature as a function of the
time agrees with the experimental results. The error between
the current numerical results and the experimental data is less
than 1%, which is mainly caused by the treatment of local
thermal equilibrium.
4. RESULTS AND DISCUSSION
4.1. Effect of TES under Constant Radiation. In this
section, the thermal and chemical performances of base case C
and non-TES case C′ are analyzed to investigate the effect of
TES under constant radiation heating condition.
As shown in Figure 5a and b, a significant temperature
gradient exists in the base case and non-TES case, which agrees
with previous studies.7,51,52 Nevertheless, the coupling of the
storage component causes a strong delay in the temperature
rise (more than 2000 s) as shown in Figure 5b. At the same
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time, the local overheating, which is recognized as one of the
main defects of solar thermal reactor,5,25,26 is alleviated. The
temperature on the absorption surface remains below 1200 K
most of the time. Meanwhile, the final temperature of the
absorption surface (TC1) is reduced by more than 200 K. This
significantly decreases the requirement of thermostable
performance of the absorption component. Specifically, a
very small temperature difference exists between TC1 and TC2
in case C, indicating the high heat transfer performance inside
the storage component. This result also proves that neglecting
the solar radiation distribution on the absorption surface is an
acceptable assumption.
Power partitioning for case C and case C′ is, respectively,
shown in Figure 5c and d to further analyze the energy
conversion in the reactor. The absorbed power is basically
divided into the sensible heat in the packed-bed, the sensible
heat in the species outlet, the radiation heat loss, and the
energy converted into the chemical form. Additionally, the
sensible and latent heat stored in the storage component is
illustrated for the base cases. η is defined as the ratio of the
different forms of energy to the total solar energy input. Figure
5d shows that 45.2% (41.1% sensible heat and 4.1% latent
heat) of the input solar energy is stored. Because of the large
temperature difference, the sensible heat represents the main
part of the storage capacity. Meanwhile, the storage material
has a relatively large specific heat and density (Table S1).
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Figure 7. (a) Wood mass conversion as a function of time in cases C and C′; and (b) char yield at different terminal temperature ranges in cases C
and C′.
Thus, the temperature on the absorption surface in case C rises
slower than that in case C′.
The lower temperature of the absorption surface results in
some notable phenomena. Although the overall heating period
of case C is prolonged by 66.2% as compared to that of case C′
(Figure 5), the total radiation heat loss even presents a slight
decrease (from 6.71 to 6.24 MJ). The sensible heat in the
species outlet is considered recyclable.53,54 Thus, it will not be
further discussed in the current work. The solar to chemical
energy conversions of cases C′ and C are only 3.3% and 1.1%,
respectively. Different from the gasification, pyrolysis is a weak
endothermic reaction.18,34 Moreover, the conversion between
the intermediate solid and char in the current numerical model
is even an exothermic reaction with an enthalpy of −210 kJ/kg.
Thus, the typical index, solar to chemical energy conversion
efficiency,7 is not suitable for the solar pyrolysis process.
A new criterion, which is based on the char production yield,
is proposed in the current work to better evaluate the
effectiveness of the solar energy input in the pyrolysis reactor.
It is defined as
m yield
Y=
Q solar Q loss (29)
In this criterion, myield is the mass of the target product and
Qloss only accounts for the radiation heat loss. Specifically, for
cases with storage (C), the energy stored in the PCM/skeleton
composite is removed from Qsolar.
The terminal temperature range from 573 to 673 K is
recommended for the slow pyrolysis for the char product.34,55
There should be a relatively large temperature difference
between the storage component and the reaction chamber to
ensure the reaction temperature. Thus, 873 K is selected as the
critical point to roughly divide the energy in the storage
component into two parts, the high-quality sensible/latent heat
and the low-quality sensible heat. The high-quality heat can be
directly used during the current pyrolysis process or the
preheating process in the next batch of feedstock. The stored
low-quality heat is used to process the first batch of the
feedstock. As the number of batch increases, the low-quality
heat stored at the first batch can be neglected as compared to
the huge amount of total solar energy input.
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Figure 6 presents the development of the melting front and
heating rate distribution as a function of the wood weight loss
to correlate the heating process and the formation of the
targeted product. The heating rate that covers the reaction
front of case C′ and case C is within the range of 0.1−0.35 K/s
(6−21 K/min) and 0.06−0.12 K/s, respectively. For such a
slow pyrolysis process, char formation is the dominant process.
The criterion Y is further expressed in the form of a
dimensionless number to compare the total char yield of the
current cases with the non-TES cases.
m yield, i m yield, i
Yi =
Q solar, i Q loss, i Q solar, i Q loss, i (30)
The value of Yc is 1.18, which means that solar energy input
is more effective when coupling with the storage component.
The total char yield and wood weight loss are presented in
Figure 7a.
Apart from the quantity of the char yield, the quality of the
char is also important. Under such low heating rates, the higher
terminal temperature results in increasing the fixed char
content for the char product, while the lower temperature
brings better compressive strengths.56,57 These two character-
istics are important for the commercial and industrial
utilization of the char. The temperature at which the
intermediate solid converts to char is defined as the terminal
temperature.57 The accumulated char yield at different
terminal temperature ranges is presented in Figure 7b to
evaluate the effect of TES on the char quality. The time when
the wood mass fraction (Figure 7a) turns to 0 is adopted to
calculate the total reaction duration.
For case C, the peak value of the char yield occurs in the
range 623−673 K, and there is a 50 K decrement as compared
to case C′, implying that the fixed char content of the char
declines.57 If maximizing the char yield is the main objective of
the reactor design, the coupling with TES can be an effective
measure to manage the char yield at the price of a slight
decline of the char quality in the fixed char content. At the
same time, the distribution of the char product becomes more
uniform (mainly produced in 623−673 K) when coupling the
pyrolysis reactor with the storage component.
2141 https://doi.org/10.1021/acs.energyfuels.2c03884
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Energy & Fuels
Figure 8. (a) Temperature response of non-TES case S′; (b) temperature response of base case S; (c) power partitioning and applied input solar
power input of non-TES case S′; and (d) power partitioning and applied input solar power input of base case S.
4.2. Effect of TES under Radiation with Short-Term
Interruptions. In this section, the thermal and chemical
performances of case S and case S′ are analyzed to investigate
the effect of TES under the radiation heating condition with
short-term interruptions.
As shown in Figure 8a, the solar-irradiated surface in case S′
suffers from a huge temperature fluctuation under 5, 10, and 20
min radiation interruptions. The maximum temperature
difference during the 20 min fluctuation even reaches 300 K.
The drastic thermal cycling stresses will induce serious safety
problems for the reactor in practical applications. By coupling
with TES, the maximum temperature difference for case S
decreases to 80 K (Figure 8b), indicating that the thermal self-
management of the solar reactor can be achieved thanks to the
storage. On the other hand, due to the thermal resistance
caused by the low conductivity of the feedstock and char, only
TC 1−3 (r−rin = 5, 12, and 13.25 cm) is influenced by
radiation interruptions. The thermal shock caused by heating
interruptions (within 20 min) does not almost affect the
temperature at TC4 and TC5.
The influence of short-term interruptions on the power
partitioning is neglective as shown in Figure 8c and d. Only the
sensible heat stored is used to buffer temperature fluctuations.
The used storage capacity during the 20 min fluctuation is as
small as 2.6% Qsolar,S, which indicates that there is a large
potential for optimizing the storage component as a function of
the targeted operation duration.
On the other hand, the sensible heat in packed-bed
decreases once the solar energy input stops in case S′. It
pubs.acs.org/EF Article
results in the temperature drops that, consequently, will affect
the quality of char. Although the power of sensible heat in
packed-bed comes down as time goes on, the sensible heat in
the packed-bed keeps growing the whole interruption by
coupling TES in case S (Figure 8d). Specifically, at the end of
the 20 min interruption, the function of the storage component
is mainly to compensate the radiation heat loss of the reaction
chamber.
As shown in Figure 9a, the heating rate near the reaction
front in case S′ decreases from 0.12−0.14 to 0.06−0.10 K/s
within 200 s. The radiation interruption results mainly in a
thermal shock in the region near the absorption surface. At this
time, the reaction front has already moved deeply inside the
reaction chamber. Thus, the heating rate of the reaction front
remains at 0.06−0.10 K/s until the end of the interruption.
This heating rate is provided by the sensible heat evolution in
the packed-bed, which corresponds to the power variation in
Figure 8a. For case S in Figure 9b, the thermal shock near the
inner surface of the storage component is smoother, and the
heating rate remains constant at approximately 0.07 K/s during
the whole process.
Figure 10a and b compares the char yield rate in different
temperature ranges as a function of time in cases S, S′, C, and
C′ to further analyze the influence of radiation interruptions on
the char quality. The char in 623−673 K serves as the main
product in case S, and the char formed in 673−723 K is the
main product in case S′. As shown in Figure 10a, the formation
rate of char in the base case is slightly influenced by radiation
interruptions. Meanwhile, in non-TES cases, the main char
2142 https://doi.org/10.1021/acs.energyfuels.2c03884
Energy Fuels 2023, 37, 2134−2148
Energy & Fuels
Figure 9. Reaction fronts and heating rate distributions: (a) the 20 min interruption in case S′; and (b) the 20 min interruption in case S.
yield rate decreases over 60% during the 20 min radiation
interruption. This reaction rate decrease is difficult to
compensate due to the break of balance between the
exothermic reaction and the endothermic reaction. As shown
in Figure 10c, the short-term interruption causes a weak
variation of the wood mass loss. Yet the char quality can be
significantly influenced (Figure 10d). For the non-TES cases,
the peak value of the char yield moves from 673−723 to 623−
673 K. Contrarily, with storage, the variations of the char yield
in the temperature ranges 623−673 and 673−723 K are
controlled to 16.2% and 25.6%, respectively (Figure 10d).
4.3. Effect of TES under Radiation with Long-Term
Interruption. In this section, the thermal and chemical
performances of cases L and L′ are analyzed to investigate the
effect of TES under the radiation heating condition including
long-term interruptions.
As shown in Figure 11, the temperature difference during
the 40 min interruption in case L′ surpasses 400 K, while the
temperature difference in case L remains lower than 100 K.
Meanwhile, the power partitioning shows that the latent heat
in TES is completely released during the 40 min interruption,
which indicates that the phase change process enables the
temperature stability. Nevertheless, for longer durations, the
temperature of the storage will rapidly drop.58 The storage
pubs.acs.org/EF Article
presents different discharging behaviors with respect to the
ratio of the latent heat to the sensible heat. During the 40 min
interruption, the discharge performance of the storage is
similar to that of parallel combined sensible-latent storage
devices because the sensible and latent heats nearly discharge
simultaneously.38,59 After 10 500 s, the discharging behavior of
TES is similar to the cascaded combined sensible-latent storage
devices, indicating that the latent heat in the component acts as
an amplifier to enlarge the effective capacity of the stored
sensible heat.60
Generally, the long-term interruption significantly influences
the power partitioning. Thus, it is necessary to calculate the
effectiveness of the solar power usage. On the basis of eq 29
and total char yield in Figure 12a, YL is calculated as 1.16. It is
slightly lower than YC . Nevertheless, it still indicates that the
solar power input becomes more effective on the total char
yield when the pyrolysis reactor is coupled with TES.
Figure 12b compares the char yield in different temperature
ranges as a function of time in cases L, L′, C, and C′ to further
evaluate the influence of long-term radiation interruptions on
the char quality. The char produced in the terminal
temperature range 623−673 K is the main product in both
cases L and L′. For non-TES cases, comparing the cases C′ and
L′, the peak value of the char yield moves from 673−723 to
2143 https://doi.org/10.1021/acs.energyfuels.2c03884
Energy Fuels 2023, 37, 2134−2148
Energy & Fuels
Figure 10. (a) Char yield rate in different temperature ranges as a function of time in the base cases; (b) char yield rate in different temperature
ranges as a function of time in the non-TES cases; (c) wood mass conversion as a function of time in cases C, C′, S, and S′; and (d) char yield at
different temperature ranges in cases C, C′, S, and S′.
623−673 K for L′, and the influence of radiation interruptions
is more significant. In case L, the variation of the char yield in
the range 623−673 K decreases from 66.8% to 17.0% by using
TES as compared to case L′. It should be noted that TES
results in a mismatch between the total char yield and the final
char yield at the complete wood conversion time. This
indicates that the variation of the char yield in the range 623−
673 K can further decrease as time elapses.
5. CONCLUSION
In this study, a novel solar pyrolysis packed-bed reactor
coupled with TES is developed. The chlorine salt infiltrated
with SiC skeleton is selected as the storage material. A two-
dimensional transient model of the developed reactor is
established and validated by experimental results in previous
studies. Different kinds of solar radiation, including the
constant solar radiation, the short-term solar interrupted
radiation, and the long-term interrupted solar radiation, are
simulated to investigate the effect of TES on the chemical and
thermal performances of the solar reactor.
The current TES design can automatically maintain the
pyrolysis process for 20−40 min when the solar radiation is
pubs.acs.org/EF Article
interrupted. During the discharging process, the discharging
behavior of TES is similar to the cascaded combined sensible-
latent storage devices if the high-quality sensible heat in the
storage has been sufficiently accumulated, indicating the
storage can provide a longer heating period for pyrolysis
process. Oppositely, the discharging behavior is closer to the
parallel combined storage devices. The latent heat dominates
the discharging, and the heating of the pyrolysis process is
more stable. During the charging process, the local overheating
and thermal cycling stresses on the absorption surface can be
alleviated by the storage. The variation of the temperature on
the absorption surface can be controlled below 100 K under
intermittent solar radiation conditions. Although the overall
heating period in non-TES cases is prolonged, the total
radiation heat loss in base cases even presents a slight decrease
by alleviating the overheating.
The effectiveness of solar power input to convert biomass to
char can be improved by coupling the solar pyrolysis reactor
with heat storage. A new criterion Y, defined as the ratio of the
total char yield and the effective solar power input, is proposed
to evaluate the effectiveness of solar power on the total char
yield. The ratio of Y values is related to the situations with and
2144 https://doi.org/10.1021/acs.energyfuels.2c03884
Energy Fuels 2023, 37, 2134−2148
Energy & Fuels pubs.acs.org/EF Article

Figure 11. (a) Temperature response of non-TES case L′; (b) temperature response of base case L; (c) power partitioning and applied input solar
power input of non-TES case L′; and (d) power partitioning and applied input solar power input of base case L.

Figure 12. (a) Wood mass conversion as a function of time in cases C, C′, L, and L′; and (b) char yield at different temperature ranges in cases C,
C′, L, and L′.

without TES. Its dimensionless form Y′ indicates that, at
constant (Yc = 1.18) and long-term interrupted (Yc = 1.16)
solar power input, the TES reduces the solar energy
consumption for the total char production by 18% and 16%,
respectively.
2145
TES makes the char quality controllable in the solar reactor.
The char quality is evaluated on the basis of the terminal
temperature and mainly produced in the ranges 623−723 K in
the current reactor. Although the feedstock and char are able
to store some high-quality sensible heat, the thermal shocks
https://doi.org/10.1021/acs.energyfuels.2c03884
Energy Fuels 2023, 37, 2134−2148
Energy & Fuels pubs.acs.org/EF Article

due to radiation interruptions cause an unrecoverable reaction

rate decrease in the range 623−723 K. In non-TES cases with
■ ACKNOWLEDGMENTS
We acknowledge funding from the National Natural Science
the condition of short-term radiation interruptions, the Foundation of China (52076098, 52111530296) and The
variation of char yield in the temperature range 623−673 K Young Top-notch Talent Cultivation Program of Hubei
is as large as 34.9%. The TES design can reduce the variation Province.
to 16.5%. In cases with long-term radiation interruptions, the
TES has a more significant effect by reducing the char yield
variation at 623−673 K from 66.8% to 17.0%. ■ NOMENCLATURE
A = area of the aperture (m2)
■
*
ASSOCIATED CONTENT
sı Supporting Information
Ai = pre-exponential constant (s−1)
Cp = specific heat (J kg−1 K)
dp = average particle diameter (m)
The Supporting Information is available free of charge at
D = gas diffusion tensor value (m2/s)
https://pubs.acs.org/doi/10.1021/acs.energyfuels.2c03884.
Ei = apparent activation energy (kg/mol)
Table S1, properties of absorption and storage materials; eSiC = emissivity of SiC
and Table S2, properties of feedstock and productions Fε = structure function
(PDF) H = heights of packed-bed domain (cm)
Δh = reaction enthalpy (kJ/kg)

■ AUTHOR INFORMATION
Corresponding Author
K = permeability (m2)
ki = reaction rate coefficient (1/s)
L = latent heat of fusion (J/kg)
Kuo Zeng − State Key Laboratory of Coal Combustion, m = mass of productions
Huazhong University of Science and Technology, Wuhan, P = pressure (Pa)
Hubei 430074, People’s Republic of China; orcid.org/ Qinlet = heat flux at the inner boundary of the absorption
0000-0001-8414-2636; Email: zengkuo666@hust.deu.cn surface (kW)
Qsolar = solar power input (kW)
Authors Q = volumetric heat source (W/m3)
Hongyang Zuo − State Key Laboratory of Coal Combustion, R = universal gas constant (8.314 J/mol·K)
Huazhong University of Science and Technology, Wuhan, rin = inner radius of the PCM/skeleton domain (cm)
Hubei 430074, People’s Republic of China rmid = outer radius of the PCM/skeleton domain (cm)
Dian zhong − State Key Laboratory of Coal Combustion, rout = radius of the packed-bed domain (cm)
Huazhong University of Science and Technology, Wuhan, S = mass transfer source term (kg/m3·s)
Hubei 430074, People’s Republic of China t = time (s)
Jun Li − State Key Laboratory of Coal Combustion, Huazhong T = temperature (K)
University of Science and Technology, Wuhan, Hubei ΔT = melting temperature range (K)
430074, People’s Republic of China Tm = melting temperature (K)
Huaqian Xu − State Key Laboratory of Coal Combustion, u⃗ = flow velocity of gaseous species (m/s)
Huazhong University of Science and Technology, Wuhan,
Greek Symbols
Hubei 430074, People’s Republic of China
Yongwen Lu − State Key Laboratory of Coal Combustion, γ = stoichiometric coefficient
Huazhong University of Science and Technology, Wuhan, ε = porosity
Hubei 430074, People’s Republic of China η = degree of pyrolysis or energy proportion
Wang Lu − State Key Laboratory of Coal Combustion, κ = extinction coefficient
Huazhong University of Science and Technology, Wuhan, λ = thermal conductivity (W m−1 K−1)
Hubei 430074, People’s Republic of China μ = dynamic viscosity (kg m−1 s−1)
Hongyu Zhou − State Key Laboratory of Coal Combustion, ρ = density (kg/m3)
Huazhong University of Science and Technology, Wuhan, ω = mass percentage
Hubei 430074, People’s Republic of China σ = Stefan−Boltzmann constant (W (m−2 K−4))
Gilles Flamant − Processes, Materials and Solar Energy Subscripts
Laboratory, PROMES-CNRS, Odeillo Font Romeu 66120, avg = average value
France bed = packed-bed
Haiping Yang − State Key Laboratory of Coal Combustion, c = char
Huazhong University of Science and Technology, Wuhan, eff = effective value
Hubei 430074, People’s Republic of China; orcid.org/ is = intermediate solid
0000-0002-8323-8879 g = gas
Hanping Chen − State Key Laboratory of Coal Combustion, l = liquid
Huazhong University of Science and Technology, Wuhan, p = particle
Hubei 430074, People’s Republic of China s = solid
Complete contact information is available at: t = tar
https://pubs.acs.org/10.1021/acs.energyfuels.2c03884 w = wood
Abbreviations
Notes PCM = phase change material
The authors declare no competing financial interest. TES = thermal energy storage
2146 https://doi.org/10.1021/acs.energyfuels.2c03884
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Energy & Fuels pubs.acs.org/EF
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