i n t e r n a t i o n a l j o u r n a l o f h y d r o g e n e n e r g y 4 8 ( 2 0 2 3 ) 1 2 4 6 1 e1 2 4 7 3

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Modeling of cooperative defect transport and

thermal mismatch in a planar solid oxide fuel cell

Sen Yang a, Yongjun Lu a,1, Bingbing Liu a,b, Qi Che a, Fenghui Wang a,*
a
Bio-inspired and Advanced Energy Research Center, Department of Engineering Mechanics, Northwestern
Polytechnical University, Xi'an, Shaanxi 710129, China
b
Huawei Digital Power Technologies Co., Ltd, Xi'an, Shaanxi 710129, China

highlights graphical abstract

Thermo-chemo-mechanical
model of SOFC considering defect
diffusion is proposed.

Defect diffusion relieves bending
of the overall multilayer structure.

The cathode stress convert
compressive to high tension stress
during defect transport.

Oxygen partial pressure is the
critical parameter for the overall
stress level.

article info abstract

Article history: Mixed ionic-electronic conducting (MIEC) membranes are widely applied as cathode ma-
Received 15 September 2022 terial in solid oxide fuel cells (SOFCs). Nonetheless, the chemical expansion of an MIEC
Received in revised form membrane caused by point defects (oxygen vacancies and small polarons) during oxygen
26 November 2022 transport induces cell failure. In this study, a multilayer thermo-chemical-mechanical
Accepted 8 December 2022 model was proposed to consider defect diffusion under sudden changes in the cathode
Available online 4 January 2023 atmosphere, thermal expansion mismatch, and mechanical bending deformation. Under
the set boundary conditions, the overall structural curvature of the multilayer system was
Keywords: relieved when the cathode was subjected to a high tensile stress. The influences of relevant
Planar solid oxide fuel cell parameters on the transient stress field were also investigated, and the overall stress of the
Defect diffusion multilayer structure decreased significantly when the oxygen partial pressure in the inlet
Transient stress distribution channel was constrained. Reducing the sintering temperature and chemical expansion
Thermo-chemo-mechanical coefficient could improve the reliability of the planar SOFC. In addition, the effect of con-
coupling straints in different directions on the multilayer system stresses is also investigated. This
study provides theoretical support for use in designing the stabilities and gas supply
strategies of planar solid fuel cells.
© 2022 Hydrogen Energy Publications LLC. Published by Elsevier Ltd. All rights reserved.

* Corresponding author.
E-mail address: fhwang@nwpu.edu.cn (F. Wang).
1
These authors contributed to the work equally and should be regarded as co-first authors.
https://doi.org/10.1016/j.ijhydene.2022.12.107
0360-3199/© 2022 Hydrogen Energy Publications LLC. Published by Elsevier Ltd. All rights reserved.
12462 i n t e r n a t i o n a l j o u r n a l o f h y d r o g e n e n e r g y 4 8 ( 2 0 2 3 ) 1 2 4 6 1 e1 2 4 7 3
Introduction
Solid oxide fuel cells (SOFCs) have drawn significant attention
owing to their attractive features such as environmental
friendliness, high conversion efficiencies, and diverse sizes
[1e3]. The factors hindering the commercialization of SOFCs
from design and manufacturing to operation have been
investigated extensively, including their carbon depositions/
gas poisoning [4,5], thermal mismatches [6,7], redox stabilities
[8,9], and active metal migrations [10e12]. Meanwhile, chem-
ical expansion during the operation of SOFCs has received
considerable attention. Mixed ionic-electronic conducting
membranes, which are cathode/electrolyte materials used in
SOFCs, undergo a series of defects reactions when storing and
transporting oxygen. The valence of the cations (small po-
larons) change, and oxygen vacancies are formed, which in-
duces chemical expansion [13e15]. The damage to the cell
caused by the resulting chemical stress cannot be
underestimated.
To our knowledge, one potentially efficient strategy to
resolve chemical expansion is the development of novel ma-
terials, e.g., the recently proposed ceria-based heterostructure
composites [16] that may overcome the limitations of the
electrolyte, and the developed Ruddlesden-Popper perovskite
(Anþ1BnO3nþ1) [17], which exhibits an oxygen-storage capacity
beyond that of a conventional perovskite, in addition to rela-
tively stable chemical expansion. The other solution is to
construct a mathematical model of the chemical expansion of
the cell to evaluate and control the parameters under the
operating conditions. Regarding the second solution, Atkinson
et al. [18,19] quantified the chemically induced stresses in
SOFC electrolytes caused by defects in doped ceria. However,
owing to the complex operating conditions of SOFCs, multiple
physical stress fields interact strongly with each other, and
thus, in addition to chemical stresses, other physical factors
were also considered. In the most advanced study, Jin et al.
[20] established a microscopic model, which coupled chemi-
cal, thermal, and structural stresses. Chemical stress signifi-
cantly influenced the stability of the electrolyte/cathode
interface. In this model, the constraints of the anode layer on
the interface between the cathode and electrolyte were not
considered, and the analytical process was regarded as a
steady-state process. In another study [21], the chemical
stress distribution in a positive-electrolyte-negative (PEN)
button battery was analyzed, and this model was still based
on a steady-state analysis. In addition, as an essential factor
leading to structural failure, the thermal mismatch stress was
not considered, and thus, the analyzed stress field was not the
working state. Dubois et al. [22] developed a model of 2D
protonic-ceramic button fuel cell, that coupled chemo-
thermo-mechanical stress. Furthermore, Wu et al. [23]
considered the chemo-electro-thermo-mechanical stress of a
3D model of a button SOFC during the fabricating and opera-
tion. Lenser et al. [24] investigated the electro-chemo-
mechanical stresses in fuel cells and electrolysis modes
based on defects in doped ceria.
Chemical stress is a transient-to-steady-state process,
which is reflected in the start-stop process of SOFCs.
1) The concentration of oxygen vacancy is a function of ox-
ygen partial pressure (PO2 ), and temperature [25], and
changes continuously as the SOFC system begins to heat
up and cool down.
2) When the atmosphere on one side of the electrode sud-
denly changes [26], which causes a sudden change in the
concentration of point defects. The point defects gradually
diffuse uniformly in the cathode, its concentration
constantly changes, and it causes a continuously changing
chemical stress distribution (transient chemical stress
distribution) in the electrode.
Therefore, transient chemical stress is vital in electrode
stability [27]. In an investigation by Euser et al. [28,29], the
transient chemical stresses in membranes were studied by
the expanding Nernst-Planck-Poisson (NPP) equation, and the
stress varied considerably with time during defect diffusion.
The PO2 on one side of a membrane suddenly changes, and the
membrane likely to fail or be damaged. However, studies have
only considered defect diffusion in investigating the distri-
bution of transient chemical stress within membranes, and
the effects of transient chemical stresses on the multilayer
structure of planar SOFCs have received little attention.
A thermal stress analysis model based on a multi-layer
elastic system has been established [30] and was well
applied to determine the thermal residual stress distributions
within planar SOFCs. Meanwhile, a model may be used to
determine the stress-strain field and change in curvature, and
structural optimize the PEN structure [31e33]. Therefore,
adding the contribution of the chemical stress term to extend
the original model is necessary to analyze the distribution of
transient chemical stress in a multi-layer system under defect
diffusion. The internal stress field of the cathode under a
sudden change in atmosphere may thus be investigated.
In this study, a multi-layer thermo-chemical-mechanical
model is proposed, considering the defect diffusion under
sudden changes in the cathode atmosphere, residual thermal
stress during fabricating period, and mechanical deformation
during structural bending. The purpose is to describe the
instantaneous stress field under realistic conditions and pro-
vide suggestions for use in designing and manufacturing
planar SOFCs.
Theory/calculation
Researchers have conducted detailed studies regarding cath-
ode materials with high mixed ionic-electronic conductivities,
from the original fluorite-ceria to the current perovskite.
Notably, the chemical expansion coefficient of the perovskite
is generally an order of magnitude lower than that of fluorite-
ceria [13]. Typical perovskite oxides include
Lax Sr1x Co1y Fey O3d (LSCF), Bax Sr1x Co1y Fey O3d (BSCF), and
Lax Sr1x MnO3 (LSM). They are the optimal candidates for use
in cathode materials for application in SOFCs, but, the doping
levels of these mixed materials lead to changes in the elec-
trochemical and mechanical performances. LSCF exhibits a
superior electrical performance in cathodes compared to that
of LSM owing to its higher ionic and electronic conductivities
 i n t e r n a t i o n a l j o u r n a l o f h y d r o g e n e n e r g y 4 8 ( 2 0 2 3 ) 1 2 4 6 1 e1 2 4 7 3 12463

[17,34,35]. In addition, LSCF displays a higher stability at

500e800  C than that of the BSCF cathode [36e38]. In addition,



BB L þ B
B L þ B0B ¼ 1 (3)
the thermo-kinetic parameters and stability of LSCF also vary
with different Fe/Co ratios. According to an experimental




VO L þ O
O L ¼3 (4)
study, the doping of Fe into the material may inhibit the
mobility of Co, enabling superior bonding of the material with





BB L þ 2 VO

L ¼ Sr0La L þ B0B L (5)
the electrolyte during sintering and reducing the coefficient of
thermal expansion. Consequently, Fe-rich compounds exhibit In these formulations, the concentration unit (½Xk L ) of each
stronger stabilities than those of Co-rich compounds [39]. ion is the lattice unit, which is related to the molar concen-
Furthermore, Y2O3 stabilized ZrO2 (YSZ) and LSCF react tration unit (½Xk ) as follows:
extensively at the interface to generate La2Zr2O7, SrZrO3, and 
spinel phases, reducing the chemical stability and electro- ½Xk  ¼ ½Xk L VM (6)
chemical performance of the SOFC after long-term operation The molar volume of LSCF6428, VM , is 3.3  10 m mol1
5 3

[38,40]. Gd-doped ceria (GDC) may be used to replace YSZ as an [21]. The defect concentrations of ½Sr0La L and ½VO

L are assumed
electrolyte in SOFCs. Therefore, La0:6 Sr0:4 Co0:2 Fe0:8 O3d as equal to the doping level. That ½Sr0La L ¼ 0:4 and the non-
(LSCF6428) and GDC were used as the respective cathode and
stoichiometric oxygen vacancy concentration ½VO

L ¼ d.
electrolyte materials in the analytical calculations in this
The equilibrium constants of the two reactions Eqs. (1) and
study as conclusion.
(2) are indicated in the form of the Gibbs free energies as
follows:
Model assumption

 
0 2  
OO L B B L DH0i  TDS0i
Before conducting the simulation, some assumptions were Ki ¼

2
¼ exp  (7)
P2O2 VO

L B RT
B L
made as shown below:



0   
1. The materials for planar SOFCs are homogeneous and BB L BB L DH0d  TDS0d
Kd ¼
 2 ¼ exp  (8)
isotropic, and comply with linear elasticity theory. BB L RT
2. The planar SOFCs are in a start-stop process (Gas supply
In Eqs. (7) and (8), DH0 and DS0 represent the standard en-
changing: N2 4 Air). The effect of applied cell voltage on
tropy and enthalpy changes of the two reactions, respectively.
the oxygen vacancy distribution is neglected [41].
R is the gas constant with the value of 8.314 J mol1K1 and T is
3. The PO2 is imposed at the cathode/air channel interface,
the temperature. Associating Eqs. (3)e(8), the functional rela-
and the effects of gas-phase flow is not considered [42,43].
tionship PO2 ¼ f ðd; TÞ is obtained. The standard enthalpy and
4. Chemical expansion of the electrolyte and anode at equi-
entropy were gained from the experimental data [47,49]. They
librium is not considered [24,44].
are then substituted into the equations. It should be stated
here that the experimental sample is LSCF6428 with a
Lanthanum vacancy (from an intentional 0.5% A-site defi-
Defect equilibrium model of LSCF6428
ciency) [47]. Table 1 shows the changes in the standard en-
thalpies and entropies changes obtained via fitting. The
During oxygen transport, LSCF6428 undergoes different defect
concentration of three mobile charge-carrying defects at a
reactions internally and many different defect equilibria
steady-state thus be obtained and used as the boundary
models have been investigated, including metallic, and itin-
condition for the defect transport model.
erant or small polaron which belong to semiconductor models
[45,46]. Semiconductor models that have received more
Defect transport model
attention are analyzed in this study [47]. Furthermore,
The conservation equation governing the concentration of the
although Co is more reactive than Fe ions, the Fe content
charged defect is:
within LSCF6428 is higher than the Co content, and thus, Co
and Fe are involved in the defect reactions [48]. The Co and Fe v½Xk 
þ V,Jk ¼ Q (9)
ions occurred in three states (Co2þ, Co3þ, and Co4þ; Fe2þ, Fe3þ, vt
and Fe4þ). The ratio of these two metals involved in the re- ½Xk  are the molar concentration of defects, and t is time. Jk
action is unclear, and B-sites were used instead of Fe and Co. represents the molar flux of the defects, and Q is a source
The incorporation Eq. (1) and the disproportionation reaction term, which is not considered in the following analysis. B
B and
shown in Eq. (2) are expressed in Kro € ge-Vink notation as:
OO are regarded as immobile. Hence, they remain
1
O2 ðgÞ þ VO

þ 2B 

B #OO þ 2BB (1)
2
Table 1 e Thermodynamic parameters of
2B
0
B #BB þ BB (2) La0:6 Sr0:4 Co0:2 Fe0:8 O3d [47].
   
In the defects reactions of LSCF6428, the charge equilib- DH0 kJ mol1 DS0 J mol1 K1
rium conditions, oxygen sites, and B-site equilibrium condi- Ki 111 64.5
tions are given by Eqs. (3)e(5), as follows: Kd 19.3 37.3
12464 i n t e r n a t i o n a l j o u r n a l o f h y d r o g e n e n e r g y 4 8 ( 2 0 2 3 ) 1 2 4 6 1 e1 2 4 7 3

Fig. 1 e Principle of chemical expansion via defect diffusion.

electroneutral. The molar flux of defects could be expressed

using the equation as

Jk ¼ uk ½Xk Vmk (10)

where uk and m ~ k represent the species mobilities and electro-

chemical potential, respectively. uk is related to the defect
diffusion coefficient, and m ~ k consists of the standard-state
chemical potential m+k , electrostatic potential F, hydrostatic
stress sh , number of charges for defects zk (z½VO

 ¼ þ 2;z½B
B  ¼ þ 1;
z½B0B  ¼  1) and the Vegard constant of chemical expansion bk .

Dk
uk ¼ (11)
RT

~ k ¼ m+k þ RT ln½XK  þ zk FF  3bk sh

m (12)

bk is assumed as independent of the species concentration

[28]. The chemical expansion coefficient of the molar unit is Fig. 2 e Total conductivity of LSCF6428 as a function of
related to that of the lattice unit, as indicated by b½VO

 ¼ oxygen partial pressures at different temperatures.
bL½V

 VM . Notably, chemical expansion results from a combi-
O

nation of lattice contraction around oxygen vacancies and
lattice expansion due to cation radius changes, ultimately
resulting in a net expansion. Nevertheless, there is not enough
information to assess the contribution of each defect indi-
vidually [29,50]. Thus, it is assumed that the net chemical
expansion is related to oxygen vacancy concentration and
b½B
B  ¼ b½B0B  ¼ 0.
According to basic mechanical theory, the hydrostatic
stress can be expressed as:
1
sh ¼ sxx þ syy þ szz
3 Xz2 F2 ½Xk 
The extended Nernst-Planck flux is expressed as:
energy Ek , and correction factors ak and єk (see Fig. 1). These
parameters can be derived by fitting the experimental con-
ductivity data [51] using 1stOpt 9.0 (7D-Soft High Technology,
Beijing, China), and the D+k and Ek values of the small polarons
were constrained based on their physical definitions. The
parameters of the diffusion coefficient of the oxygen va-
cancies were obtained from Tan et al. [52], the fitting results
are demonstrated in Fig. 2, and the defect transport parame-
ters derived from the conductivity are shown in Table 2.
The fitting results are expressed using Eq. (16).
(13)
s¼ k
Dk (16)
k
RT

zk F½Xk  3b ½Xk  F an the local charge density re can be formulated in the form
Jk ¼ Dk V½XK   Dk VF þ k Dk Vsh (14) of Poisson's equation as:
RT RT
  Xk
Ek þ єk d V , ðεr ε0 VFÞ ¼  re ¼  F k¼1 zk ½Xk  (17)
Dk ¼ D+k ð1 þ ak dÞexp  (15)
RT
Xk
The defect diffusion coefficient Dk shown in Eq. (14) is V , i ¼ F k¼1 zk Jk (18)
expressed using the pre-exponential factor D+k , activation
 i n t e r n a t i o n a l j o u r n a l o f h y d r o g e n e n e r g y 4 8 ( 2 0 2 3 ) 1 2 4 6 1 e1 2 4 7 3 12465

The system exhibits a planar geometry, and thus, sxx ¼ syy

Table 2 e La0:6 Sr0:4 Co0:2 Fe0:8 O3d defect transport
parameters. and szz ¼ 0. Layer i of the system contains a normal stress that
 can be formulated as:
Dk ðm2 s1 Þ Ek ðkJmol1 Þ ak εk ðkJmol1 Þ
!
VO$$ 1.58  106 [52] 73.60 [52] 0 0 X
sxx:i ¼ syy:i ¼ E*i ε  ai DT  ðbk D½Xk Þi (20)
B$B 5:08  105 24.98 - 4.19 - 63.97
k
B;B 2:50  106 - 3.60 - 5.48 62.95
where D½Xk  ¼ ½Xk   ½Xk 0 and ½Xk 0 is the reference defect
concentrations, assuming that the oxygen vacancy concen-
εr and ε0 are the relative permittivity and vacuum permittivity,
tration at PO2 ¼ 0:21 atm is the reference defect concentration
respectively. Solving Poisson's equation, a strictly electrically
neutral boundary condition is deemed imposed at the cath- [55]. E*i is the biaxial modulus, which is expressed as E*i ¼
P Ei =ð1  mi Þ, where mi is Poisson's ratio. ai is the coefficient of
ode/electrolyte interface ( kk¼1 zk ½Xk  ¼ 0).
thermal expansion of each layer of the material.
In the multilayer elastic system, the stress-strain distribu-
Thermal-mechanical model
tion may be determined by three parameters: ε0 , zb , and r.
These parameters are solved in the three boundary conditions
The elastic multilayer system is shown in Fig. 3. Planar SOFCs
without constrains as follows:
are considered the elastic multilayer system, the thickness of
each layer is indicated by ti , and the subscript i denotes the ZHi !
Xn X
number of layers varying from one to n. The coordinate sys-
i¼1
E*i ε0  ai DT  ðbk D½Xk Þi dz ¼ 0 (21)
tem is defined on the lower surface of the first layer, where Hi1
k
P
z; ¼ 0, with the relationship defined as: Hi ¼ ij¼1 ti ði ¼ 1  nÞ,
and thus, on the outermost surface, z ¼ Hn . Suppose the Xn ZHi
z  zb
multilayer system is stress-free state at the sintering tem- dz ¼ 0 (22)
i¼1 r
perature [53,54], when thermal and transient chemical Hi1

stresses occur under a sudden shifts in the oxygen partial

pressure on sides of the cathode at the operating temperature, Xn ZHi
in order to maintain displacement compatibility and conti- i¼1
sxx;i ðz  zb Þdz ¼ 0 (23)
nuity of the structure, the system buckles. In the multilayer Hi1

system, the total strain ε may comprise the respective uniform

The three parameters are obtained as follows:
strain and bending strain ε0 and εb . Hence, the total strain ε in
Z !
the multilayer system can be depicted as: Pn Hi X
i¼1 E*i ai DT þ ðbk D½Xk Þi
z  zb ε0 ¼
Hi1
Pn
k
(24)
ε ¼ ε0 þ εb ¼ ε0 þ (19) *
r i¼1 Ei ti

In Eq. (19), r is the radius of curvature, zb is the location of Pn *

the neutral axis. i¼1 Ei ti ð2Hi1 þ ti Þ
zb ¼ P (25)
2 ni¼1 E*i ti

Z !
Pn Hi X
3 i¼1 E*i ai DT þ ðbk D½Xk Þi  ε0 ðz  zb Þ
1 Hi1 k
¼ Pn *
(26)
r i¼1 Ei t3i þ 3t2i Hi1  zb þ 3ti Hi1  zb

The mechanical parameters of the composites are ob-

tained via the following calculations [56,57]:

Ei
Ki ¼ (27)
3ð1  2mi Þ

41
KNiGDC ¼ KGDC þ (28)
1=ðKNi  KGDC Þ þ 342 =ð3KGDC þ 4GGDC Þ

GNiGDC ¼
41
GGDC þ
1=ðGNi  GGDC Þ þ 642 ð3KGDC þ 2GGDC Þ=½5GGDC ð3KGDC þ 4GGDC Þ
(29)

9KNiGDC GNiGDC
ENiGDC ¼ (30)
3KNiGDC þ GNiGDC

aNi 4Ni KNi þ aGDC 4GDC KGDC

aNiGDC ¼ (31)
Fig. 3 e Schematic diagram of the multi-layer structure. 4Ni KNi þ 4GDC KGDC
12466 i n t e r n a t i o n a l j o u r n a l o f h y d r o g e n e n e r g y 4 8 ( 2 0 2 3 ) 1 2 4 6 1 e1 2 4 7 3

decrease as PO2 increases, whereas the trend of the concen-

Table 3 e Properties of electrode materials.
tration of ½B
B L reveals the opposite. Meanwhile, comparing
Anode Cathode Electrolyte Ni the results of the ½VO

L of LSCF6482 [28], increasing the doping
(Ni/GDC) (LSCF6428) (GDC)
ratio of Fe would enhance its stability. Fig. 4 (b) shows the
Elastic modulus 201.7 152 [58] 187 [59] 219 [57] predicted non-stoichiometry oxygen vacancy concentrations
(GPa)
at different PO2 values compared with experimental data [47].
Poisson's ratio m 0.324 0.32 [58] 0.334 [21] 0.313
The defect equilibrium model predictions are relatively small
TEC að106 =KÞ 14.95 15.3 [60] 12.63 [61,62] 16.5
ta ; tc ; te ðmmÞ 400 30 10 e compared to the experimental results, but the deviation is
within 5%. It is mainly due to the charge neutrality equations
in the model do not consider the A-site deficiency.
where Ki is the bulk modulus of material i, 4i denotes the The calculated concentrations of charged defects at
volume fraction of material i. E and G are the respective different PO2 values were imposed at the cathode/air and
modulus of elasticity and shear modulus of the material. The cathode/electrolyte interfaces as the boundary conditions in
volume fractions of Ni and GDC are assumed to be 1:1. Previ- defect diffusion. This is a conceivable assumption based on
ously studied material properties are listed in Table 3. the experiment [26], with the introduction of N2 during heat-
ing, and the PO2 values at the cathode/air and cathode/elec-
Constraint conditions trolyte interfaces are extremely low at approximately
104 atm during this period. The three mobile charge-carrying
In practice, planar SOFCs are constrained by current collectors defects within the cathode are: ½VO

L ¼ 0:11656, ½B
B L ¼
and seals [24]. Three cases, in terms of constraints, were 0:17198, and ½B0B L ¼ 0:0051, which a considered as reference
considered in this study: concentrations. When heated to a pre-set temperature, N2
stops at inlet and oxygen is injected, and the PO2 at the cath-
Case 1. The current collector prevents the bending of the ode/air interface could change abruptly to 0.21 atm. The
multilayer structure (1/r ¼ 0). Tape-casted sealant may deform concentrations of charged defects at the cathode/air interface
and accommodate this difference [63]. suddenly become: ½VO

L ¼ 0:01047, ½B
B L ¼ 0:38036, and ½B0B L ¼
0:0013, and the boundary conditions are fixed during the
Case 2. The rigid seal constrains the multilayer structure, analysis.
wherein the cell may not move laterally, but may bent (ε0 ¼ 0). Fig. 5 demonstrates the distributions of the three mobile
The collectors are ductile materials, such as Au rings [64]. charged-carrying defects concentrations and the electrostatic
potential with time at the cathode. Significantly, the diffusion
Case 3. Rigid current collectors and seals act together on a of defects in the cathode reaches equilibrium at approxi-
multi-layer structure (1/r ¼ 0, ε0 ¼ 0). mately 0.4 s. At 0.005e0.01 s, a high defect concentration
gradient is observed at approximately 5e10 mm from the
cathode/air interface. After 0.05 s, the defect diffusion rate
within the cathode slows, and the defect diffusion reaches
Results and discussion basically a steady state from 0.1 to 0.4 s, the defect diffusion
basically reaches the steady-state. The direction of ½B
B  diffu-
Transport of charged defects sion is from the cathode/air interface (high PO2 ) to the cathode/
electrolyte interface (low PO2 ), whereas ½VO

 and ½B0B  diffuse in
The relationship between PO2 and equilibrium defect con- the opposite direction, as shown in Fig. 5(aec). Notably,
centrations for LSCF6428 are obtained based on Eqs. (3)e(8), as although the defect diffusion coefficients of ½B
B  and ½B0B  are
indicated in Fig. 4 (a). The concentrations of ½B0B L and ½VO

L three or four orders of magnitude larger than that of ½VO

, the

Fig. 4 e (a) Model-predicted equilibrium defect concentrations for LSCF6428 at 1073.2 K. (b) Model-predicted non-
stoichiometry oxygen vacancy concentrations vs experimental data.
 i n t e r n a t i o n a l j o u r n a l o f h y d r o g e n e n e r g y 4 8 ( 2 0 2 3 ) 1 2 4 6 1 e1 2 4 7 3
Fig. 5 e The concentrations of charged defects and electrostatic potential transient profiles after the cell is suddenly started:




(a) VO

L , (b) B
B L , (c) B'B L , and (d) F.
time scales of diffusion during defect transport are similar.
Therefore, the electrostatic potential strongly promotes the
diffusion of oxygen vacancies.
Stress distribution and variation
The hydrostatic stress in each layer of the planar SOFC also
varies with time during defect diffusion, and the variation of
in the stress in each layer with time is shown in Fig. 6 (aec). At
the beginning of defect diffusion, the anode substrate is
slightly compressed, and the anode is subjected to tensile
stress at the interface between the anode and electrolyte. As
diffusion proceeds, the shrinkage of the cathode layer reduces
the curvature of the multilayer structure, thereby partially
releasing the stress in the anode. At the steady-state, the hy-
drostatic tensile stress decreases to 53.5 MPa at the anode-
electrolyte interface, and the stress gradient in the electro-
lyte is small owing to its thickness. After defect transport, the
compressive stress on the electrolyte increases from 53.8 to
approximately 79.9 MPa, and thus, the diffusion of defects
aggravates the compression of the electrolyte layer. The stress
relationship in the cathode layer exhibits a high degree of
nonlinearity owing to charged defects. At 0 s, compression
acts on the inner and outer interfaces of the cathode due to
thermal expansion, uniform stress, and bending stresses.
After a sudden change in PO2 on the exterior, the oxygen va-
cancy concentration decreases rapidly, and the exterior
shrinks under tension. In the initial 0e0.02s of defect diffu-
sion, the stress gradient at 5e10 mm from the cathode-air
12467
interface is large, and the cathode is easily damaged. As
defect diffusion is completed, the oxygen vacancy concen-
tration within the cathode gradually becomes uniform, and
the external stress reaches to 70.0 MPa. Brittle materials are
sensitive to a high tensile stress, which could occur potential
problems. The calculation assumes a stress-free temperature
of 1100  C [62,65].
Although the cathode stress reaches the characteristic
fracture strength of LSCF6428 [66], it does not represent the
stress level under the operating conditions: 1) PO2 is fixed at
the interface, and is not real PO2 under the operating condi-
tions. 2) This is a transient analysis, and the oxygen vacancies
diffuse into the electrolyte after the steady-state is reached.
Meanwhile, Fig. 6 (d) shows that the chemical stress caused by
the charged defects could reduce the bending of the multi-
layer system. Hence, chemical stress may induce fracturing
and damage the cathode material, yet it is beneficial for the
stability of the entire multilayer system.
Model validation
The proposed transient thermochemical-mechanical model is
validated and compared with the modeling results of similar
SOFCs in the cited references. The results are subject to de-
viations due to differences in geometry, reference tempera-
ture, and operating conditions of similar models, but these
deviations are within acceptable limits. Therefore, the com-
parison of the results is accompanied by remarks on the
conditions, and all the configurations are listed in Table 4.
12468 i n t e r n a t i o n a l j o u r n a l o f h y d r o g e n e n e r g y 4 8 ( 2 0 2 3 ) 1 2 4 6 1 e1 2 4 7 3

Fig. 6 e Variation of stress distribution and structural curvature with defect diffusion in planar SOFC: (a) Anode layer; (b)
Electrolyte layer; (c) Cathode layer; (d) structural curvature.

Table 4 e Comparison of simulation results for planar SOFCs against literature data.
This study Zhang et al. [33] Wu et al. [23] Euser et al. [28,29]

Stress-free temperature ( C) 1100e1200 1360 e e
Chemical expansion (m3 mol1 ) 7.11  107 e 8.15  107 8.15  107
Geometry Multilayer Multilayer Button-cell Single layer
Conditions Transient-state Steady-state Steady-state Transient-state
Cathode stress (MPa) 250e60 50 -1e10 330e15

Parameter study Case 1. The three layers are sintered at 1100  C [62].

The commercialization of a planar SOFC requires a good bal-
ance between the electrochemical performance and struc-
tural stability. During stress field analysis, the sintering
(stress-free) temperature of the SOFC mainly affects its re-
sidual thermal stress, resulting in the different chemical
expansion coefficients for the same material reported in the
literature and different PO2 values under the operating condi-
tions. Optimizing these parameters may improve the stability,
durability, and integrity of the SOFC during start/stop or
extreme conditions.
Effect of sintering temperature
The mismatch in the thermal expansion coefficient of each
electrode layer causes different shrinkages during cooling
after sintering, and residual thermal stress is generated in
each layer. The two cases considered are as follows:
Case 2. The anode and electrolyte are co-fired at 1100  C, and
the entire cathode is calcinated at 1200  C [56,67].
Fig. 7 indicates the influence of the sintering temperature
on the stress distribution. The cathode in Case 1 is subjected
to an intense compressive stress of approximately 259.2 MPa
with no defect diffusion. However, when the sintering tem-
perature is increased to 1200  C, the stress at the cathode
converts to a low level of compressive stress. Therefore, the
sintering temperature significantly affects the initial stress
distribution. When defect diffusion commences, the inter-
acting thermal and chemical stresses determine whether the
strains within the cathode are under tension or compression.
A lower sintering temperature can significantly reduce the
tensile stress within the cathode, mainly because a higher
stress-free temperature causes the cathode to shrink to a
 i n t e r n a t i o n a l j o u r n a l o f h y d r o g e n e n e r g y 4 8 ( 2 0 2 3 ) 1 2 4 6 1 e1 2 4 7 3
Fig. 7 e Effects of stress-free temperature: (a) the stress of each layer of cell at t ¼ 0.4s; (b) structure curvature at different
stress-free temperature.
larger extent at the operating temperature. The electrolyte is
subjected to a more significant compressive stress to ensure
the continuity and integrity of the interface. As shown in Fig. 7
(b), with the defect diffusion, the Case 2, the high stress-free
temperature experienced a reversal of curvature. Although a
higher stress-free temperature implies a decrease in curva-
ture [68], which contributes to the stability of that overall
multilayer structure. However, it causes a further increase in
the fracture probability of the electrolyte and cathode.
Therefore, the lower sintering temperature is recommended.
Nevertheless, the low sintering temperature may increase the
cell polarization resistance and thus reduce the electro-
chemical performance [69].
Effect of oxygen partial pressure
The practical oxygen partial pressure during cell operation is
related to the ambient temperature, gas flow rate, and quantity,
indicating that the oxygen partial pressure may be used as an
adjustable parameter. PO2 at the cathode/electrolyte interface is
fixed, and PO2 at the inlet gas channel is adjusted to analyze the
influence of PO2 on the stress distribution. Fig. 8 demonstrates
the stress field of the cathode after defect diffusion. It can be
Fig. 8 e Effects of oxygen partial pressure.
12469
seen the stress levels within the cathode may be efficiently
reduced by decreasing PO2 at the cathode/air interface. When
PO2 in the inlet channel is altered to 0.01 atm, the stress within
the internal cathode shifts from tension to compression, which
is critical in the safe operation of the SOFC. However, lowering
PO2 at the inlet channel should inevitably impact on the elec-
trochemical performance of the SOFC, and thus, the advan-
tages and disadvantages should be weighed.
Effects of material properties
Chemical stress within the cathode layer is related to the
chemical expansion coefficient. However, the chemical
expansion coefficient is not uniform and is influenced by the
manufacturing process, material dimensions, study condi-
tions [39,70e72], etc. The chemical expansion coefficients are
shown in Table 5. Therefore, the chemical expansion coeffi-
cient may be used to investigate its influence on the stress
field. The PO2 values at the cathode/electrolyte and cathode/air
interfaces are fixed, and the results of the calculations are
shown in Fig. 9 (a). As the chemical expansion coefficient in-
creases, the stress within the cathode increases from 69.8 MPa
to 92.8 MPa, and the stress magnitude of the stress within the
electrolyte decreases from 79.9 MPa to 57.8 MPa. Mean-
while, an increase in the chemical expansion coefficient raises
the difference in the stress at the electrolyte/cathode interface
from 210 to 383 MPa, which may lead to delamination at the
cathode/electrolyte interface. In conclusion, chemical stress
displays a more significant influence on the multilayer system
than that of residual thermal stress if the chemical expansion
coefficient increases. Porosity significantly affects the me-
chanical properties. Hence, the porosity was analyzed as a
material parameter of the electrode, as shown in Fig. 9 (b). The
porosity of LSCF6428 is linearly related to its modulus of
elasticity [73]. As the porosity increases, the tensile stress at
the cathode/air interface gradually decreases from 102 to
Table 5 e Chemical expansion coefficients of
La0:6 Sr0:4 Co0:2 Fe0:8 O3d
bL½V

 0.02153 [39,71] 0.031 [70] 0.032 [72]
O
b½VO

 (m3 mol1 ) 7.105  107 1.023  106 1.056  106
12470 i n t e r n a t i o n a l j o u r n a l o f h y d r o g e n e n e r g y 4 8 ( 2 0 2 3 ) 1 2 4 6 1 e1 2 4 7 3
Fig. 9 e Effect of the material properties on stresses. (a) Effect of chemical expansion coefficients on stresses in each layer at
0.4 s. (b) Effect of Porosity on cathode stress at 0.4 s.
Fig. 10 e Effects of the different constraints on the stress in
each layer of the electrode.
22 MPa, but the fracture strength of the cathode inevitably
decreases with increasing porosity (64 ± 4 / 21 ± 3 MPa).
Effect of constraint conditions
The assembly of a planar SOFC constrains the bending and
deformation of its structure. This causes compressive stresses
on the electrodes, with three cases described in Section 2.5.
The effect of thermal stress was not considered because the
assembly of cells at sintering temperatures is impractical. The
internal stress fields of the three constrained cases are shown
in Fig. 10. When the cell is free to bent, the stress within the
cathode decreases by approximately 10 MPa compared with a
fully free condition. The stresses are reduced by 27 and 36 MPa
in the constrained plane and fully constrained conditions.
These results consider only chemical stresses. When consid-
ering a temperature change from 20  C to 800  C, adding
constraints does not change the trend of stress described
above. However, the cathode/electrolyte interface can be
subjected to excessive compressive stresses, which would
cause delamination.
Conclusions
A coupled thermo-chemical-mechanical model for planar
SOFCs based on defect transport has been established in this
study. The effects of sintering temperature, material proper-
ties, and partial oxygen pressure on the stress distribution of
planar SOFCs were considered. The crucial conclusions are
summarized in the following points:
1. Mobile charged-carrying defects on both sides of the
LSCF6428 reaches equilibrium after approximately 0.4 s.
2. During the start-stop process of the SOFCs, before the
defect diffusion reaches equilibrium, the stress in the
cathode has already attained the characteristic fracture
strength (64 ± 4 Mpa) of LSCF6428.
3. Defect diffusion relieves the stress of the anode and elec-
trolyte while inducing the cathode stress field to change
from compressive to tensile.
4. The cathode stress field increases with increasing the
chemical expansion coefficient of LSCF6428 and the PO2 of
gas channel. Lower sintering temperature (900e1000  C)
reduces thermal stress and improves the electrochemical
performance of SOFCs.
5. The chemical stress caused by the defect transport could
lessen the bending of the multilayer system.
The conclusions have practical significance for developing
the safe operation of the battery and prolonging the life span
of planar SOFCs, especially during its sudden start-stop pro-
cess. This study could provide theoretical support for the
stable design and fabrication of planar SOFCs.
CRediT authorship contribution statement
Sen Yang: Data curation, Formal analysis, Investigation,
Methodology, Software, Visualization, Writing - original draft,
Writing - review & editing; Yongjun Lu: Investigation, Meth-
odology, Formal analysis, Writing - review & editing; Bingbing
Liu: Investigation, Methodology, Formal analysis, Writing -
 i n t e r n a t i o n a l j o u r n a l o f h y d r o g e n e n e r g y 4 8 ( 2 0 2 3 ) 1 2 4 6 1 e1 2 4 7 3
original draft; Qi Che: Methodology, Formal analysis, Writing -
review & editing; Fenghui Wang: Conceptualization, Funding
acquisition, Resources, Supervision, Writing - review &
editing;
Declaration of competing interest
The authors declare that they have no known competing
financial interests or personal relationships that could have
appeared to influence the work reported in this paper.
Acknowledgements
The authors gratefully acknowledge the support sponsored by
the National Natural Science Foundation of China (Grant
Nos.11572253) and (Grant Nos.11972302).
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