Materials Today Energy 44 (2024) 101633

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Materials Today Energy

journal homepage: www.journals.elsevier.com/materials-today-energy/

Advances in solid oxide fuel cell technologies: lowering the operating

temperatures through material innovations
Muhammad Yousaf a, c, Yuzheng Lu d, Muhammad Akbar e, Lei Lei c, Shao Jing a, *,
Youkun Tao b, **
a
College of Chemistry and Environmental Engineering, Shenzhen University, Shenzhen, Guangdong Province 518055, China
b
College of Science, Harbin Institute of Technology, Shenzhen, Guangdong Province 518055, China
c
College of Physics and Optoelectronic Engineering, Shenzhen University, China
d
School of Electronic Engineering, Nanjing Xiaozhuang University, Nanjing 211171, China
e
Key Laboratory of Ferro and Piezoelectric Materials and Devices of Hubei Province, Faculty of Physics and Electronic Science, Hubei University, Wuhan,
Hubei 430062, China

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

Article history: Solid oxide fuel cells (SOFCs) are promising for clean energy generation due to their high efficiency, fuel
Received 18 January 2024 flexibility, and status as a clean energy source with no environmental hazards. However, the challenge of
Received in revised form operating these SOFCs at elevated temperatures (800e1000
C) presents significant hurdles regarding
1 June 2024
material selection, cost-effectiveness, and device fabrication. Lowering the operational temperature of
Accepted 20 June 2024
Available online 24 June 2024
SOFCs can enhance performance and economic viability. Nevertheless, this pursuit introduces challenges
in the form of increased ohmic and polarization resistances, which detrimentally affect electrochemical
performance. High ohmic resistance and activation energy at lower temperatures reduce ionic con-
Keywords:
LT-SOFCs
ductivity and impede SOFC device efficiency. Recent advancements in materials and cutting-edge
High-performing materials technologies have addressed these issues, particularly in low-temperature operations for SOFC de-
Electrolytes vices. This review article focuses on the latest developments in material selection and advanced tech-
Electrode nologies that have demonstrated notable improvements in power output and long-term durability at
HOR&ORR functionalities lower operating temperatures, highlighting the significance of high-performing electrolyte and electrode
materials with enhanced electrochemical and fast electrocatalytic functionality to improve cell efficiency.
Additionally, the article explores the significant obstacles encountered by SOFCs at low operating
temperatures.
© 2024 Elsevier Ltd. All rights are reserved, including those for text and data mining, AI training, and
similar technologies.

1. Introduction promising electrochemical conversion devices [6e9]. The unique

characteristics of high efficiency, fuel flexibility, and low cost with
Producing renewable energy, storage, and delivery requires non-precious metal as a catalyst made SOFCs more potential elec-
continuous innovation to accomplish the goal of a clean and sus- trochemical conversion devices [10e12]. SOFCs have immense ap-
tainable energy supply [1e5]. Efficient and new technologies in the plications in portable electronic devices, transportation, combined
energy sector are the utmost requirements to fulfill the growing heat power, hybrid vehicles, and power plants [13,14]. Despite
energy demand. Fuel cells are renowned for producing numerous advantages, SOFCs face critical challenges such as high
clean energy without releasing hazardous environmental mate- operating temperature, material selection, slow start-up, mechan-
rials. Among various fuel cell types, solid oxide fuel cells (SOFCs), ical instability, compatibility issues among electrolyte and elec-
due to their high efficiency and fuel flexibility, are considered trode, and sluggish ionic conductivity on declining operating
temperature [13e18]. SOFCs operating at high temperatures face
the key challenge of sintering electrolytes at high temperatures to
get a dense structure. The interfacial problems between the elec-
* Corresponding author. trode and electrolyte are caused by dissimilar coefficients of ther-
** Corresponding author.
mal expansion [19,20]. Suitable material selection and advanced
E-mail addresses: shaojing@szu.edu.cn (S. Jing), taoyoukun@hit.edu.cn (Y. Tao).

https://doi.org/10.1016/j.mtener.2024.101633
2468-6069/© 2024 Elsevier Ltd. All rights are reserved, including those for text and data mining, AI training, and similar technologies.
M. Yousaf, Y. Lu, M. Akbar et al. Materials Today Energy 44 (2024) 101633

Nomenclature PCFC Proton Conducting Fuel Cells

AC Alternative Current
SOFC Solid Oxide Fuel Cell DC Direct Current
HOR Hydrogen Oxidation Reaction E Energy, kJ/kg
ORR Oxygen Reduction Reaction I Current
MIEC Mixed Ionic Electronic Conduction V Voltage
LT-SOFC Low-temperature solid Oxide Fuel Cell J Current density
FC Fuel Cell TPB Triple Phase Boundaries
GDC Gadolinium Doped Ceria ESB Erbia-Stabilized Bismuth
SDC Samarium Doped Ceria CO2 Carbon Dioxide
YSZ Yttria Stabilized Zirconia ASR Area Specific Resistance
ScSZ Scandia Stabilized Zirconia Rp Polarization Resistance
LSGM Lanthanum Strontium Gallium Magnesium Oxide ESB Electrochemical Impedance Spectroscopy
HT-SOFCs High-Temperature Solid Oxide Fuel Cells RE Rare Earth
CLZ Calcium Doped Lanthanum Zirconate PCE Proton Conducting Electrolytes
SLZ Strontium Doped Lanthanum Zirconate PCEC Protonic Ceramic Electrochemical Cells
I-V Current-Voltage LC Lanthanum Nickelate
I-P Current-Power SLFC Single Layer Fuel Cell

fabrication methods are key parameters for SOFCs long-term material selection is critical to reducing the operating temperature
operation [21e24]. In contrast, lowering the operating tempera- for low-temperature solid oxide fuel cells (LT-SOFCs).
ture benefits in terms of proper fuel consumption, selection of low- A high-performing anode and a potential cathode are also
cost catalysts, sealing material, and interconnectors [22,25,26]. necessary to reduce operating temperature [44e46]. The anode
However, reducing operating temperature leads to key challenges, selection microstructure of the selected material significantly en-
such as low ionic conductivity, increased electrode polarization tails electrochemical performances based on the cell configuration
resistance, and slow start-up. Conventional electrolyte yttria sta- [46]. On anode fuel, HOR catalytic functionalities take place; there-
bilized zirconia (YSZ) exhibits a high ionic conductivity of 0.1 S/cm fore, it must hold high electronic conductivity, better stability, and a
at temperatures 800e1000
C. By decreasing the temperature to high degree of thermal compatibility [47,48]. Conventionally
800
C, the ionic conductivity decreases rapidly, ultimately frequently used Ni-Zirconia anodes have drawn profound attention
affecting the cell potential [27e29]. Novel, material, and advanced at high temperatures; however, nickel particle aggregation signifi-
technologies are required to sustain the required ionic conductivity cantly decreases the anode material porosity and adversely affects
and improve ionic conductivity at low temperatures. Interestingly, fuel cell performance. Carbon deposition on Ni-YSZ also creates
gadolinium and samarium doped ceria (GDC, SDC) deliver sufficient hurdles at high temperatures that reduce cell performance [49].
high ionic conductivity at 600e800
C, showing the importance of LaCrO3, Ti0.34Nb0.66O2, and CrTi2O5 face lattice expansion due to
material selection [30e33]. It has been noticed that searching novel weak machinal strength and unsuitable anode material in reducing
electrolyte materials exhibits enhanced ionic conductivity even at atmosphere [50,51]. Ni-ScSz doped with CeO2 and lanthanum
low temperatures such as 500
C. (Dy2O3)13(Ta2O5)2(Bi2O3)85 de- strontium gallium magnesium oxide (LSGM) delivers high perfor-
livers 0.08 S/cm conductivity and 0.2 eV activation energy at 500
C, mance and low polarization resistance at low operating tempera-
further certifying that the selection of potential material signifi- tures compared to Ni-YSZ [52,53]. Ni-GDC and Ni-SDC anodes
cantly reduces operating temperature [34] perform remarkably well compared to Ni-YSZ operating at a
Another method for lowering the operating temperature is a declining temperature. With electrolyte GDC and cathode
potential catalyst with enhanced hydrogen oxidation reaction Ba0.5Sr0.5Co0.8Fe0.2O3, the configured cell delivers 1300 mW/cm2 at
(HOR) and oxygen reduction reaction (ORR) electrocatalytic 600
C, shows staggering enhancement at low temperatures by
oxidation and reduction activities. When the operating tempera- surface modification strategy by introducing an oxide ion conductor
ture is reduced below 700
C, ORR catalytic reactions get slower as a into Ni [54]. Ni-free anode material such as Cu-SDC, Cu0.2Zn0.8-
result, cell efficiency is severely affected. Poor catalytic kinetic and NSDC, Ba0.05Cu0.25Fe0.10Zn0.60-NKSDC, Sr0.94Ti0.9Nb0.1O3-CGO and
sluggish ionic conductivity increases the polarization resistance of Mn0.20FexZn0.8Ox-SDCC [55e58], have delivered exemplary perfor-
the cathode [18,35e37]. Therefore, developing a cathode with fast mance when operated fuel cell at low temperature certifies material
catalytic functionalities is necessary. An efficient cathode with modification and selection plays a crucial role in reducing operating
mixed ionic/electronic conduction (MIEC) can significantly improve temperature. This review article aims to explore the efficient ma-
catalytic functionalities [38,39]. Duan et al. have developed terials and advanced technologies that various authors have re-
BaCo0.4Fe0.4Zr0.1Y0.1O3-d (BCFZY) cathode showing remarkable ported to reduce the operating temperature of fuel cells. In addition,
enhancement in ORR catalytic functionalities at lower tempera- this work seeks to identify high-performing materials and their
tures 350e500
C [40], PrBa0.5Sr0.5Co1.5Fe0.5O5þd cathode and contribution towards lowering the operating temperature and
La0.6Sr0.4CoO3-d have delivered excellent power output at low investigate advanced materials and strategies for designing high-
operating temperatures 450e550
C. Both cathodes were estab- performing materials that exhibit superior performance at low
lished by the Hailes and Shims groups [41,42]. Another triple charge operating temperatures. This review article is structured as follows.
conducting (Hþ/e/O2) cathode Ni0.8Co0.15Al0.05LiO2-d (NCAL), has Section 2 delves into the rationale behind the need to lower the
shown remarkably fast HOR and ORR catalytic functionalities as a operating temperature of fuel cells. High-performing electrolyte
symmetrical electrode [43]. These cathode materials depict that materials and the efficient strategies employed to improve the ion

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M. Yousaf, Y. Lu, M. Akbar et al. Materials Today Energy 44 (2024) 101633

transport mechanisms are discussed in section 3. The catalytic membrane fuel cells (PEMFCs) [68], according to Albert Taranco
n
functionalities of cathode material, along with their high perfor- et al., lowering SOFC operating temperatures to 500e700
C is
mance, are discussed in section 4. Finally, section 5 addresses the crucial for commercial development due to reduced material and
challenges associated with material selection and device fabrication. system demands. High temperatures impose strict material re-
quirements and hinder commercialization. By lowering their
2. Working principle of solid oxide fuel cells working temperature, SOFCs can be made more durable, efficient,
cost-effective, safe, and compatible with other systems, making
The SOFC working principle is based on the electrochemical them more appealing for various applications. Multiple compelling
conversion of fuel and oxidant into electricity. A ceramic electro- reasons exist for reducing operating temperatures in SOFCs, as
lyte, sandwiched between an anode and a cathode constructs the follows.
SOFC. The fuel, typically hydrogen, supplied on an anode undergoes
oxidation and produces electrons. Air or O2 is supplied on the i). Higher temperatures can cause degradation of the materials
cathode as a reductant. The electrons travel through the external used in SOFCs, such as the electrolyte and electrodes,
circuit, generating electricity, while the ion passes across the lowering the fuel cells overall lifespan.
electrolyte [59e62]. The anode and cathode reactions for SOFC are ii). Dropping down the operating temperature can lower the
presented in the given equations. The operation of a typical SOFC is cost of the fuel cell by using fewer expensive materials and
depicted schematically in Fig. 1(a) with cell configuration (cathode: requiring less expensive cooling devices.
LSM þ YSZ, electrolyte: YSZ, and anode: Ni þ YSZ). Furthermore, iii). Higher operating temperatures can raise the risk of thermal
Fig. 1(b and c) shows oxygen ion conduction and proton ion runaway, a condition in which the temperature of the fuel
conduction-based SOFC. cell rises uncontrollably, potentially causing damage to the
Reaction at anode fuel cell or even an explosion.
iv). Lowering the working temperature allows for greater flexi-
2H2 þ 2O2 / 2H2 O þ 2e (1) bility in the choice of low-cost materials, thereby reducing
the overall cost of the device.
Reaction at cathode v). Lowering the working temperature can make the fuel cell
more compatible with other methods, such as trans-
O þ 4e / 2O2 (2) portation, where high temperatures can be difficult.
Overall cell reaction
3. Electrolyte for low-temperature solid oxide fuel cells
2H2 þ O2 / 2H2 O (3)
The material used for the electrolyte is determined by its high
ionic conductivity and assistance in fast ionic transport. Re-
2.1. Reason for lowering the temperature for solid oxide fuel cells searchers continually strive to improve its performance in LT-
SOFCs, and novel materials and designs are being developed to
The capacity to run at lower temperatures is a significant meet the challenges of low-temperature operation [69e71]. The
advantage of LT-SOFCs over conventional counterparts. This prop- selection of novel materials and advanced technology can help
erty reduces the thermal stress fuel cell components undergo counter the critical challenges faced by LT-SOFC when performing
during operation, improving overall system dependability and well at low temperatures [72,73]. High-performing yttria-stabilized
lifespan. Furthermore, the lower working temperature of LT-SOFCs zirconia (YSZ) employed at intermediate-temperature SOFCs don't
can contribute to cheaper material and production costs, making have sufficient ionic conductivity for low-temperature applications
this technology appealing to those looking to optimize the eco- [74]. To improve YSZ, electrolyte performance at low temperatures
nomics of their energy systems. As a result, LT-SOFCs are a potential can be achieved by decreasing electrolyte thickness; as a result, the
technology for various uses, including mobility, portable electricity, resistance decreases due to improved grain boundary/interfacial
and fixed power generation [61e63]. The fundamental challenge transport. Because of its superior ionic conductivity, YSZ is
with SOFCs is the operating temperature of 800e1000
C considered a high-performing electrolyte material with an ionic
[26,35,64], which results in material and cost limits and operational conductivity greater than 0.1 S/cm for high-temperature SOFCs.
difficulties. Recent solid oxide fuel cell experiments show extraor- Reducing the thickness of the YSZ electrolyte is also necessary to
dinarily high power densities on material modification at inter- achieve the required ASRel of 0.1 U cm2. To meet the YSZ ASRel
mediate temperatures of 600e800
C [65e67]. Nanostructured requirement, electrolyte thickness should be around 10 mm at
electrodes and high-conductivity electrolyte designs have recently 700
C and 1 mm at 500
C [72]. Constructing thin electrolytes re-
been developed to show a way to increase performance even quires advanced fabricating technology such as , spark plasma
further at lower temperatures, 350e600
C [65e67]. The reason for sintering, chemical solution deposition, atomic layer deposition,
reducing the operating temperature is well articulated by Eric D. atomic layer deposition, and pulsed laser deposition. Unfortunately,
Wachsman and Kang Taek Lee. Both perceptions are that reducing this technology is expensive and challenging to manufacture; thus,
the operating temperature of SOFCs reduces system costs, perfor- it is necessary to seek alternative approaches [5,46,75,76]. Instead
mance deterioration, and faster start-up and shutdown cycles, of using advanced technology, the second approach can be replaced
making them more suitable for portable power and transportation. by applying surface modification in the YSZ electrolyte. Yixiao Cai
Intermediate temperatures (650e800
C) provide cost-effective et al. explore a novel electrolyte of Ce0.8Sm0.2O2-deSrTiO3, designed
metallic interconnects, while low temperatures (650
C) provide for enhancing the efficiency of low-temperature solid oxide fuel
greater material flexibility and a lower balance of plant costs. cells. This electrolyte merges two types of structures, fluorite and
Operating below 350
C allows cheaper interconnects and seals and perovskite, to boost ion movement and minimize short-circuit risks
faster thermal cycling. Lower temperatures also improve theoret- from SrTiO3. The work encompasses synthesizing the material,
ical efficiency, particularly for CO fuel, despite potential efficiency constructing the fuel cell, and an in-depth analysis of its electro-
losses caused by thermally triggered polarization. This gives low- chemical performance. By high-resolution transmission electron
temperature SOFCs an advantage over proton exchange microscopy analysis, samarium-doped ceria (SDC) and strontium
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M. Yousaf, Y. Lu, M. Akbar et al. Materials Today Energy 44 (2024) 101633

Fig. 1. (a) Schematic diagram showing the operating principle of a solid oxide fuel cell (SOFC) (cathode: LSM þ YSZ, electrolyte: YSZ, and anode: Ni þ YSZ) Adopted with permission
from Ref. [59]. Copyright 2023, Royal Society of Chemistry. The working principle of SOFC. b) Oxygen-ion and c) proton conduction in a solid oxide fuel cell [60].

titanate (STO) grains are observed with distinct crystalline struc- higher than that of YSZ at the same temperature. This decrease in
tures, showing specific d-spacing measurements. The interaction performance is mainly due to the creation of resistive phases, like
between these grains is evident in the interfaces and boundaries ZrO2 during the high-temperature sintering process. The long-term
depicted in the images. A particular focus is given to an interface stability of ionic conductivity for 20ESB-YSZ sintered at 800
C was
showcasing the organized lattice of both SDC and STO, which is evaluated at 750
C using electrochemical impedance spectroscopy
evident through their respective d-spacing values. This interface is (EIS) under open circuit conditions in ambient air, as shown in
crucial, as it potentially enhances the ionic conductivity of the Fig. 2(j). Initially, conductivity was slightly decreased during the
nanocomposite. The overall crystal and microstructure attributes first 55 h. However, after this period, the ionic conductivity of
affirm the formation of an effective bulk heterostructure in the 20ESB-YSZ gradually recovered and remained stable for over 580 h,
SDCeSTO samples, as shown in Fig. 2(bed). The interface design is showing no significant degradation, thus indicating its high sta-
key to its success, facilitating rapid ion transport. A unique aspect of bility. This approach is more economical and more accessible than
the study is using the Schottky junction concept to elucidate the advanced technologies. In another work, M Yousaf et al. prepared
electrolyte characteristics of higher fuel cell performance and Ni-Zn ferrite-SDC heterostructure composites. In low-temperature
enhanced ionic conductivity. It can be seen in Fig. 2(hej). Dong Woo solid oxide fuel cells, the Ni-Zn ferrite-SDC heterostructure com-
Joh et al., developed a nanocomposite electrolyte by introducing posites are pivotal in augmenting ionic conductivity. These com-
erbia-stabilized bismuth oxide into yttria-stabilized zirconia [77]. posites merge Ni-Zn ferrite catalytic properties with the ion
The results show that the conductivity of the composite was transport functionality of SDC, enhancing the fuel cell electro-
considerably enhanced by introducing electrochemical impedance chemical efficiency. Fig. 2(kem), as interpreted from the EIS results
spectroscopy (ESB) into the electrolyte YSZ. In Fig. 2(i), the Arrhe- shows a decrease in the total ohmic resistance in the hetero-
nius data illustrated through Arrhenius plots reveal how ionic structure composite, indicating a rise in ionic conductivity. This
conductivity varies inversely with temperature. Significantly, the conductivity enhancement, or phase transformation, is evident in
conductivity of the composite increases with the addition of ESB. the Ni-Zn ferrite heterostructure membrane. The surface bound-
However, in the case of 5ESB-YSZ, the conductivity is lower than aries of Ni-Zn ferrite and SDC particles in this composite create a
YSZ alone. At 700
C, for instance, 5ESB-YSZ conductivity is 42% more efficient pathway for oxide-ion transport, potentially leading

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M. Yousaf, Y. Lu, M. Akbar et al. Materials Today Energy 44 (2024) 101633

Fig. 2. (a) A graphical illustration and (bed) HR-TEM images having an interface between the compact grains of STO and SDC heterostructure nanocomposite electrolyte, (eeg) the
ionic conductivity, I-V & I-P characteristics and Schottky Junction analysis. Reproduced with permission [73]. Copyright 2021, Springer. (hej) Nanocomposite electrolyte ESB-YSZ
with their conductivity and durability analysis. Adopted with permission from Ref. [77]. Copyright 2023, Elsewhere. (kem) XRD patterns of Ni-Zn and Ni-Zn/SDC heterostructure
with their fuel cell performance and Schematic illustration of triple phase boundaries to the performance of the device, i.e. NieZn ferrite-SDC [78]. HRTEM, high-resolution
transmission electron microscopy; STO, Strontium titanate; SDC, samarium doped ceria; ESB, electrochemical impedance spectroscopy; YSZ, yttria stabilized zirconia; XRD, X-
ray diffraction. Copyright 2020, Elsewhere.

to improved performance in the fuel cell. Moreover, this enhance- in these materials [79e81]. GDC with an electrolyte thickness of
ment is particularly noticeable in the triple-phase boundary area, a 10 mm delivers one order higher conductivity than YSZ electrolyte
critical zone for fuel cell operations. Integrating these materials of 1 mm thickness at 500
C. However in reducing conditions, the
markedly improves the overall functioning of the fuel cells, with conversion of Ce4þ to Ce3þ makes it unstable. Another approach is
significant benefits at lower operational temperatures to design novel electrolytes by using structure and interface
Gadolinia/samarium doping ceria (SDC, GDC), LSGM, and modification. This approach is more economical and not high,
dysprosium and tungsten stabilized Bi2O3 (DWSB) have improved requiring advanced fabrication technology. Several other dopants
performance and conductivity at intermediate temperatures. also exhibit, such as strontium (Sr), including yttrium (Y),
However, instability, compatibility with the anode and cathode, samarium (Sm), europium (Eu), and calcium (Ca) significantly
and chemical stability in reducing the atmosphere are severe issues improve the conductivity of ceria electrolytes and deliver high

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M. Yousaf, Y. Lu, M. Akbar et al. Materials Today Energy 44 (2024) 101633

performance [10,82,83]. Other electrolytes, such as LSGM [84]. a conductivity of 0.12 S/cm at 700
C by doping calcium and
Scandia-stabilized zirconia (ScSZ) [85,86], Calcium-doped samarium CeO2 [108]. Yanyan Liu has reported a high ionic con-
lanthanum zirconate (CLZ) [87,88], strontium-doped lanthanum ductivity of 0.12 S/cm at 600
C by doping Sm3þ, Pr3þ, and Nd3þ in
zirconate (SLZ) [89], bismuth oxide-based electrolytes (e.g. Bi2O3- ceria [101]. Rare earth dopant and co-doped ceria electrolyte ma-
doped with Sc2O3 or Y2O3) [90,91]. Compared to conventional terials, such as SmxNd0.15xCe0.85O2d [109], Ce1eaGdaeySmyO2e0.5
electrolytes, such as YSZ, the reported electrolytes show high per- [110], Ce1-xHo0.1SrxO2-d [111], Ce1exGd0.5Pr0.5O2 d [112],
formance and lower temperatures. Proton conduction-based elec- Ce0.8Sm0.2xPrxO2-d [113] have also delivered high ionic conduc-
trolytes are also being investigated as potential electrolytes LT- tivity in comparison to conventional electrolyte when operated at
SOFCs [69,70]. Proton-conducting LT-SOFCs provide advantages an intermediate temperature.
over typical SOFCs, including increased power density and faster
start-up times. Doped BaZrO3 and SrZrO3 and BaZr0.1Ce0.7Y0.2O3
(BZCY). BaZr1-xYx O3 (BZY) [92e95]. Fig. 3 compares the ionic 3.2. Proton conducting electrolytes for low-temperature solid oxide
conductivities in electrolytes reported by various authors. The re- fuel cells
ported work indicates that structural changes by using different
dopants can significantly improve ionic conductivity when The role of proton-conducting (Hþ) electrolytes in LT-SOFCs has
lowering the operating temperature. shown considerable power compared to O2 conducting electro-
lytes at 300e600
C [114e116]. PCEs have several advantages over
other electrolyte materials in LT-SOFCs. Most importantly, PCECs
3.1. Ceria-based electrolyte for lowering operating temperature exhibit higher protonic conductivity along with low activation
energy. As a result, fast ion transport occurred, leading to improved
Doped CeO2 electrolytes have several advantages in SOFCs and fuel cell performance [70,117]. Some of the most commonly studied
SOECs, including high ionic conductivity and excellent stability at PCEs for LT-SOFCs include perovskite oxides such as BaZrO3 [118],
intermediate temperatures. This type of electrolyte can also func- SrZrO3 [119], and BaCeO3 [120], BaZr0.8Y0.2O3ed [121] and remain-
tion at lower temperatures and deliver high performance by ing are mentioned in Table 1. These materials exhibit higher con-
reducing thermal loads on the cell and increasing its durability ductivity and stability. These materials are appealing candidates for
[98e100]. Doping ceria with zirconium, yttrium, gadolinium, or use in LT-SOFCs. In proton shuttles in CeO2/CeO2d coreshell
samarium can improve its ionic conductivity and oxygen ion structure, Yueming Xing et al. investigate a new core-shell elec-
diffusion. Dopant addition can also stabilize the fluorite structure of trolyte structure for proton ceramic fuel cells. This study highlights
ceria at lower temperatures and lower the sintering temperature, the enhanced proton conductivity achieved within a CeO2/CeO2d
resulting in lower manufacturing costs [101e103]. Doped ceria framework. The research unveils a distinctive mechanism of proton
oxides have been studied comprehensively as single-ion transport at the interface of the semiconductor core and shell,
substituted oxides for LT-SOFCs. However, reducing Ce4þ to Ce3þ facilitated by a high density of oxygen vacancies and a depletion
in these electrolyte types leads to electrical conduction [104,105]. In zone. This novel approach significantly improves fuel cell efficiency
a fuel cell, the electrodes are separated by the electrolyte, and the and offers fresh perspectives on proton movement in oxide mate-
electrolyte mediates the electron transfer between the electrodes. rials and the design of advanced proton conducting fuel cells
However, reducing Ce4þ to Ce3þ creates electronic short circuits if (PCFCs). Moreover, a charge separation mechanism is observed at
the Ce3þ ions come into contact with the electrodes, bypassing the the interface of CeO2d and CeO2 in a core-shell structure due to
electrolyte and reducing SOFC efficiency. As a result, the reduction electron transfer from the CeO2d shell to the CeO2 core. This results
should be halted by employing various strategies. Several efforts in an electron-depleted region on the CeO2d side and an electron-
have been made in the SOFC field to address these challenges. To enriched region on the CeO2 side. Enhanced at fuel cell operating
eliminate electronic leakage current, Virkar et al. utilize YSZ as an temperatures, thermal activation drives this separation and is
electron-blocking layer [106]. Wachsman et al. introduce co-doped driven by thermal activation, causing electron excitation. The
bismuth-oxide-based materials [68]. Simone et al. synthesized positively charged layer in the CeO2d shell limits proton migration
Bi2O3, developed alternating layers of Er2O3-stabilized Bi2O3, and and bulk infiltration by electrostatic repulsion, as shown in
demonstrated high chemical stability [107]. Banerjee et al. achieved Fig. 4(b). Consequently, proton transport is mostly surface-

Fig. 3. Conductivities of different electrolytes at different operating temperatures adopted with permission from Refs. [96,97]. Copyright 2023, Elsewhere.

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M. Yousaf, Y. Lu, M. Akbar et al. Materials Today Energy 44 (2024) 101633

Table 1
Proton conducting electrolytes for LT-SOFCs.

Electrolyte Temperature (
C) Power density mW/cm2 References

BaCe0.55 Zr0.3Y0.15O3 600 1302 [133]

BaCe0.55Zr0.3Y0.15O3 600 508 [134]
BaZr0.7Pr0.1Y0.2O3 650 108 [135]
BaCe0.6Zr0.2Y0.1Yb0.1O3ed 550 278 [136]
BaCe0.7Zr0.1Y0.2O3d 650 207 [137]
BaCe0.8Y0.2O3 600 1400 [127]
BaZr0.1Ce0.7Y0.1Yb0.1O3-d 750 1102 [138]
BaZr0.2Ce0.6Y0.1Yb0.1O3-d 650 600 [139]
BaCe0.55Zr0.3Y0.15O3-d 600 1300 [140]
BaZr0.1Ce0.7Y0.1Yb0.1O3d 750 1000 [141]
Ba(Zr0.1Ce0.7Y0.1Yb0.1)0.95Pd0.05O3d 650 724 [130]
BaCe0.5Zr0.3Dy0.2O3- d 700 290 [131]
BCZYYb4411 550 440 [140]

concentrated in the CeO2d shell, aided by weaker H-O interactions bonds and shortening O-O bond lengths, as shown in Fig. 4(h).
and lower proton diffusion activation energy than CeO2. This pro- Fig. 4(i) compares the conductivity of the ZFO-CeO2 electrolyte to
cess facilitates efficient proton transport in the electrolyte mem- other typical electrolytes reported in previous studies. It highlights
brane of the PCFC. Fig. 4(c) displays Arrhenius plots showing the that ZFO-CeO2 exhibits a significantly higher conductivity than YSZ
temperature-dependent total conductivities derived from the EIS and LSGM electrolytes. Additionally, its performance surpasses
results under fuel cell conditions. It shows that the conductivity of well-known proton conductors like BaZrO3 (BZY) and SmNiO3,
CeO2 decreases with increased heat treatment temperature, with indicating its superior conductivity properties. In another PCFC
values at 520
C being 0.16 S/cm for as-prepared CeO2, 0.12 S/cm for work, Y Xing and co-authors address the challenge of low ionic
CeO2-600 and 0.09 S/cm for CeO2-1000. The increase in heat conductivity in PCFCs. They enhance proton conduction by
treatment temperature leads to a rise in ionic activation energy, combining CeO2d with yttrium-doped barium zirconate (BZY),
indicating a challenge in ionic transportation at higher tempera- creating a semiconductor-ionic heterostructure. This novel
tures. Even the sample treated at 1000
C maintains a conductivity approach significantly increases interfacial conduction, improving
significantly higher than doped ceria, suggesting a strong ionic electrolyte performance in PCFCs and water electrolysis. The
surface conduction characteristic. In another work, Fig. 4(def) research underscores the importance of integrating
show that state-of-the-art protonic conductor BZY electrolyte de- semiconductor-ion materials and interface engineering for better
livers much higher conductivity than other oxide ion conductors proton transport and device efficiency in electrochemical energy
(SDC, LSGM, and YSZ). Fig. 4(f) provides insights into the estimated technologies. The proton transport mechanism in the CeO2d/BZY
operating temperatures for different electrolytes with a constant heterostructure is depicted in Fig. 4(k). In CeO2d, oxygen defects
thickness of 15 mm and a targeted area specific resistance (ASR) of arise along with the localization of Ce 4f state electrons, forming
0.15 U cm2. The suggested operating temperatures for BZPY10 and Ce3þ ions and creating a mix of Ce4þ and Ce3þ oxidation states.
BZY20 electrolytes are 600
C and 425
C, respectively. Highly- These oxygen vacancies facilitate the redox reaction of CeO2d,
textured BZY20 films might even operate at temperatures as low crucial for CeO2 formation. Protons move through these vacancies
as 350
C. This figure underscores the availability of effective high- and defects, forming hydroxyl radicals. Electrons produced in this
temperature proton conducting (HTPC) electrolytes for SOFCs process are confined to the surface due to positive charge repulsion,
operating at or below 600
C. Developing suitable electrode ma- creating a built-in electric field (BIEF). At 520
C, the ionic con-
terials, especially cathodes, is crucial for optimal SOFC performance ductivities for BZY-sintered, BZY, and CeO2d/BZY are observed to
at these lower temperatures. M. Yousaf and team investigated a be 0.039, 0.09, and 0.23 S/cm, respectively. The ionic conduction
semiconductor heterostructure comprising ZnFe2O4 and CeO2. The activation energies drop from 0.81 eV in BZY-sintered to 0.69 eV in
study aims to enhance proton conduction by utilizing interfacial BZY and 0.41 eV in CeO2d/BZY. This data distinctly indicates that
disordering and heterojunction effects within this heterostructure. the CeO2d/BZY heterostructure exhibits the highest ionic con-
The research reveals a marked improvement in proton conductiv- ductivity compared to the other samples, with sintered BZY
ity, positioning it as a valuable material for proton ceramic fuel showing the lowest. This suggests that ion transport on the surface
cells. Extensive material characterizations, theoretical analyses, and of these materials is much more efficient than in their bulk.
electrochemical performance evaluations were carried out to The electrochemical processes that take place in a PCFC are
deepen the understanding and optimization of proton transport, given below.
especially at low temperatures. In PCFC electrolytes, proton con- Reaction at cathode
duction occurs through two primary mechanisms: the Grotthuss
and vehicle mechanisms. The Grotthuss mechanism involves the 1
O þ 2e / O2 (4)
diffusion of Hþ ions through a network of water molecules by 2 2
forming and breaking bonds, where the Hþ ions move along and Reaction at anode
reposition at the lattice oxygen sites. Conversely, the vehicle
mechanism involves Hþ ions migrating while attached to another O2 þ H2 / H2 O þ 2e (5)
element, as seen in perovskite-structured oxides where OH for-
mation and oxygen vacancies occur. The ZFO-CeO2 heterostructure, Overall reaction:
as evidenced by HR-TEM, XPS, and density functional theory (DFT)
calculations, shows interfacial disorder primarily due to oxygen 1
O þ H2 / H2 O (6)
atom displacement at the interface, leading to oxygen defects in the 2 2
lattice. These defects potentially facilitate Hþ ion hopping along O- Hydrogen is oxidized and divided into protons and electrons at
O bonds in the Grotthuss mechanism by weakening partial MeO the anode. After splitting, electrons flow through the external
7
M. Yousaf, Y. Lu, M. Akbar et al. Materials Today Energy 44 (2024) 101633

Fig. 4. (aec) Schematic diagram of the SOFC with CeO2 core-shell particles as the electrolyte, the proton shuttles transport in the high-conducting region of the electrolyte
membrane constituted by the surface region of the CeO2d shell and their ionic conductivity analysis. Reproduced with permission [122]. Copyright 2019, ACS Publications. (def)
Schematic Illustration and proton-conduiting BZY electrolyte conductivity with oxygen-ion conductors, SDC, LSGMs, and YSZ [123]. Adopted with permission from reference [128].
Copyright 2023, Wiley. (gei) The schematic illustration of typical p-n junction formation and energy band alignment for the interpretation of the charge separation mechanism, the
proton conduction mechanism of the ZFO-CeO2 fuel cell device by following the Grotthuss and vehicle mechanism and prepared a heterostructure conductivity comparative
analysis. Reproduced with permission [124]. Copyright 2023, WILEY. (jel) Schematic illustration of the proposed design ideas for surface proton conduction enhancement, built-in
electric field, and ionic conductivity analysis. Reproduced with permission [125]. SOFC, solid oxide fuel cell; BZY, BaZr1-xYx O3; SDC, samarium doped ceria; LSGMs. lanthanum
strontium gallium magnesium oxide; YSZ, yttria stabilized zirconia. Copyright 2022, ACS Publications.

circuit to the cathode side. Simultaneously, protons pass across the high-power output of 1.4 W/cm2 [127]. On the other hand, BCY is
electrolyte and react with oxygen molecules and electrons to form not viable for long-term operation due to its chemical instability.
water. The mechanism is shown in Fig. 5, along with the conven- Kiho Bae et al. [128] have demonstrated a very high power density,
tional SOFC working principle. low ohmic resistance, and high protonic conductivity for 1 mm
Protonic conductor BaCeO3 (BCY) electrolytes show excellent thick BaCe0.55Zr0.3Y0.15O3d electrolytes. The cell exhibits Pmax
performance at low temperatures. Ito et al. demonstrated that a 1.1 W/cm2 at 600
C; even at low temperatures, 550
C BCZY de-
fuel cell operates at 400e600
C with BCY electrolyte, delivering a livers Pmax 800 mW/cm2. I-V/I-P performances and EIS data of
8
M. Yousaf, Y. Lu, M. Akbar et al. Materials Today Energy 44 (2024) 101633

BCZY electrolytes are presented in Fig. 6. In another study con- LT-SOFCs are mentioned in Table 2, having much higher peak power
ducted by Mingi Choi, controlling the chemical reaction in density than conventional doped electrolytes. The dense, thin layer
BaZr0.4Ce0.4Y0.1Yb0.1O3 electrolyte in an anode-supported PCFC, it of YSZ and a thick layer of porous, mixed ionic-electronic con-
is found that the cell delivers Pmax of 1.90 W/cm2 with a low Ro of ducting materials such as gadolinium/samarium-doped ceria are
0.060 U cm2 at 650
C and 0.082 U cm2 at 550
C [129]. By doping typical examples of heterostructure electrolytes for LT-SOFCs. The
pd in (Ba(Zr0.1Ce0.7Y0.1Yb0.1)0.95Pd0.05O3d), it is found that PCFC dense YSZ layer provides mechanical stability and prevents gas-
delivers Pmax724 mW/cm2 at 650
C, while without pd doping, the phase corrosion of the porous MIEC layer. The thick porous MIEC
similar cell exhibit (450 mW/cm2) depicting it as a promising fuel layer, on the other hand, facilitates oxygen reduction and oxygen
cell. NiBZCYYbPd anode was used, which reduced and further ion transport, allowing for quicker ionic transport. The crucial part
improved the catalytic functionality; as a result, the cell was of such a type of heterostructure is the formation of hetero-
persistently stable for 350 h [130]. BCZDy with Co-free Sr3Fe2O7- interfaces, which leads to interface superionic conduction. Wang
d cathode exhibited open circuit voltage (OCV) values of 1.090 V et al. achieved a conductivity of 0.18 S/cm in a heterostructure
and Pmax of 286 mW/cm2 at 700
C [131]. It has also been re- composite of La0.6Sr0.4Co0.2Fe0.8O3-d and Ca0.04Ce0.8Sm0.16O2-d at
ported that BaCe0.7Zr0.1Y0.2O3-d electrolyte prepared using the dip 600
C [142]. Garcia-Barriocanal et al. found a colossal ionic con-
coating technique can work even at low temperatures, such as ductivity (0.1 S/cm at 200
C) around 8-order enhancement in
200
C [132]. conductivity [143]. Yingbo Zhang et al. constructed a hetero-
structure among CeO2/a-Al2O3 electrolytes exhibiting conductivity
3.3. Heterostructures electrolyte for low-temperature solid oxide of 0.127 S/cm and Pmax 1017 mW/cm2 550
C [144]. This result
fuel cells shows that the achieved power is higher than the conventional
electrolyte in another study conducted by Jaime Liu et al., using
At low temperatures, heterostructure electrolytes are predicted Ba0.9K0.1Fe0.5Co0.5O3-d (p-type) and Sm0.075Nd0.075Ce0.85O2-d (n-
to possess exceptionally high levels of ionic conductivity. The het- type) and construct a semiconductor heterostructure between a
erostructure composites electrolytes recently exhibited consider- perovskite and fluorite material. On performing fuel cell perfor-
able performance and ionic conductivity greater than 0.1 S/cm at mance, as configured, SOFC delivers Pmax 911 mW/cm2 at 550
C
600
C. By combining different materials with complementary along with 0.14 S/cm conductivity [145]. By using a tipple con-
features and heterostructure electrolytes can increase the ionic ducting (Hþ/O2/e) cathode material BaCo0.4Fe0.4Zr0.1Y0.1O3-d and
conductivity of LT-SOFCs. Various heterostructure electrolytes for ZnO, Xia Chen has reported 643 mW/cm2 at 500
C. The

Fig. 5. SOFC with (a) a proton-conducting electrolyte and (b) an oxygen ion conductor [126]. SOFC, solid oxide fuel cell.

9
M. Yousaf, Y. Lu, M. Akbar et al. Materials Today Energy 44 (2024) 101633

Fig. 6. Fuel cell performance and EIS of PCFC with BCZY electrolyte [128]. Adopted with permission from reference [131]. EIS, electrochemical impedance spectroscopy; PCFC, proton
conducting fuel cell. Copyright 2023, Wiley.

Table 2
Heterostructures electrolyte for LT-SOFCs.

Electrolyte Temp. (
C) Power density mW/cm2 References

LiZnOeSnO2 530 376 [148]

La0.8Sr0.2Co0.8Fe0.2O3-d-Li2TiO3 550 350 [149]
SrFe0.2Ti0.8O3-d-ZnO 520 650 [150]
CeO2-CuO 550 845 [151]
Ni0.4Zn0.6 Fe2O4- Sm0.2Ce0.8O2 550 760 [78]
CeO2d@CeO2 550 650 [152]
SrFe0.75Ti0.25O3d Sm0.25Ce0.75O2d 520 920 [153]
Ce0.8Sm0.2O2-d and SrTiO3 550 892 [73]
NaCo0.5Fe0.5O2-CeO2 550 1010 [63]
NCAL-ZnO-SnO2 550 1267 [154]
CeO2d/BaZr0.8Y0.2O3 520 845 [125]
Sm0.075Nd0.075Ce0.85O2d/Al2O3 550 1312 [155]
SrTiO3/CeO2 550 745 [156]

heterostructure formation suppresses its electronic conduction, unique crystal structure and tunable properties, which reduce the
helping achieve superior OCV (1.08, 1.03e1.01 V) at 400, 450
C operating temperature of SOFCs [22,35,162]. Reducing the oper-
[146]. The mechanism of the p-n junction and its suppression of ating temperature improves the cathode’s efficiency and durability.
electronic conduction are shown in Fig. 7. Naveed Mushtaq et al. The choice of materials used in the SOFC cathode can significantly
have reported a heterostructured Ba0.5Sr0.5Fe0.8Sb0.2O3-d- impact the operating temperature. The thickness of electrolytes
Sm0.2Ce0.8O2-d that promoted fast electrocatalytic activities and and cathodes is crucial in achieving high performance. A thinner
found the heterostructure exhibits ionic conductivity >0.1 S/cm electrolyte and cathode can lower ion and electron transfer resis-
1012 mW/cm2 power density at 550
C [147]. These results suggest tance, resulting in a more efficient SOFC system. The use of nano-
that forming heterostructure electrolytes via surface modification technology can also help reduce temperature. For example, using
significantly enhances ionic conductivity and lowers activation nanostructured materials can enhance the surface area of the
energy. electrodes and promote more efficient ion and electron transfer
[36,71]. Polarization is a loss of efficiency that occurs in SOFCs when
4. Cathode material for low-temperature solid oxide fuel cells there is a mismatch between the electrochemical reaction rate and
the transport of ions and electrons. Reducing polarization resis-
This reduction reaction at the cathode is critical for a quick tance leads to high performance at low temperatures [163,164].
catalytic response. The cathode performance considerably in- The unique crystal structure of perovskites facilitates the
fluences the overall electrochemical efficiency of the SOFCs. A transport of oxide ions across the cathode and electrolyte in-
suitable cathode should have a low resistance to catalytic func- terfaces. This can reduce polarization resistance; as a result, the
tionalities, which leads to high electrochemical performance SOFC shows better catalytic functionalities [165,166]. By selecting
[157e160]. Therefore, the cathode material must have good elec- the appropriate perovskite material, it is possible to design a SOFC
trochemical functionality toward fast oxygen reduction reactions system that operates at a lower temperature without sacrificing its
[161]. The cathode material should have sufficient quick catalytic performance, thus reducing the overall cost and increasing the
activities to aid the ORR at the cathode-electrolyte interface, an system’s durability. Fe-based cathodes are a type of cathode that
essential process in SOFCs. Reducing the operating temperature of has been investigated for use in SOFCs. Fe-based materials have a
SOFCs is an important research topic, as it can improve their effi- unique electronic and ionic conductivity, making them attractive
ciency, durability, and cost-effectiveness. There are several ways to for use in SOFC cathodes [167e169]. One common ferrite-based
reduce the operating temperature. Among them, perovskite-based cathode material is LSCF. The perovskite crystal structure LSCF al-
cathode materials are considered efficient catalysts due to their lows high oxygen vacancies and ion conductivity density. LSCF is

10
M. Yousaf, Y. Lu, M. Akbar et al. Materials Today Energy 44 (2024) 101633

Fig. 7. p-n heterojunction formed at the hetero-phasic interface between BCFZY and ZnO [146]. Adopted with permission from reference [83]. BCFZY, BaCo0.4Fe0.4Zr0.1Y0.1O3-d.
Copyright 2023, Elsewhere, Ref. [149].

also a mixed ionic and electronic conductor, which can transport perovskite materials, such as LSC, exhibit high ORR functionalities
oxygen ions and electrons [170,171]. This allows for efficient oxygen and can be tailored to have optimal properties for specific appli-
reduction at the cathode-electrolyte interface. Additionally, Fe- cations. The porosity of the cathode can also affect its performance.
based cathodes have been shown to have high activity and stabil- A higher porosity can promote more efficient gas diffusion and
ity in SOFCs, making them a promising material for use on these improve the electrochemical reaction. However, too high porosity
devices. It has been reported that composite cathodes for LT-SOFCs can result in reduced mechanical strength and stability. Therefore,
offer long-term durability owing to their enhanced conductivity optimizing the cathode porosity for the specific application is
and fast catalytic functionality [167,170,172]. essential. The microstructure of the cathode, such as the size and
distribution of pores, can also affect its performance. A well-
4.1. Perovskites cathode for low-temperature solid oxide fuel cells organized microstructure with a large surface area can promote
more efficient oxygen reduction and electron transfer [181,182].
Perovskites have been widely researched and employed as po- Surface modifications, such as the deposition of catalysts or surface
tential cathode materials in SOFCs. Due to their high-oxygen coatings, can also improve the performance of the cathode. These
reduction activity, perovskites are possible cathode materials in modifications can enhance the reaction rate or protect the cathode
SOFCs. Because of their chemical stability, they are suited for high- from degradation [183,184].
temperature applications [173e175]. Perovskite materials are Zhang et al. have reported a minimum 0.119 U cm2 ASR at 550
C
compatible with a wide range of SOFC electrolytes, making them for Pr0.2Ba0.8Co0.7Fe0.3O3d, far lower than LSCF-based cathode at
adaptable and allowing the SOFC architecture to be customized to such low operating temperature [166]. Rare earth-doped
meet specific needs. Doping or substituting various elements in inPr0.2Ba0.8Co0.7Fe0.3O3d has almost 1/3 of the area-specific resis-
perovskite materials allows for fine-tuning features such as oxygen tance compared to the pristine cathode. Applying the co-doping to
reduction activity and chemical stability [176,177]. The cathode dope (Gd and Ce) in LaFeO3, as Jinpeng Li reported 0.419 W/cm2 at a
material should possess high ORR catalytic activities to facilitate the temperature of 550
C [185]. Ni0.8Co0.15Al0.05LiO2-d is a modified
ORR at the cathode-electrolyte interface in SOFCs. Due to their high perovskite oxide cathode with triple charge conduction. The fast
ORR functionalities, LSM, La1-xSrxCoO3 (LSC), and other perovskite-type electrocatalytic activity makes it an effective cathode material for
oxides are commonly used as efficient and high-performing cath- LT-SOFCs. Yuanjing Meng reported a power density of 648 mW/cm2
ode materials in SOFCs [178,179]. The selection of potential cathode in NCAL and a high OCV of 1.01 V at 550
C [43]. Naveed Mushtaq
material remarkably affects the overall performance of SOFC. Ma- developed a high-performing cathode by doping Sb in
terials with high electronic and ionic conductivity, compatibility, Ba0.5Sr0.5FeO3ed and found that a fabricated perovskite cathode
and durability are preferred cathodes [71,180]. For instance, delivering 738 mW/cm2 with the area-specific resistance (ASR) of
11
M. Yousaf, Y. Lu, M. Akbar et al. Materials Today Energy 44 (2024) 101633

0.20 U cm2 at 550
C [186]. In Sr0.95A0.05Fe0.8Nb0.1Ta0.1O3d (A ¼ Li, conducting La0.7Sr0.3Mn0.7Ni0.3O3dd, a cathode that displays Pmax
Na, and K), a Co fee perovskite, it is found that Li\K carbonates boost 386 mW/cm2 at 600
C [195]. BaxCo0.4Fe0.4Zr0.1Y0.1O3 d shows
the ORR activity with low ASR (0.12 and 0.18) U cm2 at 600
C [157]. significantly low polarization resistance and 376.27 mW/cm2 po-
The rhombohedral perovskite La0.5Sr0.5Co0.8Mn0.2O3 and hexagonal wer density at 500
C [195]. BaCo0.4Fe0.4Zr0.1Y0.1O3-d reported by
perovskite Ba0.5Sr0.5Co0.8Mn0.2O3 exhibits high ionic 3.51 S/cm and Chanho Kim et al. show fast ORR functionalities and deliver a Pmax
2.26 S/cm along with Pmax 277 mW/cm2 186 mW/cm2 at 550
C of 1.06 W/cm2 at 650
C [196]. BaZr0.2Ce0.7Y0.1O3d,- Sr4Fe4Co2O13þd
[187]. Double-layered Pr2BaNiMnO7d perovskite oxides have have shown 535 mW/cm2 and 1.065 V OCV at 550
C, representing
shown fast electrocatalytic activities at low temperatures. The it as a high-performing tipple conducting cathode owing to its fast
cathode delivers Pmax1070 mW/cm2 at 700
C with 0.084 U cm2 catalytic activities at a much lower temperature [197]. BaCo0.4-
polarization resistance [188]. A triple-charge conductor BaCo0.4- Fe0.4Zr0.1Y0.1-xZnxO3-d shows a power of 0.49 W/cm2 at 600
C [198].
Fe0.4Zr0.1Y0.1O3-d perovskite delivers 610 mW/cm2 power and an
open-circuit voltage of 1.01 V at 550
C [189]. Bi0.7Sr0.3FeO2.9-dF0.10
possesses Rp 0.12 U cm2 at 600
C [169]. Pmax of 1563 mW/cm2 is
reported for perovskite cathode Nd0.2Sr0.8Nb0.1Co0.9O3-d at 650
C 4.3. Composite cathode for low-temperature solid oxide fuel cells
with ASR 0.037 U cm2, sowing it a high performing perovskite
cathode [190]. LaxSr1-xCoO3-d cathode was prepared using facile High catalytic activities of the composite cathode can help
infiltration and achieved Pmax 1000 mW/cm2 reported at 600
C reduce the operating temperature of LT-SOFCs. A composite cath-
[168]. SrSc0.2Co0.8O3d delivered an ASR of 0.206 U cm2 and a power ode comprises multiple materials that combine to improve the
density of 564 mW/cm2 at 500
C [191]. cathode's overall performance. Composite cathodes mentioned in
Table 3 demonstrate that they can deliver high performance even at
4.2. Triple conducting cathode material low-temperature solid low operating temperatures. One approach to making composite
oxide fuel cells cathodes involves using a mixture of perovskite and spinel oxides
to enhance performance. This combination leverages the high ionic
Triple-conducting cathode materials are high-performing and conductivity of perovskite and the excellent catalytic properties of
have drawn substantial attention when operating the fuel cell at a spinel, resulting in improved performance, especially at low oper-
declining temperature. These materials are characterized by their ating temperatures. Perovskite oxides, such as LaMnO3 or LaCoO3,
ability to triple conduction oxygen ions (O2), electrons (e), and have high catalytic activity for oxygen reduction, while spinel ox-
protons (Hþ) simultaneously, which can lead to improved cell ides, such as NiFe2O4 or CoFe2O4, have high electronic conductivity.
performance and lower operating temperatures compared to Combining these two materials allows a composite cathode to have
traditional SOFCs. These materials exhibit enhanced triple charge high catalytic activity and leading performance in LT-SOFCs. Other
conduction and fast catalytic functionalities for ORR activities, composite cathodes for LT-SOFCs may include a combination of a
making them attractive candidates for LT-SOFCs. Triple-conducting perovskite oxide and an oxide with high ionic conductivity, such as
cathode materials can improve the electrochemical performance of yttria-stabilized zirconia. This can help to improve the ORR and
LT-SOFCs at low temperatures, making them a promising technol- reduce polarization losses in the fuel cell. Composite cathodes for
ogy for clean energy production. Ba0.95Fe0.7Co0.2Sc0.1O3-d, an effi- LT-SOFCs offer an encouraging approach to improving the perfor-
cient triple-conducting (Hþ/O2/e) cathode, delivers Pmax mance and durability of these fuel cells. A nanocomposite cathode
1092 mW/cm2 and 419 mW/cm2 for O-SOFCs and H-SOFCs at BaCe0.16Y0.04Fe0.8O3d by Dan Zou shows superior ORR functionality
550
C and the material is persistently stable for more than 100 h with low area-specific resistances that deliver remarkable low
[160]. Layered structured triple charge conductor Ni0.8C- resistance of 0.27 and 1.49 U cm2 at 600, 500
C presenting it as one
o0.15Al0.05LiO2-d cathode exhibits a Pmax of 648 mW/cm2 at a low of the most efficient cathode [199]. Jin Goo Lee et al. reported a
temperature of 550
C [43]. On doping F into layered structured composite core-shell fiber-structured Ba0.5Sr0.5Co0.8Fe0.2O3-
LiNi0.8Co0.15Al0.05O2-d cathodes, the SOFC delivers Pmax 591 mW/ 2

d Gd0.1Ce0.9O1.95 and found a high Pmax 2 W/cm at 550 C and is
cm2 at 550
C and are stable for 110 h without significant degra- durable for a 300 h at a current density of 1 A/cm2, suggesting that
dation [192]. BaCo0.4Fe0.4Zr0.1Y0.1O3-d perovskite developed by the such a type of cathode impressively lowers the operating temper-
Duan group shows an excellent performance at 0.65 W/cm2 at ature. Yu Chen et al. reported hierarchically porous
600
C, and even at a low temperature of 500
C, the BCFZY cathode Sm0.5Sr0.5CoO3eGd0.1Ce0.9O2d nanocathode and found them as
based PCFC deliver Pmax 0.45 W/cm2 [193]. Using self-assembly, fabricated fuel cells delivering Pmax 650 mW/cm2 at 500
C; more
nanocomposite BaCo0.7(Ce0.8Y0.2)0.3O3-d shows good mix ionic importantly, the cell is persistently stable for 500 h at 500
C
electronic conductivity, as fabricated cathode shows 985 mW/cm2 without any significant degradation. The results are displayed in
at 650
C [194]. Ning Wang et al. synthesized a triple charge Fig. 8.

Table 3
Composite cathode for LT-SOFCs.

Cathode Temp. (
C) Power density mW/cm2 References

SrCo0.4Fe0.4Zr0.1Y0.1O3edeBaCe0.6Zr0.2Y0.1Yb0.1O3ed 600 409 [136]

LaNi0.6Fe0.4O3edeSm0.5Sr0.5CoO3ed 650 728 [201]
La0.6Sr0.4Co0.2Fe0.8O3edeBaCe0.7Zr0.1Y0.1Yb0.1O3ed 550 294 [132]
La0.25Sr2.75FeNiO7ed- BaCe0.7Zr0.1Y0.1Yb0.1O3ed 550 187 [202]
Sm0.5Sr0.5CoO3eGd0.1Ce0.9O2d 500 650 [200]
Ba0.5Sr0.5Fe0.8Sb0.2O3-d-Sm0.2Ce0.8O2-d 550 1012 [147]
Sm0.2Ce0.8O2-d-Ba0.5Sr0.5Fe0.8Sb0.2O3-d 550 705 [203]
Ba0.5Sr0.5Co0.8Fe0.2O3- d Gd0.1Ce0.9O1.95 550 2000 [204]
Sm0.5 Sr0.5 CoO3- d-Ce0.8 Sm0.2 O2 600 122 [205]
La0.6Sr0.4Co0.2Fe0.8O3-d - Ce0.8 Sm0.2O2-d 500 20 [206]
PrBaCo2O5þd-BaZr0.7Y0.2Pr0.1O3-d 550 70 [207]

12
M. Yousaf, Y. Lu, M. Akbar et al. Materials Today Energy 44 (2024) 101633

Fig. 8. (a) Fuel cell performance, (b) stability test [200]. Adopted with permission from Ref. [200]. Copyright 2023, Elsevier, (c) electrochemical performance of LSM-ESB/GDC/Ni-
GDC (I-V/I-P) (d) EIS of LSM-ESB/GDC/Ni-GDC. Adopted with permission from Ref. [36]. Copyright 2023, ACS publication.

4.4. Lanthanum-based cathode material for solid oxide fuel cells performance even at low operating temperatures in the range of
(450e500
C). La0.2Sr0.8Co0.8Ce0.2O3‒d cathode-based SOFC deliv-
Lanthanum-based lanthanum nickelate (LaNiO3) and ered a Pmax of 440 mW/cm2 at 550, depicting it as a high-
lanthanum cobaltite (LaCoO3) materials. Lanthanum-based cath- performing cathode [210].
odes are long-searching cathode materials in SOFCs because of A general formula (LaMO3), where ‘M’ is a transition with mixed
their high electronic conductivity and fast catalytic activity, a ionic-electronic conductivity [38,211]. Due to enhanced catalytic
crucial reaction in fuel cells [208,209]. Lanthanum nickelate performance, it has been considered a potential cathode, showing
(LaNiO3) is a perovskite oxide with a high electronic conduction incompatibility with YSZ electrolytes, especially at declined temper-
and modest thermal expansion coefficient, which makes it a good atures because of undesirable interface reactions. However, this ma-
choice for use in SOFCs. However, it is prone to reactions with terial shows remarkably improved results at intermediate
atmospheric water vapor, which can reduce its electrical con- temperatures with doped ceria. La1-xSrxCoO3-d cathode exhibits fast
ductivity. To mitigate this issue, researchers have developed electrode activity owing to high oxygen diffusivity [212]. La1xSrx-
various techniques to protect the LaNiO3 surface, such as surface Fe1yCoyO3-d have shown fast ORR, high electrical conductivity, and
modification and coating with protective layers. Lanthanum better oxygen self-diffusion coefficients at 600 and 800
C [52]. Below
cobaltite (LaCoO3) is another popular lanthanum-based cathode 650
C, pure LSCF offers sluggish performance; however, when an
material for SOFCs. It has a good electronic conductivity and high ionic conductor is introduced, the ORR catalytic functionality of LSCF
ORR performance. High thermal stability and excellent chemical significantly improves. Jung Hoon Park et al. have shown Pmax 1.7 W/
compatibility make them promising candidates for selection as a cm2 at 650
C in a composite cathode La0.6Sr0.4Co0.2Fe0.8O3-
cathode. However, it is less conductive than LaNiO3 and can be dGd0.1Ce0.9O1.95 [213]. Cathode with low Rp achieving good perfor-
susceptible to phase changes at elevated temperatures. The mances. Therefore, a suitable cathode material should be highly
lanthanum-based cathode material depends on the specific re- conductive and compatible with middle-layer electrolytes so that it is
quirements of the SOFC and the tradeoffs between electronic low-ohmic losses can occur. Typically, ionic conductivity >100 S/cm at
conductivity, catalytic activity, and stability. Different strategies 600
C is helpful for composite cathode functionalities [52,214,215].
have been searched out to improve the conductivity of the Yi-Lin Huang reported La0.85Sr0.15MnO3-de(Bi0.8Er0.2)2O3, and the re-
lanthanum-based cathode material. Ni-foam-pasted La0.2Sr0.8- ported cathode achieved Pmax 1200 mW/cm2 at 600
C [36], and the
Co0.8Ce0.2O3‒d, reported by Jinping Wang, portrays high results are shown in Fig. 8(c and d).

13
M. Yousaf, Y. Lu, M. Akbar et al. Materials Today Energy 44 (2024) 101633

5. Challenges in material selection and device fabrication of degradation mechanisms and temperature cycling might affect
solid oxide fuel cell performance over time. Finally, actual use requires the SOFC stack
to be integrated with other system components and the develop-
Fabricating SOFCs is complicated and challenging, especially at ment of efficient startup and shutdown procedures.
high operational temperatures. Materials selection, thermal sta-
bility, and chemical compatibility are paramount requirements. 6. Future prospective
Choosing suitable materials for different fuel cell elements can be
tricky since these materials must be compatible and operate well The transition toward lower operational temperatures in SOFCs
under high-temperature and high-pressure circumstances. Aside is pivotal for commercializing SOFCs. Operating SOFCs below
from that, the electrolyte membrane is an essential component of 600
C offers significant advantages, such as reduced thermal
the SOFC, and its manufacture is a challenging procedure stress, prolonged device lifespan, and potential cost reductions
[216e218]. The electrolyte material must be chemically stable in through material and manufacturing optimizations. However,
the presence of fuel and oxidant gases in the SOFC. This is even achieving efficient performance at these reduced temperatures
more challenging for LT-SOFCs as decreasing temperature hampers poses several challenges, primarily maintaining high ionic con-
the electrochemical performances of electrolyte material with the ductivity and catalytic activity. Future research should explore new
fuel and oxidant gases. Developing stable materials in the presence electrolyte compositions with ionic/protonic conductivity capable
of these gases is critical to the long-term durability of LT-SOFCs. The of SOFCs operating at lower temperatures. Developing high-
membrane must be thin, dense, and defect-free to provide excel- performing catalysts is crucial for maintaining high catalytic ac-
lent ionic conductivity. It is difficult to achieve this level of fineness tivity and low polarization resistance in low-heat operations.
in the fabrication process. Because of the complexity of scaling up Employing nanotechnology to create materials with high surface
the fabrication process, producing large-scale SOFCs with high areas and tailored nano-scale features can significantly enhance
consistency and quality is challenging. The high-temperature sin- reaction kinetics and ion transport. Reducing the thickness of
tering process necessary for manufacturing electrodes and elec- electrolytes and electrodes reduces electrical and polarization
trolytes raises the expense of making SOFCs on a large scale. resistance, thus improving overall efficiency. Additionally, long-
Thermal control of SOFCs is also a key concern, as high-temperature term durability studies are crucial to understanding degradation
gradients within the cell can produce thermal stresses, resulting in mechanisms and material stability under reduced temperature
cracking, deformation, and cell collapse [219,220]. To enable long- conditions, leading to the development of strategies to mitigate
term operation, SOFCs must be highly durable and dependable. degradation. Cost-effective and scalable manufacturing techniques
Over time, the SOFC high-temperature and high-pressure condi- are vital for producing low-temperature SOFCs. Innovations in
tions can cause corrosion, deterioration, and performance decline. material synthesis and device fabrication can reduce costs. By
A fundamental problem in SOFC fabrication is ensuring long-term addressing these critical areas, the development of SOFCs capable
durability and reliability. The cathode material should have high of efficient operation at reduced temperatures will be significantly
ORR kinetics to facilitate the ORR efficiently. However, the ORR advanced, enhancing their commercial viability and promoting
kinetics are slower at low temperatures, leading to lower cell per- cleaner and more sustainable energy solutions.
formance. Developing materials that exhibit high ORR kinetics at
low temperatures is, therefore, a significant challenge. The cathode 7. Conclusion
material should be compatible with the electrolyte and anode
materials used in the LT-SOFC to ensure efficient electrochemical Reducing the operational temperature below 600
C is essential
reactions. Developing materials compatible with various materials for SOFC commercialization. In low operating temperatures, the
is challenging [221e223]. It requires a deep understanding of the thermal stress on the cell is reduced, which further helps to extend
material’s properties and interactions with other fuel cell compo- the SOFC device lifespan. SOFC-based devices are costly; selecting
nents. Optimizing cell assembly and anode, cathode, or electrolyte materials is essential to choosing stable materials at high temper-
thickness extensively impacts cell performance. This can be atures. Therefore, to utilize low-cost, reducing the SOFC operational
improved by utilizing different fabrication techniques, including temperature is necessary. The critical component is electrolyte
tape casting for thin films, uniaxial pressing for high-quality material must have high ionic conductivity to transport ions effi-
shapes, and screen printing for low-cost processing. These ciently. Therefore, the essential requirements are advanced strate-
methods are often combined to optimize cell fabrication. Various gies and novel materials with high ionic conductivity at low
studies have explored these designs and techniques over the past temperatures (below 600
C). In this regard, electrolyte materials
decade and demonstrated more stability and performance with hybrid ionic conductivity significantly improves peak power
improvement [15]. densities and stable voltage. Low temperature can significantly
More precisely, the assembly of SOFCs has significant hurdles, impact electrolyte electrochemical properties and performance,
principally related to material compatibility, fabrication proced- and it is essential to consider these effects when designing the
ures, and mechanical integrity. To avoid degradation at high electrolytes. The cathode is exposed to a harsh environment,
working temperatures, the materials must have appropriate ther- including high temperatures, oxidizing and reducing conditions,
mal expansion coefficients and chemical stability. High-quality and mechanical stresses. This can cause degradation and perfor-
components, especially thin, dense electrolytes and porous elec- mance loss over time, limiting the material’s lifetime and reliability.
trodes, require precise production procedures. Furthermore, pre- When operated at low temperatures, both catalytic activity and
serving the cell components' mechanical strength and structural polarization resistance, therefore, high performing cathodes with
integrity is critical for enduring operational pressures. Effective fast ORR catalytic functionalities are of utmost importance when
sealing methods are necessary to prevent gas leakage, and the in- selecting cathode materials. However, the performance is improved
terconnects must be conductive, sturdy, and corrosion-resistant. at low temperatures by employing surface and structural modifi-
The electrode microstructure and the electrolyte's thickness must cation strategies. Recent advancements in various fields, such as
be optimized for performance efficiency, but commercial viability technology, engineering, physics, and chemistry/electrochemistry,
requires cost-effective and scalable manufacturing procedures. have opened new possibilities in energy conversion and storage
Durability and longevity are also important considerations, as applications. In these domains, a fundamental understanding of
14
M. Yousaf, Y. Lu, M. Akbar et al. Materials Today Energy 44 (2024) 101633

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cludes: employment and funding grants. If there are other authors, Thermal-expansion offset for high-performance fuel cell cathodes, Nature
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Progress in durability of metal-supported solid oxide fuel cells with infil-
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