Journal of Power Sources 601 (2024) 234242

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Journal of Power Sources

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Review article

Towards a high efficiency and low-cost aqueous redox flow battery: A

short review
Zhaoxia Hou a, 1, Xi Chen a, 1, Jun Liu a, Ziyi Huang a, Yan Chen c, Mingyue Zhou b, *, Wen Liu a, **,
Henghui Zhou d
a
State Key Laboratory of Chemical Resource Engineering, College of Chemistry, Beijing University of Chemical Technology, Beijing, 100092, China
b
College of Carbon Neutrality Future Technology, China University of Petroleum, Beijing, 102200, China
c
Beijing Power Equipment Group Co., Ltd., Beijing, 102401, China
d
College of Chemistry and Molecular Engineering, Peking University, 100871, Beijing, China

H I G H L I G H T S

• Performance/cost balance is the key to low cost flow batteries

• The characteristics of various aqueous redox flow batteries are discussed
• Challenges include low energy density, slow kinetics, and instability
• Future trends favor aqueous organic and iron-based chemistries

A R T I C L E I N F O A B S T R A C T

Keywords: The aqueous redox flow battery (ARFB), a promising large-scale energy storage technology, has been widely
Energy storage researched and developed in both academic and industry over the past decades owing to its intrinsic safety and
Aqueous redox flow battery modular designability. However, compared to other technologies (e.g. Li-ion batteries), the relatively low energy
Levelized cost of storage
density, inferior efficiency, and high investment cost of the ARFB limit its further applications. Although
tremendous efforts have been made to improve the performance as well as the cost-effectiveness of ARFB by
various approaches, it is still a challenge to recognize a united and general roadmap for the next commercial-
available ARFB. Here we review the evaluation criteria for the performance of flow batteries and the develop­
ment status of different types of flow batteries. The factors affecting the performance of flow batteries are
analyzed and discussed, along with the feasible means of improvement and the cost of different types of flow
batteries, which is expected to provide useful references for the further development of high-efficiency and low-
cost flow batteries.

1. Introduction
With the growth of population and the continuous consumption of
fossil fuels, energy crises and environmental problems are becoming
increasingly prominent. Securing sustainable and environmentally
friendly energy is critical to the development of human society [1].
Renewable energy, such as solar, tidal, and wind power, provides sig­
nificant opportunities to alleviate the potential energy crisis. However,
the inherent intermittence of these renewable sources causes significant
challenges for electric grid operators [2,3]. To buffer the impact of the
intermittent problems and improve the quality of power grids, it is
necessary to develop low-cost large-scale electrical energy storage (EES)
systems [4–6]. Lithium-ion batteries (LIBs) have attracted wide atten­
tion due to their high energy density and rate capacity, which are of
great importance for various applications from portable electronic
products to electric vehicles [7,8]. However, the relatively high lev­
elized cost of storage (LCOS) and security issues have limited their ap­
plications in large-scale EES systems. The LCOS is defined as the total

* Corresponding author.
** Corresponding author.
E-mail addresses: mingyue.zhou@cup.edu.cn (M. Zhou), wenliu@mail.buct.edu.cn (W. Liu).
1
the co-first author.

https://doi.org/10.1016/j.jpowsour.2024.234242
Received 12 December 2023; Received in revised form 16 February 2024; Accepted 19 February 2024
Available online 10 March 2024
0378-7753/© 2024 Elsevier B.V. All rights reserved.
Z. Hou et al.
lifetime cost of the energy storage system divided by the cumulated
released energy of the investment, which is used to evaluate the eco­
nomic development prospects of energy storage projects [9–11]. By
contrast, ARFBs are promising candidates for large-scale energy storage
due to their modular designability, scalability, safety, and potentially
low cost on the condition of using low-cost electrolytes and increasing
the storage duration [12–14]. On the power generation and grid side, in
scenarios where volume and weight requirements are not strict, the
disadvantage of low energy density of ARFBs is no longer a limiting
factor. Its stronger security and scalability are competitive enough and
render it greater promise for the needs of long-duration and grid-scale
energy storage than LIBs. Secondly, although the cost of ARFBs is
currently higher than LIBs, the emerging low-cost ARFBs and the effect
of large-scale commercial deployment suggest a trend of fast
cost-reducing. Fig. 1 shows the components and working principle of a
typical redox flow battery (RFB). The conventional RFB consists of the
stack unit, electrolyte, external storage tanks, circulation pumps, and a
management and control unit. The electrode does not undergo redox
reactions itself, which only provides sites for electrochemical reactions.
Generally, the redox species is dissolved in the electrolyte and stored in
two tanks respectively, which are circulated through a peristaltic pump.
Unlike other batteries, this design allows for the separation of electro­
chemical reaction sites (electrodes) and the storage of active materials in
space. The battery power rating (electrode size) and capacity (tank size)
are designed to be relatively independent which provides advantages
such as excellent scalability, flexible modular designability, simple
thermal management, and high security [15].
The cost-effectiveness of ARFBs depends on the material cost and the
cycle life cost. The latter depends on the fading rate and maintenance of
active species as well as other components [16,17]. Specifically, as
shown in Fig. 1, the cost of ARFB mainly includes three parts that must
be systematically considered for comparison: active materials (energy
cost), power stack (power cost), and the operation and management
(O&M) cost of the equipment. The sum of energy and power costs is also
referred to the initial investment cost, which is mainly determined by
the bills of material cost [18]. Taking the widely used all vanadium
redox flow battery (VRFB) as an example, the system with a 4-h
discharge duration has an estimated capital cost of $447 kWh− 1, in
which the electrolyte and membrane account for 43% and 27% of the
total cost, respectively [19–21]. For electrolyte, the cost between
different systems can be reflected by the chemical price of active species,
e.g. K2S2, ZnO, K4Fe(CN)6•3H2O is 0.5, 1.3, 2 US$ kg− 1, respectively,
while the VOSO4•4H2O is 10.2 US$ kg− 1 which greatly increases the
initial cost [22].
Therefore, the path to reduce the cost of ARFB is mainly considered
from the following aspects: a) developing low-cost chemical materials
and battery stacks used in the RFB system; b) improving the physical and
chemical properties of the components for better efficiency, e.g. the
Fig. 1. Schematic illustration of a typical RFB and cost analysis. (abbreviations:
cost of power system (Cp), cost of balance-of-plant components (Cbop), the
addition to the investment cost to reach the system price (Cadd)).
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Journal of Power Sources 601 (2024) 234242
conductivity and selectivity of the membrane, the reaction activity of
active species, and the catalytic activity of the electrode; c) promoting
the cycling stability of the electrolyte, electrode, and membrane
materials.
In this review, we provide a brief introduction and overview of a low-
cost ARFB with a variety of active materials, by evaluating the electro­
chemical performance in terms of efficiency, energy density, power
density, and cycle stability. The key metrics affecting battery efficiency
are analyzed, followed by mitigation strategies and their benefits.
Finally, we provide perspectives on the future direction of the devel­
opment of high-efficiency and low-cost ARFBs.
2. Performance evaluation method of ARFBs
With the development of grid-scale EES, a variety of ARFBs have
been proposed. However, the electrochemical performance is varied due
to the different nature of the active materials. For example, the limited
solubility of K3[Fe(CN)6] in an aqueous medium leads to the relatively
low energy density of iron-based ARFBs [23,24] while the severe
crossover and slow redox kinetics of polysulfide lead to insufficient ef­
ficiency though it is highly soluble in aqueous media [25]. The inno­
vation of materials and structural optimization has been committed to
improving the performance of ARFBs, and a great deal of experimental
and simulation data has been demonstrated. It is very important to
evaluate the performance data of flow cells reliably and accurately.
Therefore, the establishment of a scientific and reasonable performance
evaluation method is the basis of battery research. Next, we will discuss
the fundamental attributes and performance parameters that are typi­
cally encountered in conventional battery performance testing methods
and analyze the main influencing factors.
2.1. Charging and discharging test
The charging and discharging test is a common method to evaluate
the performance of ARFBs [11]. The protocols for charging and dis­
charging tests commonly used in batteries are constant current and
constant voltage settings, of which the processes may repeat for multiple
charge/discharge cycles. During the test, various performance parame­
ters can be obtained, which restrict and influence each other, such as
capacity, coulombic efficiency (CE), voltage efficiency (VE), energy ef­
ficiency (EE), capacity utilization (CU), and capacity retention (CR)
[26]. The definition, calculation, and influencing factors of various
performance parameters are listed in Table 1. For the test of constant
current, the battery is first fully charged using a constant current. Once
fully charged, the battery is then discharged at a constant current. Each
reduction/oxidation half-cycle ends when a prescribed cell over­
potential is reached. However, because of high mass transport over­
potentials at the extreme state of charge (SOC) values, as well as the time
lag between the attainment of a particular SOC value in the cell and its
attainment in the reservoirs, less than 100% of the actual capacity is
accessed before the switching occurs. For the test of constant voltage,
where each half-cycle ends only after the reduction/oxidation current
has become negligible, at which point close to 100% of the available
charge is expected to have been extracted. This is strictly true if the
chosen potential limits provide large enough overpotentials to access
essentially 100% of the electrolyte capacity and side reactions at those
limits are negligible. In most studies, flow cells comprising two elec­
trolytes separated by an ion exchange membrane are used for per­
forming cycling tests. The reactant of interest usually acts as the
capacity-limiting side (CLS) with a relatively lower initial capacity of
active species.
The capacity of an ARFB is defined as the amount of charge (Ah)
stored in the electrolyte of CLS, as described in Eq (1).
nCF ( )
Cap = Ah L− 1 (1)
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Z. Hou et al. Journal of Power Sources 601 (2024) 234242

Where n is the number of transferred electrons involved in a redox
process, C is the concentration of redox species, and F is the Faraday’s
constant. The capacity is typically measured in ampere-hours (Ah) or
milliampere-hours (mAh). CE is the ratio of discharging capacity to
charging capacity which is used to measure the reversibility of the redox
reaction. Decomposition, crossover, and dendrite formation of active
substances on the CLS will cause capacity loss, which then affects CE and
CR. In addition, the self-discharge behavior on the CLS and the occur­
rence of irreversible side reactions will reduce the CE [27].
The energy density of the cell, as one of the most significant pa­
rameters for EES devices, is determined by Eq 2
Cap U0
Energy Density =
μv
Where Cap is the capacity on the CLS, U0 is the voltage of a single cell, μv
is the volume factor (μv = 1+smaller capacity/larger capacity of the
electrolyte). It can be seen that the capacity is related to the concen­
tration of the redox-active species, and U is determined by the redox
potential of the active species in anolyte and catholyte. So the energy
density is determined by the solubility and the redox potential of the
active species.
VE is the ratio of the mean discharging voltage over the mean
charging voltage at a constant current. EE is the ratio of discharge en­
ergy over charge energy at a certain current density, which also equals
the product of CE and VE. CU is the ratio of achieved capacity over
theoretical capacity. VE, EE, and CU are all affected by polarization and
current density. In general, smaller battery resistance and lower current
density will increase VE, EE, and CU. The capacity decay rate is the
capacity decay in percentage over a total test duration in terms of cycle
number or time which is used to evaluate the cycling stability. The CE,
VE, EE, CU, and CR should be considered comprehensively when
comparing the performance of flow batteries.
to a slow electrochemical reaction of the electrode. Vohm is ohmic in­
ternal resistance, which consists of the contact resistance between the
ion conducting membrane, electrode, and bipolar plate. Therefore, a
membrane with high ion conductivity is in urgent need [29]. Vtranst is
the internal resistance of concentration polarization caused by the
diffusion speed of products and reactant is far lower than that of a
chemical reaction.
The flow battery is mainly composed of two parts: an energy system
and a power system. In a flow battery, the energy is provided by the
electrolyte in external vessels and is decoupled from the power. The
power density stands for power per unit area that the battery can supply,
which is calculated by Eq 3
(2) IVcell ( )
Power Density = mW cm− 2 (3)
A
where I is the discharge current, Vcell is the output potential, and A is the
active surface area of an RFB, which is normally determined by the
effective area of the electrode. The power density is affected by many
complicated factors such as the battery voltage, conductivities of redox
species and separators together with the redox kinetics of the active
species on electrodes. Notably, operation factors including temperature,
flow rate, and flow field will also play a great role in the output of power
[26].
3. Cost analysis and application of low-cost ARFBs
3.1. Cost analysis of each component of ARFBs
The cost of flow batteries is also an important evaluation criterion.
LCOS includes all cost elements in the discharge life of the EES system
and quantifies the discounted cost per unit of discharge. Therefore,
LCOS is often used to evaluate the economic benefits of different EES
technologies. LCOS is calculated using eq. (4).

2.2. Polarization test ∑

N ∑
N
Charging cost
investment cost + O＆M cost
(1+r)n
+ (1+r)n
+ end(1+r)
of life cost
N+1

LCOS = n n
(4) [10]
VE and power density are affected by battery resistance. So an in­ ∑
N
EDischarged
crease in polarization can cause a decrease in VE and power density, n
(1+r)n

affecting the performance of the battery [28]. Battery polarization

It assumes all investment costs are incurred in the first year and sums
mainly includes electrochemical polarization, concentration polariza­
ongoing costs in each year (n) up to the system lifetime (N), discounted
tion, and ohmic polarization. Vact is the internal resistance of electro­
by the discount rate (r). The investment cost of RFBs mainly includes the
chemical polarization that deviates from the equilibrium potential due

Table 1
The parameters of RFBs to evaluate the electrochemical performance.
Definition Illustration Influence factor

GCD test
Coulombic CE = Qdischarge/Qcharge The ratio of discharge capacity over charge capacity Proton selectivity of ion exchange
Efficiency (conduction) membranes
Voltage VE = ‾Ed/‾Ec The average voltage of the discharge voltage divided by the Internal resistance of ion exchange
Efficiency average voltage of the charging voltage (conduction) membrane and stack
Energy EE = CE × VE The ratio of discharge energy over charge energy at a certain
Efficiency current density. The product of coulombic efficiency and
voltage efficiency
Capacity CU = Qa/Qt The ratio of actual capacity over theoretical capacity Voltage efficiency
Utilization
Capacity decay =(1－QN/Q1)/N Capacity decay in percentage over a total test duration cycle Comprehensive performance
rate number(N) or time(D).
D 1
=(1－Q /Q )/D
Polarization test
V act The potential deviates from the equilibrium potential Low operating current density
due to the slow electrochemical reaction of the
electrode.
V ohm Contact resistance between ion conducting film, Medium operating current density
electrode, and bipolar plate
V trans The diffusion speed of products and reactants is far High operating current density
lower than that of chemical reactions, concentration
polarization
Power density P––(I × Vcell)/A (mW cm− 2) Power output per membrane area at a certain SOC Battery polarization and voltage

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Z. Hou et al. Journal of Power Sources 601 (2024) 234242

cost of power and energy systems. O&M cost refers to the cost of oper­ Table 3
ation and maintenance of materials and equipment over its lifetime. The The performance and cost of various batteries (iron-chromium redox flow bat­
charging cost is often affected by electricity price over time, which is the tery (ICRFB), zinc-bromine redox flow battery (ZBRFB), polysulfide-
same for different technologies and thus can be set to zero for conve­ polybromide redox flow battery (PSB)).
nience. End of life cost refers to all the costs incurred to treat and recycle EES Energy Power density Cycle life Cost($
at the end of the life cycle of an EES. The energy cost includes the cost of technology density(Wh (W L− 1 KWh− 1)
L− 1)
the active material, salt, solvent, and storage tanks. In aqueous systems,
due to the low cost of solvent and salt, energy cost is mainly determined VRFB 25–35 ＜2 10000–13000 400
by the active materials as well as the storage tanks. Therefore, the energy ICRFB 13–30 10–20 ＞10000 620
ZBRFB 30–65 5000–10000 340–1350
cost of flow batteries with different types of active materials varies
＜25
PSB 20–30 ＜2 2000–2500 150–1000
greatly [18]. For example, the cost of vanadium electrolytes is 10.20 US LIB 200–500 1500–10000 1500–4500 200
$ kg− 1, which accounts for about 35% of the total cost of the battery [22, Pb-Acid 50–90 10–400 2000–4500 100–400
30]. Whereas, iron costs only 0.42 US$ kg− 1 [31], zinc costs only 1.90 Ni–Cd 15–150 80–600 2000–2500 800–2400
Na–S 150–300 140–180 2500–4500 300–500
US$ kg− 1 [32], and sulfur costs 0.29 US$ kg− 1, attributed to their nat­
ural abundance. The power cost consists of Cp, Cbop, and Cadd. Cost of
electrodes, membranes, end plate, collector, bolt, and gasket are and ensures long-term durability [34]. There are some issues with
included in Cp. Power conditioning equipment, controls, sensors, VRFBs, although they can offer distinct advantages compared to other
pumps, pipes, fans, valves, and heat exchangers are included in Cbop. flow battery systems. Due to the high cost of vanadium, vanadium-based
Cadd includes factors such as labor, depreciation, overheads, and security flow batteries lack economic advantages. The cost of vanadium elec­
deposits. Table 2 lists the cost of each component. Apparently, the use of trolyte stands at 10.2 US$ kg− 1, constituting approximately 35% of the
inexpensive electrolytes, electrode materials, and membranes can total battery cost. Similarly, the stack cost, encompassing ion exchange
reduce costs on the condition that the low-cost material exhibits similar membrane and electrode materials, accounts for another 35% of the
stability and efficiency. The performance and cost of various ARFBs and overall cost. Moreover, the initial installation cost is substantial,
other commercial batteries are summarised in Table 3. resulting in a total battery cost ranging from 433 to 640 US$ kWh− 1
Costs can also be reduced by improving the performance of RFBs [22]. Furthermore, the development of this technology has been
such as energy density, power density, and cycle life. The use of redox- hampered by solubility issues and suboptimal redox reaction kinetics.
active species with fast kinetics and low viscosity, electrolyte and Therefore, a lot of research has been carried out to reduce the cost of
membrane with high ionic conductivity, current collector with good VRFBs by changing the composition of the electrolyte, membrane
conductivity, and suitable flow field design can reduce battery over­ properties, electrode materials, etc. To improve the ionic conductivity,
potential to improve power density and energy density. As a result, the researchers often use sulfuric acid, hydrochloric acid, phosphoric acid,
size of both the stack and the electrolyte storage tanks can be cut down, and other concentrated acids as the supporting electrolyte. Wei et al.
which in turn reduces the cost of RFBs [22,33]. As for the life-span cost, [35] assembled silica in situ on the nanofiltration membrane surface and
the selection of redox substances, membranes, and electrodes with high pores to improve the ion selectivity and conductivity of the membrane in
stability can also improve the durability of RFBs, thereby reducing life the VRFBs. The ionic conductivity determines the VE of the cell, and the
cycle costs [16]. selectivity of the membrane determines the CE of the cell according to
the analysis of cell polarization behavior. To achieve high selectivity and
3.2. Key redox pairs for the development of low-cost ARFBs high conductivity of active ions, Li’s team [36] carried out the design of
the composite membrane by introducing the polyamide layer in the
3.2.1. Vanadium-based ARFBs porous membrane. The results show that the porous membrane can
VRFBs are the most developed and widely used flow batteries to date, achieve high conductivity and ion selectivity, which improves the CE
with an energy density of about 15–25 Wh L− 1, an energy efficiency of and power density of the cell. At present, graphite felt and carbon felt are
more than 80%, and a cycle life of more than 200,000 cycles [30]. The commonly used in flow batteries [37,38], however, their catalytic ac­
Schematic diagram and electrochemical profile of the ARFBs are shown tivity of electrochemical reaction of vanadium species is limited. Intro­
in Fig. 2. The VRFBs use the same elements in catholyte (VO2+/VO+ 2) ducing catalysts such as carbon materials [38,39], metals [40–42], and
and anolyte (V3+/V2+), which serves to relieve the issue of crossover, metal oxides [43–45] on the electrodes, and acid [46] or heat treatments
[47] have been investigated to improve electrochemical reaction ki­
Table 2 netics of vanadium species. Oxygen-functionalized single-walled carbon
The relevancy of key indicators, components, and costs of RFBs. nanotubes, as a superior electrocatalyst for the positive Br− /Br−3 couple
Criteria Component Essential factor Cost (US$ m− 2)
of the V/Br battery, can facilitate the reaction kinetics due to the for­
mation of active oxygen-containing functional groups on the surface,
Energy Electrolyte Redox potential Energy cost
which increase the effective surface area and catalyze the electron
density solubility
Power Electrode material Current density 10–30 transfer processes [48].
density (carbon fiber felt) Electrical
conductivity 3.2.2. Zinc-based ARFBs
Active site The study of zinc-based batteries can be traced back to the 70s of the
Membrane Selectivity 500
(fluorinated) Ionic conductivity
20th century, which mainly includes zinc-iron (Fe3+/Fe2+, 0.77 V vs
Membrane (fluorine- Stability 25 SHE), zinc-air, zinc-iodine (I− /I3− , 0.536 V vs SHE), zinc-nickel, zinc-
free) bromine (Br2/Br− , 1.087 V vs SHE), zinc-organic RFBs, etc [53–56].
Stack (End plate, × 47 Zinc-based flow batteries have a much lower chemical cost (1.9 US$
collector, bolt)
kg− 1) than VRFBs. Besides inherent safety and stability, the materials in
Pipeline (Piping and flow rate Fixed cost
Pumps) zinc-based ARFBs are abundant, which has always been the focus of
Cycle life × Stability Inverse research on EES technology [30]. Unlike other redox active species, zinc
proportional anodes can be applied over a wide pH range.
Others O&M cost Corrosivity and pH Determined by According to the pH environment, zinc-based ARFBs are divided into
Replacement interval cycle stability the system
alkaline, acidic, and neutral systems. The reactions of the zinc anode in
cost

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Z. Hou et al. Journal of Power Sources 601 (2024) 234242

Fig. 2. The schematic diagram and electrochemical profile of the various ARFBs. (a) Demonstration (b) CV curve (Reproduced with permission from Ref. [49]) (c)
Voltage profile (Reproduced with permission from Ref. [20]) of VRFB. (d) Demonstration € CV curve (Reproduced with permission from Ref. [50]) (f) Voltage profile
(Reproduced with permission from Ref. [51]) of ZIRFB. (g) Demonstration (h) CV curve (i) Voltage profile (Reproduced with permission from Ref. [31]) of AIRFB (j)
Demonstration (k) CV curve (l) Voltage profile (Reproduced with permission from Ref. [28]) of polysulfide-polyiodide redox flow battery (PSIRFB) (m) Demon­
stration (n) CV curve (o) Voltage profile (Reproduced with permission from Ref. [52]) of DHPS-iron RFB.

different environments are as follows [57]:
2+ −
Neutral or acidic : Zn + 2e ⇌Zn
Alkaline : Zn(OH)2−4 + 2e− ⇌Zn + 4OH−
In alkaline zinc-based ARFBs, zinc and ferricyanide are generally
used as active substances in the negative electrolyte and positive elec­
trolyte, respectively [58,59], which offer relatively low electrolyte cost
and a high open-circuit voltage (OCV) of up to 1.74 V. In the discharged
state, the negative electrode side is oxidized from zinc metal to basic
zincate solution, while the positive side is reduced to ferrocyanide by
(5)
ferricyanide. Compared to ferricyanide in alkaline media, Fe2+/Fe3+
and Br− /Br2 in acidic electrolytes have a higher solubility and thus
(6)
potentially higher energy density. However, in an acidic zinc-iron redox
flow battery (ZIRFB), the acidity of the solution will cause the corrosion
of zinc, the hydrolysis of the Fe2+/Fe3+, and hydrogen evolution re­
actions (HER). For acidic systems with buffer solution (e.g. HAc/NaAc),
the pH environment of the electrolyte can be maintained between 2–6,

5
Z. Hou et al.
and high CE can be achieved [60]. The poor reversibility and insufficient
kinetics of Br− /Br2 lead to a low power density although ZBRFB has a
high energy density and a low cost. In addition, the formation of zinc
dendrite will limit its cycling stability [61,62]. Compared with alkaline
and acidic systems, zinc generally forms an ARFB system with organic
substances in neutral environments, such as zinc-TEMPO, and zinc-poly
(TEMPO), which is mild and has lower requirements for ion membranes
and other components. The neutral ZIRFB also has been reported. ZnBr2
and FeCl2 were used as active species and Fe2+ inhibits hydrolysis by
complexing glycine [63]. Furthermore, the complexation of bromide
ions to zinc ions in neutral electrolytes can greatly enhance the revers­
ibility of zinc redox pairs [64].
Considering that the area capacity of zinc-based ARFB is limited by
electrodes due to the plating/stripping of the zinc, the energy is no
longer decoupled from power. In addition, zinc dendrite/accumulation
is also one of the key problems [65]. In the process of charging, the zinc
dendrite may puncture the membrane and cause the battery short cir­
cuit. During the discharging process, the accumulation of unstripped
zinc on the membrane will increase the cell resistance. The accumula­
tion issue of zinc dendrites in alkaline conditions is more serious than in
acidic and neutral conditions. The increasing concern for the above
problems has driven the research on the surface modification of elec­
trode materials, the rational design of membranes, the concentration
optimization of electrolyte solution, and the introduction of additives.
In terms of the modification of electrode materials, the direct contact
between the bulky electrolyte and the active zinc anode is prevented to
increase the over-potential of HER and block the charge transfer path
from metal zinc to water molecules. To eliminate the zinc dendrites, we
should promote the transfer of ions and electrons on the anode surface,
achieve a uniform electric field and concentration distribution, reduce
the local current density, and reduce the concentration or diffusion
polarization. Based on these ideas, the mitigation strategies related to
the anode mainly include the construction of protective layer on the
surface of the electrode material and the structural design of the zinc
metal anode [66,67]. The protective layer can inhibit the direct contact
of the electrolyte with the zinc anode and inhibit the corrosion of the
zinc group, especially in the weak acidic or high-concentration alkaline
electrolyte. At present, the reported protective layer materials mainly
include metal (In and Pd) [66,68,69], metal compound (ZnS, TiO2,
CaCO3, ZrO2) [70,71], carbon material (activated carbon, carbon
nanotubes, MOFs) [67,72], etc. In terms of ionic membranes, it mainly
aims at modifying the current commercial membrane or inducing Zn
uniform deposition to circumvent the challenges of zinc dendrites [65,
73–75]. In addition, the composite film has a stronger mechanical
Fig. 3. The historical developments and chemical price comparison of various ARFBS. Reproduced with permission from Refs. [78–81]. (Abbreviations: AIRFB for all
iron redox flow battery).
6
Journal of Power Sources 601 (2024) 234242
stability to prevent penetration by the dendrite [76], improving the
service life of the battery. The modification of the electrolyte includes
the optimization of zinc salt and the use of additives, which can reshape
the solvation structure and inhibit the zinc dendrites. Additives such as
nicotinamide [32] can reshape the solvation structure of Zn2+, and N, N,
N′ N’-Tetra(2-hydroxyethyl) ethylenediamine [77] slows down the dy­
namics of zinc deposition to prevent the formation of dendrites.
3.2.3. Iron-based ARFBs
Due to the natural abundance and low cost of iron (0.42 US$⋅Kg− 1),
iron-based flow batteries have received widespread attention in recent
years [31]. The first iron-based flow battery was proposed in the 70s of
the 20th century, with Fe (III)/Fe (II) and Cr (III)/Cr (II) serving as the
positive and negative active components, respectively and HCl as the
supporting electrolyte, which exhibited the battery voltage of 1.18 V.
The historical developments and chemical price comparison of various
ARFBs are shown in Fig. 3. However, many factors such as poor reaction
reversibility, HER side reactions, and crossover of active components
severely affect the EE of ICRFBs and pose great safety issues.
In recent years, several low-cost and high-stability iron-based redox
pairs have been developed including all-iron systems, organic-iron sys­
tems, zinc-iron systems, and sulfur-iron systems, etc. There are three
main trends: First, the use of complex ligands, such as phenanthroline,
triethanolamine, glycine, etc [82–84]; Second, the addition of polar
solvents that increase the solubility of iron complexes or reshape the
solvation structure [31]; Third, manipulation of the anions to regulate
the solubility and kinetics [85]. The use of suitable complexing agents
can effectively overcome the problem of iron ions precipitating as ferric
hydroxide at pH > 2. At the same time, the use of organic complex li­
gands can change the redox potential and the solubility of the active
species. A variety of organic ligands have been studied. For instance,
Robert F. Savinell [86] studied the ratio of glycine to Fe3+/Fe2+ as a
function of the pH of solution, showing that the optimized ratio of
glycine to Fe3+ is 1:1, at which high ligand solubility and a high redox
potential can be achieved at pH 2. Kwon [87] reported 2,2-bis(hydrox­
ymethyl)2,2,2-hyponitrotriethanol (BIS-TRIS) as an organic ligand of Fe
(BIS-TRIS) compound and constitutes an AIRFB coupled with [Fe
(CN)6]3− catholyte, which does not exhibit any side reactions after 250
cycles, exhibiting a capacity of 11.7 Ah L− 1, CE and CR of 99.8 and
99.9%, respectively.
Among all the ligands, cyanide exhibits great properties with
inherent chemical structure stability and facile kinetics, which makes
ferricyanide one of the most popular redox species for catholytes.
However, the energy density of ferricyanide-based batteries is relatively
Z. Hou et al.
low due to the limited solubility of ferricyanide (<0.8 M for K4[Fe(CN)6]
and <0.6 M for Na4[Fe(CN)6]). Based on the redox-targeting reaction of
[Fe(CN)6]4-/3- and Prussian blue (PB), Wang Qing’s team [88] designed
a redox-targeted flow battery with [Fe(CN)6]4-/3- as the redox mediator
and PB as a solid energy storage material to break the solubility limi­
tation of ferricyanide, which greatly improve the capacity of the system.
In addition, the solubility of ferricyanide can be improved by cation
exchange strategies. For instance, the solubility of Li4[Fe(CN)6] and
Li3[Fe(CN)6] is 2.32 M and 2.70 M, and the solubility of (NH4)4[Fe
(CN)6] and (NH4)3[Fe(CN)6] is1.60 M and 1.92 M, respectively.
3.2.4. S-based ARFBs
Sulfur is abundant on the earth, usually in the form of elemental
sulfur, sulfide, and sulfate. Among the existing active materials, sulfur
has a lower cost (0.29 US$ kg− 1). Elemental sulfur can react with soluble
polysulfides in aqueous solution to generate other polysulfides S2− x (x =
2–8). Sulfur species, i.e. polysulfides can achieve reasonably high
theoretical energy densities with low chemical costs due to their excel­
lent solubility in water and organic solvents, which can satisfy the
fundamental requirements of large-scale energy storage devices. In
addition, the redox process between various polysulfides is a multi-
electron reaction, thus delivering high theoretical capacity. Combined
with the above application advantages, polysulfides have been widely
used in energy storage systems, including metal-sulfur batteries, solar
cells, and RFBs.
All-liquid polysulfide-based ARFBs. The earliest research on
polysulfide-based flow batteries dates back to the 1980s [89]. Poly­
sulfide was paired with bromine, which has a high open-circuit voltage
(1.35 V). The chemical reaction and standard potential were shown in
equations (7) and (8). During the charging process, Br− was oxidized to
Br2 and complexed simultaneously to form Br−3 , while polysulfide was
reduced to a species with lower valence. The discharge process is the
opposite.
Cathode: Br−3 + 2e− ⇆ 3Br− E⊝ = 1.09 V vs. SHE (7)
Anode: S2−
4
−
+ 2e ⇆ 2S22 ⊝
E = − 0.48 V vs. SHE (8)
However, the self-discharge behavior caused by the crossover of the
active species is more serious, thus, the capacity decay is relatively fast.
The occurrence of HER and the precipitation of sulfur seriously affect
cycle stability. In addition, the solubility of Br− is low (0.21 M), as well
as the toxicity of bromine pollutes the environment, which has great
safety risks. Compared to Br2/Br− redox pairs, highly soluble I− /I−3 pairs
have a faster and highly reversible kinetic process [90], and the reaction
process is shown in Equation (9).
I−3 + 2e− ⇆ 3I− E⊝ = 0.54 V vs. SHE (9)
Polysulfide/polyiodide flow batteries exhibit lower initial invest­
ment costs (polysulfide/iodine: 85.4 US$ kWh− 1) under the same energy
density. The PSIRFB was assembled using high-concentration KI and
K2S2. The battery achieved high capacity utilization. Without capacity
decay, 50 stable cycles were realized [80].
Wei Wang et al. [25] reported a polysulfide/potassium ferricyanide
flow battery with an open-circuit voltage of 0.91 V. The neutral ferri­
cyanide and polysulfide were used as catholyte and anolyte, respec­
tively. Cheap redox materials and battery components with longer
service life can reduce investment costs. Organic compounds have the
advantages of structural diversity and flexible structural regulation,
posing great promise for energy storage applications. Taking the mo­
lecular of viologen as an example [91], the molecule shows strong
electrostatic attraction to polysulfides and inhibits the growth of lithium
dendrites, which helps to improve performance. During the redox pro­
cess, the molecule undergoes two single-electron reactions that provide
high energy density.
7
Journal of Power Sources 601 (2024) 234242
3.2.4.1. Liquid-gas polysulfide-based hybrid ARFB. Li et al. [92] sum­
marized the existing low-cost flow batteries. Among the known redox
active substances, sulfur has the lowest cost per stored charge, which is
only higher than water and air. This group then coupled oxygen re­
actions (oxygen evolution reaction (OER)/oxygen reduction reaction
(ORR)) with polysulfide chemistry to construct an exceptionally
low-cost system. With a solid electrolyte (LiSICON) used as the separator
of the flow battery, an acid-alkaline hybrid sulfur-air system was
investigated with 0.5 M Li2SO4/0.5 M H2SO4 and 1 M Li2S4/1 M LiOH as
catholyte and anolyte, respectively [92]. Based on the different con­
centrations of sulfur species, the energy density of the battery is 30~145
Wh L− 1 with the chemical cost of the active material is ~1 US$⋅kWh− 1,
which is the lowest level.
3.2.4.2. Solid-liquid polysulfide-based hybrid flow batteries. To improve
the energy density, some alkali metals with lower potential were paired
with a highly soluble negative electrolyte and separated by a glass-
ceramic membrane to avoid crossover of the active species. Lu’s [93]
group explored the electrochemical interactions of polysulfides and io­
dides, reducing the crossover of polyiodide ions and removing the use of
ion-selective ceramic membranes. In addition, the team developed a
highly reversible low-cost sulfur/manganese ARFB. The positive active
species of Mn2+/MnO2(s) has a high theoretical potential and a high
theoretical capacity (616 mAh g− 1) [94]. The battery used low-cost
active materials and circumvented the problem of zinc dendrites in
the Zn/MnO2 battery. The cycling stability under high areal capacity
(50–100 mAh⋅cm− 2) is greatly improved with the capacity retention rate
of 98% after 75 cycles at 50 mA cm− 2, which is much higher than that of
Zn/MnO2 flow batteries.
3.2.5. Organic-based ARFBs (AORFBs)
Electroactive organic molecules take advantage of natural renew­
ability, flexible designability, and sustainable production compared to
present commercial inorganic materials with uneven resource distribu­
tions [26]. The quinones were first reported as organic electroactive
material in an aqueous solution by Smith et al., in 2007 [95]. Afterward,
a series of organic molecules began to be used in ARFBs, mainly
including hydroquinone and quinone based on carbonyl (C– –O) bond
reaction, alloxazine [96], and phenazine [96,97] based on C– –N reac­
tion, viologens [98] and nitroxide radicals [99] based on doping reac­
tion. In recent years, soluble organic electroactive materials have been
widely regarded as promising candidates for low-cost and sustainable
ARFBs due to their facile molecular engineering with various functional
groups to adjust the solubility and redox potential [26].
However, the energy density of AORFBs is limited by the solubility
and redox potential of organic species in an aqueous solution, which has
been the main obstacle limiting practical application. By strategically
modifying the structures of molecules with hydrophilic hydroxyl or
sulfonate groups, the solubility of organic redox-active molecules in
aqueous electrolytes can be significantly promoted [52,100,101]. For
instance, 2,6-dihydroxyanthraquinone (2,6-DHAQ) exhibits a solubility
over 0.6 M in 1 M potassium hydroxide (KOH) solution and 7,8-dihy­
droxyphenazine-2-sulfonic acid at its near-saturation concentration
(1.4 M) exhibits an operating voltage of 1.4 V with a reversible anolyte
capacity of 67 Ah L− 1 [52]. It is worth noting that the substituting
location, number of functional groups, and the species of its
counter-cation contribute to different solubility [102,103]. Alloxazine
modified by carboxylic acid (COOH) groups is proven to increase the
aqueous solubility and deliver a desirable shift in the redox potential
[104]. With the further introduction of carboxylic acid-doped carbon
nanotube (CA-CNT) catalyst for increasing the reactivity, the redox
reactivity of alloxazine-COOH can be improved greatly because of the
role of COOH within alloxazine-COOH as a proton donor, the fortified
hydrophilic attribute of alloxazine-COOH, and the increased number of
active sites. Additionally, the use of additives, such as ethylene glycol
Z. Hou et al.
[105] and choline hydroxide [102] is another effective strategy to
improve solubility.
In terms of the redox potential governed by the energy levels of their
frontier highest occupied molecular orbital (HOMO) and lowest unoc­
cupied molecular orbital (LUMO), it can be effectively tuned through
structural functionalization. Specifically, the addition of electron-
donating groups leads to a negative shift of the redox potential while
the addition of electron-withdrawing groups leads to a positive shift
[106]. The redox potential of the organic molecules can also be influ­
enced by the solution environment due to the variation of the pH and
supporting electrolytes. For example, 2,6-DHAQ was reported by Lin
et al. used as the negative active material coupled with K3[Fe
(CN)6]/K4[Fe(CN)6] catholyte in basic KOH supporting electrolyte to
replace the toxic Br2/Br− in previously reported system. These OH−
groups on anthraquinone core structure are deprotonated to promote
solubility and get greater electron donation capacity, which contributes
to a 47% increase in OCV over previously reported systems, higher
solubility (>0.6 M at room temperature) and comparable kinetic rate in
1 M KOH to that in the previously reported acid solvent environment.
However, a key deficiency of most reported organic chemistries is
the utterly impractical capacity decay rates (>0.1 %/day) for RFB in­
stallations to reach the projected value due to the decomposition of their
organic constituents. Thus, the most challenging but imminent object in
developing AORFBs is the designation of highly stable redox-active
compounds at both discharged and charged states even at high con­
centrations (>0.5 M). The degradation of organic active species can be
attributed to both the type and structure of organic molecules and
exogenous factors (pH [107], temperature [108], oxygen tightness
[109] et al.). After the introduction of the ether-linked alkyl chains with
solubilizing carboxylate functional groups onto an anthraquinone core,
4,4’-((9,10-anthraquinone-2,6-diyl) deoxy) dibutyrate was six times
more soluble than 2,6-DHAQ at pH value of 12 and affords the lowest
ever reported capacity fade (<0.01%/day) for RFBs without rebalancing
[81]. Moreover, solvation regulation can also be a facile strategy to
extend the lifetime of organic active species. Xu et al. [110] incorporated
tetramethylammonium cations in the supporting electrolytes to interfere
with the solvation structure of DHAQ2− /DHAHQ4− anions, thereby
deactivating the chemical or electrochemical reduction of DHAHQ4−
and subsequent side reactions. The status of various redox flow batteries
Fig. 4. The status of various RFBs (VRFB, ICRFB, AIRFB, ZIRFB, PSIRFB) based
on radar diagram of key indicators. (Concentration, Power cost, Energy cost,
Open circuit voltage, Energy density).
8
Journal of Power Sources 601 (2024) 234242
is shown in Fig. 4.
Different from the abovementioned redox organic materials involved
in the protonation process in redox equilibrium, viologens are used
preferentially in neutral media thus the redox potential is independent
of pH. Radical species are involved as intermediates or products of the
reduction reaction. Methyl viologen (MV) dichloride, considered as
archetypical 4,4′ substituted bipyridine, was first reported by Wang and
Liu in RFBs with high solubility in a neutral aqueous solution (3 M in 1.5
M NaCl) [111]. When paired with nitroxide radicals or ferrocene de­
rivatives as catholytes, the constructed neutral AORFBs exhibit excellent
electrochemical performance [112,113]. Liu et al. [13] designed a
neutral AORFB composed of MV and ferrocyanide to achieve integrated
salt water desalination and energy storage. This technology offers op­
portunities to address both renewable energy production and water
scarcity through one device. TEMPO is a stable radical that can undergo
fast reversible redox transformation to corresponding oxoammonium
salt. But it still suffers from severe crossover due to the smaller size than
the ion-conductive channels in ion exchange membranes [111,114,
115]. Recently, Feng et al. [116] synthesized a class of molecularly
engineered ionic liquid-mimicking TEMPO dimers to address this chal­
lenge, one of which coupled with viologen derivatives demonstrated
unobservable capacity decay at 4 M electron concentration over 96 days
benefitted from membrane compatibility and a strong water coordina­
tion environment.
Last but not least, considering the self-decomposition characteristics
of organic molecules, physical organic chemistry, and advanced char­
acterizations that can get fundamental and practical insight at the mo­
lecular level is urgently required to further understand the degradation
mechanism of redox active molecules, thus developing higher-lasting
devices for large scale energy storage [117,118].
4. Main factors of loss and the mitigation strategies
Electrolytes, membranes, and electrodes serve as pivotal constituents
for RFBs. Their intrinsic characteristics significantly determine the
overall battery performance (Fig. 5). Consequently, interest in the
investigation of these materials has been steadily escalating. This section
provides a comprehensive assessment of the distinctive properties of
these components and an overview of current methods employed for the
improvement of CE and VE.
4.1. Key materials that affect CE
Electrolyte and CE: The CE can be affected by the self-
decomposition caused by the instability of the active substance and
the side reactions in the electrolyte. Self-decomposition is particularly
common in organic-based flow batteries, such as the bimolecular
degradation of viologen and its derivatives. The mechanism of self-
decomposition of organic species includes disproportionation, nucleo­
philic substitution, disproportionation, dimerization, and polymeriza­
tion, etc. The self-decomposition of active substances may lead to
permanent loss of active substances, resulting in capacity decay and
reduction of CE. Liu et al. [119] reported a highly stable AORFB using 1,
1′-bis[3-(trimethylammonium)propyl]-4,4′-bipyridinium tetrachloride
((NPr)2V) as the anolyte and 4-trimethylammonium-TEMPO chloride
(NMe-TEMPO) as a catholyte, with a high voltage of 1.38V and a capacity
retention rate of 99.995% per cycle. The viologen radicals can undergo a
dimeric degradation process. When compared to previously reported
methyl viologen (MV), [(NPr)2V]+ exhibited extraordinary stability
than [MV]+, which is explained by reduced dimerization caused by
higher charge repulsion from two extra positively charged propyl
ammonium pendant arms, as shown in Fig. 6c. Thus, its capacity
retention rate per cycle can reach 99.995%, and CE is close to 100%.
Side reactions and decomposition of solvents are also a major chal­
lenge, namely HER and OER in aqueous systems. For active substances
with a potential exceeding the voltage window of water splitting, the
Z. Hou et al. Journal of Power Sources 601 (2024) 234242

Fig. 5. Analysis of capacity loss mechanism in terms of efficiency in an RFB. (a) Main factors affecting CE and attenuation analysis; (b) Main factors affecting VE and
attenuation analysis.

Fig. 6. Various strategies to deal with low CE (a) The ammonium chloride-supported zinc-iodine redox flow battery (AC-ZIFB) using ammonium-based electrolyte.
Reproduced with permission from Ref. [53]. (b) Design concept of the bifunctional electrocatalysts. Reproduced with permission from Ref. [120]. (c) Proposed
favorable dimerization of [MV]+• and unfavorable dimerization of [(NPr)2V]+•. The red double arrows indicate charge repulsion between the pendent ammonium
groups. Reproduced with permission from Ref. [119]. (d) Charge-reinforced ion-selective membrane repels the negatively charged active materials (S2−
x and Ix ) from
−

crossover and alleviates free water migration. Reproduced with permission from Ref. [22]. (e) Microstructure of Paper Reinforced sulfonated poly ether ketone
(SPEEK) Membrane before and after Thermal Cross-Linking. Reproduced with permission from Ref. [121]. (f) The structural superiority of mixed matrix membrane
with highly anti-alkali microporous hollow spheres (denoted as DM-HM) under alkaline electrolyte. Reproduced with permission from Ref. [29]. (g) Schematic
illustration of Zn deposition induction mechanism. Reproduced with permission from Ref. [122]. (h) Multifunctional carbon felt-based electrode (NTCF) with
abundant N-rich defects for high-power density and long-cycle life ZBRFBs. Reproduced with permission from Ref. [62]. (i) The use of non-solvent-induced phase
separation (NIPS) with easily controllable parameter to create varieties of porous microstructures. Reproduced with permission from Ref. [123].

HER and the OER exert considerable influence, leading to reduced CE
and alterations in pH levels. In response to these challenges arising
within the electrolyte, a substantial array of enhancements has been
undertaken to ameliorate its performance. For instance, Jang et al. [120]
reported a promising electrocatalyst consisting of Ketjenblack (KB)
carbon with embedded bismuth nanoparticles (Bi–C). As shown in
Fig. 6b, Bi nanoparticles are uniformly incorporated into KB carbon by a
simple reduction process, and due to the synergistic effect of Bi and KB,
the formation of BiHx delays the reduction of H+ to inhibit hydrogen
evolution and provides an active site to enhance the Cr2+/Cr3+ redox
reaction. ICRFB with Bi–C catalyst as the negative electrode exhibited an
average CE of 97.4% during a charge-discharge cycle at room
temperature.
In hybrid flow cells, the formation of dendrites depletes the active
material and causes a decrease in CE. This problem can be resolved with
the proper design of electrolytes. Chen et al. [53] developed an AC-ZIFB
based on NH4I/NH4I3 redox pair design. The design of AC-ZIFB is shown
in Fig. 6a. The decoupling design allows electrolyte and counterions to
exist in anolyte and catholyte, respectively. NH+ 4 can reduce the for­
mation of zinc dendrites and promote the reaction kinetic process of
electrodes. The anionic properties of I− , I−3 , and I2Cl− prevent the
migration of cations through the cation exchange membrane. A constant
current cycle test with a charge-discharge current of 20 mA cm− 2 was
performed for both AC-ZIFB and conventional zinc-iodine redox flow
battery (ZIFB). The CE of AC-ZIFB remains at 99% over 100 cycles, while
conventional ZIFB has only 90% CE in about 50 cycles.
Membrane and CE: Crossover and damage of the membrane may
cause the reduction of CE. Crossover mainly refers to the transport of

9
Z. Hou et al.
active substances through the membrane leading to self-discharge or
irreversible reaction. Efforts have been made to improve the CE by
weakening the crossover of active species through the membrane. For
instance, Lu’s group [22] has created a charge-enhanced ion-selective
membrane that allows polyvinylidene fluoride (PVDF)-bound KB to
enter the Nafion membrane and reduce expansion and water absorption.
It delivered a strong polysulfide/polyiodide absorption capability to
capture and accumulate negatively charged anions, which electrostati­
cally repels active anions in the electrolyte, and thus decreases crossover
and migration of water/OH− , as shown in Fig. 6d. PSIRFB exhibited a
low capacity decay rate (0.0004% per cycle) over 1200 cycles, as well as
CE＞99.9% benefitted from the high hydrophobicity of PVDF, the high
absorption strength, and high conductivity of KB for
polysulfides/polyiodides.
SPEEK membranes are considered potential candidates to replace
expensive Nafion membranes due to their high selectivity of protons. To
overcome the poor mechanical/chemical stability of SPEEK membranes
in VRFB, Xi et al. [121] adopted a novel method by employing com­
mercial paper (copy paper, rice paper, and filter paper) as the SPEEK
scaffold and subsequently crosslinking the SPEEK by heat treatment. The
fibers of these commercial papers contain abundant hydroxyl groups,
which can interact with the sulfonic acid group of SPEEK to produce
hydrogen bonds (Fig. 6e), thereby enhancing the mechanical properties
of the membrane. Compared to the CE of the benchmark Nafion 115
membrane (92.8%), the optimized rice paper-enhanced SPEEK mem­
brane demonstrates an improved CE of 98.3% even at a high current
density of 120 mA cm− 2. Li et al. [29] developed a cost-effective
DM-HM. The daramic membrane used is a polyethylene (PE) porous
membrane, which can not only trap the highly anti-alkali inorganic
components in the PE matrix but also maintain the porous structure of
the PE polymer, thus, improving the wettability of the electrolyte. As a
result, DM-HM has strong mechanical strength to resist the growth of
zinc dendrite and excellent chemical and mechanical stability. At 80 mA
cm− 2, the alkaline ZIRFB displayed 500 stable cycles with a CE of 98.6%.
Electrode and CE: For the hybrid RFB, dendrite formation and loss
of solids are the two main problems that account for the low CE. The
formation and detachment of dendrites consume active substances,
which in turn leads to low CE, capacity attenuation, and even battery
lapse. Insufficient dissolution of solids resulting from redox reactions
involving solid-phase formation can cause electrode passivation and
reduced CE. At present, the main improvement approach for electrodes
includes thermal/chemical treatments, active site modifications, and
three-dimensional design. For instance, a multifunctional tin modified
three-dimensional carbon felt anode host material (SH) was engineered
as an anode by Li et al. [122]. The adsorption energy of Sn to zinc atoms
is higher than that of the pristine carbon felt host, which can provide
sufficient zinc nucleation sites and low nucleation overpotential for zinc
deposition. The strong interaction between Sn and Zn can effectively
avoid the aggregation of deposited Zn on the surface of the Sn layer and
avoid the fall-off of Zn from the electrode. With SH electrode design,
ZBRFB steadily demonstrated 120 cycles with an average CE of 97.2%.
Similarly, Li et al. [62] prepared a NTCF, which shows high catalytic
activity for the Br2/Br− reaction for ZBRFB. At the same time, the
reduced zinc atoms tend to be deposited uniformly in N-rich defects until
these defects are filled, which results in stable operation of ZBRFB at an
unprecedented high current density of 180 mA cm− 2 with a CE of
97.25% by using NTCF electrodes (Fig. 6h). In addition, under the high
area capacity of 40 mAh cm− 2, the zinc symmetrical flow battery can
steadily operate for 140 cycles at 80 mA cm− 2 exhibiting a CE of 98.93%.
As a general technique for creating tunable porous materials suited for
RFB electrodes, NIPS has been proposed [123]. It is shown that elec­
trodes with distinct microstructures and porosities can be produced with
different relative concentrations of scaffold-forming polyacrylonitrile to
pore-forming poly(vinylpyrrolidone). NIPS-derived electrodes made of
continuous, interconnected porous networks show great promise for
RFBs and provide a solid foundation for material innovation, offering
10
Journal of Power Sources 601 (2024) 234242
strong competition to the market’s present fiber-based electrodes.
4.2. Key materials that affect VE
VE is the ratio between the average discharging voltage and the
average charging voltage and it is mainly affected by battery resistance
and current density. Voltage hysteresis between the charge and
discharge caused by the potential difference between the two redox
molecules inevitably deteriorates the VE of RFB. The lower battery
resistance and smaller current densities usually deliver higher VE.
Additionally, the state of charge, operating temperature, and state of
health of the battery have been identified as the main parameters that
influence the VE [124]. Furthermore, VE can also be significantly
improved through the redox targeting reactions [125], the use of cata­
lysts, and the design of the flow fields [126].
Electrode and VE: The electrode provides the active sites for redox
reactions that occur in RFBs and can alter the kinetics of redox pairs. In
addition, the electrode structure can affect the concentration over­
potential, which in turn affects the VE. Insufficient redox reaction ki­
netics on the electrode lead to activation polarization, which further
reduces VE. The main strategy for increasing electrode activity is to
decorate the electrode with carbon-based or metal-based [127] de­
rivatives that can increase the active surface area or provide some cat­
alytic activity. Based on semiconductor theory, Zai et al. [128] designed
CoS2/CoS heterojunction nanoparticle materials using the hydrothermal
method. The heterojunction material contacting interface forms two
inverted spatial charge regions and excites a built-in electric field. CV
data shows that heterojunction materials (CoS2/CoS) exhibit minimal
redox peak voltage separation (0.10 V), compared to graphite felts and
monometallic sulfides. The uneven distribution of the charges within the
material enhances the charge transfer activity, and the reaction revers­
ibility of the redox active pairs can be significantly increased by the
adsorption of charged ions and the improvement of the electron-transfer
process. The PSIRFB using CoS2/CoS heterojunction materials as elec­
trodes was found to achieve stable cycling performance at 10 mA cm− 2
with a CR rate of up to 84.5%. The peak power of the CoS2/CoS electrode
battery reaches 86.2 mW cm− 2, which is much higher than the peak
power of the graphite felt electrode (8.9 mW cm− 2). The nitrogen-doped
graphene (N-G) reported by Barun et al. [129] also revealed the sur­
prisingly beneficial effects on three types of Hybrid RFBs, namely
hydrogen/vanadium cells, hydrogen/manganese cells (RHMnFC), and
polysulfide/air cells. Fig. 7b shows the polarization and power density
curves of RHMnFC. Using advanced materials such as nanomaterials can
also effectively improve the efficiency of ARFB. Park et al. [130] re­
ported an aqueous mixed zinc-manganese ARFB with a
double-membrane-based three-electrolyte using an alkaline zinc redox
couple (Zn/[Zn(OH)4]2− ) and an acidic manganese redox couple
(Mn2+/MnO2(s)). The CV curves of Mn2+/MnO2 on different electrodes
indicated that the Ipa/Ipc values on the bismuth nanoparticle embedded
carbon felt (BCF) with the metal ionic catalysts (MIC) (BCF-MIC) elec­
trode increase significantly, evidencing the enhancement of electro­
catalyst on the redox kinetics of Mn2+/MnO2 and exhibiting an EE of
89.8% at a current density of 15 mA cm− 2 (Fig. 7c). Additionally,
N-doped vertical graphene is in-situ grown on graphite felt via a
metal-free chemical vapor deposition method, which exhibits a high
specific surface area and remarkable catalytic activity [131]. The
vertical-standing nanostructure promotes the accessibility of vanadium
ions to electrode/electrolyte interfaces, effectively decreasing the mass
transport resistance of active species. The EE is significantly higher than
that of the original electrode.
Membrane and VE: The selectivity of the membrane is highly
correlated with the CE of the battery, while the conductivity of the
membrane is related to VE. The low conductivity of the membrane leads
to a decrease in VE, while the increase in conductivity often leads to a
decrease in selectivity. Thus, the trade-off between conductivity and
selectivity is especially important when improving the properties of
Z. Hou et al. Journal of Power Sources 601 (2024) 234242

Fig. 7. Various strategies to deal with low VE. (a) The CV of the catalysts deposited on glassy carbon in 4 mM NaI + 0.5 M NaCl solution and 0.06 M Na2S + 0.02 M S
+ 0.5 M NaCl solution at a scan rate of 50 mV s− 1. Reproduced with permission from Ref. [128]. (b) Polarization and power density curves using the same electrolytic
conditions with the exception of a higher hydrogen flow rate of 100 mL min− 1. Reproduced with permission from Ref. [129]. (c) CV of the catalytic effect of the
treated carbon felt with various methods. Reproduced with permission from Ref. [130]. (d) Schematic illustration of the membrane containing a hydrophobic poly
(vinylidene fluoride-total hexafluoropropylene) (PVDF-HFP) impregnated into a bacterial cellulose (BC) aerogel scaffold and interconnected proton conduction
pathways of the BC/PVDF-HFP membrane. Reproduced with permission from Ref. [132]. (e) The proposed degradation mechanisms of anions exchange membranes
(AEMs). Reproduced with permission from Ref. [133]. (f) Interleaved flow field (IFF) used in flow batteries. Reproduced with permission from Ref. [134]. (g) Ef­
ficiencies (CE and VE) of the PSIRFB cell under flow-mode in comparison with the VE achieved under the static mode at the same current density Reproduced with
permission from Ref. [80].

membrane. Improving the conductivity and chemical stability of the
membrane is of great significance to improve VE. Zhu et al. [132] re­
ported a highly conductive and selective RFBs membrane containing a
PVDF-HFP impregnated into a BC aerogel scaffold. The high proton
conductivity of the membrane stems from the intrinsic highly hydro­
philic network of BC fibrils, which serves as an osmotic pathway for
proton conduction. Meanwhile, its selectivity originates from the hy­
drophobic lamination on the BC scaffold, which functions as a barrier to
prevent the migration of vanadium ions and minimize crossover. In
addition, both BC/PVDF-HCP showed higher conductivity by comparing
the effectiveness of higher flow rates on battery performance.
In addition, temperature may also impact the efficiency of ARFBs.
Temperature affects the thermodynamics and kinetics of electro­
chemical reactions. Taking VRFB for example, higher temperature can
accelerate the kinetics of electrochemical reactions, reduce the viscosity
of electrolytes, enhance the H+ transmembrane transport, and improve
the solubility of V2+, V3+, and VO2+. In addition, high temperature can
reduce the OCV, boost the crossover, speed up the HER, and promote the
formation of V2O5 precipitation. Except for VRFBs, Lu’s team [135]
performed the test of the Sn(OH)2− 6 negolyte at 60 C. By increasing the
◦

with Nafion 115 membranes at different temperatures. At a current
density of 100 mA cm− 2, VRFBs using BC/PVDF-HFP membranes can
operate 300 cycles with an average CE of 97.56%, VE of 81.56%, and EE
of 79.49%. To balance the ionic conductivity and vanadium perme­
ability, Chen, etc. [133] have designed polysulfide-based side-­
chain-type AEMs (the side-chain-type AEMs having PTA groups and the
side-chain-type AEMs (PSf-c-PTA) with QA moieties) with a lower area
resistance and a relatively higher vanadium permeability, due to its
higher water uptake. The VRFB with PSf-c-PTA membrane delivered a
CE of 98.4% and an EE of 84.3% at a current density of 120 mA cm− 2.
Device design and VE: The device of the battery, such as flow
channel design, and flow rate will also affect VE. Typical flow field de­
signs used in RFBs are the serpentine flow field (SFF) and IFF [134]. The
structure of IFF on a porous electrode is shown in Fig. 7f. Flow rate also
has a great influence on VE. Li et al. [80] prepared a high-energy and
low-cos PSIRFB. The performance of the battery at different flow rates
(Fig. 7g) was tested, and the results showed that when the flow rate
increased within a certain range, the VE value increased because the
electrolyte flow reduced the mass transport loss of redox substances on
the electrode surface. However, once the flow rate exceeds a certain
value, the increase of the flow rate does not improve VE, as the balance
between mass transport resistance and the rate of redox reactions limits
temperature, the sluggish kinetics was improved. Furthermore, as the
temperature increased, the resistance and internal resistance of the
battery decreased [136]. Ding et al. [137] conducted redox targeting
flow battery tests at different temperatures and uncovered that the uti­
lization of solid materials increased with the increase of the activity of
redox species at high temperature.
Based on the potential cost-effectiveness and the development stage,
the roadmap of ARFBs is described in Fig. 8. The most maturely devel­
oped is VRFB, which is currently in the stage of commercialization.
However, the economic benefit of VRFB is poor because of the high cost
of vanadium. The industrialization of ICRFB is still in infancy and has
just entered the demonstration and verification stage of commerciali­
zation. ZIRFB is promising considering the cost and performance, which
is in the stage of system integration. In order to achieve the commer­
cialization of ZIRFBs, further breakthroughs are still needed in material,
chemistry, and battery design. The problem of poor power capability
and cycle stability of PSB has hindered its development, which is still in
the stage of engineering optimization. Despite the advantages of high
energy density and low cost, AORFBs are currently in the stage of
fundamental R&D. With breakthroughs in material modifications and
improvements in mass production, as well as the gradual improvement
of domestic and international industry chains, the LCOS for AORFBs is

11
Z. Hou et al.
Fig. 8. The roadmap of ARFBs.
expected to decline significantly. This could lead to further technolog­
ical breakthroughs and make them suitable for commercialization and
widespread application. The AIRFB is primarily still in the exploration
stage. Although it technically possesses the same intrinsic system
simplicity as VRFBs and has a low material cost, its development is
relatively immature when considering the battery performance, which is
mainly due to the lack of suitable active species.
5. Conclusion and perspective
To advance the widespread adoption of ARFBs, substantial research
efforts have been devoted to enhancing their performance while
simultaneously reducing costs. We comprehensively review key per­
formance metrics and cost assessment methodologies associated with
ARFBs. Achieving cost advantages is contingent upon the judicious
utilization of cost-effective materials, stack configurations, and the im­
provements of battery performance.
(1) The balance of the cost and performance. In practical appli­
cations, it is essential to adopt a holistic perspective that balances
cost considerations with battery performance. Based on the
standpoint of lifecycle levelized cost, energy cost-effectiveness,
power cost-effectiveness, and long-term stable cycling perfor­
mance are integral elements, rendering low-cost constituents
advantageous only when coupled with all three aspects.
(2) The challenges of ARFBs and paradigm-shift innovations. A
detailed cost and performance analysis of various ARFB variants
reveals persistent challenges, including low energy density,
sluggish kinetics, and instability of low-cost redox-active mate­
rials. To overcome those challenges, paradigm-shift innovations
such as new chemistries and new materials are pressingly needed
to go beyond conventional thinking.
(3) The characteristics of various ARFBs. Among current ARFB
configurations, the VRFB demonstrates the most stable perfor­
mance; however, its rapid expansion is hindered by the high cost
of active materials. Zinc-based ARFBs and iron-based ARFBs have
the advantage of low cost, but their development is seriously
hindered by dendrite formation and hydrogen evolution. The use
of organic ligands can alleviate the current problems of iron-
based ARFBs. Sulfur-based ARFBs have the advantages of low
cost and high solubility, but the electrochemical activity and ki­
netic reversibility of polysulfides are poor. AORFBs have attrac­
ted attention for their natural renewability and flexible
designability, but their low solubility and instability in aqueous
solutions are the biggest problems at present. From the perspec­
tive of material cost differences and kinetic expectations, we are
12
Journal of Power Sources 601 (2024) 234242
most optimistic about ZIRFB in the short term, and AORFB and
AIRFB in the long term.
(4) The factors affecting the performance. The factors affecting
the performance of ARFBs are varied. We present a comprehen­
sive overview of these determinants and corresponding
enhancement strategies, focusing on CE and VE. Factors affecting
CE encompass the reversibility of the electrochemical reaction,
the stability of active materials, and the membrane crossover
effect. VE, on the other hand, is subject to limitations arising from
sluggish reaction kinetics, membrane conductivity, and design-
related issues within the flow channel configuration.
Despite the existing challenges in ARFBs, there is promise for their
utilization in large-scale energy storage applications. To facilitate their
broader adoption, it is imperative to establish a rigorous and systematic
framework for evaluating ARFB performance. Moreover, ongoing efforts
are directed toward ameliorating current challenges in active materials
and optimizing various components, including electrodes, membranes,
and other devices, with the overarching goal of enhancing ARFB per­
formance and cost-effectiveness.
CRediT authorship contribution statement
Zhaoxia Hou: Writing – original draft. Xi Chen: Writing – original
draft. Jun Liu: Writing – original draft. Ziyi Huang: Writing – original
draft. Yan Chen: Writing – original draft. Mingyue Zhou: Writing –
original draft. Wen Liu: Writing – original draft. Henghui Zhou:
Writing – original draft.
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.
Data availability
No data was used for the research described in the article.
Acknowledgment
This work was supported by Beijing Municipal Natural Science
Foundation-Xiaomi Joint Project (L223011), National Natural Science
Foundation of China (51967020, 22108149). In addition, the work was
also supported by the Research and Development program in Shanxi
Province and Shanxi Energy Internet Research Institute. Mingyue Zhou
would like to thank the support from "the Fundamental Research Funds
Z. Hou et al.
for the Central Universities" (2462023QNXZ016).
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