REVIEW
Li-S Batteries
More Reliable Lithium-Sulfur Batteries: Status, Solutions
and Prospects
Ruopian Fang, Shiyong Zhao, Zhenhua Sun, Da-Wei Wang, Hui-Ming Cheng,
and Feng Li*
Lithium-sulfur (Li-S) batteries have attracted tremendous interest because
of their high theoretical energy density and cost effectiveness. The target of
Li-S battery research is to produce batteries with a high useful energy density
that at least outperforms state-of-the-art lithium-ion batteries. However,
due to an intrinsic gap between fundamental research and practical applica-
tions, the outstanding electrochemical results obtained in most Li-S battery
studies indeed correspond to low useful energy densities and are not really
suitable for practical requirements. The Li-S battery is a complex device and
its useful energy density is determined by a number of design parameters,
most of which are often ignored, leading to the failure to meet commercial
requirements. The purpose of this review is to discuss how to pave the way
for reliable Li-S batteries. First, the current research status of Li-S batteries
is briefly reviewed based on statistical information obtained from literature.
This includes an analysis of how the various parameters influence the useful
energy density and a summary of existing problems in the current Li-S battery
research. Possible solutions and some concerns regarding the construction
of reliable Li-S batteries are comprehensively discussed. Finally, insights are
offered on the future directions and prospects in Li-S battery field.
1. Introduction
The ever-increasing demand for economic and efficient energy
storage technologies has triggered the continuous exploration
of advanced battery systems.[1–4] Lithium ion batteries (LIBs),
based on lithium intercalation electrochemistry, have domi-
nated the battery market for portable electronic devices since
their successful launch in the 1990s.[5,6] At present the highest
energy density of a LIB is approaching its limit, but cannot
satisfy the requirements of emerging electric vehicles (EVs),
R. P. Fang, S. Y. Zhao, Dr. Z. H. Sun, Prof. H.-M. Cheng, Prof. F. Li
Shenyang National Laboratory for Materials Science
Institute of Metal Research
Chinese Academy of Sciences
72 Wenhua Road, Shenyang 110016, China
E-mail: fli@imr.ac.cn
Dr. D.-W. Wang
School of Chemical Engineering
University of New South Wales
Sydney, NSW 2052, Australia
Prof. H.-M. Cheng
Tsinghua-Berkeley Shenzhen Institute
Tsinghua University
Shenzhen 518055, China
DOI: 10.1002/adma.201606823
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hybrid EVs, and next-generation port-
able electronic devices.[7] In an attempt to
obtain higher energy densities, advanced
battery systems involving new electro-
chemistry and new cathode materials have
been under intense investigation in recent
years.[8–10]
Lithium-sulfur (Li-S) batteries, using
abundant elemental sulfur as the cathode
material, have become one of the most
promising candidates for next-generation
energy storage devices owing to their
high theoretical energy density and low
cost.[7,11–17] Different from the intercala-
tion electrochemistry of LIBs, Li-S bat-
teries involve a multi-electron-transfer
electrochemistry and have a high theo-
retical specific capacity of 1675 mAh g−1
based on the conversion reaction of S8 +
16 Li+ + 16 e− → 8 Li2S.[14,18] Considering
an average cell voltage of 2.2 V vs Li+/Li,
the specific energy density of a Li-S battery
has a theoretical value of 2567 Wh kg−1,
which is five times higher than that of
commercially available LIBs (387 Wh kg−1 for LiCoO2/graphite
batteries).[7] It has been estimated by Li-S battery manufac-
turers Sion Power and Oxis Energy that future Li-S batteries
are expected to have a practical gravimetric energy density of
400–600 Wh kg−1, more than twice that of state-of-the-art LIBs,
showing great potential for an EV to be driven ≈500 km between
charges.[11] The low cost of sulfur further provides such tech-
nology with economic advantages and makes it appealing for
large-scale energy storage for renewable energy sources, such
as wind and solar.[19]
Intensive research efforts have been made in the Li-S bat-
tery field, with publications growing exponentially in recent
years.[12] From the perspective of fundamental research, a long-
term target should be the formation of a basis for the future
commercialization of Li-S batteries with a high useful energy
density that at least outperforms state-of-the-art LIBs. However,
the market penetration of Li-S batteries has been impeded by
an intrinsic gap between fundamental research and practical
applications.[8,11] The primary focus of many Li-S battery papers
has been the design of advanced sulfur host materials, which
is inadequate for the evaluation of a Li-S cell. Although a high
specific capacity and good cycling stability have been achieved,
the values of these parameters have been obtained based on
the weight of sulfur in the electrode, and the corresponding
energy density based on the whole cell is often lower than that
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of LIBs.[15] Indeed, a Li-S battery is a complex device and its

performance is sensitive to a variety of design parameters such Ruopian Fang is currently a
as sulfur content, areal sulfur loading, electrode thickness, Ph.D student at the Institute
electrolyte type, electrolyte/sulfur ratio, and cycling conditions of Metal Research, Chinese
(for example, the potential window and cycling rate),[8,11,12] Academy of Sciences. She
all of which need to be considered and optimized in practical obtained her B.S. (2012)
applications. However, they are often ignored in the literature, in Materials Science and
resulting in a failure to construct reliable Li-S batteries for com- Engineering from Wuhan
mercialization. In fundamental research, the useful energy University of Technology
density of a Li-S cell must be considered and its feasibility for in China. Her research is
practical applications must be evaluated.[11] Therefore, studying focused on the design and
and optimizing cathode materials alone are not likely to lead to fabrication of novel carbon-
the successful Li-S battery commercialization. Attention needs based materials for high-
to be paid to the key design parameters in order to translate energy-density lithium-sulfur batteries.
fundamental research into commercial applications. These
include sulfur content and areal sulfur loading in the cathode, Hui-Ming Cheng is Professor
electrolyte type, and electrolyte/sulfur ratio. In addition, safety and Director of both the
concerns regarding the use of a lithium metal anode need to Advanced Carbon Research
be addressed before Li-S battery technology can be adopted for Division of Shenyang
large-scale commercialization. National Laboratory for
There are many review articles that summarize strategies Materials Science, Institute of
for the optimization of Li-S batteries and the resulting pro- Metal Research, the Chinese
gress.[14,19–22] Therefore, we do not intend to give another sum- Academy of Sciences, and the
mary here. Instead we shall try to provide a comprehensive over- Low-Dimensional Material
view of promising approaches for the construction of reliable and Device Laboratory of the
Li-S batteries from the perspective of the cell rather than only the Tsinghua-Berkeley Shenzhen
cathode materials. The fundamental scientific problems in cur- Institute, Tsinghua University.
rent Li-S battery research are discussed based on an analysis of His research activities focus on carbon nanotubes, gra-
the statistical information in the Li-S literature, and feasible solu- phene, other two-dimensional materials, energy storage
tions aimed at addressing these problems are discussed. Finally, materials, photocatalytic semiconducting materials, and
perspectives are considered with regard to producing more reli- bulk carbon materials.
able Li-S batteries with a rationally improved performance.
Feng Li is a Professor of the
Institute of Metal Research,
2. Electrochemistry and Challenges Chinese Academy of Sciences
of Li-S Batteries (IMR, CAS). He received his
Ph.D. in materials science
2.1. Electrochemistry at IMR, CAS (2001). His
main research interest is in
Sulfur has over 30 solid allotropes, among which the most nano materials for electro-
common and stable form is cyclic octasulfur (S8).[23] Figure 1 chemical energy storage and
shows a typical charge/discharge profile for a Li-S battery, it conversion.
can be seen that S8 undergoes compositional and structural
changes during the redox process, which involve the formation
of a series of soluble lithium polysulfide intermediates (Li2Sn,
3 ≤ n ≤ 8). Two obvious discharge plateaus are observed, cor-
responding to a solid (S8)→liquid (Li2Sn)→solid (Li2S2/Li2S) upper discharge plateau.[24] During the subsequent charging,
process with a gradual decrease in the sulfur chain length.[18] In Li2S is reconverted to elemental sulfur through the formation
the upper discharge plateau, S8 is first reduced to S82−, and sub- of intermediate polysulfides, resulting in a reversible cycle.
sequently to S62− and S42− with an average voltage of 2.3V (vs However, it should be noted that the theoretical capacity
Li/Li+), corresponding to a theoretical capacity of 418 mAh g−1 (1675 mAh g−1) of Li-S batteries cannot usually be achieved
(0.5 electron transfer per S atom).[14] Due to the high solubility under practical circumstances, and this will be explained in
of these long-chain polysulfides, the upper discharge plateau detail in the following sections.
shows fast reaction kinetics.[18] The lower discharge plateau
at 2.1 V (vs Li/Li+) corresponds to further reduction of poly- 2.2. Challenges
sulfides to insoluble Li2S2/Li2S, and the theoretical capacity is
1254 mAh g−1 (1.5 electron transfer per S atom).[14] Because of Despite the high-energy advantage of Li-S batteries, several
the conversion reaction between solid Li2S2 and Li2S, the reac- key challenges exist and need to be addressed for performance
tion kinetics during this stage are much slower than for the improvement and future commercialization.

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(1) The insulating nature of sulfur and Li2S:
Both sulfur and Li2S are insulating for electrons and lithium
ions, and this directly limits the electrochemical reactions and
results in low utilization of the active material. In the upper
discharge plateau, despite the fast solid-liquid reaction kinetics,
it is very challenging to achieve the theoretical capacity of
418 mAh g−1. It has been reported that even after repeated
cycles, unreacted sulfur still exists.[25] A uniform dispersion of
sulfur and good electrical contact with conductive additives are
required for the reduction of sulfur to long-chain polysulfides.
In the lower discharge plateau, because the conversion reac-
tion Li2S2 + 2Li+ + 2e− → 2Li2S involves a solid-solid process,
the polysulfides formed in the upper discharge plateau are
difficult to completely reduce to Li2S because of the sluggish
reaction kinetics.[26] Theoretically, the capacity ratio of the lower
discharge plateau to upper discharge plateau is expected to be
3,[19] but a value of ≈2.5 is more realistic. In practical condi-
tions, the incorporation of sulfur in a conductive matrix is usu-
ally required,[14,15,19,20] resulting in decreased specific capacity.
In addition, the common Li-S voltage profiles tend to show a
higher polarization in the lower discharge plateau voltage due
to limited kinetics for both electrons and lithium ions,[17,27,28]
which further results in a decrease in practical energy density.
(2) High solubility of intermediate polysulfides in the electrolyte:
Lithium polysulfides generated during the conversion reac-
tion are soluble in the most common organic electrolytes
used for Li-S batteries, which leads to some known problems,
including low Coulombic efficiency, fast capacity decay, and
high self-discharge rate.[18,29] The details of their influence can
be summarized as follows: 1) driven by the concentration gra-
dient force (from the cathode to the anode), the soluble poly-
sulfides migrate to the lithium anode where they are reduced
to insoluble Li2S, resulting in an irreversible loss of active
material and passivation of the anode; 2) during charging, the
migrating long-chain polysulfides are partially reduced to short-
chain polysulfides by the lithium anode, which then shuttle
back to the cathode driven by the electric field from the anode
to the cathode, causing the well-known “shuttle effect” with low
Figure 1.  A typical charge/discharge profile for a Li-S battery.
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charging efficiency; 3) the repetitive dissolution and redeposi-
tion of active material species leads to a rearrangement of sulfur
within the cathode, and this tends to passivate the cathode and
increase the impedance due to the inhomogeneous distribution
of insulating sulfur. Although the dissolution of polysulfides
causes many problems, it is, on the other hand, essential for
achieving high sulfur utilization. Since sulfur is not conduc-
tive, to ensure electron transport, which is a key factor during
the electrochemical process, the reduction of sulfur can only
take place on the surface of the conductive matrix. Due to the
continuous dissolution of polysulfides, the remaining sulfur is
exposed to the conductive matrix so that its reduction can pro-
gress. Therefore, the dissolution of polysulfides needs to be
rationally balanced and controlled to achieve both high sulfur
utilization and high cycling stability.
(3) The volume expansion going from sulfur to Li2S upon
lithiation:
The density of octasulfur (2.07 g cm−3) is higher than that
of Li2S (1.66 g cm−3), resulting in a large volume expansion
(≈80%) upon lithiation.[30] The repeated volume variation of the
electrode leads to pulverization of the cathode and the detach-
ment of sulfur from the cathode conductive matrix. It is dif-
ficult for the isolated sulfur to be used in the following electro-
chemical reactions due to loss of electrical contact, resulting in
a permanent capacity fade. In this regard, an appropriate void
space needs to be provided to accommodate the volume change
of the active material and preserve the structural integrity
of the cathode, which leads to a decreased volumetric energy
density of the cell. Indeed, due to the intrinsic low density of
sulfur, the volumetric energy density of Li-S batteries is not
expected to be much higher than that of state-of-the-art LIBs
(≈600 Wh L−1).[12] Therefore, the porosity of the electrode needs
to be controlled for a balance between the volumetric energy
density and performance.
(4) The use of a metallic lithium anode:
Lithium metal is an ideal anode for high energy density bat-
teries because of its high specific capacity (3860 mAh g−1) and
low reduction potential (−3.04 V vs a standard hydrogen elec-
trode).[31] However, the use of a metallic lithium anode is one of
the most challenging aspects for the commercialization of Li-S
batteries for the following reasons: 1) the formation of lithium
dendrites induced by an inhomogeneous distribution of cur-
rent density on the surface and a lithium ion concentration
gradient at the electrode/electrolyte interface causes safety con-
cerns due to the potential appearance of short circuits;[32] 2) the
repeated lithium plating/stripping process during cycling leads
to a large volume change and cracking of the lithium anode,
resulting in the formation of inactive “dead Li” that cannot par-
ticipate in the subsequent cycling and this lowers the utiliza-
tion rate of lithium;[12] 3) metallic lithium is known to be highly
reactive, and it reacts spontaneously with organic electrolytes
to form a solid electrolyte interphase (SEI), which is unstable
because of the large volume change during the lithium plating/
stripping process, resulting in the continuous irreversible con-
sumption of active lithium;[33] 4) as discussed above, due to the
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“shuttle effect”, the efficiency of the lithium anode is signifi-
cantly lowered due to the formation of a Li2S passivation layer
on its surface, which limits the cycling stability of the battery.[15]
Protection of the lithium anode or the exploration of alternative
anodes may be possible solutions to address these problems,
which we will discuss in the following sections.
3. Categories of Li-S Batteries
Based on the initial state of sulfur in the cathode, Li-S batteries
can be classified into four categories: elemental sulfur (S8),
short-chain sulfur, lithium sulfides, and catholytes. The typical
charge/discharge curves in the first two cycles for these four are
shown in Figure 2.
3.1. Elemental Sulfur (S8)
To improve the sulfur utilization and cycling stability of sulfur
cathodes, various strategies have been explored to design and
fabricate advanced sulfur composite materials by dispersing
sulfur in various conductive matrixes including carbon mate-
rials,[17,34–38] conductive polymers,[39] and conductive metal
oxides[40]/carbides.[41] In most cases, the sulfur still exists in
the form of cyclo-octasulfur (S8), and shows multi-step elec-
trochemical behavior with two discharge plateaus and the for-
mation of soluble polysulfide intermediates (Figure 2a).[17,34–36]
This type of sulfur cathode is the most widely studied system
because of the advantages of a potentially high sulfur content
in the cathode and a relatively high output voltage. Due to the
strong nucleophilic reactivity of polysulfide anions, this type
Figure 2.  Typical charge/discharge curves of a) elemental sulfur (S8), b) short-chain sulfur, c) lithium sulfide, and d) catholyte.
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of sulfur cathode is not compatible with the carbonate-based
electrolytes used for state-of-the-art LIBs because polysulfides
immediately react irreversibly with the carbonate-based sol-
vents on their formation.[42] Therefore, ether-based electrolytes,
typically with a mixture of dioxolane (DOL) and dimethox-
yethane (DME) as solvents, are used for elemental sulfur
cathodes, which enables the multi-step reduction of sulfur by
dissolving the polysulfide intermediates.[18] Due to the unavoid-
able polysulfide dissolution, considerable efforts must be made
to prevent the free migration of polysulfides to the anode. Wang
et al.[43] reported the pioneering work of elemental sulfur cath-
odes in 2008, with the use of sulfur-coated mesoporous carbon
as the cathode active material. In 2009, Nazar et al.[17] used
an ordered mesoporous carbon (CMK-3) as the sulfur host to
improve the electrical conductivity and trap the polysulfides,
resulting in an improved specific capacity and cycling perfor-
mance. Many other elemental sulfur cathode materials have
also shown improved Li-S battery performance, e.g., S/carbon
nanotubes[34] and S/TiO2.[30]
3.2. Short-Chain Sulfur
Short-chain sulfur is generally of two categories: smaller sulfur
molecules (S2–4)[37,38,44,45] and sulfurized carbon.[46–48] Smaller
sulfur molecules (S2–4) with a chain-like structure have at
least one dimension <0.5 nm, while cyclo-sulfur molecules
(S5–8) are >0.5 nm in at least two dimensions,[44] therefore the
smaller sulfur molecules can be accommodated in a micropo-
rous carbon matrix with a pore size of <0.5 nm.[37,38,45] In sul-
furized carbon, short sulfur chains are covalently bound to the
surface of a carbon matrix.[48] For example, Wang et al.[47] used
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elemental sulfur to dehydrogenate polyacrylonitrile (PAN), and
the -CN groups in the PAN form heterocycles with short sulfur
chains grafted onto the conjugated carbon to form sulfur-
ized PAN.[49] Different from the cyclic S8 molecules involving
solid-liquid-solid conversion reactions, short-chain sulfur is
discharged and charged entirely through a solid-solid phase
transition from S to the Li2S phase without the formation of
polysulfide intermediates.[37,48] Therefore, the upper discharge
plateau corresponding to the transition from S8 to S42− no
longer exists and only one single discharge plateau at ≈1.8 V
(S2–4→S2−) is observed in the voltage curves (Figure 2b).[37] In
this regard, short-chain sulfur is compatible with carbonate-
based electrolytes, and the polysulfide shuttle effect can be
completely avoided, leading to advantages of high Coulombic
efficiency and stable capacity retention.[50] However, this type
of sulfur cathode usually has a low sulfur content (usually less
than 50 wt%),[37,38,44–47] leading to significantly decreased prac-
tical specific capacity. What’s more, short-chain sulfur cathodes
have a low average voltage (≈1.9 V vs Li+/Li) compared to ele-
mental sulfur cathodes (≈2.2 V vs Li+/Li), which further lowers
the energy density.
3.3. Lithium Sulfide
As discussed above, the use of a lithium metal anode poses a
significant safety issue for the large-scale implementation of
Li-S batteries. In this regard, lithium sulfide (Li2S), the final
discharge product of sulfur, has been explored as an active
material in the cathode because fully lithiated Li2S can work
with safer lithium-free anodes (e.g., graphite, Si/Sn-based
anodes).[51–54] However, it is known that the electrochemical
activity of Li2S is even lower than that of sulfur, and a large
potential barrier (≈1V) exists at the start of charging for Li2S
so that a higher cutoff voltage (≈3.8 V) is required to overcome
this barrier and activate the Li2S (Figure 2c), resulting in a low
Coulombic efficiency for the first cycle.[54] However, the cou-
pling of Li2S and lithium-free anodes has rarely been studied
in literature. In addition, lithium sulfide cathodes are moisture
sensitive and need a dry and inert environment throughout
their fabrication and manipulation, which potentially impacts
industrial production.
3.4. Catholyte
Lithium polysulfide batteries were first reported by Rauh
et al. in 1979,[55] with dissolved polysulfides (catholyte) as the
starting active material (Figure 2d). A conductive electrode
(usually carbon materials) is required in this configuration,
and it also serves as a current collector for electron transport.[13]
Recently, several studies have shown that lithium polysulfide
systems provide better redox kinetics due to a more uniform
distribution of active materials, and the higher reaction activity
of liquid polysulfides over solid sulfur results in improved
sulfur utilization.[56–59] However, as the active polysulfides are
combined with the electrolyte, the mass of electrolyte in lithium
polysulfide batteries is significantly higher than that in the first
three types of Li-S batteries, and this contributes to the inactive
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mass and results in a decreased energy density. In practical
applications, lithium polysulfide systems show potential for use
in stationary flow batteries, and efforts must be made to mini-
mize the mass of the conductive current collector and increase
the effective sulfur concentration in the catholyte.
4. Statistical Overview and Analysis of the Current
Typical Research Results on Li-S Batteries
For Li-S batteries, the gap between fundamental research and
practical applications lies in the difference between materials
research and device design. A Li-S battery is an integrated
device, involving not only materials, but also electrode architec-
ture and cell engineering, and the energy density is one of its
most important parameters. For the materials research, atten-
tion is mostly focused on the sulfur utilization (specific capacity
based on the sulfur mass) and cycling stability of the active
materials. For electrode architecture and cell engineering,
design parameters, including the sulfur content, areal sulfur
loading and ratio of active to inactive components, play a key
role in determining the useful energy density, but are often
ignored in materials research, leading to the failure in con-
structing reliable Li-S batteries. Therefore, attention should be
extended from the materials to the whole cells with the above
design parameters taken into consideration. To obtain a high
energy density, besides high sulfur utilization and high output
voltage, the sulfur content and areal sulfur loading in the
cathode should be as high as possible, and the weight of inac-
tive components in the cell (e.g., current collectors, electrolytes)
needs to be as low as possible. In general, a reliable Li-S bat-
tery requires high energy density, high stability, high safety and
low cost, which involves the collaboration of materials research,
electrode architecture and cell engineering (Figure 3).
Because the energy density of a Li-S cell is determined by
all the above-mentioned factors, it is essential to have a com-
prehensive evaluation of them as they relate to papers on Li-S
Figure 3.  Requirements for reliable Li-S batteries.
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batteries published in recent years. On the one hand, an over-
view of the research status of Li-S batteries can provide guide-
lines for the future development in this field. On the other
hand, these parameters are not independent of each other, and
the connections between them are worth exploring to obtain a
better understanding of Li-S cell design. Here, 205 papers on
Li-S batteries from 2009 to 2016 have been selected for this
purpose.[17,25–28,30,34–41,45,46,60–248] They were selected according
to the following criteria: (1) papers studying the properties of
the sulfur cathode are preferred; (2) ≈60% have been published
since 2015; (3) the 30 most cited papers in the Li-S battery field
since 2009 are included. The information about active mate-
rials, sulfur contents, areal sulfur loadings, specific capaci-
ties, areal capacities, cycling performance, electrolyte to sulfur
ratios, and output voltage values are summarized and listed in
Table S1, and the results of statistical analysis of several key
parameters will be discussed in the following sections.
4.1. Sulfur Content and Specific Capacity
All the 205 papers provided information on sulfur content
(the sulfur weight fraction in the cathode). There are 267 data
concerning sulfur content and specific capacity, because several
papers list more than one sulfur content (Table S1).
In order to provide a reliable evaluation, sulfur contents
were calculated based on the weight of the cathode (not
including the weight of current collectors or interlayers). It is
worth mentioning that many publications only emphasize the
sulfur content in sulfur-containing composites, which is inad-
equate because the final sulfur content in the electrode, is lower
because of the addition of conductive additives and binders
during fabrication (except for freestanding electrodes). Espe-
cially for composite materials with high sulfur content, a large
amount of conductive additives is often added to the electrodes
Figure 4.  Statistical analysis of sulfur content and specific capacity: a, c) distributions from 2009 to 2014, b, d) distributions from 2015 to 2016.
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to improve their electronic conductivity and enhance the sulfur
utilization, which leads to significantly lowered sulfur con-
tents in the final electrodes. As displayed in Table S1, most
of the examined electrodes have sulfur contents in the range
41%–70%, but a few are below 40%, and several report values
lower than 30%. It is known that a low sulfur content directly
results in a lower specific capacity of the electrode. It can be
seen that the sulfur content in more than half the examined
papers is not satisfactory, in comparison with the active mate-
rial content in commercial LIBs (≈90%).[11] Distributions of
sulfur contents from 2009 to 2014 (Figure 4a) and from 2015 to
2016 (Figure 4b) show a tendency to higher values, however the
proportion of high sulfur contents above 71% is just 13.58%
even in 2015–2016.
In most papers, the specific capacity is given based on the
sulfur mass rather than the mass of the whole cathode, making
it difficult to compare different approaches reported in lit-
erature. Therefore, the specific capacities shown in Figures 4c
and 4d are given based on the electrode mass to obtain a more
convincing analysis (the specific capacities obtained at low cur-
rent densities were selected). Specific capacity is determined
by two factors: sulfur content and sulfur utilization, and the
detailed relationship between them is shown in Table S2. For
a high specific capacity, both high sulfur utilization and sulfur
content are needed; however, it is known that sulfur utiliza-
tion usually decreases with increasing sulfur content due to the
low conductivity for both lithium ions and electrons. There-
fore, sulfur content and sulfur utilization should be balanced
to achieve a high specific capacity. Typically, with a sulfur con-
tent of 70% and a sulfur utilization of 70%, a specific capacity
of 821 mAh g−1 can be achieved (Table S2). In Figure 4c, the
number of reported specific capacities below 500 mAh g−1 is
as high as 43.75% in 2009–2014, which decreases to 18.13%
in 2015–2016 (Figure 4d). However, over half of the examined
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data in 2015–2016 are below 700 mAh g−1, and the number of
reported specific capacities above 800 mAh g−1 is only 20.47%
(Figure 4d).
4.2. Areal Sulfur Loading and Areal Specific Capacity
The importance of areal sulfur loading and areal capacity needs
to be particularly emphasized. For LIBs, a typical areal capacity
of 4 mAh cm−2 is required for their use in EVs. Considering the
lower average voltage of Li-S batteries (2.2V) than that of LIBs
(3.5V), the areal capacity of Li-S batteries needs to be higher
than 6 mAh cm−2 to compete with the state-of-the–art LIBs.
The areal capacity is determined by both areal sulfur loading
and sulfur utilization, and the detailed relationship between
them is shown in Table S3, from which it can be seen that
with a low areal sulfur loading of 2 mg cm−2, the areal capacity
is only 3.35 mAh cm−2 even when 100% sulfur utilization is
achieved, indicating the importance of areal sulfur loading in
determining the areal capacity. With a typical sulfur utiliza-
tion of 70%, the areal sulfur loading needs to be improved to
at least 5 mg cm−2 to achieve an areal capacity of 6 mAh cm−2
(Table S3). Moreover, it is worth noting that, as shown in
Table S1, in some papers high sulfur contents are not accom-
panied by high areal sulfur loadings and high areal capacities
because of the small thickness of the sulfur cathode, which
make them unsuitable for practical uses in spite of their high
specific capacities.
In the 205 papers examined, 49 of 84 publications in 2009–
2014, and 106 of 121 papers in 2015–2016 provide informa-
tion about areal sulfur loading, resulting in a total of 213 areal
sulfur loading and areal capacity data, and results of the corre-
sponding analysis are shown in Figure 5. Most of the examined
Figure 5.  Statistical analysis of areal sulfur loading and areal capacity: a, c) distributions from 2009 to 2014, b, d) distributions from 2015 to 2016.
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data shows a low areal sulfur loading less than 2 mg cm−2, with
corresponding areal capacities mostly less than 2 mAh cm−2
(Table S1). Even in 2015–2016, the number of reported areal
sulfur loadings below 2 mg cm−2 is 56.58% (Figure 5b), and
corresponding areal capacities below 2 mAh cm−2 account
for 48.68% of the examined data (Figure 5d). For high areal
capacities above 6 mAh cm−2, the number of reported values
shows a small increase from 9.84% in 2009–2014 (Figure 5c)
to 14.47% in 2015–2016 (Figure 5d). It can be seen in Table S1
that even in the most recent publications in 2016, most areal
sulfur loadings are still below 2 mg cm−2, indicating that the
areal sulfur loading has not received enough attention despite
its significance. Generally, a high areal sulfur loading means an
increased electrode thickness and results in limited kinetics for
both lithium ions and electrons. Therefore, even if a high spe-
cific capacity can be achieved with a low areal sulfur loading, it
does not mean that a similar high performance can be obtained
with higher areal sulfur loadings in practical cells. Such elec-
trodes with low sulfur loadings have much lower gravimetric
energy densities than commercial LIBs, which is only reason-
able for reaction mechanism studies.
4.3. Electrolyte/Sulfur Ratio
Electrolyte to sulfur (E/S) ratio is a very important parameter
in Li-S cells. On the one hand, the electrolyte is an inactive
component, which is significant in determining the final
energy density of Li-S cells, as discussed in Figure 3. It has been
indicated that even with satisfactory sulfur contents and areal
sulfur loadings as well as high sulfur utilization, the real energy
density of a Li-S battery cannot outperform that of a commer-
cial LIB in the presence of an excessive amount of electrolyte.[11]
© 2017 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim
www.advancedsciencenews.com
Figure 6. Statistical analysis of electrolyte to sulfur (E/S) ratios from
2009–2016.
On the other hand, the amount of electrolyte has an influence
on sulfur utilization, cycling stability, and Coulombic efficiency
because the electrolyte is directly related to the polysulfide dis-
solution issue discussed in section 2.2. Therefore, the E/S ratio
is a very important parameter in determining both the elec-
trochemical performance and energy density of Li-S batteries.
However, only 32 out of the examined 205 papers provide infor-
mation on the E/S ratio, indicating that this parameter has
been neglected.
There are 59 total reported E/S ratios and the analysis results
are displayed in Figure 6. Over half of the recorded E/S ratios
are higher than 10 µL mg−1, corresponding to a weight ratio of
electrolyte to sulfur higher than 10:1 (the density of the com-
monly used ether-based electrolyte in Li-S batteries is about
1.0 mg µL−1). It has been estimated that the weight ratio of electro­
lyte to sulfur in a Li-S battery should be no higher than 4:1 to
ensure a high gravimetric energy density,[11] and a high E/S ratio
of >10 µL mg−1 would lead to a significantly reduced energy
density of a practical cell. Nevertheless, only 3 of the 59 reported
E/S ratios are lower than 4 µL mg−1. Low E/S ratios often lead
to reduced sulfur utilization and a low number of cycles because
of insufficient wetting of the electrode and continuous electro-
lyte depletion during cycling.[56] In this regard, approaches for
improved performance with low E/S ratios are worth exploring
to pave the way for the commercialization of Li-S batteries.
4.4. Electrode Size
In most papers, coin cells with a diameter of 20 mm are used to
study their electrochemical properties, while for a practical Li-S
battery, the size is much larger than that of coin cells. There-
fore, performance differences exist between the coin cells used
in materials research and the large pouch cells used in practical
applications.[249] Even for coin cells, a smaller sulfur cathode
often results in better electrochemical performance than with
a larger cathode with the same areal sulfur loading, especially
for cathodes with a high areal sulfur-loading. In this regard, the
sulfur cathode used in coin cells should have a similar area to
the lithium anode or at least larger than 1 cm2 to obtain more
convincing performance results. However, only 77 out of the
205 examined papers provide electrode sizes. In several publi-
cations, very tiny sulfur cathodes (less than 0.5 cm2) were used
to achieve better electrochemical performance.
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4.5. Cycling Conditions
For the performance evaluation of Li-S batteries, cycling sta-
bility and output voltage are key indicators, and these are not
only influenced by sulfur content, areal sulfur loading, E/S ratio
and electrode size, but are also sensitive to cycling conditions,
including the potential window and current density (cycling
rate). The cycling performance and the voltage of the second
discharge plateau of the 205 publications examined are sum-
marized in Table S1.
The potential window, especially the discharge cutoff voltage,
has a significant effect on the cycling stability of a Li-S battery.
In ether-based electrolytes, LiNO3 is often used as an addi-
tive, which serves to protect the lithium anode and suppress
the redox shuttle of polysulfides. At a discharge cutoff voltage
below 1.7V, an irreversible reduction of LiNO3 occurs on the
surface of the cathode, which lowers the reaction kinetics of
the subsequent redox processes, leading to decreased cycling
stability.[250] Therefore, with a LiNO3-containing electrolyte, a
discharge cutoff voltage of 1.8V is desirable for the good revers-
ibility of Li/S batteries (generally with a potential window of
1.8V–2.8V).
It is known that different current densities result in dif-
ferent electrochemical performance in terms of specific
capacity, cycling stability and output voltage even for the same
cell. For LIBs, a lower current density often leads to a higher
specific capacity and better stability. However, for Li-S bat-
teries, this is not the case, especially for cathodes with a low
sulfur loading. At a higher current density, although both the
specific capacity and the output voltage are lowered, higher
cycling stability can often be achieved. Because high current
densities lead to high electric field forces (from the anode to
the cathode during charging for polysulfide ions), which can
offset the polysulfide concentration gradient force (from the
cathode to the anode), resulting in suppressed polysulfide dif-
fusion to the anode and improved cycling stability. Therefore,
in many papers with low areal sulfur loadings, it is common
to see that high current densities are used to achieve high
stability regardless of decreased specific capacity and output
voltage, directly resulting in a significantly lower energy den-
sity, which is not desirable. Indeed, the cycling performance
at low current densities (often lower than 168 mA g−1) reveals
the actual role of the cathode in confining polysulfides and is
very important for the evaluation of a Li-S cell. However, many
papers have not shown data for cycling performance at low
current densities.
4.6. Economical and Ecological Concerns
Last but not least, economical and ecological concerns need
to be raised, and this is an important aspect for industrial
production. For the commercialization of Li-S batteries, the
overall energy and time demand needs to be strictly controlled,
and simple electrode configurations with easy synthesis and
low cost are preferred. As shown in Table S1, many advanced
sulfur-host materials have been specifically designed, some of
which involve a complex fabrication process with the use of
toxic raw materials, and these are not suitable for large-scale
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www.advancedsciencenews.com
use. Indeed, sophisticated sulfur cathodes are not always nec-
essary to achieve excellent electrochemical properties. Some
simple electrodes using low-cost and commercially available
materials as well as easy preparation processes result in a high
electrochemical performance, which we will highlight in the
next section.
4.7. Protocols for Reliable Li-S Batteries
From the above statistical analyses, it can be concluded that
the papers on Li-S batteries certainly indicate good progress: at
the early stage, efforts were mostly made to improve the sulfur
utilization regardless of sulfur content in the cathode; after-
wards, a high sulfur content was given increasing attention to
improve the specific capacity based on the whole cathode; in
the last two years, the importance of high areal sulfur loading
has been raised, with more research concerned with the fab-
rication of cathodes with a high sulfur loading. Nevertheless,
the attention to high sulfur contents and areal sulfur load-
ings is still inadequate (Table S1). Besides, as we have shown,
the energy density of a Li-S cell is affected by a wide range
of design parameters, many of which have not been given
the attention they deserve. With a view to constructing more
reliable Li-S batteries, we hope that the discussion presented
here will cause future research to pay more attention to the
following:
(1) High sulfur content (≥70 wt%) and high specific capacities
(≥800 mAh g−1) based on the whole cathode. It is worth men-
tioning that interlayers inserted between the sulfur cathode
and the separator have been often used in recent reports, and
the weight of such interlayers should be included because
they also belong to the cathode.
(2) High areal sulfur loadings (≥5 mg cm−2) and high areal ca-
pacities (≥6 mAh cm−2).
(3) Information on the electrolyte to sulfur ratio needs to be pro-
vided. Low E/S ratios (≤4 µL mg−1) are desired for high en-
ergy densities.
(4) Information on electrode size should be given. The cathode
should have a similar area to the lithium anode or at least
larger than 1 cm2 in coin cells.
(5) A discharge cutoff voltage of higher than 1.7V should be used
in LiNO3-containing electrolytes. Cycling performances at
low current densities are important.
(6) Simple electrodes with an easy fabrication process using low-
cost materials are preferred.
5. Possible Solutions and Some Concerns for
More Reliable Li-S Batteries
As shown in the above statistical overview, most reported Li-S
research work is far from satisfactory from the point of view of
applications, and there is still plenty of room for improvement
from the perspectives of fundamental research. In this sec-
tion, we will provide an overview of the promising approaches
towards the construction of reliable Li-S batteries from the
viewpoints of sulfur cathode, electrolyte, and anode.
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5.1. Sulfur Content and Areal Sulfur Loading
As discussed earlier, the sulfur content and areal sulfur loading
in the cathode exert a direct influence on the energy density
of a Li-S battery. Due to the trade-off between high sulfur con-
tent and high sulfur utilization, to have a high sulfur content
without sacrificing sulfur utilization is a key point. In this
regard, the construction of effective conductive matrixes is
needed to ensure the desired electrical contact of sulfur with
the electrode and facilitate efficient electron transport with the
amount of conductive agents as low as possible. In the fol-
lowing, possible solutions from three aspects will be discussed:
1) porous host materials for the sulfur; 2) construction of inter-
connected conductive networks; and 3) the use of conductive
interlayers.
For the same cathode materials, increased areal sulfur
loading means increased electrode thickness, leading to
decreased conductivities for lithium ions and electrons. The
performance obtained from thin sulfur cathodes with low
areal sulfur loadings is often not reproducible when the elec-
trode thickness is increased. For the commercialization of Li-S
batteries, an improvement of areal sulfur loading is a crucial
issue and deserves more attention. Especially for short-chain
sulfur cathodes, which have intrinsically low sulfur contents,
high areal sulfur loadings are particularly necessary for pos-
sible commercial use. We will discuss possible solutions for the
realization of high-sulfur-loaded cathodes from three aspects: 1)
conventional two dimensional (2D) current collectors; 2) layer-
by-layer (LBL) strategy; 3) 3D current collectors.
5.1.1. Porous Host Materials for Sulfur
Conductive porous materials, commonly lightweight porous
carbon materials, have been extensively studied as hosts to
accommodate sulfur within their nanopores.[14,15,19,22] On the
one hand, good electron transport can be ensured between
the conductive porous matrix and the sulfur, resulting in high
sulfur utilization. On the other hand, the porous structure
serves to confine polysulfides within the pores and suppress
their free migration to the anode, which improves cycling
stability. For achieving high sulfur contents in sulfur/porous
carbon composites, a high pore volume is required, which is
given by the following formula (taking ≈80% volumetric expan-
sion from sulfur to Li2S into consideration):
V
*d
sulfur content = 1.8
V
* d +1
1.8
where V is the pore volume of the porous carbon, and d is the
density of sulfur (2.07 g cm−3). Considering the addition of a
conductive additive and binder in the casting fabrication of the
cathodes (often 10 wt% ≈ 30 wt%), for a 70 wt% sulfur con-
tent in the cathode, a sulfur content of at least 80 wt% in the
sulfur/porous carbon composite is needed, corresponding to a
high pore volume of 3.48 cm3 g−1 for the carbon, as shown in
Table 1.
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Table 1.  Relationship between the pore volume of porous host materials
and their theoretical sulfur contents.
Sulfur content (wt%) 60 65 70 75 80 85
Pore volume (cm3 g−1) 1.3 1.62 2.03 2.61 3.48 4.93
Recently, a few groups have achieved high sulfur contents
(≥80 wt%) in sulfur/porous carbon composites with highly
porous carbon materials as the sulfur host. Song et al.[220]
reported the production of highly crumpled nitrogen-doped
graphene sheets with an ultrahigh pore volume by a simple
thermally induced expansion strategy. Li-S cells using these
wrinkled graphene sheets as both sulfur host and interlayer
achieved a high capacity of ≈1000 mAh g−1 with a high sulfur
content (≥80 wt%). In our recent work, a highly porous gra-
phene with a pore volume of 3.51 cm3 g−1 was fabricated by
the thermal exfoliation of graphite oxide, enabling a high sulfur
content in the resulting composite of 80 wt%.[26] After mixing
with a conductive additive and binder (15 wt%), the final sulfur
cathode contained 68 wt% sulfur, which is close to the above
criterion (70 wt%). Combining highly conductive graphene as
the current collector and partially oxygenated graphene as a
polysulfide-adsorption layer, a high initial specific capacity of
1500 mAh g−1 (based on sulfur) was achieved, corresponding
to a high capacity of 1020 mAh g−1 based on the whole cathode.
Besides the pore volume, pore size is another important
parameter for porous carbon materials. The pore structure has
three categories based on pore size: 1) micropores (<2 nm); 2)
mesopores (2 nm ≈ 50 nm); 3) macropores (>50 nm).[251]
Micropores lead to a high surface area and enable close elec-
trical contact with active materials by strong adsorption. How-
ever, they often result in low pore volumes for sulfur accommo-
dation and sluggish kinetics for lithium ion transport, which are
not desirable for high sulfur contents. It should be particularly
noted that small micropores with a pore size of <0.5 nm enable
the formation of small sulfur molecules (as discussed in section
3.2) and can completely solve the polysulfide shuttle effect due
to the elimination of polysulfide formation, resulting in high
sulfur utilization and good cycling stability. For mesopores and
macropores, despite the weaker adsorption with active mate-
rials, they are beneficial for electrolyte penetration, which facili-
tates lithium ion transport, and more importantly, they lead to
high pore volumes and consequently high sulfur contents.
The optimal pore size for use in Li-S batteries is not yet fully
understood. Based on the above discussion, as summarized in
Table 2, we give the following principles in tailoring the pore
size of porous carbon materials for use as the sulfur host:
(1) Mesopores and macropores are beneficial in achieving high
sulfur content, but show inferior cycling stability (ether-based
electrolytes are used). Research efforts should be focused on
trapping polysulfides and suppressing the shuttle effect.
(2) Small micropores (<0.5 nm) show advantages in high sulfur
utilization and good cycling stability due to the presence of
small sulfur molecules, but have a limited sulfur content and
a low output voltage (carbonate-based electrolytes are used).
Effort needs to be focused on the development of thick cath-
odes with high areal sulfur loadings, which we will discuss in
the following section.
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Table 2.  Advantages and disadvantages of porous carbon materials with
different pore sizes as the sulfur host.
90 Mesopores and Small micropores Large micropores
macropores (<0.5 nm) (0.5 nm–2 nm)
7.83
Electrolyte ether-based carbonate-based ether-based
Advantages high sulfur content good cycling stability should be avoided
high output voltages
Disadvantages inferior cycling low sulfur contents
stability
low output voltages
(3) Large micropores (0.5 nm−2 nm) should be avoided in the
design of sulfur host materials (when ether-based electro-
lytes are used), because they show inferior cycling stability
compared to small micropores (<0.5 nm) and low sulfur con-
tents as well as sluggish reaction kinetics compared to those
obtained with mesopores and macropores.
5.1.2. Interconnected Conductive Networks
Constructing interconnected conductive networks in the sulfur
cathode has proved to be an effective way to achieve high sulfur
utilization with a high sulfur content. The incorporation of
interconnected conductive scaffolds provides sufficient space
to accommodate the sulfur and abundant electron pathways for
the redox processes. The materials used for the construction of
such conductive networks need to meet two requirements: high
conductivity and light weight. In this respect, nanostructured
carbon materials, such as carbon nanotubes (CNTs) and gra-
phene, show overwhelming advantages.
Cheng et al.[104] explored the idea of embedding sulfur in
aligned CNTs by a simple ball-milling process, resulting in a
high sulfur content of up to 90 wt%. The sulfur powders were
crushed into small nanoparticles which were well distrib-
uted within the aligned framework of CNT arrays (Figure 7a).
The small bundles of aligned CNTs interconnected with one
another, providing a robust conductive network. With 77 wt%
sulfur content in the cathode (15 wt% binder was added), an
initial discharge capacity of 564 mAh g−1 was achieved based
on the total mass of the cathode. More recently, Papandrea
et al.[213] reported a freestanding three dimensional (3D) gra-
phene framework for a highly efficient loading of sulfur par-
ticles without binders or conductive additives (Figure 7b), and
the sulfur content in the cathode reached as high as 90 wt%.
The interconnected graphene network ensured excellent con-
ductivity and the 3D pore structure allowed efficient lithium
ion transport and served to accommodate the volume changes
during cycling. This 3D sulfur/graphene composite delivered
a high discharge capacity of 969 mAh g−1 based on the entire
cathode.
5.1.3. Conductive Interlayers
The concept of interlayers inserted between the sulfur cathode
and the polymer separator was first developed by Manthiram’s
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Figure 7. a) Scanning electron microscopy (SEM) image of a sulfur/
aligned CNT composite. The circles and arrows refer to the particles of
sulfur and aligned CNTs respectively. b) SEM image of a three dimen-
sional graphene framework with 90 wt% sulfur. a) Reproduced with per-
mission.[104] Copyright 2014, Elsevier. b) Reproduced with permission.[213]
Copyright 2016, Springer.
group,[81] and significant improvements in not only the active
material utilization but also the capacity retention were
observed with the insertion of a microporous carbon paper
between the cathode and separator. The interlayer functions as
an embedded conductive network in the cathode region that
facilitates electron transport and effectively reduces the resist-
ance, and serves to trap the migrating polysulfides and sup-
press their diffusion to the anode. As a result of the unique
advantages of such interlayers, sulfur cathodes with high sulfur
contents are able to show high sulfur utilization and good
cycling stability. Similar to the requirements for the materials
used in the construction of interconnected conductive networks
(section 5.1.2), the materials used for the conductive interlayers
also need to be highly conductive and lightweight.
Our group has extended the concept of interlayers by pro-
posing a sandwich-structured sulfur cathode configuration
using two graphene membranes. One graphene membrane
with a sulfur coating as the active material was used as a current
collector (GCC), and the other was coated on a commercial pol-
ymer separator (G-separator) as an interlayer (Figure 8a). More
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important, a pure sulfur cathode was used to give a 70 wt%
sulfur content in the cathode assembly, eliminating the complex
synthesis of a material to host the sulfur, which is desirable for
large-scale production. The sandwich-structured sulfur cathode
delivers a high specific capacity of 750 mAh g−1 at a high cur-
rent density of 6 A g−1, which is 50 times higher than that of a
cell using an aluminum current collector and a polymer sepa-
rator (Figure 8b), indicating highly efficient electron transport
in this cathode. A battery with the sandwich-structured sulfur
cathode configuration also exhibits better capacity retention on
cycling than other configurations (Figure 8c).
Although the addition of conductive interlayers contributes
to improved electrochemical performance with high sulfur con-
tents, the interlayer is a part of the cathode, which increases the
weight of inactive components and leads to a decreased sulfur
content based on the whole cathode. Therefore, the size, thick-
ness and density of the conductive interlayers should be consid-
ered to determine the sulfur content.
5.1.4. Conventional 2D Current Collectors
For the preparation of sulfur cathodes, slurry-coating is often
used to cast a slurry of active material, conductive additive,
and binder onto a flat 2D current collector. Thick sulfur cath-
odes with high areal sulfur loadings often suffer from low
sulfur utilization and high polarization. Lv et al.[147] studied
the change of the areal specific capacity as a function of
areal sulfur loading using 80 wt% S/integrated Ketjen Black
(Figure 9a), and found that above a limit of 3.5 mg cm−2,
the increase in areal capacity from the increased areal sulfur
loading cannot compensate for the decrease in sulfur uti-
lization, resulting in a decreased areal capacity despite the
increased areal sulfur loading. A gradual capacity increase
during the initial 20 cycles was observed in the cycling per-
formance of a cathode loaded with 3.5 mg cm−2 sulfur
(Figure 9b), which is caused by the electrolyte wetting within
the thick sulfur cathode. This phenomenon becomes serious
with a higher areal sulfur loading of 5 mg cm−2 (Figure 9c),
and even at a rate as low as 0.05 C, the initial discharge
capacity is only 570 mAh g−1, but increases to 1200 mAh g−1
in the 10th cycle. When the current density was increased
to 0.2 C, significantly decreased discharge capacities and
voltage plateaus were observed. These results indicate that,
for cathodes with a high sulfur-loading, electrolyte wettability
becomes a key challenge in addition to the significantly low-
ered electronic conductivity, which leads to sluggish lithium
ion transport in the cathode.
Incorporating CNTs or graphene as conductive additives
during the electrode preparation has proved to be an effec-
tive way to alleviate the above challenges for thick sulfur cath-
odes. These additives can facilitate electrolyte penetration and
increase the electronic conductivity of thick electrodes, leading
to improved electrochemical properties. In Figure 9d, when
the conventional carbon black is replaced by the same amount
of graphene and CNTs, the cell exhibits greatly improved dis-
charge capacities compared with that in Figure 9c. In recent
work reported by the Nazar group,[211,212] graphene was used as
a conductive additive to create 3D electron conductive pathways
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Figure 8.  a) Schematic of a Li-S battery with a sandwich-structured cathode. b) Rate performance of Li-S batteries with different configurations. The
improvement in specific capacity is the ratio of the capacity of a battery with a GCC/S+G-separator to that of one with an Al foil/S+separator. c) Cycling
stability of Li-S batteries with different configurations for 100 cycles. Reproduced with permission.[130]

and to promote electrolyte wetting across the thick electrodes, Besides the modification of conductive additives, tuning
resulting in high areal sulfur loadings of 3–5 mg cm−2 with binder networks is another approach to enhance electron and
improved areal capacities and cycling stabilities. ion transport in thick sulfur cathodes. Recently, Yang et al.[252]
reported a simple phase inversion method
for producing high performance Li-S bat-
teries with high sulfur loadings. By simply
immersing an aluminum foil coated with
the slurry mixture of active material, polymer
binder (polyvinylidene fluoride-hexafluoro-
propylene) and organic solvent (N-methyl pyr-
rolidone) into a water coagulation bath, phase
inversion took place immediately, resulting
in a porous electrode with interconnected
binder networks, electron paths and ion
channels. In comparison with an electrode
prepared by direct drying that had a dense
structure (Figure 10a), the morphology of the
electrode prepared by phase inversion had a
hierarchical porous skeleton with the active
material dispersed within the polymer binder
fibers (Figure 10b). As a result, Li-S cells with
this electrode had a high specific capacity
and good cycling performance with an areal
sulfur loading of 1.5 mg cm−2 (Figure 10c).
Moreover, with a higher areal sulfur loading
of 7 mg cm−2, the electrode shows an initial
discharge capacity of 951 mA h g−1 and 89%
capacity retention after 50 cycles (Figure 10d),
indicating the advantages of the phase inver-
Figure 9.  a) Dependence of areal specific capacities on the areal sulfur loadings at 0.1C. b)
−2 sion method in improving the performance
Cycling stability of a cathode loaded with 3.5 mg cm sulfur. c) Discharge profiles of a cathode
loaded with 5 mg cm−2 sulfur and using carbon black (super P) as the conductive additive of cathodes with a high sulfur loading.
(10 wt%). d) Discharge profiles of a cathode loaded with 4.7 mg cm−2 sulfur using graphene For sulfur cathodes with 2D current col-
(5 wt%) and CNTs (5 wt%) as conductive additives. Reproduced with permission.[147] lectors, a high sulfur content is required for

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and ion transport, but also effectively trap

soluble polysulfide intermediates within the
cathode. Moreover, the areal sulfur loading
can be easily increased by increasing the
number of sulfur layers. Consequently, a
six-sulfur-layer cathode can have an ultra-
high areal sulfur loading of 11.4 mg cm−2
and a high initial discharge capacity of
995 mA h g−1, corresponding to an areal
capacity of 11.3 mA h cm−2. It also main-
tains a reversible capacity of 650 mA h g−1
after 100 cycles, showing good cycling sta-
bility (Figure 11b). Based on this concept,
Yuan et al.[126] reported the fabrication of a
freestanding S/CNT paper electrode with
a sulfur loading of 6.3 mg cm−2, which
was further increased to 17.3 mg cm−2 by
stacking three S/CNT paper electrodes,
resulting in a high areal capacity of
15.1 mAh cm−2. Li et al.[146] designed a “pie”-
structured freestanding sulfur cathode with
a sulfur loading of 3.6 mg cm−2, in which
Figure 10.  Cross-sectional morphology of electrodes prepared by the a) phase inversion and b) multichannel carbon nanofibers are the
direct drying methods. c) Cycling performance of Li-S cells with electrodes prepared by phase
“filling” and amino-functionalized graphene
inversion and direct drying at 0.2 C. d) 50 cycles at 0.05 C with an areal sulfur loading of
7.0 mg cm−2 (phase inversion). Reproduced with permission.[252] is the “crust”. After stacking three layers, a
high sulfur loading of 10.8 mg cm−2 and an
areal capacity greater than 8 mAh cm−2 were
the realization of a high areal sulfur loading. The challenges achieved along with good stability for 50 cycles.
for thick sulfur cathodes include the need to solve the problem
of decreased electronic and ionic conductivities, and modifying
conductive additives and binder networks during electrode 5.1.6. Three-dimensional Current Collectors
preparation show promise in achieving both high performance
with high areal sulfur loadings. Aluminum foil is usually used as the current collector for the
sulfur cathode to guarantee electrical connection between the
cathode and the external circuit, and active materials need to
5.1.5. Layer-by-Layer Strategy be intimately attached to the current collector to facilitate elec-
tron transport. In this case, for thick sulfur cathodes with a
Freestanding sulfur cathodes have been considered a prom- high sulfur-loading, long electron diffusion pathways from the
ising option for achieving high sulfur contents, as they do not current collector to the surface of the electrode often result in
include additional binders, conductive addi-
tives and current collectors compared with
electrodes produced using slurry-coating.[19]
Carbon nanomaterials such as CNTs,[34]
carbon fibers[146] and graphene[100] have been
widely used for the construction of free-
standing electrodes, because they tend to
form interwoven conductive networks, which
enhance the sulfur utilization even without
the presence of conductive additives (as dis-
cussed in section 5.1.2). For freestanding
sulfur cathodes, a layer-by-layer (LBL) strategy
has proved to be a simple and effective way to
achieve high areal sulfur loadings.
The concept of the LBL strategy was
introduced by the Manthiram group[154] to
obtain high-areal-capacity sulfur cathodes,
with the use of freestanding porous carbon
nanofiber layers (Figure 11a). Such LBL Figure 11.  a) Schematic of LBL sulfur cathodes. b) Cycling performance of a cell with a six-
cathodes not only facilitate fast electron sulfur-layer cathode (11.4 mg cm−2). Reproduced with permission.[154]

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significantly reduced sulfur utilization. Moreover, the stability
of aluminum in organic electrolytes remains a problem, and
it suffers severe electrochemical corrosion during cycling,[216]
which further results in a loss of local electrical contact of sulfur
with the current collector and an increased internal resistance
of the cell. In this regard, 3D current collectors, which embed
cathode materials in a 3D support matrix, not only function
as an inner conductive scaffold to guarantee the desired elec-
trical contact with active materials, but also provide sufficient
space for a large amount of active material and to trap the poly-
sulfides during cycling. Li-S batteries using 3D current collec-
tors have demonstrated great promise for the construction of
high sulfur-loaded electrodes with improved stability.
Chung et al.[90] reported the fabrication of 3D sulfur-nickel
foam cathodes by a simple paste-absorption method with
an areal sulfur loading of 2 mg cm−2. The sulfur-nickel foam
cathode provided an excellent internal electron transport net-
work by ensuring intimate contact between the sulfur and the
nickel foam and served as a cage to retain the polysulfides in
the cathode region, leading to a stable cycle life with a high
discharge capacity retention rate of 92% after 50 cycles. Cheng
et al.[105] designed a 3D aluminum foam-CNT scaffold as a cur-
rent collector for Li-S batteries that enabled high areal sulfur
loadings ranging from 7.0 to 12.5 mg cm−2. A high initial dis-
charge capacity of 6.02 mAh cm−2 (860 mAh g−1) was achieved
for an electrode loaded with 7.0 mg cm−2 sulfur. However,
the intrinsic high density of metal foams may result in a sig-
nificantly reduced overall energy density. In this regard, light-
weight carbonaceous materials are preferable for building 3D
current collectors.
Miao et al.[114] reported the easy and low-cost synthesis of
sulfur/carbon fiber cloth cathodes with high areal sulfur load-
ings ranging from 3.8 to 8.0 mg cm−2. The carbon fiber cloth
consisted of interconnected carbon fibers and sulfur was
Figure 12.  a) SEM image of the hollow carbon fiber foam. b) SEM image and c) 3D X-ray microtomography image of the S/hollow carbon fiber foam
electrode with an areal sulfur loading of 10.8 mg cm−2. d) Areal capacities of three S/hollow carbon fiber foam electrodes with different sulfur loadings
at different cycles. e) Schematic of sulfur reduction process in the S/hollow carbon fiber foam electrode with high electrolyte absorbability. Reproduced
with permission.[190]
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distributed homogeneously within the 3D conductive network
with no large sulfur particles observed, which is beneficial for
achieving a high sulfur utilization even at high sulfur load-
ings. A high specific capacity of 1100 mAh g−1 was retained
after 50 cycles with an areal sulfur loading of 6.7 mg cm−2, cor-
responding to a high areal capacity of 7.37 mAh cm−2. In our
recent work,[190] a hollow carbon fiber foam was synthesized by
the carbonization of natural cotton (Figures 12a), and this was
used as a 3D current collector to accommodate a large amount
of sulfur-multiwall CNT-carbon black hybrids (90 wt% sulfur)
(Figure 12b), enabling ultrahigh areal sulfur loadings of
6.2-21.2 mg cm−2. The carbon fibers had lengths of several hun-
dred micrometers and formed a long-range conductive network
with uniformly distributed micrometer-size sulfur clusters
(Figure 12c). The resulting electrodes showed good cycling sta-
bilities as well as high areal capacities with areal sulfur loadings
of 6.2, 10.8, and 16.5 mg cm−2 (Figure 12d). A mechanism was
proposed to account for the intriguing electrochemical perfor-
mance of these electrodes: the 3D foam-like structure of the
current collector enables high amount of electrolyte uptake,
and serves to localize the polysulfides dissolved in the electro-
lyte within the cathode region and prevent their diffusion to
the lithium anode, resulting in lower active material loss and
enhanced cycling stability (Figure 12e).
5.2. Electrolyte
For the liquid organic electrolyte systems used in Li-S batteries,
ether-based electrolytes are most widely used, while carbonate-
based ones are only suitable for short sulfur-chains (as dis-
cussed in section 3). The use of ether-based electrolytes gives
rise to the dissolution and re-deposition of polysulfides and
enables a high sulfur utilization. However, they also cause the
© 2017 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim
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“shuttle effect” and have a great impact on the electrochemical
properties. Therefore, parameters concerning the use of elec-
trolytes are of great importance for the optimization of perfor-
mance. Here we will discuss the use of ether-based electrolytes
in Li-S batteries from two aspects: concentration and amount.
Then solid and gel electrolytes used in Li-S batteries will be
introduced and discussed.
5.2.1. Electrolyte Concentration
The dissolution of lithium polysulfides in electrolytes causes a
series of problems including fast capacity decay and low Cou-
lombic efficiency (Section 2.2). The concentration of lithium
ions in electrolytes plays a key role in the solubility of poly-
sulfides according to the principle of dissolution equilibrium.
In this regard, increasing the lithium salt concentrations in
the electrolytes is a promising way to decrease the solubility
of lithium polysulfides. Suo et al.[253] reported a new class
of “solvent-in-salt” (SIS) electrolytes with high lithium salt
(Li[CF3SO2)2N]: LiTFSI) concentrations up to 7 mol L−1, which
is close to the saturation limit. The use of such a high con-
centration electrolyte led to decreased dissolution of lithium
polysulfides and improved cycling stability (Figure 13a). In
addition, the Coulombic efficiency reached nearly 100% after
the first cycle owing to effective alleviation of the polysulfide
shuttle effect in the charging process (Figure 13b), while other
less-concentrated electrolytes (2 mol L−1 and 4 mol L−1) exhib-
ited apparent Coulombic efficiencies greater than 100% (here
Coulombic efficiency = charge capacity/discharge capacity),
indicative of the polysulfide “shuttle effect”. Moreover, the “sol-
vent-in-salt” electrolyte can effectively suppress the formation
of lithium dendrites because of the ultrahigh lithium salt con-
centration and high viscosity. With ultra-high lithium salt con-
centrations, the balance of cations (Li+) and anions (TFSI−) is
maintained near the metallic lithium anode. The space charge
created by TFSI− depletion is minimal, which is unfavorable for
dendrite growth and contributes to improved safety.
Despite the above advantages of high concentration electro-
lytes, several concerns need to be taken into consideration in
practical conditions. First, a high salt concentration often leads
to high viscosity and results in high polarization with a lowered
output voltage. Second, the density of electrolytes is increased
Figure 13.  a) Cycling performance and b) Coulombic efficiency of sulfur cathodes in ether-
based electrolytes with different concentrations (SIS 2#: 2 mol L−1 LiTFSI, SIS 4#: 4 mol L−1
LiTFSI, SIS 7#: 7 mol L−1 LiTFSI). Reproduced with permission.[253] Copyright 2013, Macmillan
Publishers Limited.
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with an increase of lithium salt concentration, leading to an
increased percentage of inactive components and a decreased
energy density. Third, the significantly increased cost of the
lithium salt in high concentration electrolytes is not econom-
ical. Therefore, for a practical Li-S battery it remains to be seen
whether the performance improvement due to high concentra-
tion electrolytes can compensate for the above three concerns
needs and further exploration is needed.
5.2.2. Electrolyte Amount
As discussed in section 4.3, the electrolyte to sulfur ratio
influences not only the energy density, but also the electro-
chemical properties of Li-S batteries. A lower amount of elec-
trolyte leads to a decreased amount of dissolved polysulfides
and suppressed shuttle effect, but also to sluggish lithium ion
transport, especially at high current densities, due to its poor
wetting ability. A higher amount of electrolyte lowers both the
gravimetric and volumetric energy densities. However, more
electrolyte can improve the cycle life because the depletion of
electrolyte during cycling is one of the major reasons for the
failure of high sulfur-loaded electrodes.[56] The importance of
the electrolyte amount has been highlighted in several reports.
Zheng et al.[24] investigated the influence of the sulfur/elec-
trolyte ratio on Li-S battery performance and found that, with
an optimized E/S ratio of 20 µL mg−1 (corresponding to
50 g L−1 in Figure 14), a good balance between electrolyte
viscosity, wetting ability, diffusion rate of dissolved polysulfides
and nucleation/growth of solid Li2S/Li2S2 was established along
with significantly reduced corrosion of the lithium metal anode
(Figure 14). Cheng et al.[254] tuned the polysulfide shuttle effect
by adjusting the E/S ratios, and a Li-S cell with a high initial
discharge capacity of 1053 mAh g−1 at a high rate of 1 C and
an ultralow decay rate of 0.049% per cycle during 1000 cycles
was obtained with a E/S ratio of 24 µL mg−1 (corresponding to
1.28 mol L−1 in this report).
Nevertheless, the reported optimized E/S ratios for max-
imum electrochemical performance are often higher than
10 µL mg−1. As discussed earlier, an E/S ratio less than or equal
to 4 µL mg−1 should be used in a practical Li-S battery to ensure
a high energy density. Therefore, more work needs to be done
to improve the electrochemical performance and energy density
with the use of small amounts of electrolyte.
5.2.3. Solid and Gel Electrolytes
As discussed in section 2.2, the inevitable dis-
solution of polysulfides and safety concerns
regarding the use of a metallic lithium anode
in liquid electrolytes are two main challenges
in the commercialization of Li-S batteries.
In this respect, the use of solid electrolytes
instead of liquid electrolytes is technically a
viable approach to completely inhibit the dis-
solution of polysulfides and increase the sta-
bility of the lithium anode. In addition, solid
electrolytes show advantages of high thermal
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Figure 14.  a) Charge/discharge profiles and b) cycling performance of Li-S cells with different
sulfur/electrolyte ratios. Discharge capacities delivered at c) ca. the 2.3 V plateau and d) the
2.1 V plateau (and below) during cycling. Reproduced with permission.[24] Copyright 2013, The
Electrochemical Society.
stability, high mechanical strength, and non-flammability.[15]
The most frequently used solid electrolytes in Li-S batteries are
based on a Li2S-P2S5 system,[255,257,258] which consists of lithium
sulfides and phosphorous pentasulfides with a certain molar
ratio. Nagata et al.[255] studied the performance of all-solid-state
Li-S cells using Li1.5PS3.3 (60Li2S-40P2S5 [mol%]) as the solid
electrolyte (Figure 15a), and found that an activated-carbon-
based composite electrode exhibited the best performance
because of the high surface area of activated carbon, which
enables sufficient electrical contact with sulfur at nanoscale and
improved sulfur utilization. Consequently, an excellent cycling
performance with a reversible capacity of over 1600 mAh g−1
after 100 cycles was achieved in the cell (Figure 15b).
Gel-polymer electrolytes also show promise in solving the
problems associated with polysulfides. Hassoun et al.[256]
replaced the common liquid organic solution electrolyte with a
gel-type polymer membrane, which contains liquid regions in
a polymer envelope (Figure 15c). The exterior polymer sheath
acts as a physical barrier that prevents direct contact of the elec-
trode components with the liquid. It also inhibits the dissolu-
tion of polysulfides from the cathode and protects the lithium
anode. The feasibility of this concept was demonstrated with
a Li2S/C cathode and a lithium anode in the gel-polymer elec-
trolyte, and the cell had a high capacity and good reversibility
(Figure 15d).
Despite the great promise of solid and gel electrolytes in
solving the challenges regarding the polysulfides and the
lithium anode, the lithium-ion conductivity of these electrolytes
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is significantly lower than liquid electrolytes.
The high interfacial resistance between elec-
trodes and electrolytes remains a problem,
leading to a large voltage hysteresis and a
lower output voltage (Figure 15a and d).
5.3. Anode
With the significant improvements in the
development of sulfur cathodes, the anode,
which is a major limiting factor in the use
of Li-S batteries as practical energy storage
devices, has recently attracted much more
attention. As discussed in section 2.2,
metallic lithium is the most promising anode
candidate due to its high specific capacity
and low electrochemical potential. However,
challenges including lithium dendrite forma-
tion, unstable solid electrolyte interfaces and
volume changes lead to safety concerns, low
Coulombic efficiency, and short cycle life.
Therefore, the stability of the lithium metal
anode may determine the fate of Li-S bat-
teries. Three aspects of the stabilization of the
lithium anode will be discussed: 1) stabiliza-
tion of the interface between the anode and
the electrolyte; 2) a 3D lithium host; and 3)
a “lithiophilic” lithium host. The use of alter-
native anodes such as carbon and silicon will
also be introduced.
5.3.1. Stabilization of the Interface
Because metallic lithium is highly reactive in organic electro-
lytes, strategies for improving the stability and uniformity of
the interfaces between the lithium anode and electrolytes have
been explored to suppress dendrite formation and stabilize
the solid electrolyte interphase (SEI). Most approaches focus
on a modification of liquid electrolytes by either adjusting the
electrolyte components or optimizing additives to control SEI
formation.[259–262]
The addition of LiNO3 to ether-based electrolytes has proved
to significantly improve the Coulombic efficiency and cycle life
of Li-S batteries, because LiNO3 participates in the formation
of a passivation layer on the lithium surface, which prevents
further reactions between lithium and the polysulfides.[263,264]
However, due to the volume change of the lithium anode, the
passivation layer grows continuously with the progressive con-
sumption of LiNO3, which is ineffective in suppressing lithium
dendrite formation during long-term cycling. Although it is
very difficult to achieve sufficient passivation of the lithium
anode in liquid electrolytes,[265] Ding et al.[260] proposed a self-
healing electrostatic shielding mechanism that can fundamen-
tally alter lithium dendrite formation by using an electrolyte
additive cation (such as cesium or rubidium ions) with a lower
reduction potential than the standard Li/Li+ (Figures 16a–16d).
During the initial stage of the lithium deposition process, some
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Figure 15.  a) Charge/discharge curves of an all-solid-state Li-S cell containing a composite cathode based on activated carbon, Ketjen black, and
acetylene black. b) Cycling performance of an all-solid-state Li-S cell containing an activated carbon-based composite cathode. c) A photograph of the
gel-type polymer membrane. d) The initial 3 cycle charge/discharge curves of a Li2S/C electrode in the gel-polymer electrolyte. a, b) Reproduced with
permission.[255] Copyright 2014, Elsevier. c–d) Reproduced with permission.[256]

protuberant tips were unavoidably formed due to fluctuations
in this system (Figure 16a), which caused a strong electrical
field, and lithium preferentially deposited around the tips to
form lithium dendrites. Additive cations with a lower reduc-
tion potential accumulated in the vicinity of the tips to form
an electrostatic shield (Figure 16b), which could enable the
subsequent lithium deposition in the adjacent regions of the
anode (Figure 16c) until a smooth deposition layer was formed
(Figure 16d), leading to suppressed lithium dendrite forma-
tion. Consequently, the lithium layer resulted in a distinctive
improvement in anode surface quality with the elimination
of lithium dendrite growth (Figure 16e) compared to that in a
control electrolyte without cesium ion additives (Figure 16f).
In addition, the cesium or rubidium ions were not consumed
during the lithium deposition due to the low reduction poten-
tial and thus remained effective for many cycles. However, the
Coulombic efficiency was relatively low (76.6%) due to the poor
SEI layer formed on the lithium metal surface. In general, from
the perspective of liquid electrolytes, a good combination of
electrolyte solvent, salt, additive and their concentrations needs
to be explored for both the high Coulombic efficiency and high
safety (dendrite free) of the lithium metal anode.
Alternatively, ex situ coated mechanically stable artificial
layers, such as polymer or solid-state blocking layers,[266–268]
have been proposed to block the dendrite penetration. These
interfacial layers stabilize the interface of the lithium anode
with the liquid electrolytes, leading to improved Coulombic
efficiency and safety. However, these approaches rely on the
principle of physical confinement to suppress the lithium den-
drite penetration, and cannot change the intrinsic behavior
of the lithium dendrite growth, and are therefore not reliable
during long-term cycling.
5.3.2. 3D Lithium Hosts
Generally, a planar lithium metal foil is directly used as the
anode of lithium batteries, and the initial plating of lithium on
the planar substrate is prone to the inhomogeneous deposition
of lithium particles on which lithium dendrites may then grow.
In this regard, constructing a 3D host to accommodate lithium
deposition shows promise in preventing dendrite growth.
Yang et al.[269] reported a 3D Cu current collector with a
submicrometer-sized skeleton and high electroactive surface
area that improved the electrochemical deposition behavior of
lithium. For planar current collectors, the initially deposited
small Li particles function as charge centers when charges accu-
mulate at their sharp tips in the electric field (Figure 17a), and
the subsequent deposition of lithium on these sharp tips results
in the growth of Li dendrites. In comparison, on a 3D Cu foil,
numerous protuberant tips on the submicrometer fibers func-
tion as the charge centers and nucleation sites, and the electric
field is roughly uniform so that the charges are homogeneously
dispersed along the Cu skeleton (Figure 17b). The lithium is

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Figure 16.  a–d) Illustration of the lithium deposition process based on a
self-healing electrostatic shielding mechanism. SEM images of the mor-
phologies of lithium films formed in the electrolytes e) with and f) without
cesium ion additives. Reproduced with permission.[260] Copyright 2013,
American Chemical Society.
therefore expected to nucleate and grow on the submicrometer
Cu fibers in nanosized lumps, fill the spaces between them
and eventually form a relatively smooth Li surface. As a result,
a relatively flat lithium surface is obtained on the 3D Cu foil
after depositing 2 mAh cm−2 of lithium (Figure 17c). The cor-
responding atomic force microscope (AFM) image shows an
undulating topography with gentle slopes with a height differ-
ence of <2.5 µm (Figure 17d). Therefore, the accommodation of
the lithium anode on the 3D Cu foil remarkably suppresses den-
drite growth, and significantly improves the safety of the lithium
anode. Cheng et al.[270] have fabricated a 3D nanostructured
anode with metallic lithium contained in a fibrous Li7B6 matrix,
which had stable long cycling performance and high Coulombic
efficiency in Li-S batteries. This 3D nanostructured LiB alloy
anode not only reduced the current density and decreased the
growth rate of Li deposits, but also limited the final size of
the deposited lithium on the nanostructured matrix, leading
to the dendrite-free morphology of the anode at the macroscale.
5.3.3. Lithiophilic Lithium Hosts
It is known that a lithium anode shows a continuous volume
change during lithium plating/stripping, and the resulting
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huge internal stress fluctuations and floating interface cause
anode pulverization during continuous cycling. Moreover, the
SEI on the lithium surface strongly correlates with the dimen-
sional stability of the anode, which becomes unstable and tends
to collapse during the drastic volume changes, resulting in
continuous electrolyte decomposition and exacerbated lithium
dendrite growth. Therefore, it is necessary to build a host with
good lithium affinity (lithiophilicity) for metallic lithium. Good
lithiophilicity enables the strong binding between lithium and
host, which is critical for achieving both a uniform lithium dis-
tribution during synthesis and a low lithium nucleation barrier
during cycling.
Lin et al.[271] reported a composite lithium metal anode that
exhibits small dimensional changes (≈20%) during cycling
and good mechanical flexibility. The anode was prepared by
infusing molten lithium into a lithiophilic, layered reduced gra-
phene oxide (rGO) film with uniform nanoscale gaps between
the rGO layers (Figure 18a). After lithium infusion, these gaps
were filled with lithium and the layered structure was main-
tained (Figure 18b). Because of the abundant nucleation sites
and the almost complete interfacial protection provided by the
rGO layers, the Li–rGO film remained smooth without observ-
able cracks or dendrites on the surface after ten stripping/
plating cycles at a relatively high current density of 3 mA cm−2
(Figure 18c). The large number of 2D lithium interlayers greatly
increased the activated surface area for lithium nucleation and
deposition. In addition, the rGO layer acted as a stable artificial
interface because the graphene layers maintained a stable SEI
and accommodated dimension fluctuations. Therefore, with the
stable rGO at the interface and a small dimension change, SEI
cracking and lithium dendrite growth were highly suppressed.
As a result, galvanostatic cycling of a symmetric Li–rGO elec-
trode exhibited stable voltage profiles with little hysteresis, and
flat voltage plateaus were observed throughout the cycling,
while the Li foil showed a gradual increase in hysteresis with
cycling and a sudden voltage drop was detected with big voltage
changes in the later cycles, which was explained by an internal
short-circuit with Li dendrite penetration (Figure 18d). Based
on the concept of constructing lithiophilic lithium hosts, Liu
et al.[33] designed a polyimide matrix with a conformal layer
of zinc oxide to render the surface lithiophilic, so that molten
lithium could be drawn into the matrix, producing a nano-
porous lithium electrode. The polymeric backbone enabled
uniform lithium stripping/plating with the lithium confined in
the matrix, allowing minimum volume changes and effective
dendrite suppression.
5.3.4. Alternative Anodes
Considering the significant challenges related to a lithium
metal anode, several alternative anodes have been explored
for Li-S batteries.[53,272–275] For example, Brückner et al.[272]
demonstrated stable Li-S cells with silicon-carbon (Si-C) and
all-carbon anodes. When the sulfur cathode was coupled with
a metallic lithium anode, the cell was able to achieve revers-
ible cycling for 135 cycles at 167 mA g−1 (Figure 19a). How-
ever, when the same cathode was cycled at 836 mA g−1 (after
three cycles at 167 mA g−1), the cell failed rather quickly after
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reason for the low cycling stability with a lim-

ited amount of electrolyte especially at high
current densities. In comparison, when the
sulfur cathode was coupled with a pre-lithi-
ated Si-C anode, the cell showed good cycling
stability for more than 1300 reversible cycles
with high Coulombic efficiency of 99.8% in
the 1390th cycle (Figure 19c). It should also
be noted that the excess lithium in this cell
was only 60%, and the enhanced cycle sta-
bility could be attributed to the fact that a
stable SEI was formed on the Si-C anode
and the electrolyte was not consumed during
cycling. The cycling performance of the cell
with an all-carbon anode was also investi-
gated with excess lithium of only 10%, and
stable cycling for more than 550 cycles was
observed with no cell failure (Figure 19d).
The above results demonstrate good poten-
tial for the use of alternative anodes beyond
metallic lithium in Li-S batteries. However,
the electrochemical potential of lithiated
carbon-based anodes was higher than that of
elemental lithium, which might result in a
Figure 17.  Illustration of the electrochemical deposition processes of Li metal on a) a planar decrease in the energy density of the full cell.
current collector and b) a 3D current collector. The distribution of electrons within the current
collectors in the electric field is schematically shown with the dashed lines illustrating the
possible positions where Li would be deposited. c) Side view SEM image and d) AFM height
6. Summary and Outlook
image of 2 mA h cm−2 of lithium deposited on a 3D Cu foil with a submicrometer skeleton.
Reproduced with permission.[269] Copyright 2015, Macmillan Publishers Limited. We have overviewed the research status of
Li-S batteries by analyzing the statistical
45 cycles (Figure 19b). This could be attributed to rapid elec- information provided in 205 Li-S battery research papers over
trolyte depletion due to the unstable SEI on the lithium anode. the last 8 years, and comprehensively discussed how the var-
In this regard, the metallic lithium anode may be the main ious parameters, including sulfur content, areal sulfur loading,

Figure 18. SEM images of a) a layered rGO film, b) a layered Li–rGO film, and c) the surface of a Li–rGO film after 10 galvanostatic cycles at
3 mA cm−2. d) Galvanostatic cycling of a symmetric Li–rGO electrode (blue) and bare Li foil (red) at 3 mA cm−2. Insets: detailed voltage profiles for a
Li–rGO electrode with the number of cycles indicated. Reproduced with permission.[271] Copyright 2016, Macmillan Publishers Limited.

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in order to promote the Li-S battery tech-

nology.[276] Modification of the conductive
additives and binders, a multi-layer electrode
configuration, and 3D electrode design show
effectiveness in the fabrication of cathodes
with a high sulfur loading. Nevertheless,
more work should be done for the realization
of the desired sulfur utilization of more than
80% (corresponding to a specific capacity of
1340 mAh g−1 based on sulfur mass) with a
sulfur content higher than 70% and an areal
sulfur loading high than 5 mg cm−2.

(2) Electrolyte:

The appropriate use of electrolytes plays

a very important role in the commercializa-
tion of Li-S batteries. Currently, challenges
remain for both liquid electrolytes and solid
or gel electrolytes. Further improvements
Figure 19. Discharge capacity and Coulombic efficiency of a sulfur cathode coupled with need to be explored to balance the advantages
a metallic lithium anode cycled at a) 167 mA g−1 and b) 836 mA g−1 after three cycles at and disadvantages of the different electrolyte
167 mA g−1. c) Discharge capacity and Coulombic efficiency of a sulfur cathode coupled with systems to achieve both high energy density
a Si-C anode cycled at 836 mA g−1 after three cycles at 167 mA g−1. d) Discharge capacity and
−1
Coulombic efficiency of a sulfur cathode coupled with an all-carbon anode cycled at 334 mA g .
and improved safety. For liquid electrolyte
Reproduced with permission.[272] systems, the concentrations of lithium salt
in the electrolyte need to be optimized to
electrolyte type, electrolyte/sulfur ratio, and cycling conditions, balance the reaction kinetics of polysulfides and overall energy
affect the useful energy density. Most Li-S batteries reported so density. Low amounts of electrolyte should be used with the
far are accompanied by low areal sulfur loadings and a great desired electrode wettability. In view of the safety concerns of
excess of electrolyte, leading to low practical energy densities the lithium anode, the mechanism of lithium dendrite forma-
that have no chance of outperforming state-of-the-art LIBs even tion in liquid electrolytes needs further investigation. The fea-
if full sulfur utilization is achieved. Therefore, there is still a sible approaches for electrolyte modification should be explored
long way to go before Li-S battery technology becomes commer- to protect the lithium anode (for example, the use of electrolyte
cially available. With the aim of paving the way to more reliable additives). More innovations are required for Li-S batteries to
Li-S batteries with commercial applications, attention needs to be able to use solid or gel electrolytes which promise high level
be paid not only to materials research, but also to the electrode of safety.
architecture and cell engineering. From the perspective of fun-
damental research, we have emphasized that high sulfur con- (3) Anode
tents, high areal sulfur loadings and low electrolyte-to-sulfur
ratios are essential requirements for achieving high practical The challenge of the anode is one of the most critical bar-
energy density of a Li-S device, and these parameters should be riers to the use of Li-S batteries. Despite its advantages for high
optimized. Besides, problems related to a lithium metal anode energy density, a lithium metal anode is unstable in liquid
in the Li-S system still remain a great challenge and further organic electrolytes and the safety concerns regarding lithium
developments are needed for the stabilization and protection of dendrite formation greatly impede its use in practical cells.
the anode. There are two aspects to the protection of the lithium anode:
Several suggestions with respect to the development of dif- passivation of the lithium metal surface and hosting metallic
ferent components in a Li-S battery are generalized as follows: lithium in a prepared matrix. It should be noted that common
electrolytes are often used to investigate the stability of the
(1) Sulfur cathode: lithium anode in the literature, however, the interface prop-
erties of the lithium anode become more complicated in Li-S
For achieving high sulfur contents, novel conductive mate- batteries with the presence of mobile polysulfides. Therefore,
rials need to be explored for effective accommodation of the the feasibility of the approaches reported for lithium anode sta-
active material, including the synthesis of host materials for bilization need further verification. To produce a safe lithium
the sulfur and the design of sulfur adsorption materials (for anode with long-term cyclability, a better understanding on the
example, conductive interlayers). Any addition of inactive mate- formation and evolution of a surface passivation layer on the
rials in the cathode needs to be taken into consideration. For lithium anode needs exploration to provide more insight into
high areal sulfur loadings, more importance is attached to the the fade mechanisms of the anode. In addition, considering
cathode architectures. Research on scale-up prototypes of Li-S the lithium metal degradation (including the formation of a
cells with practically high loading and per unit area are desired surface passivation layer and “dead” Li), the excess over the

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stoichiometric amount of lithium metal used to pair with the
sulfur cathode needs to be rationally controlled for a balance
between performance and overall energy density. For alterna-
tive anodes, although the safety concerns can be effectively
addressed, the main drawback is the decrease of energy den-
sity, which needs further optimization to compete with other
lithium-based battery systems.
From the practical perspective, the following aspects need
more deep thinking and deserve more research effort for
achieving significant breakthroughs in the development of Li-S
battery field.
(1) Understanding of fundamental reaction mechanism:
The conversion reaction mechanism of Li-S batteries
involves a series of structural and compositional changes of
multiple intermediates, which is very complicated and has not
been fully understood. As the electrochemical properties are
closely related to the formation of polysulfide intermediates,
advanced characterizations, for example by in situ and ex situ
observations, are needed to investigate the reaction kinetics
and dynamic changes of active materials during the redox pro-
cess. Advances in the fundamental understanding of the elec-
trochemical reactions taking place in a Li-S cell are expected to
provide precise guidelines for the design of Li-S batteries.
(2) Solid-state Li-S batteries
The use of lithium metal anode brings a major advantage to
Li-S batteries with respect to energy density, but the safety issue
causes a great challenge. Construction of solid-state batteries
with solid electrolytes is among the most promising ways to ful-
fill the safety expectation. As the development of solid-state bat-
teries is still at a early stage, many issues, for example, mobility
of lithium ions in solid electrolytes and interfacial kinetics
between solid electrolytes and active materials, remain to be
solved to guarantee stable operation of a solid-state Li-S cell.
(3) Integrated consideration of electrode and cell
Optimization of a Li-S cell requires the collaboration of elec-
trodes, current collectors, separators and electrolytes. For the
design of active materials in Li-S batteries, integrated consid-
eration of these components is expected to provide more con-
vincing results.
(4) Target driven design of Li-S batteries
For energy storage applications, performance indicators
include gravimetric energy density, volumetric energy density,
power density, cycle life, and high/low temperarure properties.
It is necessary to explore the specific applications of Li-S bat-
teries and determine the detailed performance requirements
for target-driven design of their different components.
Overall, the commercial availability of Li-S batteries requires
further scientific and technical development. More research
needs to be done with emphasis on their integral design, and
reliable Li-S batteries with a satisfactory performance need
continuous optimization of the sulfur cathode, lithium anode,
Adv. Mater. 2017, 1606823
1606823  (21 of 25)
www.advmat.de
and electrolyte to meet the goal of market penetration. In addi-
tion, simple, sustainable and scalable fabrication approaches
for the components in the Li-S cell are greatly needed because
cost-effectiveness is very important for industrial-scale produc-
tion. Reports that the energy density of a 37 Ah Li-S battery
reached 566 Wh kg−1 at room temperature and 616 Wh kg−1
at 50 °C,[277] indicate that there are promising prototypes of
high energy density Li-S batteries. It is believed that Li-S battery
technology could be applicable in transportation and large-scale
grid energy storage in the near future.
Supporting Information
Supporting Information is available from the Wiley Online Library or
from the author.
Acknowledgements
This work was supported by the Ministry of Science and Technology
of China (2016YFA0200100, 2016YBF0100100, 2014CB932402), NSFC
(Nos. 51521091, 51525206, 51372253, 51272051 and U1401243),
“Strategic Priority Research Program” of the Chinese Academy of
Sciences (XDA09010104), the Key Research Program of the Chinese
Academy of Sciences (Grant No. KGZD-EW-T06), and the CAS/SAFEA
International Partnership Program for Creative Research Teams. The
authors thank Dr. Lixiao Miao in National Center for Nanoscience and
Technology for helpful discussions.
Keywords
batteries, high energy, lithium, sulfur
Received: December 18, 2016
Revised: February 22, 2017
Published online:
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