Please cite this article in press as: Bhargav et al.
, Lithium-Sulfur Batteries: Attaining the Critical Metrics, Joule (2020), https://doi.org/10.1016/
j.joule.2020.01.001
COMMENTARY
Lithium-Sulfur
Batteries:
Attaining
the Critical
Metrics
Amruth Bhargav,1 Jiarui He,1
Abhay Gupta,1
and Arumugam Manthiram1,*
Amruth Bhargav is a PhD student in the
Materials Science and Engineering
graduate program at the University of
Texas at Austin. He obtained his B.E.
in Mechanical Engineering from Visves-
varaya Technological University, India,
in 2013 and a Master of Science in Me-
chanical Engineering from Indiana Uni-
versity-Purdue University Indianapolis
in 2016. His research mainly focuses
on lithium-sulfur and lithium-organo-
sulfur batteries.
Dr. Jiarui He is a postdoctoral fellow in
the Texas Materials Institute at the Uni-
versity of Texas at Austin. He obtained
his B.E. (2012) and his PhD (2018) in
electronic information materials and
devices from the University of Elec-
tronic Science and Technology of
China. His research interests are in the
area of electrochemical conversion
and storage materials. He has authored
more than 76 publications, with 3,000
citations and an h-index of 33 (Google
Scholar).
Abhay Gupta is a PhD student in the
Materials Science and Engineering
graduate program at the University of
Texas at Austin. He received his
bachelor’s degree from the Hildebrand
Department of Petroleum and Geosys-
tems Engineering at the University of
Texas at Austin in 2016. His research
mainly focuses on lithium-sulfur batte-
ries with an emphasis on low-tempera-
ture performance.
Professor Arumugam Manthiram is the
Cockrell Family Regents Chair in engi-
neering and the Director of Texas
Materials Institute and the Materials
Science and Engineering program at
the University of Texas at Austin. His
research interests are in the area of
materials for rechargeable batteries
and fuel cells, including novel syn-
thesis approaches, advanced char-
acterization, and prototype device
fabrication. He has authored more
than 800 publications, with 60,000 ci-
tations and an h-index of 123 (Google
Scholar). See https://www.sites.utexas.
edu/manthiram for further details.
Introduction
Lithium-sulfur (Li-S) batteries represent
a potential step-change advance in hu-
manity’s ability to electrochemically
store energy, because of the high
gravimetric capacity and low cost of
sulfur. We are now on the precipice
of the next phase of Li-S research,
where new developments must
palpably contribute to making the
Li-S technology commercially relevant.
To take this leap, the Li-S community
should recognize the shortcomings in
the parameters being used in current
cell designs and deliberately move to-
ward those that can fully realize the
high-energy density promise of Li-S
batteries. In this Commentary, we
outline key areas for improvement in
the Li-S technology. Although this
commentary is organized on subsys-
tem by subsystem basis, many of these
challenges are interdependent. The
following subsections present parame-
ters that are critical to consider in Li-S
research and provide a roadmap for
overcoming the obstacles that have
prevented the technology’s implemen-
tation to date. Finally, we introduce the
‘‘five 5s’’—the critical metrics that are
essential for meeting the high-energy
target of Li-S systems.
Joule 4, 1–6, February 19, 2020 ª 2020 Elsevier Inc.
Cathode
The cathode has received the largest vol-
ume of work among all Li-S cell compo-
nents in academic literature. Here, we
seek to highlight the critical challenges re-
maining in this area and also call attention
to the unique interplay between sulfur
and the electrolyte. The electrochemistry
of the Li-S battery relies on the formation
of soluble lithium polysulfide (LiPS) inter-
mediates during charge and discharge.
These redox-active species dissolve into
the electrolyte and mediate the reaction
kinetics of charge-transfer in solution,
which in effect regulates the achievable
capacity in the cell. The dissolution of
the sulfur active material into the electro-
lyte highlights the need to consider the
cathode and electrolyte in conjunction,
rather than as separate decoupled en-
tities. For this reason, this section first
delves into parameters governing just
the sulfur electrode and then proceeds
to highlight metrics that best account for
the dependencies of the cathode on the
electrolyte.
Use of Carbon
The majority of sulfur cathodes in the
literature employ composite frame-
works containing significant amounts
of conductive carbon (up to 50 wt %).1
This is to overcome the low electronic
conductivity of sulfur. However, the
addition of large amounts of conduc-
tive filler deprecates the cell-level spe-
cific energy. Therefore, minimization
of carbon content in the cathode is crit-
ical to prioritize when optimizing the
sulfur cathode. Similar to Li-ion battery
cathodes, the carbon content should
ideally be reduced to below 5%. Addi-
tionally, minimization of carbon content
can be highly beneficial to the following
three parameters:
a. Porosity: Various carbons and
their composites used in Li-S
cathodes have a high surface
area (100–1500 m2 g 1) and low
tap density (0.1–0.3 g cm 3).2
1
 Please cite this article in press as: Bhargav et al., Lithium-Sulfur Batteries: Attaining the Critical Metrics, Joule (2020), https://doi.org/10.1016/
j.joule.2020.01.001

A B C they are sufficiently bound.

Contact angle = 125° Contact angle = 35°
Carbon Sulfur LiCoO2 Non-polar carbon interacts
weakly with the polar LiPSs in
solution (as seen in Figure 1D),
resulting in poor binding and
electron transfer. Consequently,
there is an incomplete conver-
1 g sample each Hydrophobicity of carbon host Hydrophilicity of polar host sion of LiPS and generation of
D E F an electronically insulating thin
500 600
E/S ratio L mg-1) E/S ratio L mg-1)
film of Li2S, which reduces the
Specific Energy (Wh kg-1)

Specific Energy (Wh kg-1)

2 3 2 3
500
400 4 5 4 5 attainable capacity.3 A sulfur
400
100% S Utilization (%)
host should be both conductive
300 90%
300 80%
and electrocatalytic. Such hosts
70%
200 60% can simultaneously facilitate
200 50%
40% LiPS binding (as observed in the
LiPS LiPS LiPS
100 100 case of polar hosts in Figure 1D)
2 4 6 8 10 12 1 2 3 4 5 6 7 8
+C + polar
host
Sulfur Loading (mg cm-2) E/C Ratio ( L [mAh]-1) while promoting electron trans-
fer, boosting its conversion and
Figure 1. Critical Cathode Parameters attainable capacity. In addition,
(A) A visual comparison of the density of microporous carbon (Ketjenblack EC-600JD), sulfur, and a
a thin, lightweight layer of such
Li-ion battery cathode, LiCoO 2 . The powders were tapped to ensure efficient packing.
polar materials could also be
(B) Interaction between water and carbon, showing its high hydrophobicity.
(C) Interaction of water with a polar host on carbon, showing greatly improved hydrophilicity. incorporated as an interlayer on
(D) A simple polysulfide-absorption test comparing carbon and a polar host. The transparent the separator to simultaneously
solution in the case of polar host shows its strong interaction with polysulfides. improve utilization and polysul-
(E) Analytical model showing the effect of sulfur loading on energy density at various E/S ratios.
fide confinement.
(F) Model showing the effect of E/C ratio (with subsequent points corresponding to increased sulfur
utilization as indicated) has on the specific energy at various E/S ratios.
Sulfur Loading
Another critical parameter to consider
The density of microporous car- based redox of LiPSs, which in when designing the sulfur cathode is
bon, sulfur, and an established turn relies on facile ion transport. the areal sulfur loading, in mg cm 2.
Li-ion battery material like This is encouraged when the Higher sulfur loading increases
LiCoO2 is visually compared liquid electrolyte can completely the areal capacity of the cathode
through the photograph in Fig- envelop (i.e., wet) the cathode (mA h cm 2). This maximizes the spe-
ure 1A. The density of carbon is particles. The hydrophobicity of cific energy of the cell, because the
strikingly low, being four and carbon resists wetting by the po- increased fraction of active material off-
nine times less dense than, lar electrolyte, as seen in Fig- sets the ‘‘dead weight’’ present from
respectively, sulfur and LiCoO2. ure 1B. Therefore, high carbon the various inactive components like
Therefore, the increased use of content in the cathode curtails the current collectors and separator.
carbon results in a highly porous wetting, resulting in poor ion The dynamic effect of sulfur loading
cathode. Large amounts of elec- transport and lowering the cell on specific energy is modeled in Fig-
trolytes are required to suffi- capacity. Hydrophilic hosts or ure 1E. In this model, the specific
ciently wet all the surfaces in surface treatments can enhance energy of a Li-S battery is plotted
such a cathode, adding appre- wettability (Figure 1C) and as a function of areal sulfur loading,
ciable weight to the cell and di- thereby facilitate electrolyte assuming that the cathode contains
minishing the specific energy. infiltration and promote LiPS 70 wt % sulfur and achieves
In order to obtain a dense cath- conversion. 1,000 mA h g 1 (~60% utilization).
ode with minimized electrolyte c. Interaction: The sulfur host matrix Further information about this model
uptake, a sulfur host should at the cathode forms the primary is provided in the Supplemental Infor-
possess low surface area (<100 electron conduction pathway for mation. It is evident that irrespective
m2 g 1) and high tap density the various redox-active species of the electrolyte amount, a sulfur
(0.7–1 g cm 3). during cycling. Effective electron loading of <4 mg cm 2 is insufficient
b. Wettability: The sulfur conversion transfer between the LiPS and to outbalance the weight of inactive
reaction depends on solution- conductive host occurs when cell components. Future investigations

2 Joule 4, 1–6, February 19, 2020

 Please cite this article in press as: Bhargav et al., Lithium-Sulfur Batteries: Attaining the Critical Metrics, Joule (2020), https://doi.org/10.1016/
j.joule.2020.01.001
into the sulfur cathode should strive for
sulfur loadings of >5 mg cm 2 in order
to obtain practically relevant results.
Electrolyte-to-Sulfur (E/S) Ratio
The electrolyte constitutes the largest
weight fraction of a Li-S cell. Hence, it
represents the most important lever in
altering the specific energy of the cell.
As highlighted above, the electrolyte
and the sulfur are coupled owing to
the formation of electrolyte-soluble
LiPSs. Maximizing specific energy thus
necessitates the consideration of the
electrolyte volume used in the cell
with respect to the amount of sulfur in
the cathode. Electrolyte/sulfur (E/S)
ratio (expressed in mL mg 1) is a param-
eter that accurately captures this de-
pendency, as depicted in the model in
Figure 1E. This shows that for a given
loading, reducing the E/S ratio greatly
improves the specific energy. A 50%
or higher gain in specific energy can
be achieved by lowering the E/S ratio
from 5 to 2 mL mg 1. As mentioned
above, one way to optimize the E/S ra-
tio is to tune the porosity of a cathode.
Although researchers are beginning to
recognize the significance of this
metric, a large portion of Li-S research
output still continues to use E/S ratios
>20 mL mg 1 or simply neglects to
report E/S ratio altogether.1,4–6 This
fails to meet the standards of what is
needed in order to realistically evaluate
the improvements being reported.
Therefore, to fairly gauge the improve-
ments in cathode design and make
relevant improvements to specific en-
ergy, the community must focus on
reducing the E/S ratio below 5 mL mg 1.
Electrolyte-to-Capacity (E/C) Ratio
Conventional ether-based electrolytes
can dissolve up to 8 M sulfur in the
form of LiPSs in solution.5 Therefore,
at low E/S ratios, the dissolved LiPS
concentration can be driven toward
the saturation point of the electrolyte.
The onset of electrolyte saturation by
LiPS presents a barrier to further disso-
lution of active material, inhibiting the
conversion of remaining sulfur to Li2S.
Thus, at limited electrolyte conditions,
the sulfur utilization and capacity deliv-
ered by the cell tends to be poor. This
interplay between electrolyte amount
and sulfur utilization can be described
by the parameter of electrolyte/capac-
ity (E/C) ratio, defined as the amount
of electrolyte used per unit of discharge
capacity delivered in a cell (expressed
in g [A h] 1 or mL [mA h] 1). E/C ratio
is a consequence of sulfur utilization in
the cell and thus cannot be directly
controlled like the E/S ratio. However,
as E/C ratio links the inactive weight of
the electrolyte to the capacity derived
by the cell, it is an effective determinant
of specific energy. This effect at
different E/S ratios has been modeled
in Figure 1F. As expected, for a given
E/S ratio, a higher sulfur utilization max-
imizes the specific energy, which is re-
flected by a minimized E/C ratio. This
can also be looked at from a specific-
energy standpoint. In order to achieve
325 W h kg 1, for example, a cathode
operating at a low E/S ratio of 2 mL
mg 1 can achieve the target specific
energy with only 60% sulfur utilization
(corresponding to ~1,000 mA h g 1,
or an E/C ratio of 2 mL [mA h] 1). Alter-
natively, a cathode operating at a high
E/S ratio of 5 mL mg 1 can achieve this
energy density so long as the sulfur uti-
lization is 90% (~1,500 mA h g 1 or E/C
ratio of 3.3 mL [mA h] 1). This example
emphasizes that the E/C ratio is a mea-
sure of the effectiveness of the electro-
lyte in enabling utilization for a given
cathode architecture. The E/C ratio
can be minimized by modulating prop-
erties such as wettability and interac-
tion as detailed above. Therefore,
beyond just lowering the E/S ratio
below 5 mL mg 1, cathodes must be de-
signed to also lower the E/C ratio below
5 mL (mA h) 1 to realistically evaluate
new improvements.
Electrolyte
The electrolyte plays a critical role in
the Li-S battery, beyond just ensuring
excellent ionic conductivity. As
described previously, the nature of
discharge in Li-S batteries relies on the
dissolution of redox-active LiPS, which
mediates the reaction kinetics of charge
transfer. This presents unique chal-
lenges and opportunities when devel-
oping and optimizing Li-S battery
electrolytes. Due to the solution-medi-
ated reaction mechanisms, the Li-S
electrolyte must be able to accommo-
date and solvate a wide array of lithium
polysulfide species. However, although
the dissolution of lithium polysulfides is
essential, this also presents the conse-
quence of parasitic shuttling of active
material to the anode. This leads to sig-
nificant active material loss over the
course of cycling. An additional consid-
eration is the long-term stability of the
reactive lithium-metal anode in the
presence of the chosen electrolyte.7
Therefore, the electrolyte must simulta-
neously guarantee satisfactory ionic
conductivity, favorable solubility of
LiPSs, minimization of the LiPS shuttle
effect, and long-term stability with the
Li-metal anode. The predominantly
used ether-based electrolyte repre-
sents the currently best-identified
compromise among this myriad of con-
siderations. This electrolyte displays
quite favorable ionic conductivity and
LiPS solubility. Additionally, ethers
display relatively high stability with Li-
metal in comparison to other classes
of polar aprotic solvents. The effort to
minimize LiPS shuttling and further
extend the long-term stability with Li-
metal presents significant opportu-
nities for liquid electrolytes and
will require continued exploration of
new electrolyte solvents, salts, and
additives.
There are also opportunities for explo-
ration of new electrolyte frameworks,
such as solid-state electrolytes as well
as sparingly solvating electrolytes. In
sparingly solvating electrolytes, the sol-
vent is entirely coordinated by the salt
in order to prevent dissolution of LiPS.
In both systems, the circumvention of
Joule 4, 1–6, February 19, 2020 3
 Please cite this article in press as: Bhargav et al., Lithium-Sulfur Batteries: Attaining the Critical Metrics, Joule (2020), https://doi.org/10.1016/
j.joule.2020.01.001
A
600
E/S ratio
Specific Energy (Wh kg-1)
500 2 3
4 5
400
300
200
100
0 5 10
N/P ratio
Figure 2. Critical Anode and Cell Geometry Parameters
(A) Model showing the variation of specific energy as a function of N/P ratio at various E/S ratios. Li
anode was retrieved from a cycled (B) coin cell after 300 cycles and (C) pouch cell after 40 cycles,
showing vastly different Li deposition morphologies.
LiPS dissolution requires the battery to
rely on solid-state reduction from
elemental sulfur to Li2S. This can pre-
sent significant benefits for minimiza-
tion of LiPS shuttling and long-term
stability with Li metal. However, it also
presents key difficulties in terms of re-
action kinetics, particularly when using
high sulfur loadings and minimal
carbon content required for practical
implementation.
Given the diversity of approaches avail-
able, it is vital to keep in mind that the
implementation of any new electrolyte
framework must strive to meet the pa-
rameters outlined in this commentary.
Through continued development of
conventionally solvating, sparingly sol-
vating, and solid-state electrolytes, the
stringent design requirements of the
Li-S battery could finally be met.
Anode
Designing high-energy-density Li-S
cells necessitates the use of a Li-metal-
based anode, both to offset the low
operating voltage (~2.1 V versus Li/
Li+) and match the high capacity of sul-
fur. However, enabling the stable
cycling of the Li-metal anode denotes
one of the most formidable challenges
and largest areas for improvement
in Li-S batteries. In this section, we
look at how parameters like excess
Li, anode architecture, and electrolyte
4 Joule 4, 1–6, February 19, 2020
B C
L mg-1)
3 mm 1 cm
15 20
Li anode from coin Li anode from pouch
cell after 300 cycles cell after 40 cycles
degradation are key for unlocking Li-S
performance.
Negative-to-Positive (N/P) Capacity
Ratio
Negative/positive (N/P) ratio is defined
as the areal capacity of the Li anode
(negative electrode) to that of the sulfur
cathode (positive electrode). An ideal
Li-S full cell would operate at an N/P ra-
tio of 1.8 However, excess Li is required
to offset the Li loss occurring due to
electrolyte decomposition and solid-
electrolyte interphase (SEI) formation.
The excess Li comes at the cost of spe-
cific energy. The impact of N/P ratio on
cell-level specific energy as a function
of different E/S ratios has been
modeled in Figure 2A. When the N/P
ratio is R20, the excess Li weight penal-
izes specific energy, limiting it to
around 150 W h kg 1. As the N/P ratio
approaches unity, the specific energy
increases by 100% to 200%, depending
on the E/S ratio used. Additionally, the
use of low N/P ratios amplifies the gains
to specific energy brought about by
reducing E/S ratio. For example, at an
N/P ratio of 5, the specific energy in-
creases by 56% when the E/S ratio is
reduced from 5 to 2 mL mg 1. Typical
Li-S cells unfortunately use thick Li-foils
(>500 mm or N/P R20) as the anode.
Beyond simply lowering specific en-
ergy, this excess also compensates for
Li loss during cycling, obfuscating the
true cycle life. Therefore, in order to
augment the improvements brought
about by reducing E/S and E/C ratios,
the community should work toward us-
ing thin Li-foils (N/P ratio <5). This
would vastly improve both gravimetric
and volumetric energy density, while
providing a realistic view of cycle life.
Anode Architecture
Li is a relatively soft metal, with a Mohs
hardness of 0.6, whereas that of a metal
like copper (Cu) is 3. This lack of robust-
ness prevents it from being able to be
rolled into thin, mechanically stable
foils. For this reason, thin (50 mm) Li foils
generally contain a Cu foil backing.
Because Cu is very dense (8.9 g cm 3
versus 0.534 g cm 3 for Li), it contrib-
utes nearly 75% of the mass of such an
anode, dramatically reducing its effec-
tive capacity.9 Cu also gets corroded
by LiPSs. These issues hinder the use
of thin Li foils in this format and hamper
the reduction of N/P below 5. There-
fore, future Li-S research must focus
on employing thin Li anodes wherein
the Li is infused into lightweight,
robust, and lithiophilic host matrices.10
This will help minimize inactive current
collector weight while also lowering
the N/P ratio.
Electrolyte Decomposition
Repeated cycling of Li anode to high
capacities involves the stripping and
plating of several microns of Li metal.
Exposure of the electrolyte to fresh Li
surfaces in each cycle leads to their con-
sumption and a continuous growth of
insulating SEI. This problem is further
exacerbated by the non-uniform de-
posits of high-surface-area Li metal
with mossy and dendritic morphology.
Particularly in the limited electrolyte en-
vironments that practical Li-S operation
requires, this reduces the amount of
electrolyte available for stable cathode
operation, leading to premature cell
failure.11 The instability of the Li-metal
anode likely represents the single
greatest obstacle to implementation
of the Li-S battery. It is thus imper-
ative to understand the Li-anode
 Please cite this article in press as: Bhargav et al., Lithium-Sulfur Batteries: Attaining the Critical Metrics, Joule (2020), https://doi.org/10.1016/
j.joule.2020.01.001
Figure 3. Attaining Critical Metrics for Li-S Batteries
(A) The five 5s showing the critical metrics required for high-energy-density Li-S batteries.
(B) Schematic showing the main issues leading to a low-energy-density configuration and the key changes to overcome these limitations toward a high-
energy-density configuration.
degradation behavior in the unique
polysulfide-rich environment of Li-S
batteries.8 Continued understanding
of these unique interfaces could enable
the development of additives or artifi-
cial SEI layers that could eventually
overcome the challenges intrinsic to
Li-metal anode.12
Cell Geometry
A final overarching consideration is the
cell testing geometry. Studies are
generally conducted in coin-cell geom-
etries in order to evaluate the funda-
mental performance of a new material
in a high-throughput manner. However,
the implementation of battery materials
at large size scales brings about new
challenges that coin-cell testing fails to
highlight. For example, at a coin-cell
level, uniform Li stripping and plating
can be observed (Figure 2B). In
contrast, at the large size scales of
pouch-cells, uneven current densities
across the anode can cause wide varia-
tions in the deposited morphology,
which affects cycling behavior (Fig-
ure 2C). Another downside of coin cells
is the ineffective volume utilization. In a
typical 2032-type cell, <2% of the vol-
ume is occupied by the cell compo-
nents. Whereas, in a vacuum-sealed
soft-packing pouch cell, >65% of the
volume is utilized. This helps in the opti-
mization of important parameters like
E/S ratio and stack pressure. Therefore,
testing new materials in large pouch-
cell geometries can help obtain realistic
assessments of new modifications. The
evaluation of new materials at size
scales relevant to commercial
implementation prioritizes the consid-
eration of industry-relevant parame-
ters. This will hopefully discourage the
use of materials that cannot be pro-
duced at scale and hone the commun-
ity’s attention to practical solutions.
Conclusion: The Five 5s for High-
Energy Li-S Cells
The history of Li-ion batteries demon-
strates that concerted efforts in recog-
nizing and tackling the key technical
challenges form the bedrock for their
commercial success. Li-S technology
can undergo a similar transformation,
provided the research community is in
unison on maximizing the system-level
specific energy. This target can be
simplified as the achievement of the
following five metrics, which we title
the ‘‘five 5s’’ as shown in Figure 3A: sul-
fur loading >5 mg cm 2, carbon con-
tent <5%, E/S ratio <5 mL mg 1, E/C
ratio <5 mL (mA h) 1, and N/P ratio <5
in pouch-type cells. This would enable
the transition from a heavy, voluminous
low-energy configuration shown in Fig-
ure 3B to a light-weight and compact
high-energy system as depicted in Fig-
ure 3B. It is important to note that the
attainment of these metrics does not
necessarily signal the culmination of
the development path for Li-S batte-
ries. Rather, it points to the minimum
metrics that the community must strive
to achieve in putting our best foot for-
ward toward making Li-S batteries a
reality.
SUPPLEMENTAL INFORMATION
Supplemental Information can be
found online at https://doi.org/10.
1016/j.joule.2020.01.001.
ACKNOWLEDGMENTS
The authors would like to thank the
support by the U.S. Department of En-
ergy, Office of Basic Energy Sciences,
Division of Materials Science and
Engineering under award number DE-
SC0005397.
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1MaterialsScience and Engineering Program and
Texas Materials Institute, University of Texas at
Austin, Austin, TX 78712, USA
*Correspondence: rmanth@mail.utexas.edu
https://doi.org/10.1016/j.joule.2020.01.001