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@ARTICLE{Ohno:902688,
author = {Ohno, Saneyuki and Zeier, Wolfgang G.},
title = {{T}oward {P}ractical {S}olid-{S}tate {L}ithium–{S}ulfur
{B}atteries: {C}hallenges and {P}erspectives},
journal = {Accounts of materials research},
volume = {2},
number = {10},
issn = {2643-6728},
address = {Washington, DC},
publisher = {ACS Publications},
reportid = {FZJ-2021-04475},
pages = {869 - 880},
year = {2021},
abstract = {The energy density of the ubiquitous lithium-ion batteries
is rapidly approaching its theoretical limit. To go beyond,
a promising strategy is the replacement of conventional
intercalation-type materials with conversion-type materials
possessing substantially higher capacities. Among the
conversion-type cathode materials, sulfur constitutes a
cost-effective and earth-abundant element with a high
theoretical capacity that has a potential to be
game-changing, especially within an emerging solid-state
battery configuration. Employment of nonflammable solid
electrolytes that improves battery safety and boosts the
energy density, as lithium metal anodes are also viable. The
long-standing inherent problem of conventional
lithium–sulfur batteries, arising from the reaction
intermediates dissolved in liquid electrolytes, can be
eliminated with inorganic solid ion conductors. In
particular, the highly conducting and easily processable
lithium-thiophosphates have successfully enabled the
lab-scale solid-state lithium–sulfur cells to achieve
close-to-theoretical capacities. For applications requiring
safe, energy-dense, lightweight batteries, solid-state
lithium–sulfur batteries are an ideal choice that could
surpass conventional lithium-ion batteries.Nevertheless,
there are challenges specific to practical solid-state
lithium–sulfur batteries, beyond the typical challenges
inherent to solid-state batteries in general. While the
conversion reaction of sulfur realizes a large specific
capacity, the associated significant total volume changes of
the active material results in contact losses among the
cathode components and, consequently, decreases reversible
capacity. Additionally, the ionically and electronically
insulating active material requires composite formation with
solid electrolytes and electron-conductive additives to
secure sufficient ion and electron supply at a triple-phase
boundary. However, the compositing process itself makes the
carrier transport pathways very tortuous and requires the
balancing of carrier transport and optimization of the
attainable energy density. Lastly, the requirement of a high
interfacial area to establish sufficient triple-phase
boundaries promotes the degradation of the solid
electrolytes, and the formation of less-conductive
interphases further deteriorates the transport in the
composites.This Account focuses on the challenges associated
with developing practical solid-state lithium–sulfur
batteries and provides an overview over recently developed
concepts to tackle these critical challenges: (1)
Introduction of the conversion efficiency to enable
quantitative assessments of the impact of chemo-mechanical
failure. (2) For long-term cycling, the electrolyte
degradation at the interface and the electrochemical
activity of the formed interphases come into play. Practical
stability tests with increased interfacial areas and
subsequently altered reversal potentials can quantify the
magnitude of the electrolyte degradation and confirm
influences of reversible redox activity of the interphases.
(3) Monitoring the effective conductivity in the composites
clarifies correlations between transport and cyclability,
further highlighting the need of quantitative measurements
to address the composite carrier transport. (4) Impedance
spectroscopy combined with transmission-line model analysis
as a function of applied potentials can visualize the
stability window of good effective ion transport to utilize
both the capacity contributions from redox-active
interphases and the high ionic conductivity. In the end, a
roadmap toward the practical solid-state lithium–sulfur
batteries will be presented.},
cin = {IEK-12},
ddc = {620},
cid = {I:(DE-Juel1)IEK-12-20141217},
pnm = {1223 - Batteries in Application (POF4-122) / LISZUBA -
Lithium-Schwefel-Feststoffbatterien als Zukunftsbatterie
(03XP0115B)},
pid = {G:(DE-HGF)POF4-1223 / G:(BMBF)03XP0115B},
typ = {PUB:(DE-HGF)16},
UT = {WOS:000711029400004},
doi = {10.1021/accountsmr.1c00116},
url = {https://juser.fz-juelich.de/record/902688},
}