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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},
}