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@ARTICLE{Luether:1025077,
      author       = {Luether, Marco J. and Gomez-Martin, Aurora and Jiang,
                      Shi-Kai and Schmuch, Richard and Placke, Tobias and Hwang,
                      Bing-Joe and Winter, Martin},
      title        = {{I}s the ‘{S}ingle-{C}rystal’ {A}pproach {T}ruly
                      {F}easible for {N}i-{R}ich {L}ayered {O}xides? – a {F}air
                      and {R}ealistic {P}erformance {C}omparison in
                      {N}cm||{G}raphite {C}oin {C}ells},
      journal      = {Meeting abstracts},
      volume       = {MA2023-01},
      number       = {2},
      issn         = {1091-8213},
      address      = {Pennington, NJ},
      publisher    = {Soc.},
      reportid     = {FZJ-2024-02665},
      pages        = {487 - 487},
      year         = {2023},
      note         = {Hierbei handelt es sich lediglich um einen Abstract.},
      abstract     = {Secondary particle cracking induced by anisotropic volume
                      change during cycling has been identified as a major failure
                      mechanism of state-of-the-art Ni-rich layered oxide cathodes
                      like Li[NixCoyMnz]O2 (x + y + z = 1, NCMxyz where x ≥ 0.8)
                      as it allows surface-related degradation phenomena such as
                      inactive phase formation, transition metal dissolution and
                      ongoing electrolyte decomposition to continue on newly
                      formed, highly reactive surface cycle after cycle.1 The
                      approach of designing 'single-crystal' (SC) particles is
                      believed to mitigate this issue by replacing polycrystalline
                      secondary agglomerates (PC) by well-separated micron-sized
                      primary particles that can prolong the cycle life of the
                      material by improving its morphological integrity.2Particle
                      cracking in layered oxide cathode materials is exacerbated
                      with increasing Ni-content which qualifies the
                      'single-crystal' approach especially for Ni-rich NCMs (x ≥
                      0.8). Despite this, meaningful long-term cycling studies are
                      still scarce as two main challenges obstruct a fair
                      evaluation of the 'single-crystal' approach: The synthesis
                      of Ni-rich SC-NCMs is not straightforward as the conditions
                      required for enhanced crystal growth (e. higher calcination
                      temperature and/or a molten-salt environment requiring a
                      washing step) are inherently damaging to Ni-rich materials.3
                      This often leads to comparisons between materials where
                      factors other than morphology cannot be excluded (e.g.
                      synthesis from different precursors, different
                      post-processing steps, undisclosed dopants/coatings in
                      commercial materials, etc.). The larger crystal size of
                      SC-NCMs compared to PC-NCMs is believed to cause kinetic
                      limitations impacting achievable capacities and rate
                      performance.4 As a consequence, either the 'single-crystal'
                      sample is cycled in a lower state-of-charge window despite
                      the same same upper cut-off voltage or the polycrystalline
                      reference sample is cycled at an unnecessarily high voltage.
                      Both conditions favor the 'single-crystal' material.The
                      objective of this work was to establish a fair comparison
                      between the two morphologies. For this purpose, a series of
                      'single-crystal' Li[Ni0.8Co0.1Mn0.1]O2 (SC-NCM811) materials
                      with varying particle sizes where synthesized. To
                      deconvolute the effect of particle size and morphology from
                      other influences, a molten salt-assisted synthesis was
                      followed, so that bulk properties of SC-NCMs remained
                      constant and PC-NCM reference samples could be synthesized
                      from the same home-made precursors and with the same
                      post-processing steps. The samples were thoroughly
                      characterized in terms of physicochemical properties and
                      their electrochemical performance was evaluated in NCM||Li
                      and NCM||Graphite coin cells. The performance of PC- and
                      SC-NCM811 was compared at the same upper cutoff voltage and
                      again at the same state-of-charge window to compare the
                      materials as fairly as possible.References:(1) de Biasi, L.;
                      Schwarz, B.; Brezesinski, T.; Hartmann, P.; Janek, J.;
                      Ehrenberg, H. Chemical, Structural, and Electronic Aspects
                      of Formation and Degradation Behavior on Different Length
                      Scales of Ni-Rich NCM and Li-Rich HE-NCM Cathode Materials
                      in Li-Ion Batteries. Advanced Materials2019, 31 (26).
                      https://doi.org/10.1002/adma.201900985.(2) Zhao, W.; Zou,
                      L.; Zhang, L.; Fan, X.; Zhang, H.; Pagani, F.; Brack, E.;
                      Seidl, L.; Ou, X.; Egorov, K.; Guo, X.; Hu, G.; Trabesinger,
                      S.; Wang, C.; Battaglia, C. Assessing Long‐Term Cycling
                      Stability of Single‐Crystal Versus Polycrystalline
                      Nickel‐Rich NCM in Pouch Cells with 6 MAh Cm −2
                      Electrodes. Small2022, 2107357, 2107357.
                      https://doi.org/10.1002/smll.202107357.(3) Langdon, J.;
                      Manthiram, A. A Perspective on Single-Crystal Layered Oxide
                      Cathodes for Lithium-Ion Batteries. Energy Storage
                      Mater2021, 37, 143–160.
                      https://doi.org/10.1016/j.ensm.2021.02.003.(4) Ryu, H. H.;
                      Namkoong, B.; Kim, J. H.; Belharouak, I.; Yoon, C. S.; Sun,
                      Y. K. Capacity Fading Mechanisms in Ni-Rich Single-Crystal
                      NCM Cathodes. ACS Energy Lett2021, 6 (8), 2726–2734.
                      https://doi.org/10.1021/acsenergylett.1c01089.},
      cin          = {IEK-12},
      ddc          = {540},
      cid          = {I:(DE-Juel1)IEK-12-20141217},
      pnm          = {1221 - Fundamentals and Materials (POF4-122)},
      pid          = {G:(DE-HGF)POF4-1221},
      typ          = {PUB:(DE-HGF)16},
      doi          = {10.1149/MA2023-012487mtgabs},
      url          = {https://juser.fz-juelich.de/record/1025077},
}