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@ARTICLE{Krger:906588,
      author       = {Kröger, Till-Niklas and Harte, Patrick and Klein, Sven and
                      Beuse, Thomas and Börner, Markus and Winter, Martin and
                      Nowak, Sascha and Wiemers-Meyer, Simon},
      title        = {{D}irect investigation of the interparticle-based
                      state-of-charge distribution of polycrystalline {NMC}532 in
                      lithium ion batteries by
                      classification-single-particle-{ICP}-{OES}},
      journal      = {Journal of power sources},
      volume       = {527},
      issn         = {0378-7753},
      address      = {New York, NY [u.a.]},
      publisher    = {Elsevier},
      reportid     = {FZJ-2022-01539},
      pages        = {231204 -},
      year         = {2022},
      abstract     = {The presented case study provides mesoscopic insights into
                      the state-of-charge (SOC) distribution of battery electrodes
                      containing layered transition metal oxides with
                      Li(Ni0.5Mn0.3Co0.2)O2 (NMC532). The application of
                      classification-single-particle inductively coupled plasma
                      optical emission spectroscopy (CL-SP-ICP-OES) enables the
                      rapid screening of the lithium content of individual cathode
                      active material (CAM) particles achieving a statistically
                      viable elucidation of the mesoscale SOC distribution between
                      different particles of the electrode. The results reveal the
                      evolution of a persistent mesoscale SOC heterogeneity of the
                      electrode upon delithiation at slow rates and extensive
                      relaxation times as confirmed by time-of-flight secondary
                      ion mass spectrometry (ToF-SIMS). The implications of local
                      chemical and structural ramifications of the investigated
                      NMC532 for heterogeneous active material utilization are
                      thoroughly discussed. Furthermore, it is found that the
                      evolved SOC heterogeneity of the electrode is strongly
                      dependent on the current density. The correlation to the
                      decreased capacity utilization is further investigated with
                      a straightforward quantification approach revealing a
                      considerable contribution to capacity fading by persistently
                      inactive lithium in the CAM. The results highlight the
                      importance of the analysis of persistent mesoscale SOC
                      heterogeneity as a potential capacity fade mechanism in
                      layered lithium transition metal oxide-based battery
                      electrodes.},
      cin          = {IEK-12},
      ddc          = {620},
      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},
      UT           = {WOS:000782426900005},
      doi          = {10.1016/j.jpowsour.2022.231204},
      url          = {https://juser.fz-juelich.de/record/906588},
}