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@ARTICLE{Nowak:851174,
      author       = {Nowak, Sascha and Winter, Martin},
      title        = {{T}he {R}ole of {C}ations on the {P}erformance of {L}ithium
                      {I}on {B}atteries: {A} {Q}uantitative {A}nalytical
                      {A}pproach},
      journal      = {Accounts of chemical research},
      volume       = {51},
      number       = {2},
      issn         = {1520-4898},
      address      = {Columbus, Ohio},
      publisher    = {American Chemical Soc.},
      reportid     = {FZJ-2018-04874},
      pages        = {265 - 272},
      year         = {2018},
      abstract     = {Lithium ion batteries are nowadays the state-of-the-art
                      power sources for portable electronic devices and the most
                      promising candidate for energy storage in large-size
                      batteries, e.g., pure and hybrid vehicles. However, the
                      degradation of the cell components minimizes both storage
                      and operation lifetime (calendar and cycle life), which is
                      called aging. Due to the numerous different aging effects,
                      in either the single constituents or their interactions with
                      each other, many reports about methodologies and techniques,
                      both electrochemical and analytical, can be found in the
                      literature. However, quantitative data about the degradation
                      effects were seldom stated. One important effect is the
                      cation distribution and migration during operation. Metal
                      dissolution and metal migration of the cathode and the
                      corresponding deposition of these metals on the graphitic
                      anode are known harmful degradation effects, especially for
                      the formed solid electrolyte interphase on the surface of
                      the anode. Depending on the applied cell chemistries and
                      therefore the cathode material, different mechanisms were
                      reported so far. For lithium manganese oxide based cells,
                      the acidification of the electrolyte due to composition of
                      the conduction salt is attributed as the main source of
                      metal migration. Due to subsequent loss of manganese from
                      the cathode, the overall performance of the cell is
                      seriously impaired. Based on the obtained observations, this
                      degradation mechanism was adapted to lithium nickel cobalt
                      manganese based cells as main cause of the capacity fading.
                      However, with the help a developed total X-ray fluorescence
                      method and additional surface and electrolyte
                      investigations, the proposed HF based mechanism was
                      disproven. Instead, the migration was directly associated
                      with material defects or mechanical spalling of the
                      particles. Furthermore, with the obtained quantitative data
                      of the migrated transition metals on the anode and
                      separator, the contribution on the capacity fade was
                      determined. It ranged only the ‰ region and could
                      therefore be excluded as the main source of the capacity in
                      these lithium ion batteries. Nevertheless, the oxidation
                      state of the cations is hardly accessible; but would provide
                      further information about the exact migrating mechanisms.In
                      addition, lithium can be “lost” or immobilized during
                      charge/discharge and is therefore no longer available as an
                      electrochemically active cation. For example, the formation,
                      reformation, and growth of the solid electrolyte interphase
                      and cathode electrolyte interphase leads to an increased
                      active lithium loss during cycling. The investigations on
                      this topic are frequently reported in literature; however,
                      quantitative data on the actual lithium distribution
                      throughout the cell are relatively few. Furthermore, the
                      exact amount of lost lithium in the in the respective
                      interphases is so far not available. In order to determine
                      quantitatively the lithium distribution within the cell,
                      inductively coupled plasma-based method was applied. For
                      laboratory test cells, the lithium that was lost to the
                      housing of the cell was 32 times higher than that for pouch
                      bag cells. Furthermore, the determined concentration of
                      lithium in the interphases ranged only from 2 to $4\%.$
                      However, the investigations need to be repeated with isotope
                      labeled material (6Li) in order to obtain statements that
                      are more precise.},
      cin          = {IEK-12},
      ddc          = {540},
      cid          = {I:(DE-Juel1)IEK-12-20141217},
      pnm          = {131 - Electrochemical Storage (POF3-131)},
      pid          = {G:(DE-HGF)POF3-131},
      typ          = {PUB:(DE-HGF)16},
      pubmed       = {pmid:29381052},
      UT           = {WOS:000426014500008},
      doi          = {10.1021/acs.accounts.7b00523},
      url          = {https://juser.fz-juelich.de/record/851174},
}