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@ARTICLE{Wagemaker:20185,
      author       = {Wagemaker, M. and Singh, D.P. and Borghols, W.J.H. and
                      Lafont, U. and Haverkate, L. and Peterson, V.K. and Mulder,
                      F.M.},
      title        = {{D}ynamic {S}olubility {L}imits in {N}anosized {O}livine
                      {L}i{F}e{PO}(4)},
      journal      = {Journal of the American Chemical Society},
      volume       = {133},
      issn         = {0002-7863},
      address      = {Washington, DC},
      publisher    = {American Chemical Society},
      reportid     = {PreJuSER-20185},
      pages        = {10222 - 10228},
      year         = {2011},
      note         = {This work is a contribution from the Delft Energy
                      Initiative (DEI). Financial support from Shell is
                      acknowledged for the Sustainable Mobility grant funding
                      D.P.S. The Netherlands Organization for Scientific Research
                      (NWO) is acknowledged for both beam time at ISIS and the
                      CW-VIDI grant of M.W. The authors thank Ron Smith for
                      assistance with the neutron diffraction experiments at
                      POLARIS (ISIS), Michela Brunelli and Mark Johnson at D20
                      (ILL), and Vladimir Pomjakushin at HRPT (PSI). We thank the
                      Alistore network for providing access to the TEM
                      measurements.},
      abstract     = {Because of its stability, nanosized olivine LiFePO(4) opens
                      the door toward high-power Li-ion battery technology for
                      large-scale applications as required for plug-in hybrid
                      vehicles. Here, we reveal that the thermodynamics of
                      first-order phase transitions in nanoinsertion materials is
                      distinctly different from bulk materials as demonstrated by
                      the decreasing miscibility gap that appears to be strongly
                      dependent on the overall composition in LiFePO(4). In
                      contrast to our common thermodynamic knowledge, that
                      dictates solubility limits to be independent of the overall
                      composition, combined neutron and X-ray diffraction reveals
                      strongly varying solubility limits below particle sizes of
                      35 nm. A rationale is found based on modeling of the diffuse
                      interface. Size confinement of the lithium concentration
                      gradient, which exists at the phase boundary, competes with
                      the in bulk energetically favorable compositions.
                      Consequently, temperature and size diagrams of nanomaterials
                      require complete reconsideration, being strongly dependent
                      on the overall composition. This is vital knowledge for the
                      future nanoarchitecturing of superior energy storage devices
                      as the performance will heavily depend on the disclosed
                      nanoionic properties.},
      keywords     = {J (WoSType)},
      cin          = {PGI-4 / JCNS (München) ; Jülich Centre for Neutron
                      Science JCNS (München) ; JCNS-FRM-II / JCNS-2},
      ddc          = {540},
      cid          = {I:(DE-Juel1)PGI-4-20110106 /
                      I:(DE-Juel1)JCNS-FRM-II-20110218 /
                      I:(DE-Juel1)JCNS-2-20110106},
      pnm          = {Grundlagen für zukünftige Informationstechnologien /
                      Großgeräte für die Forschung mit Photonen, Neutronen und
                      Ionen (PNI)},
      pid          = {G:(DE-Juel1)FUEK412 / G:(DE-Juel1)FUEK415},
      experiment   = {EXP:(DE-MLZ)External-20140101},
      shelfmark    = {Chemistry, Multidisciplinary},
      typ          = {PUB:(DE-HGF)16},
      pubmed       = {pmid:21598941},
      UT           = {WOS:000292715600050},
      doi          = {10.1021/ja2026213},
      url          = {https://juser.fz-juelich.de/record/20185},
}