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@ARTICLE{Bobrov:917131,
      author       = {Bobrov, Gleb and Kedzior, Stephanie A. and Pervez, Syed
                      Atif and Govedarica, Aleksandra and Kloker, Gabriele and
                      Fichtner, Maximilian and Michaelis, Vladimir K. and Bernard,
                      Guy M. and Veelken, Philipp M. and Hausen, Florian and
                      Trifkovic, Milana},
      title        = {{C}oupling {P}article {O}rdering and {S}pherulitic {G}rowth
                      for {L}ong-{T}erm {P}erformance of
                      {N}anocellulose/{P}oly(ethylene oxide) {E}lectrolytes},
      journal      = {ACS applied materials $\&$ interfaces},
      volume       = {15},
      number       = {1},
      issn         = {1944-8244},
      address      = {Washington, DC},
      publisher    = {Soc.},
      reportid     = {FZJ-2023-00363},
      pages        = {1996–2008},
      year         = {2023},
      abstract     = {Development of lithium-ion batteries with composite solid
                      polymer electrolytes (CPSEs) has attracted attention due to
                      their higher energy density and improved safety compared to
                      systems utilizing liquid electrolytes. While it is well
                      known that the microstructure of CPSEs affects the ionic
                      conductivity, thermal stability, and mechanical
                      integrity/long-term stability, the bridge between the
                      microscopic and macroscopic scales is still unclear. Herein,
                      we present a systematic investigation of the distribution of
                      TEMPO-oxidized cellulose nanofibrils (t-CNFs) in two
                      different molecular weights of poly(ethylene oxide) (PEO)
                      and its effect on Li+ ion mobility, bulk conductivity, and
                      long-term stability. For the first time, we link local
                      Li-ion mobility at the nanoscale level to the morphology of
                      CPSEs defined by PEO spherulitic growth in the presence of
                      t-CNF. In a low-MW PEO system, spherulites occupy a whole
                      volume of the derived CPSE with t-CNF being incorporated in
                      between lamellas, while their nuclei remain particle-free.
                      In a high-MW PEO system, spherulites are scarce and their
                      growth is arrested in a non-equilibrium cubic shape due to
                      the strong t-CNF network surrounding them. Electrochemical
                      strain microscopy and solid-state 7Li nuclear magnetic
                      resonance spectroscopy confirm that t-CNF does not partake
                      in Li+ ion transport regardless of its distribution within
                      the polymer matrix. Free-standing CSPE films with low-MW PEO
                      have higher conductivity but lack long-term stability due to
                      the existence of uniformly distributed, particle-free,
                      spherulite nuclei, which have very little resistance to Li
                      dendrite growth. On the other hand, high-MW PEO has lower
                      conductivity but demonstrates a highly stable Li cycling
                      response for more than 1000 h at 0.2 mA/cm2 and 65 °C and
                      more than 100 h at 85 °C. The study provides a direct link
                      between the microscopic dynamic, Li-ion transport, bulk
                      mechanical properties and long-term stability of the derived
                      CPSE and, and as such, offers a pathway towards design of
                      robust all-solid-state Li-metal batteries.},
      cin          = {IEK-9},
      ddc          = {600},
      cid          = {I:(DE-Juel1)IEK-9-20110218},
      pnm          = {1223 - Batteries in Application (POF4-122)},
      pid          = {G:(DE-HGF)POF4-1223},
      typ          = {PUB:(DE-HGF)16},
      pubmed       = {36592370},
      UT           = {WOS:000908362500001},
      doi          = {10.1021/acsami.2c16402},
      url          = {https://juser.fz-juelich.de/record/917131},
}