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@ARTICLE{Oldiges:845915,
      author       = {Oldiges, K. and Diddens, Diddo and Ebrahiminia, M. and
                      Hooper, J. B. and Cekic-Laskovic, I. and Heuer, A. and
                      Bedrov, D. and Winter, M. and Brunklaus, G.},
      title        = {{U}nderstanding transport mechanisms in ionic
                      liquid/carbonate solvent electrolyte blends},
      journal      = {Physical chemistry, chemical physics},
      volume       = {20},
      number       = {24},
      issn         = {1463-9076},
      address      = {Cambridge},
      publisher    = {RSC Publ.},
      reportid     = {FZJ-2018-03113},
      pages        = {16579-16591},
      year         = {2018},
      abstract     = {To unravel mechanistic details of the ion transport in
                      liquid electrolytes, blends of the ionic liquid (IL)
                      1-butyl-1-methylpyrrolidinium
                      bis(trifluoromethylsulfonyl)imide (Pyr14TFSI), ethylene
                      carbonate (EC) and dimethyl carbonate (DMC) with the
                      conducting salts lithium hexafluorophosphate (LiPF6) and
                      lithium bis(trifluoromethylsulfonyl)imide (LiTFSI) were
                      investigated as a function of the IL concentration.
                      Electrochemical impedance, Pulsed Field Gradient Nuclear
                      Magnetic Resonance (PFG NMR) and Raman spectroscopy
                      supported by Molecular Dynamics (MD) simulations allowed the
                      structural and dynamic correlations of the ion motions to be
                      probed. Remarkably, we identified that though the individual
                      correlations among different ion types exhibit a clear
                      concentration dependence, their net effect is nearly
                      constant throughout the entire concentration range,
                      resulting in approximately equal transport and transference
                      numbers, despite a monitored cross-over from carbonate-based
                      lithium coordination to a TFSI-based ion coordination. In
                      addition, though dynamical ion correlation could be found,
                      the absolute values of the ionic conductivity are
                      essentially determined by the overall viscosity of the
                      electrolyte. The IL/carbonate blends with a Pyr14TFSI
                      fraction of ∼10 $wt\%$ are found to be promising
                      electrolyte solvents, with ionic conductivities and lithium
                      ion transference numbers comparable to those of standard
                      carbonate-based electrolytes while the thermal and
                      electrochemical stabilities are considerably improved. In
                      contrast, the choice of the conducting salt only marginally
                      affects the transport properties.},
      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:29873343},
      UT           = {WOS:000436032900029},
      doi          = {10.1039/C8CP01485J},
      url          = {https://juser.fz-juelich.de/record/845915},
}