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The importance of batteries to sustainable energy is widely recognized. Lithium-ion batteries (LIBs) not only power handheld electronics but also are increasingly being implemented in electric vehicles and \"smart-grid\" applications to store energy from intermittent solar and wind sources, making sustainable energy a reality. Unfortunately, LIBs contain a highly flammable solvent and can exhibit catastrophic failure, as was brought to the public's attention by the Boeing 787, Samsung Galaxy Note 7, hoverboard, and Tesla battery fires. Thus, realizing the full potential of LIBs in large-scale systems requires the development of nonflammable electrolytes. Perfluoropolyether (PFPE)-based electrolytes address many of the shortcomings of conventional carbonate-based electrolytes or polymer electrolytes such as poly(ethylene oxide). PFPE-based electrolytes transport lithium more efficiently than conventional electrolytes, which has important implications on long-term battery performance. PFPEs make interesting electrolyte solvents because they are nonflammable, nonvolatile, liquid across a broad temperature range, chemically stable, and interact favorably with the anion of fluorinated salts. In this work, the molecular underpinnings for ion transport in PFPE electrolytes will be established by systematically probing how PFPE structure affects electrolyte performance including ionic conductivity, diffusivity, and transference number. End group polarity, end group concentration, and PFPE molecular weight all have important implications on electrolyte performance. 781b155fdc