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Kerner, Manfred,Lim, Du-Hyun,Jeschke, Steffen,Rydholm, Tomas,Ahn, Jou-Hyeon,Scheers, Johan Elsevier 2016 Journal of Power Sources Vol.332 No.-
<P><B>Abstract</B></P> <P>The overall safety of Li-ion batteries is compromised by the state-of-the-art electrolytes; the thermally unstable lithium salt, lithium hexafluorophosphate (LiPF<SUB>6</SUB>), and flammable carbonate solvent mixtures. The problem is best addressed by new electrolyte compositions with thermally robust salts in low flammability solvents. In this work we introduce electrolytes with either of two lithium nitrile salts, lithium 4,5-dicyano-1,2,3-triazolate (LiDCTA) or lithium 4,5-dicyano-2-trifluoromethylimidazolide (LiTDI), in solvent mixtures with high flashpoint adiponitrile (ADN), as the main component. With sulfolane (SL) and ethylene carbonate (EC) as co-solvents the liquid temperature range of the electrolytes are extended to lower temperatures without lowering the flashpoint, but at the expense of high viscosities and moderate ionic conductivities. The anodic stabilities of the electrolytes are sufficient for LiFePO<SUB>4</SUB> cathodes and can be charged/discharged for 20 cycles in Li/LiFePO<SUB>4</SUB> cells with coulombic efficiencies exceeding 99% at best. The excellent thermal stabilities of the electrolytes with the solvent combination ADN:SL are promising for future electrochemical investigations at elevated temperatures (> 60 °C) to compensate the moderate transport properties and rate capability. The electrolytes with EC as a co-solvent, however, release CO<SUB>2</SUB> by decomposition of EC in presence of a lithium salt, which potentially makes EC unsuitable for any application targeting higher operating temperatures.</P> <P><B>Highlights</B></P> <P> <UL> <LI> Solvents and salts with nitrile groups are combined into novel electrolytes. </LI> <LI> Sulfolane in adiponitrile provides thermally stable, high flashpoint electrolytes. </LI> <LI> LiDCTA and LiTDI electrolytes have high oxidation stability (4.5 V vs Li+/Li°). </LI> <LI> Ethylene carbonate is decomposed into CO2 in the presence of lithium salt. </LI> </UL> </P> <P><B>Graphical abstract</B></P> <P>[DISPLAY OMISSION]</P>