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Lithium salts with low coordinating anions likebis(trifluoromethanesulfonyl)imide (TFSI) have been the state-of-the-art forPEO-based 'dry' polymer electrolytes for three decades. Plasticizing PEO withTFSI-based ionic liquids (ILs) to form ternary solid polymer electrolytes(TSPEs) increases conductivity and Li$^+$ diffusivity. However, the Li$^+$transport mechanism is unaffected compared to their 'dry' counterpart andessentially coupled to the dynamics of the polymer host matrix, which limitsLi$^+$ transport improvement. Thus, a paradigm shift is hereby suggested: Theutilization of more coordinating anions such astrifluoromethanesulfonyl-N-cyanoamide (TFSAM), able to compete with PEO forLi$^+$ solvation to accelerate the Li$^+$ transport and reach higher Li$^+$transference number. The Li-TFSAM interaction in binary and ternary TFSAM-basedelectrolytes was probed by experimental methods and discussed in the context ofrecent computational results. In PEO-based TSPEs, TFSAM drastically acceleratesthe Li$^+$ transport (increased Li$^+$ transference number by 600$\%$ andLi$^+$ conductivity by 200-300$\%$) and computer simulations reveal thatlithium dynamics are effectively re-coupled from polymer to anion dynamics.Finally, this concept of coordinating anions in TSPEs was successfully appliedin LFP$||$Li metal cells leading to enhanced capacity retention (86$\%$ after300 cycles) and an improved rate performance at 2C.

Are Weakly Coordinating Anions Really the Holy Grail of Ternary Solid  Polymer Electrolytes Plasticized by Ionic Liquids? Coordinating Anions to the  Rescue of the Lithium Ion Mobility