Li-O₂ batteries have been recently considered as next generation of energy storage systems for electric vehicle application due to their high specific energy densities, which are comparable to gasoline [1]. Li-O₂ batteries however suffer poor cycling and reachability due to a sever electrolyte decomposition [2]. It has been shown that the electrolyte decomposition by-products such as lithium carbonate species gradually cover the surface of cathodes and shuts down the batteries quickly [3]. Although many attempts have been made to overcome the detrimental formation of these carbonate species on the surface of cathode, their formation and electrolyte instability still remains a very big challenge in this filed [4]. Recently, it has been reported that tailoring the coordination of Li ion and solvent molecules in Li-O₂ battery electrolytes is a promising method to improve the electrolyte stabilities [5,6].

In this study, we report that the inclusion of inorganic fillers in gel polymer electrolytes using different salt concentration can reduce the electrolyte decomposition by-products such as lithium carbonate species during the Li-O₂ battery cycling. The improved electrochemical performance of Li-O₂ batteries can be attributed to the interaction of filler with Li salt which in turn can tailor the interaction of Li ion and solvent molecules. To asses our hypothesis different electrochemical tests including in-depth electrochemical impedance spectroscopy, lithium transference number measurements along with other characterization methods such as Raman spectroscopy has been used.

[1] G. Girishkumar, B. McCloskey, A.C. Luntz, S. Swanson, W. Wilcke, Lithium-air battery: Promise and challenges, J. Phys. Chem. Lett. 2010,1, 2193–2203.

[2] B. D. McCloskey, C. M. Burke, J. E. Nichols and S. E. Renfrew, Chem. Commun., 2015, 51, 12701–12715

[3] S. A. Freunberger, Y. Chen, N. E. Drewett, L. J. Hardwick, F. Bardé and P. G. Bruce, Angew. Chemie - Int. Ed., 2011, 50, 8609–8613

[4] R. Younesi, G.M. Veith, P. Johansson, K. Edstrom, T. Vegge, Lithium salts for advanced lithium batteries: Li-metal, Li-O2, and Li-S, Energy Environ. Sci.,2015, 8, 1905–1922.

[5] F. Li, T. Zhang, Y. Yamada, A. Yamada and H. Zhou, Adv. Energy Mater., 2013, 3, 532–538.

[6] B. Liu, W. Xu, P. Yan, X. Sun, M. E. Bowden, J. Read, J. Qian, D. Mei, C. M. Wang and J. G. Zhang, Adv. Funct. Mater., 2016, 26, 605–613.