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Although various types of nanoparticle have been ubiquitously employed as additives to promote the practical performances of composite polymer electrolytes (CPEs) in lithium-ion batteries, the influence of the type of chemical bond between the core and canopy of the modified nanoparticle on the properties of CPEs has rarely been investigated. Herein, two types of nanoparticle additive, namely, ionic bond modified nanoparticles (IBNs) and covalent bond modified nanoparticles (CBNs), were prepared conveniently based on nanosilica with different particle sizes in order to optimize the overall performance of the electrolyte. Furthermore, the CPEs were fabricated by doping IBNs or CBNs as well as lithium salts within a poly(ethylene oxide) matrix and their electrochemical properties were investigated. The dramatic enhancement of the ionic conductivity of the CPEs resulted from the addition of fillers into the system, and the improvement became more significant when the fillers were IBNs that used the smaller silica nanoparticle as the core segment, due to the increased chain mobility, as estimated by the smaller Tg value. Moreover, a broad electrochemical stability window was obtained in the presence of IBNs, and the lithium-ion transference number of the system containing lithium bis(trifluoromethanesulfonimide), which has large anions in the structure, was almost two times higher than the CPEs using lithium perchlorate as the lithium source. Therefore, the synergistic effects of the filler structures and the electrolyte compositions are the key factors to improve the electrochemical performances of CPEs.

Solid polymer electrolyte based on ionic bond or covalent bond functionalized silica nanoparticles