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Abstract
A new class of freestanding cross-linked hybrid polymer electrolytes (HPEs) with POSS as the cross-linker was prepared by a one-step free radical polymerization reaction. Octavinyl octasilsesquioxane (OV-POSS) with eight functional corner groups was used to provide cross-linking sites for the connection of polymer segments and the required mechanical strength to separate the cathode and anode. The unique cross-linked structure offers additional free volume for the motion of EO chains and provides fast and continuously interconnected ion-conducting channels along the nanoparticles/polymer matrix interface. The HPE exhibits the highest ionic conductivity of 1.39 × 10−3 S cm−1, as well as excellent interfacial compatibility with the Li electrode at 80°C. In particular, LiFePO4/Li cells based on the HPE deliver good rate capability and long-term cycling performance with an initial discharge capacity of 152.1 mAh g−1 and a capacity retention ratio of 88% after 150 cycles with a current density of 0.5 C at 80°C, demonstrating great potential application in high-performance LIBs at elevated temperatures.
Highlights
Lithium ion batteries (LIBs) have attracted intensive attention by virtue of the high output voltage, low self-discharge rate, large energy density, no memory effect, and environmental friendly nature (Dunn et al, 2011; Qu et al, 2014; Xu, 2014; Zhang et al, 2018)
Different from most of the reported polymer electrolytes with POSS as a nanofiller, here a new class of freestanding cross-linked hybrid polymer electrolytes (HPEs) membranes with POSS as the cross-linker was prepared by a one-step free radical polymerization reaction based on our previous work (Zhang et al, 2016b)
Where Ii+j represents the integral area of the resonance peaks at 5.88–6.07 ppm from the unreacted vinyl protons of POSS, Ia represents the integral area of the resonance peaks at 1.92 ppm from the reacted vinyl protons of POSS, Ie represents the integral area of the resonance peak of protons from CH2 units in SMA segments at 1.23 ppm and Ig represents the integral area of the resonance peak from the protons of CH2-CH2-O (EO) units in PEGMEM segments at 3.41–4.32 ppm
Summary
Lithium ion batteries (LIBs) have attracted intensive attention by virtue of the high output voltage, low self-discharge rate, large energy density, no memory effect, and environmental friendly nature (Dunn et al, 2011; Qu et al, 2014; Xu, 2014; Zhang et al, 2018). The HPE containing 5 wt.% POSS exhibits the highest ionic conductivity of 3.94 × 10−5 S cm−1 at 25◦C and 1.39 × 10−3 S cm−1 at 80◦C, much higher than that of the PEGMEM/SMA polymer electrolyte (Table 2) and other PEO based solid polymer electrolytes (Table S1).
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