Developing solid polymer electrolytes (SPEs) has been proved to be a promising way to realize the commercialization of solid lithium batteries. Compared between different types of polymer structures, previous studies have shown that polyether based SPEs (e.g. polyethylene oxide) with network structure reveal good balance between ionic conductivity and mechanical strength, strong capability to suppress lithium dendrite growth and elongate cycling life, and good compatibility with commercialized lithium iron phosphate (LFP) cathode. However, there are still several drawbacks limiting the further progress in battery use. First, the strong binding between lithium ions and ether groups lowers lithium ion transference number and thus reduces the tolerant current density in lithium plating/stripping. Second, the low oxidative decomposition voltage of polyether prevents its application in high power batteries. Third, the defects occurred during crosslinking will behave as weak points which could render the break of the network and thus decrease the cycling life. To further push forward the performance, we developed SPEs with interpenetrating network structure based on our previously reported PEO single network. In order to address the above drawbacks, we selected different types of second networks with specific functions, respectively. The incorporation of poly(propylene carbonate) (PPC) can triply increase the lithium ion transference number, modify the solid electrolyte interface (SEI) and make it be stably cycled under a state-of-the-art high current density. The involvement of poly(acrylonitrile) (PAN) can improve the anodic oxidative voltage to over 5 V and make the SPE workable in NMC batteries. The addition of ultra-high molecular weight PEO in the network can extensively increase the toughness and triply elongate the cycling life. In addition, the application of our network SPE is not limited in lithium battery field. It can also support the stable cycling with metallic sodium electrode. The full solid battery using our SPE and δ-NaxV2O5 cathode can deliver a state-of-the-art high capacity of 305 mAh g-1. In summary, we believe our study on SPE networks could enlighten the future development of solid batteries from the perspective of both chemistry and structure.

Designing solid polymer electrolyte networks for high performance lithium batteries and beyond

Macromolecular Chemistry: The Second Century

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ACS Spring 2020 National Meeting & Expo

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