Solid-state lithium (Li) batteries promise both high energy density and safety while existing solid-state electrolytes (SSEs) fail to satisfy the rigorous requirements of battery operations. Herein, novel polyoxometalate SSEs, Li PW O and Li PMo O , are synthesized, which exhibit excellent interfacial compatibility with electrodes and chemical stability, overcoming the limitations of conventional SSEs. A high ionic conductivity of 0.89 mS cm and a low activation energy of 0.23 eV are obtained due to the optimized three-dimensional Li migration network of Li PW O . Li PW O exhibits a wide window of electrochemical stability that can both accommodate the Li anode and high-voltage cathodes. As a result, all-solid-state Li metal batteries fabricated with Li/Li PW O /LiNi Co Mn O display a stable cycling up to 100 cycles with a cutoff voltage of 4.35 V and an areal capacity of more than 4 mAh cm , as well as a cost-competitive SSEs price of $5.68 kg . Moreover, Li PMo O homologous to Li PW O was obtained via isomorphous substitution, which formed a low-resistance interface with Li PW O . Applications of Li PW O and Li PMo O in Li-air batteries further demonstrate that long cycle life (650 cycles) can be achieved. This strategy provides a facile, low-cost strategy to construct efficient and scalable solid polyoxometalate electrolytes for high-energy solid-state Li metal batteries.
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