Silicon-based
materials have been regarded as the most promising
anodes for high-energy batteries, when combined with high- voltage/capacity
nickel-rich layered cathodes. However, challenges arise from unstable
electrode/electrolyte interphases on the anode and cathode as well
as from safety hazards associated with highly flammable commercial
electrolytes. Herein, we rationally design a nonflammable cyclic phosphate-based
electrolyte to tune the electrode/electrolyte interphase components
by controlling the reduction of a cyclic phosphate and Li salt. This
strategy enables the electrolyte to form a highly elastic, robust
inorganic–polymeric interphase on microsized silicon-based
anodes that can accommodate the immense volume changes. Furthermore,
by generating a stable polymeric interphase on the surface of the
cathode as well, a SiO|LiNi0.6Mn0.2Co0.2O2 cell demonstrated an extremely high energy density of ∼590
Wh·kg–1 with 71.4% capacity retained over 300
cycles and high Coulombic efficiency of 99.9%. This interfacial regulation
strategy is of vital importance for designing new electrolytes for
high-energy-density batteries.
The Li dendrite issue is the major barrier that limits the implement of Li metal anode practically, especially at high current density. From the perspective of the nucleation and growth mechanism of the Li dendrite, we rationally develop a novel Prussian blue analogues (PBA)-derived separator, where tuning the metal ions bestows the PBAs with open metal site to confine anion movement and thereby afford a high Li + transference number (0.78), and PBA with ordered micropores could act as an ionic sieve to selectively extract Li + and thereby homogenize Li + flux. This demonstrates a highly reversible Li plating/stripping cycling for 3000 h at a practically high current density (5.0 mA cm −2 ). Consequently, a high loading Li||LiFeO 4 battery (∼10.0 mg cm −2 ) demonstrates ultralong cycling life at high current densities (∼5.1 mA cm −2 ). This work highlights the prospect of optimizing PBAs in regulating ion transport behavior to enable high-power Li metal batteries.
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