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Stable solid electrolyte interphase (SEI) with high Li+‐ion conductivity is desperately desired for lithium (Li) metal anodes. However, it remains challenging to build a robust SEI rationally for the Li‐metal anodes in carbonate electrolytes. Herein, a heterogeneous nitride‐rich SEI that consists of organic nitrides on the surface and inorganic nitrides inside by stepwise‐reduction electrolyte design is constructed. The heterogeneous structure endows SEI with the capability to capture and distribute Li+ on the surface and facilitate internal Li+ transportation, leading to the redistributed Li+ flux and uniform Li electrodeposition. With the newly‐formulated carbonate electrolyte, Li||Cu cells deliver a high Coulombic efficiency of 98.0% after 300 cycles at 0.5 mA cm‐2 and 0.5 mAh cm‐2. Meanwhile, superb cycling stability is also determined with full Li‐metal cells using LiNi1/3Mn1/3Co1/3O2 and high‐loading LiFePO4 (12.0 mg cm−2) cathodes. This study provides a promising strategy to regulate the SEI components and stabilize the Li anodes by rational electrolyte design. [ABSTRACT FROM AUTHOR]

Herein, nanosized fumed silica (FS) with poor electrical conductivity is used as an "electron inhibitor" between Li metal and garnet solid electrolyte (SE) to prevent lithium dendrite growth. The FS demonstrated its effectiveness in preventing the fast lithium dendrite propagation during the long-term lithium stripping and plating processes, leading to an enhanced battery performance. We believe this study could help shed light on such electron inhibitors in constructing all-solid-state batteries (ASSBs) with superior cycling performance. [ABSTRACT FROM AUTHOR]