In situ Interlock Interface through Facial Makeup of Quasi‐Solid Electrolyte with Silver Gauze Enabling Uniform Lithium Nucleation and Tip Potential Distribution

ABSTRACT Quasi‐solid polymer electrolyte (QSPE) matching lithium metal anode (LMA) enables high energy density and safety of solid‐state lithium metal battery (SSLMB). However, lithium dendrite growth is a key bottleneck for SSLMB practical application, which is attributed to the uneven lithium deposition. The non‐uniform lithium nucleation and “tip effect” induced uneven potential distribution are the primary causes. Herein, we propose to in situ construct an interlock interface through QSPE (PPAIA) with facial silver (Ag) gauze makeup immediate contacting with LMA. Li‐Ag alloy is in situ formed through the immediate contact of Ag in PPAIA with LMA, which decreases the nucleation barrier to uniform lithium nucleation thermodynamically. And the electronic conductive Ag is directly exposed around the Li nuclei to disperse accumulated charges and uniform tip potential distribution, leading to homogeneous Li ions diffusion kinetically. Consequently, homogeneous Li deposition solves the lithium dendrite growth problem. The Li||Li symmetric cell operates stably for 600 h at 0.2 mA cm −2 . The LFP||Li battery retains 95% initial capacity after 850 cycles at 1 C, and the NCM811||Li battery maintains 83% capacity retention after 800 cycles at 0.5 C. This research opens a new avenue for addressing the lithium dendrite growth issue by in situ formed interlock interface between QSPE and LMA.