Lithium Dendrite Suppression and Enhanced Interfacial Compatibility Enabled by an Ex Situ SEI on Li Anode for LAGP-Based All-Solid-State Batteries

Abstract

The electrode–electrolyte interface stability is a critical factor influencing cycle performance of All-solid-state lithium batteries (ASSLBs). Here, we propose a LiF- and Li3N-enriched artificial solid state electrolyte interphase (SEI) protective layer on metallic lithium (Li). The SEI layer can stabilize metallic Li anode and improve the interface compatibility at the Li anode side in ASSLBs. We also developed a Li1.5Al0.5Ge1.5(PO4)3–poly­(ethylene oxide) (LAGP-PEO) concrete structured composite solid electrolyte. The symmetric Li/LAGP-PEO/Li cells with SEI-protected Li anodes have been stably cycled with small polarization at a current density of 0.05 mA cm–2 at 50 °C for nearly 400 h. ASSLB-based on SEI-protected Li anode, LAGP-PEO electrolyte, and LiFePO4 (LFP) cathode exhibits excellent cyclic stability with an initial discharge capacity of 147.2 mA h g–1 and a retention of 96% after 200 cycles.

Design of a Multifunctional Interlayer for NASCION‐Based Solid‐State Li Metal Batteries

“…b) Voltage profiles of symmetric cells with LAGP‐IL interlayer operated at a high current density, 1.0 mA cm −2 , and a high capacity density of 1.0 mAh cm −2 . c) Comparison of cycling performance of symmetric cell with LAGP‐IL interlayer with that of recent publications [ 23,25–28,50–57 ] (a‐ref. [50], b‐ref.…”

Synthesis and Properties of NaSICON‐type LATP and LAGP Solid Electrolytes

“…Later, LAGP (x = 0.5)/PPC-LiFSI (PPC = poly(propylene carbonate), LiFSI = lithium bis(fluorosulfonyl)imide)c omposite solide lectrolyte was studied. Ci et al [105] mixed LAGP (from melt quenching) with PEO to form ac omposite solid electrolyte, which exhibited an ionic conductivity of 0.9 10 À4 Scm À1 at 50 8C. Ci et al [105] mixed LAGP (from melt quenching) with PEO to form ac omposite solid electrolyte, which exhibited an ionic conductivity of 0.9 10 À4 Scm À1 at 50 8C.…”

“…[106] The full battery (Li as the anode, LFP as the cathode) showeda stable charge/discharge capacity (138.3 mAh g À1 at 0.1C)a nd high capacity retention of 97.1 %a fter 100 cycles. Ci et al [105] mixed LAGP (from melt quenching) with PEO to form ac omposite solid electrolyte, which exhibited an ionic conductivity of 0.9 10 À4 Scm À1 at 50 8C. The assembled batteries with a structureo fL i(SEI)/LAGP-PEO/LFP (SEI = solid-electrolyte interphase) exhibited excellent cyclic stability, with an initial discharge capacity of 147.2 mAh g À1 and ar etention of 96 %a fter 200 cycles.…”

Reducing interfacial resistance of a Li1.5Al0.5Ge1.5(PO4)3 solid electrolyte/electrode interface by polymer interlayer protection

“…17 To address these challenges, polymer electrolyte layers were proposed to protect the ceramic layer from directly contacting the lithium metal and uniform the Li + ux on the lithium surface, which inhibit lithium dendrite nucleation. [18][19][20][21][22][23][24][25] Moreover, gel electrolyte interlayers were introduced in ceramic-based solid state batteries, which displayed a remarkable wettability toward the Li surface, with high ionic conductivity at room temperature thanks to the composition of the polymer and liquid. 26,27 However, a detailed analysis of the interfacial resistance of the multilayer LAGPbased composite electrolyte has been rarely reported, and the interaction between the ceramic layer and the polymer layer has yet to be understood.…”