Low Resistance–Integrated All‐Solid‐State Battery Achieved by Li₇La₃Zr₂O₁₂ Nanowire Upgrading Polyethylene Oxide (PEO) Composite Electrolyte and PEO Cathode Binder

Abstract

All-solid-state lithium metal battery is the most promising next-generation energy storage device. However, the low ionic conductivity of solid electrolytes and high interfacial impedance with electrode are the main factors to limit the development of all-solid-state batteries. In this work, a low resistance-integrated all-solid-state battery is designed with excellent electrochemical performance that applies the polyethylene oxide (PEO) with lithium bis(trifluoromethylsulphonyl)imide as both binder of cathode and matrix of composite electrolyte embedded with Li 7 La 3 Zr 2 O 12 (LLZO) nanowires (PLLN). The PEO in cathode and PLLN are fused at high temperature to form an integrated all-solid-state battery structure, which effectively strengthens the interface compatibility and stability between cathode and PLLN to guarantee high efficient ion transportation during long cycling. The LLZO nanowires uniformly distributed in PLLN can increase the ionic conductivity and mechanical strength of composite electrolyte efficiently, which induces the uniform deposition of lithium metal, thereby suppressing the lithium dendrite growth. The Li symmetric cells using PLLN can stably cycle for 1000 h without short circuit at 60 °C. The integrated LiFePO 4 /PLLN/Li batteries show excellent cycling stability at both 60 and 45 °C. The study proposed a novel and robust battery structure with outstanding electrochemical properties.

High-Performance 3-D Fiber Network Composite Electrolyte Enabled with Li-Ion Conducting Nanofibers and Amorphous PEO-Based Cross-Linked Polymer for Ambient All-Solid-State Lithium-Metal Batteries

“…The Li deposition first helped improve the interfacial contact by filling the interfacial gaps, while continuous Li deposition led to diminished interfacial contact and resulted in decreased Coulombic efficiency in latter cycles. Similar trend was also observed in solid-state LiFePO 4 batteries using PEO-based solid electrolytes [54][55][56][57]. Overall, the Coulombic efficiency is 97.8% after 100 cycles.…”

Liquid Polydimethylsiloxane Grafting to Enable Dendrite‐Free Li Plating for Highly Reversible Li‐Metal Batteries

“…Modifying the electrolyte separator by loading functional or polar paste to adsorb or react with bigger anions of solute would achieve a higher Li‐ion transport number and therefore homogenous Li plating . Applying high‐module solid or quasi‐solid electrolyte can mechanically suppress the Li dendrite growth, however under a cost of low ionic conductivity and high interfacial barrier. Modulating the SEI components by adding electrolyte additives of low content appears to be a facile solution to reinforce the SEI film and therefore retard the Li protuberance.…”

High Uptake and Fast Transportation of LiPF6 in a Porous Aromatic Framework for Solid‐State Li‐Ion Batteries

“…The voltage versus time profiles of the battery under each current density corresponding to the rate capacity test were shown in Figure e. The voltage profiles were very stable, and there was no obvious fluctuation under different current densities, indicating good circularity and stable interface of the battery . Figure f further compares the cycling performance LiFePO 4 ∥LiPF 6 @ PAF‐1∥Li cell and other SSLIBs that have been well studied. LiFePO 4 ∥LiPF 6 @PAF‐1∥Li cell exhibits high capacity with robust electrochemical stability and importantly, it sustained rigorous long‐term current density as high as 4C.…”

“…f) Cycling performance of Li/LiFePO 4 cells with other SSEs and LiPF 6 @PAF‐1 in long term cycles (first 100 cycles). (LLZO‐containing PCPSE, CPMEA‐LATP base PCPSE, Cathode‐supported PPAL, PEO 20 ‐LiTFSI‐MXene 0.02 , LPC@UM, PLLN …”