Developing High-Energy, Stable All-Solid-State Lithium Batteries Using Aluminum-Based Anodes and High-Nickel Cathodes

Abstract

Aluminum (Al) exhibits excellent electrical conductivity, mechanical ductility, and good chemical compatibility with high-ionic-conductivity electrolytes. This makes it more suitable as an anode material for all-solid-state lithium batteries (ASSLBs) compared to the overly reactive metallic lithium anode and the mechanically weak silicon anode. This study finds that the pre-lithiated Al anode demonstrates outstanding interfacial stability with the Li₆PS₅Cl (LPSCl) electrolyte, maintaining stable cycling for over 1200 h under conditions of deep charge–discharge. This paper combines the pre-lithiated Al anode with a high-nickel cathode, LiNi_0.8Co_0.1Mn_0.1O₂, paired with the highly ionic conductive LPSCl electrolyte, to design an ASSLB with high energy density and stability. Using anode pre-lithiation techniques, along with dual-reinforcement technology between the electrolyte and the cathode active material, the ASSLB achieves stable cycling for 1000 cycles at a 0.2C rate, with a capacity retention rate of up to 82.2%. At a critical negative-to-positive ratio of 1.1, the battery’s specific energy reaches up to 375 Wh kg⁻¹, and it maintains over 85.9% of its capacity after 100 charge–discharge cycles. This work provides a new approach and an excellent solution for developing low-cost, high-stability all-solid-state batteries.