Lithium dendrite prevention for wide-temperature-range solid-state batteries

Benefiting from their high theoretical capacity and extremely negative potential, lithium metal anodes (LMAs) are considered the “holy grail” in the high-energy all solid-state lithium-metal battery (ASSLMB) industry. However, commercialization of ASSLMBs has been hindered by severe interfacial reactions and the growth of crystalline Li dendrites throughout the cycling process. Here, we successfully suppressed the nucleation and growth of Li crystals by introducing polydopamine (PDA) into Li₅.₅PS₄.₅Cl₁.₅ (LPSCl) electrolyte. After the charging process, a uniformly distributed amorphous Li layer was obtained, accompanied by numerous LiOH nanocrystals. Both experimental observations and theoretical calculations confirmed that the hydroxyl radicals from PDA are crucial for preventing the formation of Li dendrites. In addition, the PDA-coated LPSCl particles facilitate the formation of an organic-inorganic hybrid SEI during electrochemical cycling, thereby reinforcing interfacial mechanical integrity and enhancing Li⁺ conduction. Compared to conventional Li batteries, the PDA1 %-LPSCl-based batteries demonstrated superior electrochemical performance over 1000 cycles at a rate of 0.8 C with a capacity retention of 80.0 %. Furthermore, the proposed battery delivers 157.6 mAh g⁻¹ at −30°C (0.1 C), demonstrating exceptional low-temperature operability. Therefore, this work offers valuable insights for enhancing the performance and reliability of future battery technologies.