An ultrathin conformal layer of dry-coated Li+-conductive glass–ceramic for single-crystalline nickel-rich cathode towards all-solid-state lithium batteries

• Published in: Chemical engineering journal (Lausanne, Switzerland : 1996) Switzerland : 1996), 2025-01, Vol.503, p.158152, Article 158152
• Main Authors: Wang, Yaping, Ding, Jianxiang, Liu, Xiong Xiong, Cao, Mufan, Gao, Min, Pan, Long, Sun, ZhengMing
• Format: Article
• Language: English
• Subjects: Dry coating; Glass–ceramic phosphates; Interfacial stability; Single-crystalline nickel-rich cathode; Sulfide solid electrolyte
• ISSN: 1385-8947
• DOI: 10.1016/j.cej.2024.158152

•Ultrathin GCP coating achieved via cost-effective dry processing due to glass-ceramic's unique fusibility.•GCP coating inhibits sulfide oxidation, enhances charge transfer, and boosts Li+ diffusion.•SCNCM@GCP retains 86.1% capacity after 100 cycles, with an initial capacity of 161.9 mAh g⁻¹ at 0.2C. All-solid-state lithium batteries pairing nickel-rich oxide cathodes with nonflammable solid electrolytes deliver greatly combined safety and high-energy–density merits. However, the oxide cathodes possess high oxidability and easily oxidize solid electrolytes, such as sulfides and polymers, leading to great interfacial resistance and rapid performance degradation. Herein, by employing single-crystalline LiNi0.83Co0.11Mn0.06O2 (SCNCM) as typical oxide cathode, we propose a Li+-conductive glass–ceramic phosphate (GCP) as an ultrathin conformal layer using a cost-effective dry processing strategy. The GCP conformal layer possesses triple appealing advantages: (i) GCP melts at a relatively low temperature (∼790 °C) and spreads out to improve the coating coverage, effectively blocking the interfacial oxidation of solid electrolyte by high-oxidative cathode. (ii) The melted GCP adheres tightly to the cathode surface, alleviating the delamination of coating layer on the cathode during long-term cycling. (iii) GCP possesses excellent Li+ conductivity of 0.29 mS cm−1, facilitating the charge transfer and Li+ diffusion processes. These functions contribute to diminishing interfacial resistance increases across cycling, improving longterm cycling stability of SCNCM cathodes. Consequently, the SCNCM@GCP shows excellent interfacial stability with sulfide solid electrolyte, possessing an outstanding capacity retention of 86.1 % after 100 cycles with a high initial specific discharge capacity of 161.9 mAh/g at 0.2C (72.4 % and 130.2 mAh/g for SCNCM).