Construction of composite lithium with high adhesion work and fast ionic conductivity by black phosphorus for solid-state lithium batteries

• Published in: Nano energy 2024-12, Vol.132, p.110356, Article 110356
• Main Authors: Li, Zongyang, Tang, Desha, Wang, Wenjie, Li, Chen, Deng, Rongrui, Fang, Yongheng, Wang, Yumei, Xu, Chaohe, Wang, Ronghua
• Format: Article
• Language: English
• Subjects: Adhesion work; Li+ diffusion coefficient; Lithium composite anode; LLZTO; Solid-state lithium metal batteries
• ISSN: 2211-2855
• DOI: 10.1016/j.nanoen.2024.110356

Li6.4La3Zr1.4Ta0.6O12 (LLZTO) based solid-state lithium metal batteries (SSLMBs) have a broad application prospect because of the nonflammable nature as well as the high energy density. However, the loose contact and the contact degradation of Li/LLZTO in the stripping process result in the serious lithium dendrites growth. Herein, these issues are addressed by a composite lithium anode (CLA), which is prepared through the reaction between black phosphorus and molten lithium. In comparison to pure lithium, a higher adhesion work (722.67 mJ m−2) and Li+ diffusion coefficient (2.45×10−12 cm2 s−1) are achieved for CLA, thus assuring the intimate interfacial contact of CLA/LLZTO interface during the lithium stripping process. As a result, a small interfacial resistance of 3.7 Ω cm2, a high critical current density of 1.5 mA cm−2, and extra-long cycle life of 8200 h at 0.3 mA cm−2 are achieved for CLA symmetric cell at 25 ºC. More importantly, the full cell coupled with high mass loading LiFePO4 cathode (10.6 mg cm−2) still shows a large discharge capacity of 156.3 mAh g−1 and cycles stably at 25 ºC. This work provides an alternative approach to develop the long lifespan and high capacity of SSLMBs. [Display omitted] •Composite lithium anode with large Li+ diffusion coefficient was constructed by adding black phosphorus into molten lithium.•The in-situ formed Li3P can strengthen the initial interfacial contact and promote the Li+ diffusion coefficient of lithium.•The composite lithium shows lower interfacial tension of 364.1 mN m−1 and higher adhesion work of 722.67 mJ m−2 to LLZTO.•The full cell coupled with high mass loading LiFePO4 cathode delivers a large discharge capacity of 156.33 mAh g–1 at 25 ºC.