Achieving stable lithium metal anodes via the synergy of electrostatic shielding and the high Li+ flux inorganic interphase

Jiangtao Yu¹,Xinyu Ma¹,Xiuyang Zou²,Yin Hu¹,Mingchen Yang¹,Jinhua Yang¹,Shipeng Sun¹,Feng Yan(严锋)^1,3*

¹College of Chemistry, Chemical Engineering and Materials Science, SoochowUniversity, Suzhou, 215123, China.

²School of Chemistry and Chemical Engineering, Huaiyin Normal University, Huaian 223300, China

³State Key Laboratory for Modification of Chemical Fibers and Polymer Materials, College of Materials Science and Engineering, Donghua University, Shanghai, China

Energy Environ. Sci.,2024,17, 4519-4530

Abstract:Uncontrolled dendrite growth and slow Li⁺transport kinetics at the anode/electrolyte interface severely hamper the practical applications of lithium metal batteries (LMBs). Herein, a high-charge density cationic polymer, poly(octaallyltetraazacyclo-decane nitrate) (POTA-NO₃), was developed as an anodic protective layer to moderate Li⁺deposition and enhance Li⁺transport efficiency. According to Li⁺deposition characteristics and simulation, POTA-NO₃with multiple positive charge sites provided excellent electrostatic shielding and enhanced Li⁺desolvation process to the anodes. Meanwhile, anions generated a robust and high Li⁺flux inorganic SEI to inhibit the polymer cationic layer and electrolyte decomposition. With the POTA-NO₃protective layer, Li||Li symmetric batteries achieved a stable cycling of 6300 h at a high current density of 5 mA cm^-2with a capacity of 5 mA h cm^-2. Furthermore, the POTA-NO₃-protected Li||LiCoO₂batteries exhibited a capacity retention of over 80% after 1400 long-term cycles at 1C. This work opens up the possibility for the development of stable lithium anodes.

链接：https://pubs.rsc.org/en/content/articlelanding/2024/ee/d4ee00399c