Enhanced Interphase Ion Transport via Charge-Rich Space Charge Layers for Ultra-Stable Solid-State Lithium Metal Batteries

Li, Jin1; Chen, Junjie1; Xu, Xiaosa1; Wang, Zhenyu1; Shen, Jiadong1; Sun, Jing1; Huang, Baoling1; Zhao, Tianshou1,2

2024-09-01

10.1002/aenm.202402746

ADVANCED ENERGY MATERIALS   影响因子和分区

1614-6832

1614-6840

["The significant interfacial resistance between solid electrolyte-electrode interfaces is a major bottleneck for the practical application of solid-state lithium batteries. This resistance is primarily caused by the formation of space charge layers (SCLs), resulting from the redistribution of ionic carriers at the interface between dissimilar materials with varying chemical potentials, which lead to insufficient carriers and sluggish lithium-ion transport. In this study, a conjugated structure polymer is constructed through in situ polymerization onto the oxide electrolyte, forming charge-rich SCLs on the organic/inorganic interface, and enabling the interfacial layer to maintain superior ion transfer and contact. The Li solid NMR spectra and computational study suggest that optimized SCLs offer effective pathways for Li+ conduction in the electrolyte, thereby enhancing the interfacial conduction. Furthermore, the designed electrolyte induces the formation of an inorganic-rich interphase layer on the lithium anode, enabling rapid lithium-ion transport and uniform Li deposition. Consequently, the lithium symmetric cell with this electrolyte operates for more than 5100 h, while LiFePO4/Li solid-state batteries can stably cycle up to 800 times at 5 C. This interfacial modification strategy provides a new perspective for the rational design of the charge-rich SCLs and advances the understanding of the SCLs inside the electrolyte.","This study introduces a simple and scalable method for designing high-conductive composite polymer electrolytes by forming charge-rich space charge layers. The conjugated structure polymer (P-DOL) coated LLZTO (Li6.4La3Zr1.4Ta0.6O12) compositing with PVDF-HFP modulate Li+ transport pathways and strengthen the electrode/electrolyte interfacial compatibility. With these advantages, the composite electrolyte leads to a superior interfacial stability and lithium stripping/plating kinetics. image"]

interfacial conduction lithium metal batteries solid-state electrolytes space charge layers

SCI

英语

通讯

Research Grants Council of the Hong Kong Special Administrative Region[R6005-20] ; Research Grants Council of the Hong Kong Special Administrative Region, China[2023B0303000002] ; Guangdong Major Project of Basic and Applied Basic Research[FSNH22EG07]

Chemistry ; Energy & Fuels ; Materials Science ; Physics

Chemistry, Physical ; Energy & Fuels ; Materials Science, Multidisciplinary ; Physics, Applied ; Physics, Condensed Matter

WOS:001307397700001

WILEY-V C H VERLAG GMBH

Web of Science

1.Hong Kong Univ Sci & Technol, Dept Mech & Aerosp Engn, Kowloon, Clear Water Bay, Hong Kong 999077, Peoples R China
2.Southern Univ Sci & Technol, Dept Mech & Energy Engn, Shenzhen 518055, Peoples R China

Li, Jin,Chen, Junjie,Xu, Xiaosa,et al. Enhanced Interphase Ion Transport via Charge-Rich Space Charge Layers for Ultra-Stable Solid-State Lithium Metal Batteries[J]. ADVANCED ENERGY MATERIALS,2024.

Li, Jin.,Chen, Junjie.,Xu, Xiaosa.,Wang, Zhenyu.,Shen, Jiadong.,...&Zhao, Tianshou.(2024).Enhanced Interphase Ion Transport via Charge-Rich Space Charge Layers for Ultra-Stable Solid-State Lithium Metal Batteries.ADVANCED ENERGY MATERIALS.

Li, Jin,et al."Enhanced Interphase Ion Transport via Charge-Rich Space Charge Layers for Ultra-Stable Solid-State Lithium Metal Batteries".ADVANCED ENERGY MATERIALS (2024).