1. Enhancing interfacial Li+ transport and dielectric properties in poly(ethylene oxide)-based all-solid electrolytes via inactive g-C3N4 nanosheets filler incorporation.
- Author
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Li, Zhixuan, Zhang, Weijian, Chen, Yue, Lin, Qiaoquan, Zhang, Long, Tao, Jianming, Kolosov, Oleg V., Li, Jiaxin, Lin, Yingbin, and Huang, Zhigao
- Abstract
• Second harmonic resonance-enhanced electrostatic force microscopy demonstrates that the g-C 3 N 4 additives create distributed nano-capacitors at the SPE-lithium interface, acting as "shock absorbers" for sudden changes in current densities. • The distribution of relaxation time constant (DRT) measurements validates the ability of the g-C 3 N 4 filler to effectively mitigate battery aging caused by anode interface degradation. • X-ray photoelectron spectroscopy (XPS) reveals the formation of a stable interfacial layer with lithium metal due to the reduction of nitrogen-containing organic groups in g-C 3 N 4. The advancement of all-solid-state Li metal batteries (ASSLMBs) faces a major challenge in the growth of lithium dendrites on the anode-electrolyte interface. In this study, we propose a dual-filler approach using poly(ethylene oxide) (PEO)-based solid polymer electrolytes (SPEs) that combine Li 1.4 Al 0.4 Ti 1.6 (PO 4) 3 (LATP) ion-conductive particles with graphitic carbon nitride (g-C 3 N 4) nanosheets. Analysis through second harmonic resonance enhanced electrostatic force microscopy and critical current density (CCD) tests reveal that the g-C 3 N 4 additives form nano-capacitors at the SPE-lithium interface, effectively reducing sudden changes in current densities. The distribution of relaxation time constant (DRT) measurements confirms that the g-C 3 N 4 filler suppresses uncontrolled Li dendrite growth, effectively mitigating battery aging caused by anode interfacial degradation. Furthermore, X-ray photoelectron spectroscopy (XPS) analysis indicates that the nitrogen-containing organic groups in g-C 3 N 4 are reduced to form a stable interfacial layer with lithium metal. As a result of these enhancements, the electrolyte demonstrates remarkable interfacial stability in Li/Li symmetrical cells at 0.65 mA/cm
2 and delivers promising performance in assembled Li-LiFePO 4 batteries, achieving a reversible capacity of 121.6 mAh/g at 1 C after 200 cycles. These findings highlight the potential of dual-filler PEO-based SPEs for promoting interfacial lithium-ion transport in all-solid-state Li metal batteries. [Display omitted] [ABSTRACT FROM AUTHOR]- Published
- 2024
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