材料科学
磷腈
电解质
离子电导率
锂(药物)
电导率
聚合物
化学工程
电化学
X射线光电子能谱
电极
复合材料
物理化学
化学
医学
工程类
内分泌学
作者
Vahid Jabbari,Vitaliy Yurkiv,Golam Rasul,Abhijit H. Phakatkar,Farzad Mashayek,Vahid Jabbari
标识
DOI:10.1016/j.ensm.2023.02.009
摘要
Parasitic reactions inevitably occur at the interface of lithium (Li) metal and polymer electrolytes due to ultrahigh Li reducibility coupled with poor interfacial stability or ionic conductivity. This leads to significant capacity loss and inferior lifespan of Li metal batteries (LMBs). Herein, we engineered a stable solid electrolyte interphase (SEI) layer at the interface of Li metal and polyethylene oxide (PEO) electrolyte via incorporation of phosphazene molecules. The phosphazene-solid polymer electrolyte (P-SPE) shows a significantly higher long-term stability against Li metal anode when compared with non-modified SPE. Using cryogenic transmission electron microscopy (cryo-TEM) and X-ray photon spectroscopy (XPS), Li3N, LiF, Li3P and Li3PO4 nanocrystals were identified in the SEI layer. The Li|Li cell with P-SPE cycle for 1800 cycles at 0.2 mA cm‒2. The Li||LFP cells with P-SPE deliver a specific capacity of ∼150 mAh g−1 and ∼120 mAh g−1 at 1C and 2C charge/discharge rates, respectively, with up to 80% capacity retention after 500 and 1000 cycles, respectively. Critical role of phosphazene-modified SEI in improving electrochemical performance is further investigated by density function theory (DFT) and ab-initio molecular dynamic (AIMD) calculations. This study offers a promising approach for engineering a stable and ion-conductive Li|polymer electrolyte interface for long lifespan LMBs.
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