Ultrathin and Non‐Flammable Dual‐Salt Polymer Electrolyte for High‐Energy‐Density Lithium‐Metal Battery,Advanced Functional Materials

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Ultrathin and Non‐Flammable Dual‐Salt Polymer Electrolyte for High‐Energy‐Density Lithium‐Metal Battery
Advanced Functional Materials ( IF 18.5 ) Pub Date : 2021-02-23 , DOI: 10.1002/adfm.202010261
Xidong Lin ₁ , Jing Yu ₁ , Mohammed B. Effat _{1,

2} , Guodong Zhou ₁ , Matthew J. Robson ₁ , Stephen C. T. Kwok _{1,

3} , Haijun Li ₄ , Shiying Zhan ₄ , Yongliang Shang ₄ , Francesco Ciucci _{1,

3,

5}

Affiliation

Rechargeable batteries with Li‐metal anodes and Ni‐rich LiNi_xMn_yCo_zO₂ (x + y + z = 1, NMC) cathodes promise high‐energy‐density storage solutions. However, commercial carbonate‐based electrolytes (CBEs) induce deteriorative interfacial reactions to both Li‐metal and NMC, leading to Li dendrite formation and NMC degradation. Moreover, CBEs are thermally unstable and flammable, demonstrating severe safety risks. In this study, an ultrathin and non‐flammable dual‐salt polymer electrolyte (DSPE) is proposed via lightweight polytetrafluoroethylene scaffold, poly(vinylidene fluoride‐co‐hexafluoropropylene) polymeric matrix, dual‐salt, and adiponitrile/fluoroethylene carbonate functional plasticizers. The as‐obtained DSPE exhibits an ultralow thickness of 20 µm, high room temperature ionic conductivity of 0.45 mS cm⁻¹, and a large electrochemical window (4.91 V versus Li/Li⁺). The dual‐salt synergized with functional plasticizers is used to fabricate a stable interface layer on both anode and cathode. In‐depth experimental and theoretical analyses have revealed the formation of stable interfaces between the DSPE and the anode/cathodes. As a result, the DSPE effectively prevents Li/DSPE/Li symmetric cell from short‐circuiting after 1200 h, indicating effective suppression of Li dendrites. Moreover, the Li/DSPE/NMC cell delivers outstanding cyclic stability at 2 C, maintaining a high capacity of 112 mAh g⁻¹ over 1000 cycles.

中文翻译：

超薄且不易燃的双盐聚合物电解质，用于高能量密度锂金属电池

具有锂金属阳极和富镍NiNi _x Mn _y Co _z O ₂（x + y + z = 1，NMC）阴极的可充电电池有望提供高能量密度的存储解决方案。但是，商用碳酸盐基电解质（CBE）会引起锂金属和NMC的界面反应恶化，从而导致锂枝晶的形成和NMC的降解。此外，CBE具有热稳定性和易燃性，显示出严重的安全隐患。在这项研究中，通过轻质的聚四氟乙烯支架，聚偏二氟乙烯共聚物，提出了一种超薄且不易燃的双盐聚合物电解质（DSPE）。六氟丙烯）聚合物基体，双盐和己二腈/氟代碳酸亚乙酯功能增塑剂。如此获得的DSPE具有20μm的超低厚度，0.45 mS cm ^-1的高室温离子电导率和较大的电化学窗口（4.91 V vs. Li / Li ⁺）。与功能增塑剂协同作用的双盐用于在阳极和阴极上制造稳定的界面层。深入的实验和理论分析表明，DSPE与阳极/阴极之间形成稳定的界面。结果，DSPE有效地防止了1200 h后Li / DSPE / Li对称电池短路，这表明Li树枝状晶体得到了有效抑制。此外，Li / DSPE / NMC电池在2 C时具有出色的循环稳定性，可在1000次循环中保持112 mAh g ^-1的高容量。

更新日期：2021-04-22

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