Porous polyamine/PEO composite solid electrolyte for high performance solid-state lithium metal batteries,Journal of Materials Chemistry A

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Porous polyamine/PEO composite solid electrolyte for high performance solid-state lithium metal batteries
Journal of Materials Chemistry A ( IF 10.7 ) Pub Date : 2021-10-08 , DOI: 10.1039/d1ta04599g
Chenghan Li ₁ , Shi Zhou ₁ , Lijie Dai ₁ , Xuanyi Zhou ₁ , Biao Zhang ₁ , Liwen Chen ₁ , Tao Zeng ₁ , Yating Liu ₁ , Yongfu Tang ₂ , Jie Jiang ₁ , Jianyu Huang _{1,

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Affiliation

Solid polymer electrolytes (SPEs) have attracted much attention due to their better safety and flexibility. However, the low ionic conductivity and narrow electrochemical window impede their applications in PEO-based solid-state batteries. Here we report the synthesis of a new SPE comprising PEO with 1 wt% fluoromethyl modified polyamine (PAN-FMP) as a filler that has high ionic conductivity and a wide electrochemical window. The LiFePO₄ (LFP)/SPE/Li cell delivers an initial capacity of 124 mA h g⁻¹ at 1C with a capacity retention of 83% after 1000 cycles. Moreover, the electrochemical stability window of the SPE has been widened up to 4.8 V, which makes it compatible with high voltage cathodes such as LiNi_0.8Co_0.1Mn_0.1O₂ (NMC811). The enhanced ionic conductivity of the SPE originates from the PAN-FMP filler rich in –CF₃ groups that interact with ether oxygen on the PEO segment and make ether oxygen form loose ion pairs with Li⁺ ions, thus inhibiting the rearrangement and crystallization of PEO and enhancing Li⁺ ion transport of the SPE. The long cycle life of the full cell is attributed to the formation of a LiF-rich-solid electrolyte interface (SEI) layer due to PAN-FMP promoting the defluorination of TFSI⁻. The LiF SEI layer enables uniform lithium metal deposition, and prevents the growth of lithium dendrites. The low-cost, simple preparation method and superior electrochemical performance of the SPE with an organic PAN-FMP filler thus provide a new strategy to enable high voltage and high energy density polymer based solid-state batteries.

中文翻译：

用于高性能固态锂金属电池的多孔聚胺/PEO复合固体电解质

固态聚合物电解质（SPEs）因其更好的安全性和柔韧性而备受关注。然而，低离子电导率和狭窄的电化学窗口阻碍了它们在基于 PEO 的固态电池中的应用。在这里，我们报告了一种新 SPE 的合成，该 SPE 包含 PEO 和 1 wt% 氟甲基改性多胺 (PAN-FMP) 作为填料，具有高离子电导率和宽电化学窗口。LiFePO ₄ (LFP)/SPE/Li 电池在 1C 时提供124 mA hg ^-1的初始容量，1000 次循环后容量保持率为 83%。此外，SPE 的电化学稳定性窗口已加宽至 4.8 V，使其与高电压正极兼容，例如 LiNi _0.8 Co _0.1 Mn _0.1O ₂ (NMC811)。SPE 增强的离子电导率源于富含 -CF ₃基团的 PAN-FMP 填料与 PEO 链段上的醚氧相互作用，使醚氧与 Li ⁺离子形成松散的离子对，从而抑制 PEO 的重排和结晶并增强SPE 的Li ⁺离子传输。全电池的长循环寿命归因于 PAN-FMP 促进 TFSI 脱氟，形成了富含 LiF 的固体电解质界面 (SEI) 层^-. LiF SEI 层可实现均匀的锂金属沉积，并防止锂枝晶的生长。具有有机 PAN-FMP 填料的 SPE 的低成本、简单的制备方法和优异的电化学性能为实现高电压和高能量密度聚合物基固态电池提供了新的策略。

更新日期：2021-10-27

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