Recent research progress of interface for polyethylene oxide based solid state battery

Liu Yu-Long; Xin Ming-Yang; Cong Li-Na; Xie Hai-Ming

doi:10.7498/aps.69.20201588

Abstract

Polyethylene oxide(PEO) based solid-state batteries have high safety and high energy density, making them suitable for next-generation energy storage devices. However, their energy density reaches a limitation due to the narrow electrochemical window of PEO solid electrolyte. The electrode materials that are compatible with PEO electrolyte is less, thus handering it from being put into wide application. At the PEO/electrode interface, there are side reactions between anode/PEO and PEO cathode. Some strategies are proposed to reduce the side reactions, electrochemical performances of solid-state batteries are improved. To understand the change of interface, several advanced characterizations are employed, which can offer scientific evidence of increasing the interface stability in the future.

Keywords:

Authors and contacts

National & Local United Engineering Laboratory for Power Battery, Faculty of Chemistry, Northeast Normal University, Changchun 130024, China

Corresponding author: Cong Li-Na, congln816@nenu.edu.cn ; Xie Hai-Ming, xiehm136@nenu.edu.cn

Funds: Project supported by the Special Fund of Key Technology Research and Development Projects, China (Grant Nos. 20180201097GX, 20180201099GX, 20180201096GX), the Key Subject Construction of Physical Chemistry of Northeast Normal University, the R&D Program of Power Batteries with Low Temperature and High Energy, the Science and Technology Bureau of Changchun, China (Grant No. 19SS013), the Young Scientists Fund of the National Natural Science Foundation of China (Grant No. 21905041), the Natural Science Foundation of the Education Department of Jilin Province, China (Grant No. JJKH20190265KJ), the Special Foundation of the Industrial Technology Research and Development of Jilin Province, China (Grant No. 2019C042), and the Fundamental Research Funds for the Central Universities (Grant No. 2412020QD006)

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Cited By

图 1 PEO基聚合物电解质固态电池发展概况.

Figure 1. Overview of the PEO polymer based solid-state battery.

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图 2 PEO基固态电解质与负极的反应　(a) 锂的不均匀沉积形成的锂枝晶^[29]; (b)锂金属沉积的原位电镜扫描图片^[32]; (c) 锂金属沉积的循环伏安曲线^[34]

Figure 2. Anode side reaction in PEO based solid state battery: (a) Lithium dendrite formation during deposition^[29]; (b) in-situ SEM images of lithium deposition^[32]; (c) C-V curves of lithium deposition/dissolution^[34].

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图 3 负极界面改善策略　(a) 锂金属表面修饰^[47]; (b) 有机-无机复合电解质^[49]; (c)嵌段聚合物^[54]

Figure 3. Strategies to improve the anode stability^[47]: (a) Surface modification of Li metal; (b) organic-inorganic composite electrolyte^[49]; (c) triblock co-polymer^[54].

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图 4 负极界面表征　(a)常规XPS^[56]; (b)原位SEM^[35]; (c)同步辐射CT^[61]

Figure 4. Advanced characterization of anode interface: (a)Lab-XPS^[56]; (b)in-situ SEM^[35]; (c) synchrotron X-ray microtomography^[61].

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图 5 传统电池及全固态锂电池体系质量能量密度和体积能量密度预测与比较图^[67]

Figure 5. Prediction of volumetric and gravimetric energy density for traditional battery and all solid-state battery.

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图 6 正极表面改性　(a) 固相法制备的5 wt.% c-LATP包覆的LiCoO₂的SEM图片^[76]; (b) 前驱体包覆方法获得的Li_1.3Al_0.3Ti_1.7(PO₄)₃改性LiCoO₂的SEM图片^[77]; (c) 溶液方法制备的0.5 wt% LATP均匀包覆的LiCoO₂的SEM图片^[75]; (d)在2.8−4.5 V截止电压下, LATP包覆及未包覆改性的NCM622在1 C倍率下的循环曲线 (1 C = 190 mA/g)^[79]; (e) 高温煅烧过程中LATP包覆改性及未包覆NCM622的表面演化示意图^[79]; (f) 定量分析LATP包覆改性及未包覆改性NCM622的XPS 的O1s和P2p^[79]

Figure 6. Cathode interface engineering: (a) SEM image of 5 wt.% c-LATP coated LiCoO₂^[76]; (b) SEM image of LATP precursor coated LiCoO₂^[77]; (c) SEM image of 0.5 wt.% LATP coated LiCoO₂ by solution method^[75]; (d) charge discharge curve of NMC622 at 1 C rate between 2.8−4.5 V (1 C = 190 mA/g)^[79]; (e) schematic diagram of LATP coated and un-coated NMC during high temperature sintering^[79]; (f) XPS O1s and P2p of LATP coated and un-coated NMC^[79].

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图 7 (a) 示意图说明ALD/MLD技术解决固态电池界面问题^[80]; (b) ALD技术制备的LNO包覆NCM811的TEM图^[81]; (c) 示意图说明包覆改性前后的NCM811正极在长循环后层状结构降解及晶格氧的损失情况^[81]; (d) 对比改性前后NCM811在60 ℃, 0.2 C倍率下循环性能曲线^[81]; (e) LTO包覆LiCoO₂颗粒和LTO包覆LiCoO₂正极(极片包括活性材料, 导电碳和粘结剂)的示意图^[71]; (f) 示意图说明电沉积方法制备PAN包覆NCM523^[91]

Figure 7. (a) Schematic diagram of ALD/MLD in stabilizing cathode interface^[80]; (b) TEM image of ALD LNO coated NCM811^[81]; (c) illustration of structure degradation and oxygen release of coated and uncoated NCM811^[81]; (d) cycling performance of coated and uncoated NCM811 NCM811 at 60 ℃, 0.2 C rate^[81]; (e) illustration of ALD LTO coated LiCoO₂particle and LTO coated LiCoO₂electrode^[71]; (f) illustration of PAN coated NCM 523 by electrodeposition^[91].

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图 8 (a) DSM-SPE电解质膜的结构示意图^[105]; (b) DSM-SPE电解质膜循环10次后, XPS测试LiCoO₂正极表面F1s和B1s谱图^[105]; (c) SPE, DSM-SPE, 和PEO-LiTFSI电解质组装的LiCoO₂/Li固态电池在2.8−4.3 V电压范围, 60 ℃, 0.1 C倍率下循环性能曲线^[105]; (d) 原位聚合形成CEI膜及组装固态电池的示意图^[92]; (e) LiCoO₂|PEO-SPE|Li和CEI膜改性的LiCoO₂|PEO-SPE|Li在不同循环圈数放电态的EIS曲线, 及等效电路图和相应的拟合结果对比图^[92]; (f) LiCoO₂|PEO-SPE|Li和CEI膜改性的LiCoO₂|PEO-SPE|Li在3.0−4.2 V电压范围, 0.5 C倍率下的循环性能曲线^[92]

Figure 8. (a) Demonstration of DSM-SPE solid electrolyte based solid battery^[105];(b) F1s and B1s XPS spectra of LiCoO₂ electrode after 10 cycles^[105]; (c) cycling performance of LiCoO₂/Li cell with SPE, DSM-SPE, and PEO-LiTFSI electrolyte at 60 ℃, 0.1 C rate between 2.8−4.3 V^[105]; (d) illustration of in- situ CEI film formation and solid state battery assembly^[92]; (e) EIS spectra of LiCoO₂|PEO-SPE|Li and CEI modified LiCoO₂|PEO-SPE|Li at different cycles^[92]; (f) cycling performance of LiCoO₂|PEO-SPE|Li and CEI modified LiCoO₂|PEO-SPE|Li at 0.5 C rate between 3.0−4.2 V^[92].

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图 9 (a) LATP包覆层的TEM和SAED图^[77]; (b) LATP包覆层的STEM和EDS图^[77]; (c) Mg掺杂的LiCoO₂的放大STEM和EELS图^[77]; (d) Mg掺杂的LATP- LiCoO₂ 和LATP- LiCoO₂的C-AFM图^[77]; (e) 完全充电态的NCA颗粒在21周循环后的2D-FF-TXM^[106]; (f) 完全电态的NCA颗粒在21周循环后的3D-FF-TXM^[106]; (g) 未进行循环及循环后的NCA电极在高分辨率下的BIB-SEM图^[106]

Figure 9. (a) TEM and SAED of LATP coating layer^[77]; (b) STEM and EDS of LATP coating layer^[77]; (c) STEM and EELS of Mg doped LiCoO₂^[77]; (d) C-AFM of LATP coated Mg-LiCoO₂ and LATP- LiCoO₂^[77]; (e) 2D-FF-TXM of NCA particle after 21 cycle^[106]; (f) 3D-FF-TXM of NCA particle after 21 cycle^[106]; (g) BIB-SEM of NCA electrode before and after cycling^[106].

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