Polymeric Electrolytes for Solid‐state Lithium Ion Batteries: Structure Design, Electrochemical Properties and Cell Performances

Su, Gang; Zhang, Xin; Xiao, Min; Wang, Shuanjin; Huang, Sheng; Han, Dongmei; Meng, Yuezhong

doi:10.1002/cssc.202300293

Cited by 5 publications

(2 citation statements)

References 198 publications

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“…Solid-state batteries have recently attracted significant attention due to their high thermal stability and solid electrolyte with zero leakage [8]. Solid-state electrolytes are expected to solve the safety problems caused by liquid electrolytes [9,10]. Solid electrolytes include solid polymer electrolytes (SPEs) and solid inorganic electrolytes (SIEs) [11,12].…”

Section: Introductionmentioning

confidence: 99%

Covalent Organic Framework Enhanced Solid Polymer Electrolyte for Lithium Metal Batteries

Ma,

Zhong,

Huang

et al. 2024

Molecules

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High ionic conductivity, outstanding mechanical stability, and a wide electrochemical window are the keys to the application of solid-state lithium metal batteries (LMBs). Due to their regular channels for ion transport and tailored functional groups, covalent organic frameworks (COFs) have been applied to solid electrolytes to improve their performance. Herein, we report a flexible polyethylene oxide-COF-LZU1 (abbreviated as PEO-COF) electrolyte membrane with a high lithium ion transference number and satisfactory mechanical strength, allowing for dendrite-free and long-time cycling for LMBs. Benefiting from the interaction between bis(triflfluoromethanesulonyl)imide anions (TFSI−) and aldehyde groups in COF-LZU1, the Li+ transference number of the PEO-5% COF-LZU1 electrolyte reached up to 0.43, much higher than that of neat PEO electrolyte (0.18). Orderly channels are conducive to the homogenous Li-+ deposition, thereby inhibiting the lithium dendrites. The assembled LiFePO4|PEO-5% COF-LZU1/Li cells delivered a discharge specific capacity of 146 mAh g−1 and displayed a capacity retention of 80% after 200 cycles at 0.1 C (60 °C). The Li/Li symmetrical cells of the PEO-5% COF-LZU1 electrolyte presented a longer working stability at different current densities compared to that of the PEO electrolyte. Therefore, the enhanced comprehensive performance of the solid electrolyte shows potential application prospects for use in LMBs.

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Section: Introductionmentioning

confidence: 99%

Covalent Organic Framework Enhanced Solid Polymer Electrolyte for Lithium Metal Batteries

Ma,

Zhong,

Huang

et al. 2024

Molecules

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“…However, unfortunately, the high reactivity of the lithium anode causes continuous parasitic reaction with electrolytes, rapidly forming an uneven and unstable solid electrolyte interface (SEI) on the anode surface, leading to uneven current density distribution and heterogeneous deposition of Li + . This results in the preferential deposition of Li + on local areas of the lithium metal anode, further inducing the formation of lithium dendrites [ 9 , 10 ]. These dendrites can trigger a series of issues, such as “dead lithium”, volume expansion, and battery short circuits, significantly hindering the commercialization of LMBs.…”

Section: Introductionmentioning

confidence: 99%

Long-Term Stable Cycling of Dendrite-Free Lithium Metal Batteries Using ZIF-90@PP Composite Separator

LYU,

Zhang,

Huang

et al. 2024

Nanomaterials

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Lithium metal batteries (LMBs) are anticipated to meet the demand for high energy density, but the growth of lithium dendrites seriously hinders its practical application. Herein, we constructed a kind of composite separator (ZIF-90@PP) consisting of zeolite imidazole framework-90 (ZIF-90) and polypropylene (PP) to promote the uniform deposition of Li+ and inhibit the growth of lithium dendrites. The aldehyde groups interacting with TFSI− and the nitrogen-containing negative groups attracting Li+ of ZIF-90 can facilitate the dissociation of LiTFSI to release more Li+, thus alleviating the influence of space charge near the electrode surface and accelerating the transfer of Li+. Not only does the excellent electrolyte wettability of ZIF-90 enhance the electrolyte retention capacity of the separator, but the orderly nano-channels in ZIF-90 also restrict the free migration of anions and homogenize the distribution of Li+. Consequently, the functional separator achieves a long-term stable Li plating/stripping cycling for over 780 h at 2 mA cm−2. Moreover, an impressive average coulombic efficiency of 98.67% at 0.5 C after 300 cycles is realized by Li || LFP full cells based on ZIF-90@PP with a capacity retention rate of 71.22%. The high-rate and long cycling performance of the modified Li || LFP cells further demonstrates the advantages of the ZIF-90@PP composite separator.

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Designing weakly and strongly solvating polymer electrolytes: Systematically boosting high‐voltage lithium metal batteries

Wang,

Zhang,

Huang

et al. 2024

SusMat

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Practical high‐voltage lithium metal batteries hold promise for high energy density applications, but face stability challenges in electrolytes for both 4 V‐class cathodes and lithium anode. To address this, we delve into the positive impacts of two crucial moieties in electrolyte chemistry: fluorine atom (‐F) and cyano group (‐CN) on the electrochemical performance of polyether electrolytes and lithium metal batteries. Cyano‐bearing polyether electrolytes possess strong solvation, accelerating Li+ desolvation with minimal SEI impact. Fluorinated polyether electrolytes possess weak solvation, and stabilize the lithium anode via preferential decomposition of F‐segment, exhibiting nearly 6000‐h stable cycling of lithium symmetric cell. Furthermore, the electron‐withdrawing properties of ‐F and ‐CN groups significantly bolster the high‐voltage tolerance of copolymer electrolyte, extending its operational range up to 5 V. This advancement enables the development of 4 V‐class lithium metal batteries compatible with various cathodes, including 4.45 V LiCoO2, 4.5 V LiNi0.8Co0.1Mn0.1O2, and 4.2 V LiNi0.5Co0.2Mn0.3O2. These findings provide insights into design principles centered around polymer components for high‐performance polymer electrolytes.

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Polymeric Electrolytes for Solid‐state Lithium Ion Batteries: Structure Design, Electrochemical Properties and Cell Performances

Cited by 5 publications

References 198 publications

Covalent Organic Framework Enhanced Solid Polymer Electrolyte for Lithium Metal Batteries

Covalent Organic Framework Enhanced Solid Polymer Electrolyte for Lithium Metal Batteries

Long-Term Stable Cycling of Dendrite-Free Lithium Metal Batteries Using ZIF-90@PP Composite Separator

Designing weakly and strongly solvating polymer electrolytes: Systematically boosting high‐voltage lithium metal batteries

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