Ultrahigh Elastic Polymer Electrolytes for Solid-State Lithium Batteries with Robust Interfaces

Zheng, Tianxiang; Cui, Ximing; Chu, Ying; Li, Haijuan; Pan, Qinmin

doi:10.1021/acsami.1c20243

Cited by 24 publications

(11 citation statements)

References 36 publications

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“…[30] Wen's group has designed and fabricated several SN-based electrolytes for LMBs. [31][32][33][34] These SN-based electrolytes are successfully used as solid-state electrolytes. The reason why SN was rarely employed as the major component of a liquid electrolyte is its insufficient reductive compatibility in contact with Li anode.…”

mentioning

confidence: 99%

Smart Deep Eutectic Electrolyte Enabling Thermally Induced Shutdown Toward High‐Safety Lithium Metal Batteries

Zhang

Han

et al. 2022

Advanced Energy Materials

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hydrogen electrode), lithium metal is regarded as a promising anode candidate for next-generation high-performance lithium batteries (LMBs) technology. [1][2][3] However, the highly reactive Li metal anode, being incompatible with the stateof-the-art carbonate-based electrolytes, induces unwanted electrolyte decompositions and unstable solid electrolyte interface (SEI) during electrochemical cycling. It is also noted that the repeated Li stripping and plating results in uncontrollable Li dendrites growth as well as rapid anode pulverization. [4][5][6][7] Although the ether-based electrolytes possess relatively better (electro)chemical compatibility with Li metal, yet their low oxidation stability makes them challenging for high-voltage LMBs. [2,[8][9][10][11][12] Notably, most of carbonate and ether electrolytes are volatile and flammable, posing severe safety threats to the implementation of LMBs. In order to tackle these challenges, several promising electrolyte-design proposals, such as adopting solid-state electrolytes, developing flame-retardant electrolytes, and engineering ionic liquid electrolytes, have been widely explored. [13][14][15][16][17][18][19][20][21][22][23][24][25][26][27][28] These strategies have mitigated these challenges to some extent, yet they, unfortunately, lead to higher viscosities and/or lower ionic conductivities, undermining the overall electrochemical performance of LMBs. [29] Hence, formulating an advanced electrolyte that possesses simultaneously a wide electrochemical window, a high ionic conductivity, and improved safety characteristic is highly desirable for advancing the development of high-voltage and highsafety LMBs.Succinonitrile (SN)-based electrolyte is one of the most promising electrolytes for high-performance LMBs owing to its high oxidative stability and fast ionic conduction capability. [30] Wen's group has designed and fabricated several SN-based electrolytes for LMBs. [31][32][33][34] These SN-based electrolytes are successfully used as solid-state electrolytes. The reason why SN was rarely employed as the major component of a liquid electrolyte is its insufficient reductive compatibility in contact with Li anode. [35,36] Previous reports demonstrate that the Lewis bases (e.g., Li metal) could easily extract the SN α-hydrogen Severe safety concerns and uncontrollable lithium dendrites are major challenges for commercializing high-voltage lithium metal batteries (LMBs) utilizing state-of-the-art carbonate-based electrolytes. Herein, a new type of deep eutectic electrolyte (succinonitrile/1,3,5-trioxane/lithium difluoro(oxalato) borate (DFOB), abbreviated as DEE) with a thermally induced smart shutdown function is presented to ameliorate the aforementioned issues. In this delicately designed DEE, 1,3,5-trioxane (TXE) can participate in the Li + primary solvation shell and form an unique solvation structure (Li + -SN-TXE-DFOB − ), which is favorable to enhance the Li/electrolyte interfacial compatibility. It is demonstrated that a 4.45 V LiCoO 2 /Li battery using t...

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confidence: 99%

Smart Deep Eutectic Electrolyte Enabling Thermally Induced Shutdown Toward High‐Safety Lithium Metal Batteries

Zhang

Han

et al. 2022

Advanced Energy Materials

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“…The preparation of GPEs through the conventional method typically involves the soaking of polymer films in liquid electrolytes. However, this ex situ approach suffers from the limitation of only allowing direct contact between the GPE and the topmost layer of the electrode, necessitating the use of additional liquid electrolytes to ensure proper interface contact . In contrast, in situ GPEs are considered a more viable option for integration .…”

Section: Introductionmentioning

confidence: 99%

“…However, this ex situ approach suffers from the limitation of only allowing direct contact between the GPE and the topmost layer of the electrode, necessitating the use of additional liquid electrolytes to ensure proper interface contact. 11 In contrast, in situ GPEs are considered a more viable option for integration. 12 In this approach, the monomer and initiator are added to the liquid electrolyte during battery manufacture, with the initiator decomposing to generate free radicals that initiate polymerization.…”

Section: Introductionmentioning

confidence: 99%

Laponite-Supported Gel Polymer Electrolyte with Multiple Lithium-Ion Transport Channels for Stable Lithium Metal Batteries

Wang

Jin

Huang

et al. 2023

ACS Appl. Mater. Interfaces

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Lithium metal batteries have emerged as a promising candidate for next-generation power systems. However, the high reactivity of lithium metal with liquid electrolytes has resulted in decreased battery safety and stability, which poses a significant challenge. Herein, we present a modified laponitesupported gel polymer electrolyte (LAP@PDOL GPE) that was fabricated using in situ polymerization initiated by a redoxinitiating system at ambient temperature. The LAP@PDOL GPE effectively facilitates the dissociation of lithium salts via electrostatic interaction and simultaneously constructs multiple lithiumion transport channels within the gel polymer network. This hierarchical GPE demonstrates a remarkable ionic conductivity of 5.16 × 10 −4 S cm −1 at 30 °C. Furthermore, the robust laponite component of the LAP@PDOL GPE forms a barrier against Li dendrite growth while also participating in the establishment of a stable electrode/electrolyte interface with Si-rich components. The in situ polymerization process further improves the interfacial contact, enabling the LiFePO 4 /LAP@PDOL GPE/Li cell to exhibit an impressive capacity of 137 mAh g −1 at 1C, with a capacity retention of 98.5% even after 400 cycles. In summary, the developed LAP@PDOL GPE shows great potential in addressing the critical issues of safety and stability associated with lithium metal batteries while also delivering improved electrochemical performance.

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“…All‐solid‐state electrolytes have been explored for new generations of energy storage devices, 17 and particularly quasi‐solid/hybrid composite polymer electrolytes have shown advantages in cycle stability with different battery chemistries 18 . Unfortunately, currently reported polymer/gel electrolytes possess a combination of either high ionic conductivity but low mechanical properties, 19 or high mechanical properties but low ionic conductivity 20 . Therefore, the reported cells have high mechanical properties but unsatisfactory electrochemical performance, or good electrochemical performance but insufficient mechanical strength.…”

Section: Introductionmentioning

confidence: 99%

A quasi‐solid polymer electrolyte‐based structural battery with high mechanical and electrochemical performance

Singer,

Hsieh,

Jin

et al. 2023

EcoMat

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Structural batteries are attractive for weight reduction in electric transportation. For their practical applications excellent mechanical properties and electrochemical performance are required simultaneously, which remains a grand challenge. In this study, we present a new scalable and low‐cost design, which uses a quasi‐solid polymer electrolyte (QSPE) to achieve both remarkably improved flexural properties and attractive energy density. The QSPE has a high ionic conductivity of 1.2 mS cm−1 and retains 91% capacity over 500 cycles in graphite/NMC532 cells. Moreover, the resulting structural batteries achieved a modulus of 21.7 GPa and a specific energy of 127 Wh kg−1 based on the total cell weight, which to our knowledge is the highest reported value above 15 GPa. We further demonstrate the application of such structural batteries in a model electric car. The presented design concept enables the industrialization of structural batteries in electric transportation and further applications to improve energy efficiency and multifunctionality.image

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Ultrahigh Elastic Polymer Electrolytes for Solid-State Lithium Batteries with Robust Interfaces

Cited by 24 publications

References 36 publications

Smart Deep Eutectic Electrolyte Enabling Thermally Induced Shutdown Toward High‐Safety Lithium Metal Batteries

Smart Deep Eutectic Electrolyte Enabling Thermally Induced Shutdown Toward High‐Safety Lithium Metal Batteries

Laponite-Supported Gel Polymer Electrolyte with Multiple Lithium-Ion Transport Channels for Stable Lithium Metal Batteries

A quasi‐solid polymer electrolyte‐based structural battery with high mechanical and electrochemical performance

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