Boosting Fast‐Charging Capability of High‐Voltage Li Metal Batteries with Ionic Liquid Modified Ethereal Electrolyte

Ding, Kai; Begin, Elijah J.; Yuan, Shouyi; Zhong, Mingyang; Wang, Yang; Zhang, Yingjie; Zeng, Xiaoyuan; Bao, Junwei Lucas; Wang, Yonggang

doi:10.1002/aenm.202302443

Cited by 16 publications

(1 citation statement)

References 63 publications

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“…S14) reveal the expansion of charge transfer resistance ( R ct ) and surface film impedance ( R f ) upon cycles for both HE-SC-N88 and SC-NCM88. The fast-growing R ct and R f should result from the deposition of Li-insulative by-products as a result of surface side reactions and ceaseless microcracks propagation upon repeated cycles ( 30 , 31 ). Notably, a slower increasing trend in both R ct and R f occurs for the case of HE-SC-N88, rather than a radical progress of SC-NCM88.…”

Section: Resultsmentioning

confidence: 99%

High-entropy doping promising ultrahigh-Ni Co-free single-crystalline cathode toward commercializable high-energy lithium-ion batteries

Liang,

Su,

Sun

et al. 2024

Sci. Adv.

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The development of advanced layered Ni-rich cathodes is essential for high-energy lithium-ion batteries (LIBs). However, the prevalent Ni-rich cathodes are still plagued by inherent issues of chemomechanical and thermal instabilities and limited cycle life. For this, here, we introduce an efficient approach combining single-crystalline (SC) design with in situ high-entropy (HE) doping to engineer an ultrahigh-Ni cobalt-free layered cathode of LiNi 0.88 Mn 0.03 Mg 0.02 Fe 0.02 Ti 0.02 Mo 0.02 Nb 0.01 O 2 (denoted as HE-SC-N88). Thanks to the SC- and HE-doping merits, HE-SC-N88 is featured with a grain-boundary-free and stabilized structure with minimal lattice strain, preventing mechanical degradation, reducing surface parasitic reactions, and mitigating oxygen loss. Accordingly, our HE-SC-N88 cathode demonstrates exceptional electrochemical properties particularly with prolonged cycling stability under strenuous conditions in both half and full cells, and the delayed O loss–induced phase transitions upon heating. More meaningfully, our design of HE doping in redefining the ultrahigh-Ni Co-free SC cathodes will make a tremendous progress toward industrial application of next-generation LIBs.

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Section: Resultsmentioning

confidence: 99%

High-entropy doping promising ultrahigh-Ni Co-free single-crystalline cathode toward commercializable high-energy lithium-ion batteries

Liang,

Su,

Sun

et al. 2024

Sci. Adv.

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High Ion‐Conductive Interphase Enabled by Nitrate‐Ionic Liquid Additive for Low‐Temperature Lithium Metal Batteries

He,

Tu,

Sun

et al. 2024

Adv Funct Materials

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The development of high‐performance low‐temperature lithium metal batteries (LMBs) is hindered by severe lithium dendrite growth and sluggish charge transfer, both of which can be effectively addressed by constructing a robust solid electrolyte interphase (SEI) with improved Li+ transport kinetics. Compared to the soft organic SEI layers, LiF‐rich SEI shows sufficient mechanical strength to impede lithium dendrite growth, however, its extremely low ionic conductivity (≈10−13 S cm−1) hinders Li+ transport kinetics at low temperatures. Herein, a quasi‐ionic liquid (QIL, [Li(15‐crown‐5)]NO3) additive with rich NO3− is developed by introducing 15‐crown‐5 into LiNO3, which induces the in situ formation of SEI with abundant Li3N. Impressively, this Li3N SEI exhibits superior lithium affinity and lower ionic diffusion barriers as learned from empirical and computational studies, suggesting that it may be powerful to conquer the sluggish Li+ kinetics at low temperature. With the assistance of QIL additive, Li/LiCoO2 cells with a high mass loading of 11.5 mg cm−2 demonstrate stable cycling for 250 cycles without any capacity decay at ‐20 °C. This work opens an emerging avenue to construct high‐performance low‐temperature LMBs by manipulating SEI composition.

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Molecular Crowding Solid Polymer Electrolytes for Lithium Metal Battery by In Situ Polymerization

Zhou,

Chen,

Yang

et al. 2024

Advanced Energy Materials

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Solid‐state polymer electrolytes (SPEs) require high ionic conductivity and dense contact with the electrodes for high‐performance lithium‐metal solid‐state batteries. However, massive challenges such as poor ionic migration ability, low antioxidant ability, and lithium dendrite formation still remain unresolved. These issues severely restrict its practical applications. Herein, a new type of solid‐state polymer electrolyte with a molecular crowding feature is rationally designed by in situ polymerization of a precursor containing poly (ethylene glycol) diacrylate (PEGDA) and 1,2‐dimethoxyethane (DME). Noticeably, the prepared SPE expands the electrochemical window to 4.7 V with a high lithium‐ion transfer number of 0.55 and a superior ionic conductivity of 3.6 mS cm−1 at room temperature. As a result, the lithium symmetrical batteries achieve stable cycles with more than 3000 h with no lithium dendrites at a current density of 0.5 mA cm−2. Importantly, this design provides dense contact of solid‐state polymer electrolytes with the porous cathode and lithium anode, allowing the assembled winding‐type solid‐state pouch cells with outstanding cycling stability of 81.7% retention for more than 340 cycles at room temperature. It shows excellent adaption to widely practical technology with large‐scale battery production, offering a new solution for the future development of solid‐state polymer lithium‐metal batteries.

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Boosting Fast‐Charging Capability of High‐Voltage Li Metal Batteries with Ionic Liquid Modified Ethereal Electrolyte

Cited by 16 publications

References 63 publications

High-entropy doping promising ultrahigh-Ni Co-free single-crystalline cathode toward commercializable high-energy lithium-ion batteries

High-entropy doping promising ultrahigh-Ni Co-free single-crystalline cathode toward commercializable high-energy lithium-ion batteries

High Ion‐Conductive Interphase Enabled by Nitrate‐Ionic Liquid Additive for Low‐Temperature Lithium Metal Batteries

Molecular Crowding Solid Polymer Electrolytes for Lithium Metal Battery by In Situ Polymerization

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