High-Energy and Long-Cycling All-Solid-State Lithium-Ion Batteries with Li- and Mn-Rich Layered Oxide Cathodes and Sulfide Electrolytes

Du, Wubin; Shao, Qinong; Wei, Yiqi; Yan, C. T.; Gao, Panyu; Lin, Yue; Jiang, Yinzhu; Liu, Yongfeng; Yu, Xuebin; Gao, Mingxia; Sun, Wenping; Pan, Hongge

doi:10.1021/acsenergylett.2c01637

Cited by 39 publications

(29 citation statements)

References 48 publications

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“…These experimental results demonstrate that the rapid solution synthesis using excess sulfur and the mixed solvent of ACN, THF, and EtOH can apply to a synthesis method for a broad range of sulfide SEs. 44,45 These experimental results reported here demonstrate that Li 6 PS 5 Cl prepared by the solution synthesis method using excess elemental sulfur provides high ionic conductivity and relatively stable battery performance.…”

Section: Solubility Of 5li 2 S•p 2 S 5 •2licl•xs Solutionmentioning

confidence: 54%

Rapid Solution Synthesis of Argyrodite-Type Li₆PS₅X (X = Cl, Br, and I) Solid Electrolytes Using Excess Sulfur

et al. 2023

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All-solid-state lithium-ion batteries (ASSLBs) have the potential to be the next-generation energy storage systems because of their high safety features. However, one of the major challenges to the commercialization of ASSLBs is the development of well-established large-scale manufacturing techniques for solid electrolytes (SEs). Herein, we synthesize Li 6 PS 5 X (X = Cl, Br, and I) SEs in a total of 4 h by a rapid solution synthesis method using excess elemental sulfur as a solubilizer and reasonable organic solvents. In the system, trisulfur radical anions stabilized by a highly polar solvent increase the solubility and reactivity of the precursor. Raman and UV−vis spectroscopies reveal the solvation behavior of halide ions in the precursor. This result demonstrates that the solvation structure modified by the halide ions determines the chemical stability, solubility, and reactivity of chemical species in the precursor. The prepared Li 6 PS 5 X (X = Cl, Br, and I) SEs show ionic conductivities of 2.1 × 10 −3 , 1.0 × 10 −3 , and 3.8 × 10 −6 S cm −1 at 30 °C, respectively. Our study provides a rapid synthesis of argyrodite-type SEs with high ionic conductivity.

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Section: Solubility Of 5li 2 S•p 2 S 5 •2licl•xs Solutionmentioning

confidence: 54%

Rapid Solution Synthesis of Argyrodite-Type Li₆PS₅X (X = Cl, Br, and I) Solid Electrolytes Using Excess Sulfur

et al. 2023

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“…Wh kg -1 以上的高能量密度发展目标，而且有机电解液易泄露、易腐蚀、易燃烧等特性也导致液态锂电池存在严重的安全隐患 [3,4] 。与液态锂电池相比，采用固态电解质的全固态锂电池(All-soild-state lithium battery，ASSLB)具有高安全性、高能量密度、长寿命等优点，有望解决目前液态锂电池存在的上述问题，是实现 2025年单体电池能量密度达到500 Wh kg -1 目标的关键技术之一 [5,6] 。目前，正极材料仍然是决定全固态锂电池能量密度的关键因素。因此，选择更高容量的正极材料对于提高全固态锂电池的能量密度至关重要 [7,8] 。富锂锰基层状氧化物正极材料(1-x)LiTMO 2 • xLi 2 MnO 3 (0< x≤ 1，TM=Ni，Co，Mn)的阴离子和阳离子可以在高工作电压下协同参与氧化还原反应，能提供高放电比容量(> 250 mAh g -1 )和能量密度(> 900 Wh kg -1 ) ，并且还具有热稳定性更高、原料成本低等优点 [9,10] 。此外，通过取代 Li 2 TMO 3 (TM=Ti [11] ，Zr [12] ，Ir [13] ，Ru [14] ) 中的 TM 元素，也可以获得不同类型的高容量富锂层状氧化物正极材料。近年来，图1 富锂正极材料在全固态锂电池中的发展历史概览 [18][19][20][21][22][23][24][25][26][27][28][29][30] Fig. 1.…”

Section: 引言unclassified

“…1. Development history of lithium-rich cathodes in all-solid-state lithium batteries [18][19][20][21][22][23][24][25][26][27][28][29][30] .…”

Section: 引言mentioning

confidence: 99%

“…当前固态电解质体系可分为聚合物固态电解质和无机固态电解质。以聚环氧乙烯(polyethylene oxide, PEO)为代表的聚合物固态电解质具有高可塑性、易加工等优点，但室温锂离子电导率低(10 -8 −10 -6 S cm -1 )且需要高温运行等问题导致其在富锂全固态锂电池应用上存在较大的瓶颈 [40] 。无机固态电解质如以 Li 7 P 3 S 11 、Li 9.54 Si 1.74 P 1.44 S 11.7 Cl 0.3 、Li 10 GeP 2 S 12 、Li 6 PS 5 Cl 为代表的硫化物固态电解质 [41] ，以 Li 3 YCl 6 、 Li 3 InCl 6 为代表的卤化物固态电解质 [42] 和以钙钛矿型料安全性，镍元素提高材料能量密度，钴元素提高材料导电性和结构稳定性 [47] 。在液态电池中，目前普遍以高镍或无钴作为发展目标 [48,49] 。而在固态电池中，由于电子传输阻力较大，仍需要一定量的钴以提升材料的电子电导性。基于对富锂正极材料本征特性的探究， Pan 等 [20] 通过调整 0.5LiNi 0.33 Co 0.33+x Mn 0. 于在充电状态下由氧氧化还原反应触发的氧化氧) [18] ；(b) LRCox 和 LRCo10@yLN 正极的电子电导率，离子电导率和 C2/m 相含量 [20] ；(c)(LPSCl+VGCF)|LPSCl|Li-In 电池在 2.0−4.8…”

Section: 富锂全固态锂电池研究进展unclassified

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Research advance of lithium-rich cathode materials in all-solid-state lithium batteries

Yang¹,

Hu²,

Jin³

et al. 2023

Acta Phys. Sin.

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The development of all-solid-state lithium batteries with high energy density, long cycle life, low cost and high safety is one of the important directions for the development of next-generation lithium-ion batteries. Lithium-rich cathode materials have been widely used in liquid lithium batteries for their higher discharge specific capacity (> 250 mAh g-1) and energy density (> 900 Wh kg-1), due to the synergistic redox of anions and cations, as well as their high thermal stability and low raw material cost. With the rapid development of high-performance lithium-rich cathode materials and solid-state electrolytes in all-solid-state lithium batteries, the application of lithium-rich cathode materials in all-solid-state lithium batteries is expected to break through to the target of 500 W h kg-1 energy density of lithium-ion batteries. In this review, we firstly elaborate the failure mechanism of lithium-rich cathode materials in all-solid-state lithium batteries. The poor electronic conductivity, irreversible redox reaction of anionic oxygen and structute transformation during the electrochemical cycling of lithium-rich cathode materials lead to the low initial coulomb efficiency, poor cycling stability and voltage decay. In addition, the high operating voltage of lithium-rich cathode materials (> 4.5 V vs. Li/Li+) exposes the cathode/electrolyte to not only conventional interfacial chemical reactions, but the released oxygen also aggravates the interfacial electrochemical reactions, which put higher demands on the interfacial stability of the cathode/electrolyte. Therefore, the intrinsic characteristics of lithium-rich cathode materials and the severe interfacial reaction of lithium-rich cathode/electrolyte greatly limit the application of lithium-rich cathode materials in all-solid-state lithium batteries. Then, we review the research progress of lithium-rich cathode materials in various solid-state electrolyte systems in recent years. The higher room temperature ionic conductivity and wider voltage window of inorganic solid-state electrolytes provide opportunities for the application of lithium-rich cathode materials in all-solid-state lithium batteries. At present, the application of lithium-rich cathode materials in all-solid-state lithium batteries has been initially explored on the basis of sulfide, halide and oxide solid-state electrolyte systems, and important progress has been made in studies including composite cathode preparation methods, interfacial reaction mechanisms and activation mechanisms. Finally, we summarize the current research focus of lithium-rich cathode all-solid-state lithium batteries and propose several strategies for their future outlook. Strategies such as the regulation of cathode material components, the construction of lithium ion and electron transport pathways within the composite cathode, and the interfacial modification of cathode materials have been shown to have significant effects in solving the failure problem.

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“…Significant advances have also been made recently including both anodes (i.e., graphite-based Li-free 3D anode, 18 hard carbons, 19 silicon, 20 etc.) and cathodes (i.e., LiNiO 2 , 21 Liand Mn-rich layered oxides, 22 etc.) in the SSBs.…”

mentioning

confidence: 99%

Advances in Solid-State Batteries, a Virtual Issue, Part II

Chapman

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et al. 2023

ACS Energy Lett.

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High-Energy and Long-Cycling All-Solid-State Lithium-Ion Batteries with Li- and Mn-Rich Layered Oxide Cathodes and Sulfide Electrolytes

Cited by 39 publications

References 48 publications

Rapid Solution Synthesis of Argyrodite-Type Li₆PS₅X (X = Cl, Br, and I) Solid Electrolytes Using Excess Sulfur

Rapid Solution Synthesis of Argyrodite-Type Li₆PS₅X (X = Cl, Br, and I) Solid Electrolytes Using Excess Sulfur

Research advance of lithium-rich cathode materials in all-solid-state lithium batteries

Advances in Solid-State Batteries, a Virtual Issue, Part II

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High-Energy and Long-Cycling All-Solid-State Lithium-Ion Batteries with Li- and Mn-Rich Layered Oxide Cathodes and Sulfide Electrolytes

Cited by 39 publications

References 48 publications

Rapid Solution Synthesis of Argyrodite-Type Li6PS5X (X = Cl, Br, and I) Solid Electrolytes Using Excess Sulfur

Rapid Solution Synthesis of Argyrodite-Type Li6PS5X (X = Cl, Br, and I) Solid Electrolytes Using Excess Sulfur

Research advance of lithium-rich cathode materials in all-solid-state lithium batteries

Advances in Solid-State Batteries, a Virtual Issue, Part II

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Rapid Solution Synthesis of Argyrodite-Type Li₆PS₅X (X = Cl, Br, and I) Solid Electrolytes Using Excess Sulfur

Rapid Solution Synthesis of Argyrodite-Type Li₆PS₅X (X = Cl, Br, and I) Solid Electrolytes Using Excess Sulfur