Regulate the lattice oxygen activity and structural stability of lithium-rich layered oxides by integrated strategies

Yuan, Shenghua; Zhang, Hongzhou; Song, Dawei; Ma, Yue; Shi, Xixi; Li, Chunliang; Zhang, Lianqi

doi:10.1016/j.cej.2022.135677

Cited by 22 publications

(8 citation statements)

References 50 publications

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“…This can lead to an increase in the oxidation state of Ni 2+ as a compensatory measure to balance the overall charge. On the other hand, as shown in Figure b, the Co 2p 3/2 binding energy is measured at 780.8 eV, a value matches to the reported binding energy of Co 3+ in layered LiMO 2 (where M stands for Ni, Co, and Mn). , In Figure c, the Mn 2p spectra reveal a Mn 2p 3/2 peak that fits well as a single peak with a binding energy of 642.7 eV. This observation is consistent with the presence of Mn 4+ ions, as observed in manganese-based layered compounds .…”

Section: Resultssupporting

confidence: 85%

Advanced TiO₂/Al₂O₃ Bilayer ALD Coatings for Improved Lithium-Rich Layered Oxide Electrodes

Chen,

Hsieh,

et al. 2024

ACS Appl. Mater. Interfaces

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Surface modification is a highly effective strategy for addressing issues in lithium-rich layered oxide (LLO) cathodes, including phase transformation, particle cracking, oxygen gas release, and transition-metal ion dissolution. Existing single-/ double-layer coating strategies face drawbacks such as poor component contact and complexity. Herein, we present the results of a low-temperature atomic layer deposition (ALD) process for creating a TiO 2 /Al 2 O 3 bilayer on composite cathodes made of AS200 (Li 1.08 Ni 0.34 Co 0.08 Mn 0.5 O 2 ). Electrochemical analysis demonstrates that TiO 2 /Al 2 O 3 -coated LLO electrodes exhibit improved discharge capacities and enhanced capacity retention compared with uncoated samples. The TAA-5/AS200 bilayer-coated electrode, in particular, demonstrates exceptional capacity retention (∼90.4%) and a specific discharge capacity of 146 mAh g −1 after 100 cycles at 1C within the voltage range of 2.2 to 4.6 V. The coated electrodes also show reduced voltage decay, lower surface film resistance, and improved interfacial charge transfer resistances, contributing to enhanced stability. The ALD-deposited TiO 2 /Al 2 O 3 bilayer coatings exhibit promising potential for advancing the electrochemical performance of lithium-rich layered oxide cathodes in lithium-ion batteries.

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Section: Resultssupporting

confidence: 85%

Advanced TiO₂/Al₂O₃ Bilayer ALD Coatings for Improved Lithium-Rich Layered Oxide Electrodes

Chen,

Hsieh,

et al. 2024

ACS Appl. Mater. Interfaces

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“…XRD tests were completed, and the XRD patterns of the obtained materials are shown in Figure . Both the materials correspond to α-NaFeO 2 layered structures, including the monoclinic phase part Li 2 MnO 3 (C2/m) and the hexagonal phase part LiMO 2 ( R 3̅ m ). , The (006)/(012) and (108)/(110) bimodal splitting of the material is obvious, indicating that the material has a good layer structure. , In addition, there is no significant shift in the (003) and (104) peak of the LRO@LZO-1% compared with the LRO material, which indicates that the Li 2 ZrO 3 is not doped into the internal lattice of the material. Combined with the analysis of the distribution of Zr in Figure , it can be shown that LZO is successfully coated on the primary particles of the material.…”

Section: Resultsmentioning

confidence: 92%

“…. 27,28 The (006)/(012) and ( 108)/ (110) bimodal splitting of the material is obvious, indicating that the material has a good layer structure. 29,30 In addition, there is no significant shift in the (003) and (104) peak of the LRO@LZO-1% compared with the LRO material, which indicates that the Li 2 ZrO 3 is not doped into the internal lattice of the material.…”

Section: Resultsmentioning

confidence: 96%

Lithium-Ion Conductor Li₂ZrO₃-Coated Primary Particles To Optimize the Performance of Li-Rich Mn-Based Cathode Materials

Chen

Cao

et al. 2023

ACS Appl. Mater. Interfaces

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A lithium-rich manganese-based cathode material (LRMC) is currently considered as one of the most promising next-generation materials for lithium-ion batteries, which has received much attention, but the LRMC still faces some key scientific issues to break through, such as poor rate capacity, rapid voltage, capacity decay, and low first coulomb efficiency. In this work, homogeneous Li2ZrO3 (LZO) was successfully coated on the surface of Li1.2Mn0.54Ni0.13Co0.13O2 (LRO) by molten salt-assisted sintering technology. Li2ZrO3 has good chemical and electrochemical stability, which can effectively inhibit the side reaction between electrode materials and electrolytes and reduce the dissolution of transition metal ions. Thus, the as-prepared LRO@LZO composites are expected to improve the cycling performance. It can be found that the discharge specific capacity of LRO is 271 mAh g–1 at 0.1 C, and the capacity retention rate is still 93.7% after 100 cycles at 1 C. In addition, Li2ZrO3 is an excellent lithium-ion conductor, which is prone to increasing the lithium-ion transfer rate and improving the rate capacity of LRO. Therefore, this study provides a new solution to improve the structure stability and electrochemical performance of LRMCs.

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“…所示。目前，人们对于全固态锂电池中富锂正极材料氧释放而导致的界面问题仍存在争议。尽管 Kanno 等 [29] 证明在全固态薄膜电池中致密的固体界面可以避免液态锂电池中的电解液分解、锰离子溶解和 Li 2 MnO 3 的氧析出等问题，有助于稳定 Li 2 MnO 3 正极的表面结构，但目前多数研究结果仍认为高压正极材料在全固态锂电池中会发生氧释放导致界面降解，并且需要通过正极材料界面改性以提高正极 /电解质界面的稳定性，如图 2(c)所示 [34,35] 。因此，富锂正极材料的界面问题在不同电解质体系中情况可能存在差异，需要对不同电解质体系下的界面反应机制和原理进行进一步研究。第三，电化学-机械力学失效。不可逆的晶格氧损失将不可避免地加速结构畸变，使得循环过程中不利的层状结构向尖晶石结构转变，表现为严重的电压衰减和容量衰减 [36,37] ，最终导致富锂全固态锂电池的失效。近期有研究表明 [38,39] ，晶格氧损失会导致层状氧化物正极出现应力应变畴，进而诱发孔洞和裂纹，而且正极材料的体积变化和界面反应会导致正极/电解质的力学失效。因此，富锂正极材料中氧的氧化还原反应不可逆性以及相变导致的体积变化，有可能使富锂全固态锂电池存在更严重的电化学-机械力学失效，但该研究目前仍处于初始阶段，所以其相关报道较少。图2 富锂固态复合正极界面电子和离子迁移的示意图 [21] composite cathode with modified Li-rich cathode materials [21] .…”

Section: 富锂正极材料在全固态锂电池中的失效机制unclassified

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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Regulate the lattice oxygen activity and structural stability of lithium-rich layered oxides by integrated strategies

Cited by 22 publications

References 50 publications

Advanced TiO₂/Al₂O₃ Bilayer ALD Coatings for Improved Lithium-Rich Layered Oxide Electrodes

Advanced TiO₂/Al₂O₃ Bilayer ALD Coatings for Improved Lithium-Rich Layered Oxide Electrodes

Lithium-Ion Conductor Li₂ZrO₃-Coated Primary Particles To Optimize the Performance of Li-Rich Mn-Based Cathode Materials

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

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Regulate the lattice oxygen activity and structural stability of lithium-rich layered oxides by integrated strategies

Cited by 22 publications

References 50 publications

Advanced TiO2/Al2O3 Bilayer ALD Coatings for Improved Lithium-Rich Layered Oxide Electrodes

Advanced TiO2/Al2O3 Bilayer ALD Coatings for Improved Lithium-Rich Layered Oxide Electrodes

Lithium-Ion Conductor Li2ZrO3-Coated Primary Particles To Optimize the Performance of Li-Rich Mn-Based Cathode Materials

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

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Advanced TiO₂/Al₂O₃ Bilayer ALD Coatings for Improved Lithium-Rich Layered Oxide Electrodes

Advanced TiO₂/Al₂O₃ Bilayer ALD Coatings for Improved Lithium-Rich Layered Oxide Electrodes

Lithium-Ion Conductor Li₂ZrO₃-Coated Primary Particles To Optimize the Performance of Li-Rich Mn-Based Cathode Materials