Partially Lithiated Microscale Silicon Particles as Anode Material for High‐Energy Solid‐State Lithium‐Ion Batteries

Poetke, Stephanie; Cangaz, Şahin; Hippauf, Felix; Haufe, Stefan; Dörfler, Susanne; Althues, Holger; Kaskel, Stefan

doi:10.1002/ente.202201330

Cited by 14 publications

(8 citation statements)

References 67 publications

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“…To rationalize this, we first checked whether this comes from incomplete lithiation in full cells due to the N/P ratio of 1.3 (ref. 37 ). The In/InLi|LPSCl|Si cells were cycled at 0.1C with a cutoff at a specific capacity of 2,700 mAh g –1 (which is the same degree of lithiation in full cells) for comparison.…”

Section: Se-free Si Anodes In Si|lpscl|ncm@lbo Full Cellsmentioning

confidence: 99%

Chemo-mechanical failure mechanisms of the silicon anode in solid-state batteries

Huo,

Jiang,

Bai

et al. 2024

Nat. Mater.

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Silicon is a promising anode material due to its high theoretical specific capacity, low lithiation potential and low lithium dendrite risk. Yet, the electrochemical performance of silicon anodes in solid-state batteries is still poor (for example, low actual specific capacity and fast capacity decay), hindering practical applications. Here the chemo-mechanical failure mechanisms of composite Si/Li6PS5Cl and solid-electrolyte-free silicon anodes are revealed by combining structural and chemical characterizations with theoretical simulations. The growth of the solid electrolyte interphase at the Si|Li6PS5Cl interface causes severe resistance increase in composite anodes, explaining their fast capacity decay. Solid-electrolyte-free silicon anodes show sufficient ionic and electronic conductivities, enabling a high specific capacity. However, microscale void formation during delithiation causes larger mechanical stress at the two-dimensional interfaces of these anodes than in composite anodes. Understanding these chemo-mechanical failure mechanisms of different anode architectures and the role of interphase formation helps to provide guidelines for the design of improved electrode materials.

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Section: Se-free Si Anodes In Si|lpscl|ncm@lbo Full Cellsmentioning

confidence: 99%

Chemo-mechanical failure mechanisms of the silicon anode in solid-state batteries

Huo,

Jiang,

Bai

et al. 2024

Nat. Mater.

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“…为有效提高硅负极的稳定性, 补偿硅纳米颗粒在充放电过程中反复的大体积膨胀和收缩, 2021 年, Dörfler 团队 [20] 完全锂化的微米级硅颗粒体积膨胀高达 300%, 后续会发生颗粒粉化, 进而导致容量衰减更为迅速. 该团队 [21] 为进一步解决硅负极比容量和循环稳定性两者不能兼顾的窘境, 探索使用单一非晶硅作为电池负极. 非晶硅是指部分锂化的硅仅在边缘处被锂化, 体积仅膨胀 66%, 晶体硅转化为非晶锂硅合金(a-Li x Si)的两相区域, 如图 2a 所示.…”

Section: 基于无机固态电解质构建的高镍三元/石墨 (或硅碳)高比能固态锂离子电池unclassified

Research Progress of High-energy-density Solid-state Lithium Ion Batteries Employing Ni-rich Ternary Cathodes

Zhang,

Yuan,

Zhang

et al. 2023

Acta Chimica Sinica

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To achieve carbon peaking and carbon neutrality goals, increasing the share of non-fossil energy consumption and accelerating the growth of clean, low-carbon and sustainable energy are highly desirable in developing a clean and diversified energy supply system. In this retrospect, new energy vehicles have become an ideal substitute for the traditional fuel vehicles due to their green, low-carbon, clean and sustainable characteristics, and have promising development in the future transportation industry. However, the continuously increasing demand for longer range and safety performance in electric vehicles has challenged the state-of-the-art liquid-state lithium-ion batteries. At present, the conventional lithium-ion batteries based on the traditional carbonate liquid-state electrolyte face many potential safety issues, such as leakage, volatility, combustion and explosion. In addition, their energy density reaches closely to their theoretical upper limit. Therefore, breakthroughs in battery storage technologies are urgently needed. Solid-state lithium-ion batteries, which are built with solid-state electrolytes and Ni-rich cathodes/graphite (or silicon-carbon) electrodes are the most promising battery technologies combining high energy density and improved safety property. An in-depth literature survey shows that considerable progress in the construction of high safety, high energy density Ni-rich cathodes/graphite (or silicon-carbon) solid-state lithium-ion batteries have been achieved recently. Hence, this review mainly summarizes the research progress and the development of Ni-rich cathodes/graphite (or silicon-carbon) solid-state lithium-ion batteries using inorganic solid electrolytes and polymer solid electrolytes. Moreover, the remaining challenges and future development trends of Ni-rich cathodes/graphite (or silicon-carbon) solid-state lithium-ion batteries are also discussed and presented. It is expected that the current review would contribute to the

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“…Importantly, the F‐Si pouch cell delivered high energy densities of 413 Wh kg −1 , 1022 Wh L −1 due to large SiMPs of a high tap density, ensuring high energy densities per unit mass and volume (Figure 6d ; Tables S1 and S2 , Supporting Information). [ 63 , 64 , 65 , 66 , 67 , 68 ] Instead of relying on expensive nano‐sized Si materials or creating void spaces to accommodate volume expansion, the approach adopts large particles of 5 µm, thereby achieving high energy density and notable stability. A highly dense, interconnected system afforded a capacity retention of 77.0% after 150 cycles, implying a major stride toward the realization of high‐energy and stable batteries (Figure 6e ).…”

Section: Structural Enhancement Through the Introduction Of Covalent ...mentioning

confidence: 99%

Formulating Electron Beam‐Induced Covalent Linkages for Stable and High‐Energy‐Density Silicon Microparticle Anode

Je,

Son,

Han

et al. 2024

Advanced Science

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High‐capacity silicon (Si) materials hold a position at the forefront of advanced lithium‐ion batteries. The inherent potential offers considerable advantages for substantially increasing the energy density in batteries, capable of maximizing the benefit by changing the paradigm from nano‐ to micron‐sized Si particles. Nevertheless, intrinsic structural instability remains a significant barrier to its practical application, especially for larger Si particles. Here, a covalently interconnected system is reported employing Si microparticles (5 µm) and a highly elastic gel polymer electrolyte (GPE) through electron beam irradiation. The integrated system mitigates the substantial volumetric expansion of pure Si, enhancing overall stability, while accelerating charge carrier kinetics due to the high ionic conductivity. Through the cost‐effective but practical approach of electron beam technology, the resulting 500 mAh‐pouch cell showed exceptional stability and high gravimetric/volumetric energy densities of 413 Wh kg−1, 1022 Wh L−1, highlighting the feasibility even in current battery production lines.

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Partially Lithiated Microscale Silicon Particles as Anode Material for High‐Energy Solid‐State Lithium‐Ion Batteries

Cited by 14 publications

References 67 publications

Chemo-mechanical failure mechanisms of the silicon anode in solid-state batteries

Chemo-mechanical failure mechanisms of the silicon anode in solid-state batteries

Research Progress of High-energy-density Solid-state Lithium Ion Batteries Employing Ni-rich Ternary Cathodes

Formulating Electron Beam‐Induced Covalent Linkages for Stable and High‐Energy‐Density Silicon Microparticle Anode

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