The promise of alloy anodes for solid-state batteries

Lewis, John A.; Cavallaro, Kelsey A.; Liu, Yuhgene; McDowell, Matthew T.

doi:10.1016/j.joule.2022.05.016

Cited by 112 publications

(84 citation statements)

References 105 publications

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“…23,26 Unlike conventional liquid-cell architectures, solid electrolytes (SEs) with their specific mechanical properties can apparently mitigate the issues related to the strong silicon volume change. 27,28 External stack pressure applied to SSBs appears to ensure good interfacial contact, thereby retaining cycling stability. Thus, silicon anodes may provide a realistic opportunity to achieve high energy density and long cycling stability in SSBs, and it is worth considering this in more detail.…”

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confidence: 99%

Silicon as Emerging Anode in Solid-State Batteries

Huo

Janek

2022

ACS Energy Lett.

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Silicon is one of the most promising anode materials due to its very high specific capacity (3590 mAh g −1 ), and recently its use in solid-state batteries (SSBs) has been proposed. Although SSBs utilizing silicon anodes show broad and attractive application prospects, current results are still in an infant state in terms of electrochemical performance, analytical characterization and mechanistic understanding. This paper aims to summarize current achievements and remaining challenges for the use of silicon anodes in SSBs and to provide a perspective for SSB cells with high energy density. Three types of cells with their specific type of silicon anode (i.e., thin-film cells, powder-pressed pellet-type cells, and sheet-type pouch cells) are reviewed, from their electro-chemo-mechanical behavior to microstructure optimization. Future directions for research of silicon anodes in SSBs are outlined, such as quantifying the partial ionic/ electronic conductivity of silicon anodes, clarifying their interfacial stability, and investigating their chemo-mechanical stability.

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confidence: 99%

Silicon as Emerging Anode in Solid-State Batteries

Huo

Janek

2022

ACS Energy Lett.

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“…On the other hand, it has been reported that the use of lithium alloys can help to form a more stable interface with the solid electrolyte, and various lithium alloys have been used as anodes ,− or as interlayers between lithium metal and solid electrolyte. − The improved morphological stability of the interface has often been attributed to a fast lithium diffusivity in lithium alloys. ,,, During stripping, vacancies formed at the interface would quickly be refilled, while during plating the fast lithium diffusion into the bulk of the anode alloy would maintain the activity of lithium at the interface below one and limit the accumulation of lithium atoms at the interface. A number of alloys have been reported to have lithium diffusivities significantly exceeding lithium self-diffusivity, with chemical diffusion coefficients between 10 –8 and 10 –6 cm 2 ·s –1 at room temperature measured by galvanostatic or potentiostatic electrochemical titration techniques in liquid electrolytes. ,− Among these lithium alloys, the Li-Mg system has attracted particular interest. ,, Mg has an exceptionally wide solubility range in Li, with the β-phase region spanning from 0 to 70 at.% Mg (see Figure a), so that there may be no phase transformation during electrochemical cycling of Li-Mg giving better microstructural stability .…”

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On the Relative Importance of Li Bulk Diffusivity and Interface Morphology in Determining the Stripped Capacity of Metallic Anodes in Solid-State Batteries

et al. 2022

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Lithium metal self-diffusion is too slow to sustain large current densities at the interface with a solid electrolyte, and the resulting formation of voids on stripping is a major limiting factor for the power density of solid-state cells. The enhanced morphological stability of some lithium alloy electrodes has prompted questions on the role of lithium diffusivity in these materials. Here, the lithium diffusivity in Li-Mg alloys is investigated by an isotope tracer method, revealing that the presence of magnesium slows down the diffusion of lithium. For large stripping currents the delithiation process is diffusion-limited, hence a lithium metal electrode yields a larger capacity than a Li-Mg electrode. However, at lower currents we explain the apparent contradiction that more lithium can be extracted from Li-Mg electrodes by showing that the alloy can maintain a more geometrically stable diffusion path to the solid electrolyte surface so that the effective lithium diffusivity is improved.

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“…are expected to be potential anodes for high-energy-density ASSBs because of their much higher capacity than graphite anodes. [27][28][29][30][31][32] As the most abundant metal elements in the Earth's crust, Al anode has attracted great attention because of the advantages including high capacity (≈990 mAh g −1 , from Al to Li-Al), suitable operating potential (≈0.3 V vs Li + /Li), and low cost. [27,33] Until now, various Li-Al alloy anodes with different forms have been developed, including particles, nanowires, thin films, and composite structures for the liquid organic electrolyte-based cells.…”

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Long‐Cycling All‐Solid‐State Batteries Achieved by 2D Interface between Prelithiated Aluminum Foil Anode and Sulfide Electrolyte

Fan

Ding

et al. 2022

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All‐solid‐state batteries (ASSBs) with alloy anodes are expected to achieve high energy density and safety. However, the stability of alloy anodes is largely impeded by their large volume changes during cycling and poor interfacial stability against solid‐state electrolytes. Here, a mechanically prelithiation aluminum foil (MP‐Al‐H) is used as an anode to construct high‐performance ASSBs with sulfide electrolyte. The dense Li–Al layer of the MP‐Al‐H foil acts as a prelithiated anode and forms a 2D interface with sulfide electrolyte, while the unlithiated Al layer acts as a tightly bound current collector and ensures the structural integrity of the electrode. Remarkably, the MP‐Al‐H anode exhibits superior lithium conduction kinetics and stable interfacial compatibility with Li6PS5Cl (LPSCl) and Li10GeP2S12 electrolytes. Consequently, the symmetrical cells using LPSCl electrolyte can work at a high current density of 7.5 mA cm−2 and endure for over 1500 h at 1 mA cm−2. Notably, ≈100% capacity is retained for the MP‐Al‐H||LPSCl||LiCoO2 full cell with high area loadings of 18 mg cm−2 after 300 cycles. This work offers a pathway to improve the interfacial and performance issues for the application of ASSBs.

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The promise of alloy anodes for solid-state batteries

Cited by 112 publications

References 105 publications

Silicon as Emerging Anode in Solid-State Batteries

Silicon as Emerging Anode in Solid-State Batteries

On the Relative Importance of Li Bulk Diffusivity and Interface Morphology in Determining the Stripped Capacity of Metallic Anodes in Solid-State Batteries

Long‐Cycling All‐Solid‐State Batteries Achieved by 2D Interface between Prelithiated Aluminum Foil Anode and Sulfide Electrolyte

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