Towards Optimised Cell Design of Thin Film Silicon-Based Solid-State Batteries via Modelling and Experimental Characterisation

Vadhva, Pooja; Boyce, Adam M.; Hales, Alastair; Pang, Mei-Chin; Patel, Anisha B.; Shearing, Paul R.; Li, Ruihe; Rettie, Alexander J. E.

doi:10.1149/1945-7111/ac9552

Cited by 5 publications

(11 citation statements)

References 31 publications

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“…When normalizing the Si concentration gradient, it was the maximum amount of Si lithiation that was achieved during cycling that was used. Experimental evidence of partial Si lithiation was observed previously using differential capacity analysis for these cells …”

Section: Results and Discussionmentioning

confidence: 60%

“…Experimental evidence of partial Si lithiation was observed previously using differential capacity analysis for these cells. 38 The Si strain was considerably greater when the higher diffusion coefficient was implemented (Figure 2e) due to increased Si lithiation, which resulted in greater strains but also increased cell capacity. In addition, the Si strain was more homogeneous through the electrode than with the slower experimental diffusion coefficient (Figure 2e), which can be directly linked to the Li concentration gradients throughout the electrode due to diffusion-related transport limitations.…”

Section: Resultsmentioning

confidence: 99%

“…The 2D mesh consisted of approximately 4000 quadratic elements with 94,000 degrees of freedom, while the solutions were found to be mesh-independent. The Parallel Direct Sparse Solver (PARDISO) was used to solve the discretized transport, electrochemistry, and solid mechanics equations, using the numerical procedure previously outlined …”

Section: Model Formulationmentioning

confidence: 99%

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Silicon-Based Solid-State Batteries: Electrochemistry and Mechanics to Guide Design and Operation

Vadhva,

Boyce,

Patel

et al. 2023

ACS Appl. Mater. Interfaces

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Solid-state batteries (SSBs) are promising alternatives to the incumbent lithium-ion technology; however, they face a unique set of challenges that must be overcome to enable their widespread adoption. These challenges include solid–solid interfaces that are highly resistive, with slow kinetics, and a tendency to form interfacial voids causing diminished cycle life due to fracture and delamination. This modeling study probes the evolution of stresses at the solid electrolyte (SE) solid–solid interfaces, by linking the chemical and mechanical material properties to their electrochemical response, which can be used as a guide to optimize the design and manufacture of silicon (Si) based SSBs. A thin-film solid-state battery consisting of an amorphous Si negative electrode (NE) is studied, which exerts compressive stress on the SE, caused by the lithiation-induced expansion of the Si. By using a 2D chemo–mechanical model, continuum scale simulations are used to probe the effect of applied pressure and C-rate on the stress–strain response of the cell and their impacts on the overall cell capacity. A complex concentration gradient is generated within the Si electrode due to slow diffusion of Li through Si, which leads to localized strains. To reduce the interfacial stress and strain at 100% SOC, operation at moderate C-rates with low applied pressure is desirable. Alternatively, the mechanical properties of the SE could be tailored to optimize cell performance. To reduce Si stress, a SE with a moderate Young’s modulus similar to that of lithium phosphorous oxynitride (∼77 GPa) with a low yield strength comparable to sulfides (∼0.67 GPa) should be selected. However, if the reduction in SE stress is of greater concern, then a compliant Young’s modulus (∼29 GPa) with a moderate yield strength (1–3 GPa) should be targeted. This study emphasizes the need for SE material selection and the consideration of other cell components in order to optimize the performance of thin film solid-state batteries.

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Section: Results and Discussionmentioning

confidence: 60%

Section: Resultsmentioning

confidence: 99%

Section: Model Formulationmentioning

confidence: 99%

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Silicon-Based Solid-State Batteries: Electrochemistry and Mechanics to Guide Design and Operation

Vadhva,

Boyce,

Patel

et al. 2023

ACS Appl. Mater. Interfaces

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“…[8][9][10] However, the main drawback of employing silicon as an anode are the high volume changes during the lithiation/delithiation process (300 %). [11][12][13] Since silicon itself is not sufficiently electronically or ionically conductive and needs conductive additives to perform well, the electrodes in Si-based are often composites of the active material, a SE and an electronically conductive additive such as carbon. [14][15][16] Si-based composites with carbon as a conductive additive have been widely explored as potential candidates for use in lithium-ion batteries as well as solid-state-batteries.…”

Section: Introductionmentioning

confidence: 99%

“…Hence other materials are researched as possible high capacity anodes, such as silicon which is considered to be one of the most promising materials to be employed as an anode active material, it shows a high specific capacity (3590 mAh g −1 ) and low lithiation potential (0.4 V vs. Li + /Li) compared to other anode materials [8–10] . However, the main drawback of employing silicon as an anode are the high volume changes during the lithiation/delithiation process (300 %) [11–13] . Since silicon itself is not sufficiently electronically or ionically conductive and needs conductive additives to perform well, the electrodes in Si‐based are often composites of the active material, a SE and an electronically conductive additive such as carbon [14–16] …”

Section: Introductionmentioning

confidence: 99%

Investigating the Influence of the Effective Ionic Transport on the Electrochemical Performance of Si/C‐Argyrodite Solid‐State Composites

Rudel

Rana

Ruhl

et al. 2023

Batteries & Supercaps

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Solid‐state batteries have the potential to outperform conventional lithium‐ion batteries, as they offer higher energy densities, necessary for the increasing demand for portable energy storage. Silicon‐graphite composites are considered to be one of the most promising alternatives to the lithium metal anode due to their low lithiation potential and resistance against dendrite formation. Since these composites show insufficient ionic conductivity, a fast‐conducting solid electrolyte is needed to facilitate the charge carrier transport. Optimizing the volume fractions of the solid electrolyte is crucial to ensure sufficient charge carrier transport and achieve the optimal performance. In this work, the influence of the charge carrier transport in a silicon on graphite (Si/C)/argyrodite solid electrolyte composite on the electrochemical performance is studied. By systematically varying the ratio of the Si/C to solid electrolyte, it was found that the effective ionic conductivity of the electrode composite improves exponentially with increasing content of the solid electrolyte, which in turn leads to an increase in the specific capacity of the composite across all C‐rates. This study highlights the importance of understanding and customizing charge carrier transport properties in solid‐state anode composites to achieve optimum electrochemical performance.

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Modeling and simulation of chemo-elasto-plastically coupled battery active particles

Schoof,

Niermann,

Dyck

et al. 2024

Comput Mech

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As an anode material for lithium-ion batteries, amorphous silicon offers a significantly higher energy density than the graphite anodes currently used. Alloying reactions of lithium and silicon, however, induce large deformation and lead to volume changes up to 300%. We formulate a thermodynamically consistent continuum model for the chemo-elasto-plastic diffusion-deformation behavior of amorphous silicon and it’s alloy with lithium based on finite deformations. In this paper, two plasticity theories, i.e. a rate-independent theory with linear isotropic hardening and a rate-dependent one, are formulated to allow the evolution of plastic deformations and reduce occurring stresses. Using modern numerical techniques, such as higher order finite element methods as well as efficient space and time adaptive solution algorithms, the diffusion-deformation behavior resulting from both theories is compared. In order to further increase the computational efficiency, an automatic differentiation scheme is used, allowing for a significant speed up in assembling time as compared to an algorithmic linearization for the global finite element Newton scheme. Both plastic approaches lead to a more heterogeneous concentration distribution and to a change to tensile tangential Cauchy stresses at the particle surface at the end of one charging cycle. Different parameter studies show how an amplification of the plastic deformation is affected. Interestingly, an elliptical particle shows only plastic deformation at the smaller half axis. With the demonstrated efficiency of the applied methods, results after five charging cycles are also discussed and can provide indications for the performance of lithium-ion batteries in long term use.

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Towards Optimised Cell Design of Thin Film Silicon-Based Solid-State Batteries via Modelling and Experimental Characterisation

Cited by 5 publications

References 31 publications

Silicon-Based Solid-State Batteries: Electrochemistry and Mechanics to Guide Design and Operation

Silicon-Based Solid-State Batteries: Electrochemistry and Mechanics to Guide Design and Operation

Investigating the Influence of the Effective Ionic Transport on the Electrochemical Performance of Si/C‐Argyrodite Solid‐State Composites

Modeling and simulation of chemo-elasto-plastically coupled battery active particles

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