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Due to the complex mesostructure and components of composite active layers in lithium-ion battery (LIB) electrodes, coupled with the concentration-dependent material properties and eigenstrains, efficiently estimating the effective modulus of the active layers remains a great challenge. In this work, the classic Mori–Tanaka method is found to be unable to estimate the modulus of the active layer. By realizing the importance of the mesostructure feature, a rod-rod model is proposed. The resulting modulus is expressed analytically. It is shown that the rod-rod model can accurately estimate the modulus evolution of the active layer if the material properties of the components and the evolution of volume fractions are known in advance. Moreover, a simplified rod-rod model is also developed to reduce the complexity of the proposed method. By knowing the volume fractions at two arbitrary states of charge and subsequently determining two constants, the simplified model can estimate the modulus efficiently. Considering both its accuracy and its simplicity, the simplified rod-rod model is the most suitable for the estimation. Thus, the methods developed in this work provide a new perspective for analyzing the material properties of composite active layers in LIB electrodes. [ABSTRACT FROM AUTHOR]

Abstract Partial lithiation strategies for silicon composite electrodes are experimentally investigated in this article. Two types of partial lithiation, i.e. voltage- and capacity-control strategies, are presented. Capacity loss and irreversibility of silicon electrodes are significantly suppressed by either partial lithiation strategy without any complicated modifications or treatments. The capacity of partially lithiated silicon electrodes is even higher than that of fully lithiated one after certain cycles. The images of scanning electron microscope suggest that the mechanical damage generated in partially lithiated electrodes is less than that in fully lithiated one. Furthermore, after dozens of cycles with partial lithiation, capacity decay also slows down in subsequent full charge-discharge cycles. The presented experimental results suggest that the partial lithiation strategy relieves the coupled mechanical-electrochemical degradation and is a promising approach for the long-term use of silicon composite electrodes. [ABSTRACT FROM AUTHOR]

This article demonstrates the design of charging strategies for lithium ion batteries with considering the balance between diffusion induced stress and total charge time for two- and three-stage charge methods. For the two-stage galvanostatic-potentiostatic charge method the low mechanical stress can be achieved without increasing total charge time by switching the galvanostatic to the potentiostatic at the time moment when the lithium concentration at the surface of particles reaches the limit c ¯ surf = 0 . A three-stage method, which consists of an initial galvanostatic stage of high current, a galvanostatic stage of low current and a potentiostatic ending stage, is suggested. Employing the initial galvanostatic stage of high current is helpful not only in accelerating the charge process, but also in controlling the mechanical stress once the electrical current and time duration of the initial galvanostatic stage are properly designed. [ABSTRACT FROM AUTHOR]

The state of charge (SOC) or the depth of discharge (DOD) to and the time to delamination onset and the critical size for delamination, which are potentially important in lithium ion battery design for preventing the patterned thin film electrodes from delamination, are investigated. A theoretical approach based on the cohesive model is proposed to formulate the time to and the SOC (or DOD) to delamination onset, as well as the critical size for patterned disk-like electrodes. It is found that for negative electrode the delamination initiation is dominated by mode-II during cell charging and by mode-I during cell discharging. For positive electrode both delamination modes are theoretically possible during cell charging. When the electrochemical load factor i ¯ is very high, the mode-I delamination is possible and an optimal size of electrodes exists for a given maximum i ¯ . The SOC to mode-II delamination onset decreases significantly with increasing dimensionless radius, being independent of i ¯ . When the mode-II is the dominated mode the critical size for delamination exists, and a formula for the critical size for delamination has been deduced, which is proportional to interface ductility and inversely proportional to maximum volumetric strain. [ABSTRACT FROM AUTHOR]

Abstract: A semi-analytical method based on the cohesive model has been developed to investigate the progressive growth of interface delamination in an axisymmetric thin film electrode driven by diffusion-induced stresses under the assumption that the electrode remains elastic during the Li-ion diffusion process. The evolutions of the cohesive zone and debonding zone with respect to charging time have been predicted. The cohesive zone propagates in an accelerating manner and the debonding zone advances in a slowing down manner. The key parameters that control the interfacial stresses and delamination have been identified from the obtained governing equations. And according to the discussions on the key parameters, design insights into the geometry, charging velocity and material properties of the electrode have been provided. [Copyright &y& Elsevier]

Lithium (Li) concentration-dependent mechanical properties are crucial to the performance and durability of lithium ion batteries. Here, we report an in situ measurement of the evolution of elastic modulus and partial molar volume of commercial graphite electrodes. A bending model is developed to analyze the relationship between large curvature changes and materials properties. The curvature changes of the electrode are captured using a CCD camera during electrochemical cycling. Composite graphite electrodes with different thickness ratios are chosen as the working electrode. The modulus and partial molar volume are extracted which are both associated with the stress evolution of electrodes. The results show that the elastic modulus increases during the second lithiation process, while the partial molar volume shows a stage change corresponding to the phase change of graphite materials. These results are important for the mechanical modeling and provide basic information for the commercial graphite electrodes. Image 1 • Lithium concentration-dependent mechanical properties were measured in situ. • A mechanics model was developed to analyze the curvature deformation of electrodes. • Elastic modulus and partial molar volume of the commercial graphite electrode were reported. [ABSTRACT FROM AUTHOR]

• An analytical model was established to characterize the mode-II energy release rate. • A novel plasticity-assisted zero-degree peeling test was proposed to obtain a stable crack propagation stage. • The effect of dimensionless stress, indices of hardening, and load transfer length on energy release rate were analyzed. • An excellent agreement between the theoretical calculation and numerical result was demonstrated. Lithium-ion batteries integrate heterogeneous materials such as active layers and current collectors, resulting in interfaces prone to delamination during the charge/discharge process. The mode-II energy release rate is a key index to evaluate the interfacial adhesion properties and structural integrity of electrodes. In this study, an analytical model considering the energy balance principle and a nonlinear constitutive model was established to characterize the mode-II energy release rate. A novel plasticity-assisted zero-degree peeling test (PAZDPT) is proposed to obtain a stable crack propagation stage where the peeling force is determined to calculate the mode-II energy release rate. Several parameter studies were conducted to verify the approximation of the stress distributions and simplification of the analytical model. The accuracy of the analytical model was validated against finite-element calculations. The results demonstrated an excellent agreement between the theoretical calculation and numerical results. Moreover, PAZDPT is conducive to steady crack propagation because it restricts the energy accumulation around the crack tip. The analytical model and newly proposed PAZDPT can also be extended to determine the mode-II energy release rate of other types of interfaces in bilayer thin-film materials. [ABSTRACT FROM AUTHOR]

• A general computational approach is introduced to evaluate the equivalent stiffness of various FLIBs. • The equivalent stiffness indicators, including tensile/compressive, bending, and torsion stiffnesses, are introduced by battery repeated unit cells with periodic boundary conditions. • The homogenized ABD stiffness matrix is obtained to evaluate the flexibility in different directions and deformation modes. • The connecting part is optimized, further enhancing the battery's deformability. Flexible batteries have recently developed significant advancements in structural design, diverging substantially from traditional battery architectures. However, conventional mechanical testing methods and metrics, tailored for standard battery structures, prove inadequate when evaluating the flexibility of these innovative designs. How to assess the mechanical performance of diverse structural configurations of flexible batteries poses a considerable challenge. In this study, a general computational approach is proposed to evaluate the equivalent stiffness of flexible lithium ion batteries (FLIBs) by analyzing the force–deformation response of a repeated unit cell (RUC), thereby enabling a comprehensive comparison of different FLIB designs. Moreover, to further enhance their deformability, the interconnected supple components of FLIBs have been optimized. This research lays a critical foundation for comparing the mechanical performance and optimizing the design of flexible batteries in the future. [ABSTRACT FROM AUTHOR]

Mechanical properties and lithiation-induced stress are crucial to the performance and durability of lithium-ion batteries. Here, we report the evolution of elastic modulus and stress in a silicon/polyvinylidene fluoride (PVDF) composite electrode coated on a copper foil, along with a model for analyzing the large change in the radius of curvature of the composite electrode/copper foil cantilever. The radius of curvature of the cantilever is captured by a video camera during lithiation/delithiation. The elastic modulus of the composite electrode decreases from about 0.64 GPa to 0.18 GPa during lithiation. It decreases further to about 0.10 GPa after delithiation, which is caused by the fracture of the electrode. The magnitude of the compressive stress increases lineally during lithiation and decreases suddenly to reach a steady state value during delithiation. [ABSTRACT FROM AUTHOR]