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The interfacial debonding between the active layer and the current collector has been recognized as a critical mechanism for battery fading, and thus has attracted great efforts focused on the related analyses. However, much still remains to be studied regarding practical methods for suppressing electrode debonding, especially from the perspective of mechanics. In this paper, a pre-strain strategy of current collectors to alleviate electrode debonding is proposed. An analytical model for a symmetric electrode with a deformable and limited-thickness current collector is developed to analyze the debonding behavior involving both a pre-strain of the current collector and an eigen-strain of the active layers. The results reveal that the well-designed pre-strain can significantly delay the debonding onset (by up to 100%) and considerably reduce the debonding size. The critical values of the pre-strain are identified, and the pre-strain design principles are also provided. Based on these findings, this work sheds light on the mechanical design to suppress electrode degradation. [ABSTRACT FROM AUTHOR]

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]

In this study, a system of automatic microparticle patterning that could enable the separation, trapping, and translation of single microbeads in liquid suspension using negative dielectrophoresis (DEP) tweezers was presented to form a single-bead pattern. A microchip with integrated electrodes was flipped and placed above the substrate through a micromanipulator. Microparticles laying on the substrate could be displaced to different positions relative to the electrodes on the microchip, and only the selected particles would be trapped by the electric fields generated from electrodes. Vision-based approaches were used to evaluate the necessary information, such as the gap distance and the positions of electrodes and microparticles in the image. A strategy for separating nearby particles was proposed to achieve single-bead patterning with high accuracy. A controller was used to guide the microparticles toward the position for trapping while avoiding flow disturbance. Different strategies were simulated to decrease the patterning time and find the minimum traveling distance and the best route of movement. The optimization problem is NP-hard. Hence, global optimization algorithms, such as genetic algorithm, particle swarm optimization, and ant colony optimization (ACO), were simulated, and the results were compared with those of the local optimization method. The comparison results showed that ACO obtained the best performance among the methods. The strategy for constructing high-quality microparticle patterns was also examined through experiments. Orange fluorescent polystyrene beads suspended in 6-aminohexanoic acid solution were considered and successfully patterned on a glass substrate by using the proposed system. Note to Practitioners—Micropatterning is an effective tool for pharmaceutical research and drug discovery. However, the reliability of results depends on the quality of patterns. Existing approaches, such as microfluidic devices, are limited to create a pattern from one chip for single use, and the entire process is sealed and isolated from the environment. In this study, a multielectrode microchip combined with a vision-based micromanipulator is introduced to create a novel noncontact approach for microparticle patterning, which offers high flexibility and guarantees the quality of the constructed patterns. The electrodes on the chip can be selectively energized to determine the shape of the final pattern. A real-time screening is performed so that the micromanipulator will only guide the particles in good condition for selection. An optimization algorithm is implemented to aid the particle selection with the electrodes, allowing high-quality microparticle patterns to be constructed in a short time for various applications. [ABSTRACT FROM AUTHOR]

Prelithiation has been intensively investigated in high-capacity lithium-ion batteries (LIBs). However, the optimization of prelithiation degrees for long service life of LIBs still remains a challenge. The positive efffect of prelithiation on suppressing degradation of LIBs, besides directly pursuing the high first Coulomb efficiency which has been widely reported in the literature, is revealed and discussed based on an analytical model focusing on the interfacial delamination in electrodes. For full charge-discharge cycling, well-designed prelithiation can effectively suppress the delamination and reduce the debonding size by approximately 25%, compared with the case without prelithiation. For the strategy combining partial charge-discharge cycling and prelithiation, the largest reversible capacity without debonding can be significantly improved by approximately 100% with well-designed prelithiation. This work is expected to provide a prelithiation design principle and further improve the mechanical stability of 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]

A fully coupling model for the diffusion induced finite elastoplastic bending of bilayer electrodes in lithium-ion batteries is proposed. The effect of the mechanical stress on the lithium diffusion is accounted for by the mechanical part of the chemical potential derived from the Gibbs free energy along with the logarithmic stress and strain. Eight dimensionless parameters, governing the stress-assisted diffusion and the diffusion induced elastoplastic bending, are identified. It is found that the finite plasticity starting from the interface of the bilayer increases the chemical potential gradient and thereby facilitates the lithium diffusion. The full plastic flow makes the abnormal lithium concentration distribution possible, i.e., the concentration at the lithium inlet can be lower than the concentration at the interface (downstream). The increase in the thickness of the active layer during charging is much larger than the eigen-stretch due to lithiation, and this excess thickening is found to be caused by the lithiation induced plastic yield. [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]

This paper discovers and reveals a phenomenon of feigned death induced by partial delithiation in silicon composite electrodes. Unexpected extremely rapid capacity fading occurs in the initial dozens of the cycles with low upper cut-off voltages. By looking into the irreversibility, the crack, the elemental analysis and the thickness/weight of the electrode, it suggests that the rapid capacity fading is not induced by degradation. Additionally, by providing a reboot with full delithiation, the capacity can be recovered completely, which confirms the integrity of the electrode. This novel type of capacity fading is named by "feigned death" to distinguish it from the "true death" caused by degradation. It is further confirmed that the feigned death is caused by the asymmetric phase transformation between crystalline and amorphous phases in silicon electrodes. When the depth of lithiation is high enough to generate the c-Li 3.75 Si phase but the depth of delithiation is too low to eliminate the generated crystalline phase, the feigned death is triggered. The findings of this work provide an in-depth understanding of the electrochemical performance of Si-based electrodes. • The impact of partial delithiation on cycling performances of silicon electrodes is revealed. • Feigned death of silicon electrodes is discovered. • Feigned death is caused by the asymmetric phase transformation of lithiated silicon. [ABSTRACT FROM AUTHOR]

An analytical model of mechanical contact problems in composite electrodes of lithium-ion batteries is developed in this article. Two typical types of mechanical contact, namely contact between particles and contact between particle and current collector, are investigated. Key parameters that affect the contact problem are identified from the analytical solution. High uniformity of the particle size is found to be critical to the electrode. Furthermore, a soft current collector could significantly reduce the contact stress and hence is also suggested. It is figured out that contact stress is comparable to or even higher than the diffusion-induced stress under free-expansion state, even if the mechanical constraint in electrodes is weak. To highlight the significance of contact stress, an electrochemical cycling verification experiment which involves a charging pause is conducted. Both analytical and experimental results indicate that the mechanical contact plays a crucial role in the evaluation of mechanical stability of lithium-ion battery electrodes. • Analytical solutions of PP and PC contact are established. • The contact stress can be higher than the diffusion-induced stress. • The stress within the active particle is mainly induced by mechanical contacts. [ABSTRACT FROM AUTHOR]

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]

The present study consists in the development of an analytical model and the performance of 180° peeling tests aimed at evaluating the interfacial adhesive properties of graphite electrodes of lithium–ion batteries in different charging/discharging states. In order to determine the interfacial peeling strength, uniaxial tensile tests were conducted and an analytical model was used to obtain the elastic modulus of copper foil and the graphite active layer in different charging/discharging states. Results of the application of the interfacial peeling strength analytical model indicate that the interfacial peeling strength between graphite active layer and current collector does not depend exclusively on the energy release rate but also on the strain energy stored in the collector as a consequence of the expansion of the active layer associated with the insertion within it of lithium ions. The results of the 180° peeling tests indicate that the interfacial peeling strength of the fully charged electrode is larger than the corresponding parameters measured in the fresh, soaked, and fully discharged electrodes. The predictions based on the analytical model and the experimental data collected on the interfacial peeling strength are in good agreement with each other. Image 107001 [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]