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Thick electrodes whose active materials have high areal density may improve the energy densities of lithium-ion batteries. However, the weakened rate abilities and cycle lifetimes of such electrodes significantly limit their practical applications. In this study, a modified two-dimensional model was built to evaluate the influence of the electrode structure on the lithiation process. Gradient electrodes with different particle sizes along the thickness direction are designed and fabricated via a two-layer coating process. The gradient design in the thickness direction is confirmed by three-dimensional digital microscopy, energy-dispersive spectroscopy, X-ray diffraction, and scanning electron microscopy. Galvanostatic charge/discharge cycling tests and electrochemical impedance spectroscopy are performed to investigate the electrochemical properties of the fabricated gradient electrodes. The simulation results indicate that the gradient electrode structure can enhance the utilization of electrode particles on the current collector side and alleviate the nonuniformity of the solid-phase Li concentration along the thickness direction. High electrochemical performance and long-term cycling stability of the designed gradient electrodes are verified by electrochemical test. The gradient structure fabricated via multi-layer coating processes can be used to improve the electrochemical performance of thick electrodes. [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]