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despite the current lack of understanding of how and where the cracks propagate, it is known that the crack is generated at the delithiated states of the particles, the localization of which has been suggested as a practical means of dealing with the problem of severe crack generation. in this study, we focus on the crack generation under the condition of homogeneous phase transformation, where the crack is not observed experimentally. in addition, the crack is not observed for the cases where the crack-propagation is not induced by the phase transformation. to quantitatively understand how the crack generation is generated, numerical simulations of crack generation under the condition of homogeneous phase transformation are conducted. by varying the impact speed from 5 to 60 m/s and the normal cohesive strength from 5 to 35 mpa, it is found that the crack is induced by the localized contraction due to mechanical instability. the more stable particle as a crack-free state is formed by the higher cohesive strength and is more dominant with the lower impact speed. the model is experimentally validated by the numerical results of rosakis et al. (p. 899). moreover, from the intrinsic structural instability caused by heterogeneous phase transformation and anisotropic strain changes, the effect of micro-crack generation for the crack-free state is estimated and discussed.

it has been shown that the defect generation at the delithiated states of particles induces a significant capacity degradation of ncm cathodes. in-situ cyclic testing was performed on ncm811 particles dispersed in a binder system, and the results showed that the more severe the crack, the greater the capacity degradation. in addition, a drop in the coulombic efficiency was observed with increasing overpotentials. from our fundamental understanding, we suggest that the crack generation is caused by the localized contraction of primary particles with a mechanical instability induced by the heterogeneous phase transformation and anisotropic strain changes. it is expected that the crack-free state is more stable with the higher cohesive strength and more dominant with the lower impact speed.


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