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Surface stresses, in nano-sized anode particles undergoing chemomechanicalinteractions, have a relaxing effect on the diffusion-induced stresses thusimproving the mechanical endurance of the particles, whereas, the compressiveeffect of surface stresses degrades the electrochemical performance. However,this straightforward prediction of an improved mechanical performance ischallenged in this work. Silicon nanowires undergoing huge volumetric changesduring lithiation, may undergo significant axial length-increase, which servesas an important criterion in determining the mechanical performance of SiNWs.Interestingly, surface stresses tend to reduce the length-increase underpotentiostatic charging condition, but under galvanostatic charging, thelength-increase gets enhanced, thus degrading the mechanical performance of theSiNWs. To further make the study more inclusive, the nanowire is modelled witha constraining material at its core, and a competitive analysis is presentedfor the overall performance of the anode particles under the combined effectsof surface stresses and constraining material. The mathematical model is basedon large deformation theory, considering two-way coupling of diffusion-inducedstresses and stress-enhanced diffusion. It is hoped that this study willprovide a fresh perspective in designing next-generation lithium-ion batteryparticles.

Rethinking battery degradation in presence of surface effects: mechanical versus electrochemical peformance mediated by charging condition