Diffusion-induced stress and delamination of layered electrode plates with composition-gradient

• Diffusion-induced stress of composition-gradient electrode plates is formulated.
• Delamination of composition-gradient electrode plates is investigated.
• Symmetric NE-gradient active plates can alleviate stresses and retard delamination.
• PE-gradient bilayer active plates can alleviate stresses and retard delamination.

Diffusion-induced stress can result in failure of layered electrodes in lithium-ion batteries during the process of fast lithiation and delithiation. Recent studies have demonstrated that the electro-chemo-mechanical properties of compositions-gradient nanoparticles are superior to those of homogeneous ones. In light of this aspect, we develop a theoretical model to probe the effects of composition-gradient on the stress evolution in layered electrodes. Our analysis concludes that, compared with the corresponding homogeneous structure, symmetrical negative-exponent gradient active plates or positive-exponent gradient bilayer electrodes can significantly reduce the maximum compressive stress and the stress drop at the electrode–collector interface, while the energy release rate of interface delamination is slightly weakened by it. These results, again, show that the composition-gradient could improve the mechanical performance of electrodes in lithium-ion batteries, and are instrumental to the design of electrode structures.