The mechanical stability of aqueous binder and conductive composites (BCC) is the basis of the long-term service of composite electrodes in advanced secondary batteries. To evaluate the stress evolution of BCC in composite electrodes during electrochemical operation, we established an electrochemical–mechanical model for multilayer spherical particles that consists of an active material and a solid-electrolyte-interface (SEI)-enclosed BCC. The lithium-diffusion-induced stress distribution was studied in detail by coupling the influence of SEI and the viscoelasticity of inorganic-filler-doped polymeric bonding material. It was found that tensile hoop stress plays a critical role in determining whether a composite electrode is damaged or not—and circumferential cracks may primarily initiate in BCC, rather than in other electrode components. Further, the peak tensile stress of BCC is at the interface with SEI and does not occur at full lithiation due to the relaxation nature of polymer composite. Moreover, mechanical damage would be greatly misled if neglecting the existence of SEI. Finally, the structure integrity of the binder and conductive system can be effectively improved by (1) increasing the carbon black content as much as possible in the context of meeting cell capacity requirements—it is greater than 27% and 50% for sodium alginate and the mixtures of carboxy styrene butadiene latex and sodium carboxymethyl cellulose, respectively, for composite graphite anode; (2) reducing the elastic modulus of SEI to less than that of BCC; (3) decreasing the lithiation rate.
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