The Role of Surface Free Energy in Binder Distribution and Adhesion Strength of Aqueously Processed LiNi$_{0.5}$ Mn$_{1.5}$O$_{4}$ Cathodes

This study identifies the critical aspects of binder distribution and mechanical integrity in aqueously processed LNMO cathodes, employing a comprehensive approach involving surface characterization techniques, adhesion strength testing, and electrochemical characterization. The investigation includes the use of the Washburn and Sessile Drop methods for surface free energy analysis, revealing key insights into the interfacial free energy of adhesion between cathode constituents. The results explain the formation of carbon-binder-domains and their impact on adhesion strength, with a particular focus on the conductive additives' (CA) surface area. The study demonstrates the effectiveness of reducing CA surface area and employing alternative conductive additives, such as vapor-grown carbon fibers (VGCF), in improving adhesion strength and mitigating capacity fade attributed to delamination during cycling. Furthermore, the research emphasizes the role of heat treatment beyond the melting point of the polyvinylidene fluoride (PVDF) latex binder, showcasing its influence on wetting and enhancing mechanical integrity. The presented methodology provides a valuable tool for predicting and optimizing binder distribution, offering insights into improving the overall performance and reliability of aqueously processed cathodes for advanced lithium-ion batteries.