Actual market requirements for storage systems highlight the limits of graphite as an anode for Li-ion batteries. Lithium metal can represent a suitable alternative to graphite due to its high theoretical specific capacity (about 3860 mAh g−1) and low negative redox potential. However, several aging mechanisms, such as dendrite growth, lithium loss and the formation of an unstable SEI, decrease the performances of Li-based batteries. A suitable strategy to better understand and study these mechanisms could be the development of an electrochemical model that forecasts the aging behaviour of a lithium-metal battery. In this work, a P2D aging electrochemical model for an Li-based cell was developed. The main innovation is represented by the combination of two aspects: the substitution of graphite with metallic lithium as an anode and the implementation of SEI growth on the metallic lithium surface. The calibration of the model, based on experimental measurements and the successive validation, led to us obtaining a good accuracy between the simulated and experimental curves. This good accuracy makes the developed P2D aging model a versatile and suitable approach for further investigations on Li-based batteries considering all the aging phenomena involved.
Lithium‐ion battery performance and sustainability increasingly depend on “inactive” components such as polymer binders and current collectors. Replacing conventional N‐methyl‐2‐pyrrolidone/polyvinylidene fluoride processing with water‐based manufacturing requires binders that combine mechanical cohesion, interfacial stability, and ionic transport, together with current collectors resistant to corrosion and high‐voltage degradation. Here, two aqueous binder formulations—sodium carboxymethyl cellulose (NaCMC) + SX8684(A)‐64 and NaCMC + TRD202A—are investigated in LiNi 0.5 Mn 1.5 O 4 (LNMO) cathodes cast on bare and carbon‐coated aluminum foils. Spectroscopic and thermogravimetric analyses identify SX8684(A)‐64 as a single‐phase polymethacrylate with minimal swelling (~2%–3% mass uptake), whereas TRD202A exhibits a hybrid acrylic/fluoropolymer architecture, multistage degradation, and pronounced gel‐like swelling (>30%). Morphological analysis shows porosities of 67%–71% and tortuosities of 2.4–3.7, with TRD202A on carbon‐coated aluminum producing the most open and least tortuous architecture. Intermittent current interruption measurements confirm that this configuration provides the lowest resistance, while delivering >100 mAh g −1 at 5 C, >45 mAh g −1 at 15 C, and >80% capacity retention over 100 cycles. These results demonstrate the importance of co‐designing binder chemistry and current‐collector surfaces for scalable, sustainable aqueous LNMO cathodes.