This paper presents a comprehensive study of the influences of lamination at both electrode-separator interfaces of lithium-ion batteries consisting of LiNi1/3Mn1/3Co1/3O2 cathodes and graphite anodes. Typically, electrode-separator lamination shows a reduced capacity fade at fast-charging cycles. To study this behavior in detail, the anode and cathode were laminated separately to the separator and compared to the fully laminated and non-laminated state in single-cell format. The impedance of the cells was measured at different states of charge and during the cycling test up to 1500 fast-charging cycles. Lamination on the cathode interface clearly shows an initial decrease in the surface resistance with no correlation to aging effects along cycling, while lamination on both electrode-separator interfaces reduces the growth of the surface resistance along cycling. Lamination only on the anode-separator interface shows up to be sufficient to maintain the enhanced fast-charging capability for 1500 cycles, what we prove to arise from a significant reduction in growth of the solid electrolyte interface.
The accumulation of solid electrolyte interphases (SEI) in graphite anodes related to elevated formation rates (0.1C, 1C and 2C), cycling rates (1C and 2C), and electrode-separator lamination is investigated. As shown previously, the lamination technique is beneficial for the capacity aging in graphite-LiNi1/3Mn1/3Co1/3O2 cells. Here, surface resistance growth phenomena are quantified using electrochemical impedance spectroscopy (EIS). The graphite anodes were extracted from the graphite NMC cells in their fully discharged state and irreversible accumulations of lithium in the SEI are revealed using neutron depth profiling (NDP). In this post-mortem study, NDP reveals uniform lithium accumulations as a function of depth with lithium situated at the surface of the graphite particles thus forming the SEI. The SEI was found to grow logarithmically with cycle number starting with the main formation in the initial cycles. Furthermore, the EIS measurements indicate that benefits from lamination arise from surface resistance growth phenomena aside from SEI growth in superior anode fractions.
1 March 2019 in Journal of Electroanalytical Chemistry
Atmospheric corona plasma activation was used at varied energy input levels to modify microsurfaces of cathodes and anodes, previous to assembly into lithium‐ion batteries. Correlations of the plasma activation grade are evaluated considering electrode topography, crystal structure change, electrolyte wetting characteristics, as well as C–rate capability and cycling stability. This reveals upper limits for plasma modification, as well as direct dependencies of possible hydrophilicity changes on electrode composition. Deeper insights into electrochemical impacts are gained by the application of electrochemical impedance spectroscopy, showing changes in C–rate capability to arise from changes in the cathode crystal lattice.
This study shows the feasibility of the Electrospinning method as a process step for advanced and fast production Li ion cells. Lamination is a key technology for Lithium-ion battery production. It bares different advantages, such as a fast production line speed by fixing the separator to the electrodes. Unfortunately, this technology is inapplicable for separator and electrode formulations not based on thermoplastic binders. Using Electrospinning, this disadvantage can be overcome. In our study, beaded PVDF polymer nanofibres were spun onto a fibre-reinforced, inorganic-filled separator. This modified separator was then laminated onto a NMC111-cathode using a temperature profile of 110/110/120°C within the laminator. After Lamination, the separator was pulled-off again and placed in a SEM to see the adhesive behaviour of the applied polymer. The information gathered with SEM clearly shows a successful lamination of the separator to the electrode.