Comparative Evaluation of LMR-NCM and NCA Cathode Active Materials in Multilayer Lithium-Ion Pouch Cells: Part I. Production, Electrode Characterization, and Formation

A lithium- and manganese-rich layered transition metal oxide (LMR-NCM) cathode active material (CAM) is processed on a pilot production line and assembled with graphite anodes to ≈7 Ah multilayer pouch cells. Each production step is outlined in detail and compared to NCA/graphite reference cells. Using laboratory coin cell data for different CAM loadings and cathode porosities, a simple calculation tool to extrapolate and optimize the energy density of multilayer pouch cells is presented and validated. Scanning electron microscopy and mercury porosimetry measurements of the cathodes elucidate the effect of the CAM morphology on the calendering process and explain the difficulty of achieving commonly used cathode porosities with LMR-NCM cathodes. Since LMR-NCMs exhibit strong gassing during the first cycles, a modified formation procedure based on on-line electrochemical mass spectroscopy is developed that allows stable cycling of LMR-NCM in multilayer pouch cells. After formation and degassing, LMR-NCM/graphite pouch cells have a 30% higher CAM-specific capacity and a ≈5%-10% higher cell-level energy density at a rate of C/10 compared to NCA/graphite cells. Rate capability, long-term cycling, and thermal behavior of the pouch cells in comparison with laboratory coin cells are investigated in Part II of this work.