First-Principles Simulations for the Surface Evolution and Mn Dissolution in the Fully Delithiated Spinel LiMn2O4.

摘要: The interfacial stability between the cathode and electrolyte is an essential issue in development of high-energy-density long-life lithium-ion batteries. deterioration capacity dominated by Mn dissolution makes LiMn2O4 a representative case for studying evolution interfaces. Here, we use ab initio molecular dynamics (AIMD) method to simulate interface reaction ethylene carbonate (EC) molecules (110) surface completely delithiated where most severe observed experiment. It found that intrinsic oxygen loss on will drive initial migration atoms while reducing them. EC decompose after transferring electrons atoms, its decomposition products further promote dissolution. In addition, are competitive relationship when atoms. This work provides complete picture step-by-step along with spinel system also scope study transition-metal other materials electrolytes.