Adsorption of propylene carbonate on the Li Mn₂O₄ （100） surface investigated by DFT+U calculations

【摘要】 Understanding the mechanism of the interfacial reaction between the cathode material and the electrolyte is a significant work because the interfacial reaction is an important factor affecting the stability, capacity, and cycling performance of Li-ion batteries. In this work, spin-polarized density functional theory calculations with on-site Coulomb energy have been employed to study the adsorption of electrolyte components propylene carbonate（PC） on the LiMn₂O₄（100） surface.The findings show that the PC molecule prefers to interact with the Mn atom on the LiMn₂O₄（100） surface via the carbonyl oxygen（O_c）, with the adsorption energy of-1.16 e V, which is an exothermic reaction. As the adsorption of organic molecule PC increases the Mn atoms coordination with O atoms on the（100） surface, the Mn³⁺ ions on the surface lose charge and the reactivity is substantially decreased, which improves the stability of the surface and benefits the cycling performance.更多还原

【Abstract】 Understanding the mechanism of the interfacial reaction between the cathode material and the electrolyte is a significant work because the interfacial reaction is an important factor affecting the stability, capacity, and cycling performance of Li-ion batteries. In this work, spin-polarized density functional theory calculations with on-site Coulomb energy have been employed to study the adsorption of electrolyte components propylene carbonate（PC） on the LiMn₂O₄（100） surface.The findings show that the PC molecule prefers to interact with the Mn atom on the LiMn₂O₄（100） surface via the carbonyl oxygen（O_c）, with the adsorption energy of-1.16 e V, which is an exothermic reaction. As the adsorption of organic molecule PC increases the Mn atoms coordination with O atoms on the（100） surface, the Mn³⁺ ions on the surface lose charge and the reactivity is substantially decreased, which improves the stability of the surface and benefits the cycling performance.更多还原