Abstract
Dissolution of Mn from lithium manganate spinel has hindered its commercialization as a cathode material in Li-ion batteries. This dissolution has been widely attributed to disproportionation of near-surface Mn(III), in the presence of acid, with the resultant divalent Mn being vulnerable to dissolution. To what extent moisture in the cell (as opposed to the organic electrolyte) acts as the solvent for Mn ions has not been established. Simulations by Leung show that a small displacement of trivalent Mn from its equilibrium site at an LiMn2O4(001)/ethylene carbonate interface leads to its reduction to Mn(II). In the present work, thermodynamic integration is performed based on first-principles molecular dynamics simulations within the Blue-Moon ensemble to investigate the detachment of Mn ions at the LiMn2O4(001)/water interface. The results show that reduction of Mn(III) to Mn(II) occurs also in the case of an aqueous interface. The simulations were performed for both neutral and acidic water (in the pres...
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