We have applied a recently developed ab initio grand canonical Monte Carlo (aiGCMC) method to study the electrode reaction of Sb in the sodium ion battery (SIB). By allowing Na to exchange between the system and a virtual reservoir, while fixing the number of Sb and the volume-per-Sb of the system, our aiGCMC simulations have shown that extra Na atoms can hardly be charged into the system even under 0 V electrode potential referencing to the Na bulk. This result predicts that the over 300% volume change always happens in the Na-Sb battery regardless of the morphology of the electrode material, and therefore the effort of reducing capacity drop during the charging-discharging cycles should focus on stabilizing and recovering the nanoporous structure during discharging. On the other hand, we have also modified the aiGCMC algorithm to explore NaxSb intermediates during the charging process. We have discovered a meta-stable Na2Sb phase with the energy penalty of only 10 meV per atom if decomposed into NaSb and Na3Sb. This is the first a meta-stable Na2Sb phase is predicted. Our work provides insights for a detailed understanding of the charging dynamics in Sb based SIB.

<i>Ab initio</i> grand canonical Monte Carlo simulations for the sodiation and desodiation of NaxSb in sodium ion battery

Macromolecular Chemistry: The Second Century

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ACS Spring 2020 National Meeting & Expo

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Ab initio grand canonical Monte Carlo simulations for the sodiation and desodiation of NaxSb in sodium ion battery