Using a novel electrochemical phase-field model, we question the common
belief that LixFePO4 nanoparticles separate into Li-rich and Li-poor phases
during battery discharge. For small currents, spinodal decomposition or
nucleation leads to moving phase boundaries. Above a critical current density
(in the Tafel regime), the spinodal disappears, and particles fill
homogeneously, which may explain the superior rate capability and long cycle
life of nano-LiFePO4 cathodes.Comment: 27 pages, 8 figure