Several electrode materials, such as LiFePO 4 , have a thermodynamic driving force toward phase separation. However, phase separation inside the electrode particles can be suppressed when the particles are nanosized. In this case, each individual particle remains monophasic, but phase separation can occur between particles via Li redistribution. Here, we investigate the dynamics of Li redistribution when the equilibrium potential is size dependent. We perform simulations of the charge-discharge cycle in a two-particle cell and in a 65-particle agglomerate. The difference in particle equilibrium potentials can lead to an asymmetry between lithiation and delithiation of an electrode, in which the order of transformation of the particles during lithiation and delithiation is reversed. This effect is more significant at low currents but almost negligible at high currents.LiFePO 4 (LFP) is a promising Li-ion battery material due to its thermal stability, long lifespan, and low toxicity. 1,2 As shown in experiments, LFP has a thermodynamic driving force toward phase separation. 3 However, it has been proposed that phase separation inside the particles ("intraparticle phase separation") may be prevented in nanoparticulate electrodes. [4][5][6] In this case, the particles remain monophasic, and instead Li can be redistributed between them to reduce their free energy and reach a stable state in a process we refer to as the "interparticle phase separation." This process has been the focus of several publications, 1,7-13 including our previous studies of particle-interaction dependence on particle position, 14 connectivity 15 and size. 15,16 The tendency for particles to remain monophasic leads to a discrete transformation of the particles at low currents. 7 This discrete transformation is believed to be responsible for several characteristics of LFP, such as a thermodynamic voltage hysteresis 7 and a memory effect. 17 It has been recently predicted that it also causes the current density at the particle surface to be nearly independent of cell C-rate. 13 Particle size affects (de)lithiation dynamics in multiple forms. In the first form, as explored in our previous studies, 15,16 the surface-tovolume ratio difference allows smaller particles to reach the miscibility gap faster and to initiate interparticle phase separation. A second form is the difference in the equilibrium potential between particles of different radii. A dependence of the equilibrium potential on the particle size can stem from the difference in surface-to-volume ratio between particles of different sizes, 18 which causes the total surfaceto-bulk free energy ratio to change with size. Another source of size dependence may be the change in stress in the host structure caused by the Gibbs-Thomson effect. 19,20 For LFP particles, several studies have suggested that smaller LFP particles exhibit higher equilibrium potentials than larger particles. 19,21 In this study, we incorporate the dependence of the equilibrium potential on the particle size into our pre...