TY - JOUR U1 - Zeitschriftenartikel, wissenschaftlich - begutachtet (reviewed) A1 - Horstmann, Birger A1 - Gallant, Betar A1 - Mitchell, Robert A1 - Bessler, Wolfgang G. A1 - Shao-Horn, Yang A1 - Bazant, Martin Z. T1 - Rate-Dependent Morphology of Li2O2 Growth in Li–O2 Batteries JF - The Journal of Physical Chemistry Letters N2 - Compact solid discharge products enable energy storage devices with high gravimetric and volumetric energy densities, but solid deposits on active surfaces can disturb charge transport and induce mechanical stress. In this Letter, we develop a nanoscale continuum model for the growth of Li2O2 crystals in lithium–oxygen batteries with organic electrolytes, based on a theory of electrochemical nonequilibrium thermodynamics originally applied to Li-ion batteries. As in the case of lithium insertion in phase-separating LiFePO4 nanoparticles, the theory predicts a transition from complex to uniform morphologies of Li2O2 with increasing current. Discrete particle growth at low discharge rates becomes suppressed at high rates, resulting in a film of electronically insulating Li2O2 that limits cell performance. We predict that the transition between these surface growth modes occurs at current densities close to the exchange current density of the cathode reaction, consistent with experimental observations. KW - Lithiumbatterie KW - Lithium KW - Morphologie Y1 - 2013 SN - 1948-7185 SS - 1948-7185 U6 - https://doi.org/10.1021/jz401973c DO - https://doi.org/10.1021/jz401973c PM - 26296168 AX - 1307.6621 VL - 4 IS - 24 SP - 4217 EP - 4222 ER -