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During the screening of active materials (AMs) for lithium-ion batteries, the solid-state lithium diffusion coefficient ( D  Li ) is one of the most relevant descriptors used to evaluate the relevance of an AM candidate. However, for a given compound, the D  Li values reported in literature span over several orders of magnitude. Therefore, through the case study of LiNi 1/3 Mn 1/3 Co 1/3 O 2 cathode AM, new physical insights are provided to explain the dispersion of D  Li values obtained through galvanostatic intermittent titration technique (GITT) . For the first time, a 3D electrochemical model (accounting for the carbon-binder domain) fed with experimental inputs is capable of highlighting the limitations of the most widely used equation for deriving D  Li . Through our model, we show that these limitations arise from the influence of the carbon-binder domain location throughout the electrode and the non-homogeneous AM phasedistribution and particle size.

the journal of physical chemistry letters

Mesoscale Effects in the Extraction of the Solid-State Lithium Diffusion Coefficient Values of Battery Active Materials: Physical Insights from 3D Modeling