While it is well-known that electrode conductivity has a critical impact on rateperformance in battery electrodes, this relationship has been quantified only by computer simulations. Here we investigate the relationship between electrode conductivity and rateperformance in Lithium-Nickel-Manganese-Cobalt-Oxide (NMC) cathodes filled with various quantities of carbon black, single-walled carbon nanotubes and graphene. The electrode conductivity is always extremely anisotropic with the out-of-plane conductivity, which is most relevant to rate-performance, roughly ×1000 smaller than the in-plane conductivity. For all fillers the conductivity increases with filler loading although the nanotube-filled electrodes show by far the most rapid increase. Fitting capacity versus rate curves yielded the characteristic time associated with charge/discharge. This parameter increased linearly with the inverse of the out-of-plane conductivity, with all data points falling on the same master curve.Using a simple mechanistic model for the characteristic time, we develop an equation which matches the experimental data almost perfectly with no adjustable parameters. This implies that increasing the electrode conductivity improves the rate-performance by decreasing the RC charging time of the electrode. This model shows the effect of electrode resistance on the rateperformance to become negligible in almost all cases once the out-of-plane conductivity of the 2 electrode exceeds 1 S/m. Our results show that this can be achieved by including <1wt% singlewalled carbon nanotubes in the electrode.

Two-dimensional (2D) materials show great potential for use in battery electrodes and are believed to be particularly promising for high-rate applications. However, there does not seem to be much hard evidence for the superior rate performance of 2D materials compared to non-2D materials. To examine this point, we have analyzed published rate-performance data for a wide range of 2D materials as well as non-2D materials for comparison. For each capacity−rate curve, we extract parameters that quantify performance which can then be analyzed using a simple mechanistic model. Contrary to expectations, by comparing a previously proposed figure of merit, we find 2D-based electrodes to be on average ∼40 times poorer in terms of rate performance than non-2D materials. This is not due to differences in solidstate diffusion times which were similarly distributed for 2D and non-2D materials. In fact, we found the main difference between 2D and non-2D materials is that ion mobility within the electrolyte-filled pores of the electrodes is significantly lower for 2D materials, a situation which we attribute to their high aspect ratios.

Over the past 15 years, two-dimensional (2D) materials have been studied and exploited for many applications. In many cases, 2D materials are formed by the exfoliation of layered crystals such as transition-metal disulfides. However, it has recently become clear that it is possible to exfoliate nonlayered materials so long as they have a nonisotropic bonding arrangement. Here, we report the synthesis of 2D-platelets from the earth-abundant, nonlayered metal sulfide, iron pyrite (FeS2), using liquid-phase exfoliation. The resultant 2D platelets exhibit the same crystal structure as bulk pyrite but are surface passivated with a density of 14 × 1018 groups/m2. They form stable suspensions in common solvents and can be size-selected and liquid processed. Although the platelets have relatively low aspect ratios (∼5), this is in line with the anisotropic cleavage energy of bulk FeS2. We observe size-dependent changes to optical properties leading to spectroscopic metrics that can be used to estimate the dimensions of platelets. These platelets can be used to produce lithium ion battery anodes with capacities approaching 1000 mAh/g.

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