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Increasing the energy density of lithium‐ion batteries requires the discovery of new electrode materials capable of achieving very high areal capacity. Here, liquid phase exfoliation is used to produce nanosheets of SnP3, a 2D material with extremely high theoretical capacity of 1670 mAh g−1. These nanosheets can be fabricated into solution‐processed thin films for use as lithium storing anodes. To maximize their performance, carbon nanotubes are incorporated into the electrodes to simultaneously enhance conductivity and toughness. As a result, electrodes of thickness >300 µm can be produced, which display active‐mass‐normalized capacities (≈1657 mAh g−1Active) very close to the theoretical value. These materials show maximum specific (≈1250 mAh g−1Electrode) and areal (>20 mAh cm−2) capacities, which are at the state‐of‐the‐art for 2D‐based electrodes, coupled with good rate performance and stability. In combination with commercial cathode materials, full‐cells are fabricated with areal capacities of ≈29 mAh cm−2 and near‐record energy densities approaching 1000 Wh L−1. [ABSTRACT FROM AUTHOR]

Many promising supercapacitor electrode materials have high resistivity and require conductive additives to function effectively. However, the detailed role of the additive is not understood. Here, this question is resolved by applying a quantitative model for resistance-limited supercapacitor electrodes to Co(OH)2-nanosheet/carbon nanotube composites. Without nanotubes, theory predicts and experiments show that while the low-rate capacitance increases linearly with electrode thickness, the high rate capacitance decreases with thickness due to slow charging. Experiments supported by theory show that nanotube addition has two effects. First, the nanotube network effectively distributes charge, increasing the intrinsic electrode performance to the limit associated with its accessible surface area. Second, at high-rate, the increased electrode conductivity shifts the rate-limiting resistance from electrode to electrolyte, thus removing the thickness-dependent capacitance falloff. Furthermore, the analysis quantifies the out-of-plane conductivity of the nanotube network, identifies the cross-over from resistance-limited to diffusion-limited behavior, and allows full electrode modeling, facilitating rational design. [ABSTRACT FROM AUTHOR]

Abstract: Many promising supercapacitor electrode materials have high resistivity and require conductive additives to function effectively. However, the detailed role of the additive is not understood. Here, this question is resolved by applying a quantitative model for resistance‐limited supercapacitor electrodes to Co(OH)2‐nanosheet/carbon nanotube composites. Without nanotubes, theory predicts and experiments show that while the low‐rate capacitance increases linearly with electrode thickness, the high rate capacitance decreases with thickness due to slow charging. Experiments supported by theory show that nanotube addition has two effects. First, the nanotube network effectively distributes charge, increasing the intrinsic electrode performance to the limit associated with its accessible surface area. Second, at high‐rate, the increased electrode conductivity shifts the rate‐limiting resistance from electrode to electrolyte, thus removing the thickness‐dependent capacitance falloff. Furthermore, the analysis quantifies the out‐of‐plane conductivity of the nanotube network, identifies the cross‐over from resistance‐limited to diffusion‐limited behavior, and allows full electrode modeling, facilitating rational design. [ABSTRACT FROM AUTHOR]