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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]

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 (FeS 2 ), 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 × 10 18 groups/m 2 . 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 FeS 2 . 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.

Nanocomposite strain sensors, particularly those consisting of polymer-graphene composites, are increasingly common and are of great interest in the area of wearable sensors. In such sensors, application of strain yields an increase in resistance due to the effect of deformation on interparticle junctions. Typically, widening of interparticle separation is thought to increase the junction resistance by reducing the probability of tunnelling between conducting particles. However, an alternative approach would be to use piezoresistive fillers, where an applied strain modifies the intrinsic filler resistance and so the overall composite resistance. Such an approach would broaden sensing capabilities, as using negative piezoresistive fillers could yield strain-induced resistance reductions rather than the usual resistance increases. Here, we introduce nanocomposites based on polyethylene oxide (PEO) filled with MoS 2 nanosheets. Doping of the MoS 2 by the PEO yields nanocomposites which are conductive enough to act as sensors, while efficient stress transfer leads to nanosheet deformation in response to an external strain. The intrinsic negative piezoresistance of the MoS 2 leads to a reduction of the composite resistance on the application of small tensile strains. However, at higher strain the resistance grows due to increases in junction resistance. MoS 2 -PEO composite gauge factors are approximately -25 but fall to -12 for WS 2 -PEO composites and roughly -2 for PEO filled with MoSe 2 or WSe 2 . We develop a simple model, which describes all these observations. Finally, we show that these composites can be used as dynamic strain sensors.

Titanium disulfide is a promising material for a range of applications, including lithium-ion battery (LIB) anodes. However, its application potential has been severely hindered by the tendency of exfoliated TiS2 to rapidly oxidize under ambient conditions. Herein, we confirm that, although layered TiS2 powder can be exfoliated by sonication in aqueous surfactant solutions, the resultant nanosheets oxidise almost completely within hours. However, we find that upon performing the exfoliation in the solvent cyclohexyl-pyrrolidone (CHP), the oxidation is almost completely suppressed. TiS2 nanosheets dispersed in CHP and stored at 4 °C in an open atmosphere for 90 days remained up to 95% intact. In addition, CHP-exfoliated nanosheets did not show any evidence of oxidation for at least 30 days after being transformed into dry films even when stored under ambient conditions. This stability, probably a result of a residual CHP coating, allows TiS2 nanosheets to be deployed in applications. To demonstrate this, we prepared lithium ion battery anodes from nano : nano composites of TiS2 nanosheets mixed with carbon nanotubes. These anodes displayed reversible capacities (920 mA h g-1) close to the theoretical value and showed good rate performance and cycling capability.

Molybdenum dioxide (MoO 2 ) is a layered material which shows promise for a number of applications in the electrochemical energy storage arena. Mostly studied as a bulk layered material, MoO 2 has not previously been exfoliated in large quantities. Here we demonstrate the liquid phase exfoliation of MoO 2 in the solvent isopropanol, yielding reasonable amounts of good quality nanosheets. However, we found that, when dispersed in isopropanol under ambient conditions, MoO 2 nanosheets are gradually oxidized to higher oxides such as MoO 3 over a period of days. Conversely, if the nanosheets are processed into dried films immediately after exfoliation, and before oxidation has had a chance to progress, the nanosheets are relatively stable under ambient conditions, remaining unoxidised unless the films are heated. We also found that MoO 2 nanosheets can be size selected by controlled centrifugation and show size-dependent optical properties. This allows us to propose spectroscopic metrics which allow concentration- and size-estimation from extinction spectra. Finally, we found that liquid-exfoliated MoO 2 nanosheets could be used to produce lithium ion battery anodes with capacities of up to 1140 mA h g -1 ., Competing Interests: There are no conflicts of interest to declare., (This journal is © The Royal Society of Chemistry.)