While liquid exfoliation is a powerful technique to produce defect-free nanosheets in large quantities, its usefulness is limited by broad nanosheet thickness distributions and low monolayer contents. Here we demonstrate liquid processing techniques, based on iterative centrifugation cascades, which can be designed to achieve either highly efficient nanosheet size-selection and/or monolayer enrichment. The resultant size-selected dispersions were used to establish quantitative metrics to determine monolayer volume fraction, as well as mean nanosheet size and thickness, from standard spectroscopic measurements. Such metrics allowed us to design and optimize centrifugation cascades to enrich liquid exfoliated WS₂ dispersions up to monolayer contents of 75%. Monolayer-rich dispersions show relatively bright photoluminescence with narrow line widths (<35 meV) indicating the high quality of the nanosheets. The enriched dispersions display extinction spectra with distinct features, which also allow the direct estimation of monolayer contents.

Identifying cheap, yet effective, oxygen evolution catalysts is critical to the advancement of water splitting. Using liquid exfoliated Co(OH)₂ nanosheets as a model system, a simple procedure is developed to maximize the activity of any oxygen evolution reaction nanocatalyst. First the nanosheet edges are confirmed as the active areas by analyzing the catalytic activity as a function of nanosheet size. This allows the authors to select the smallest nanosheets (length ≈50 nm) as the best performing catalysts. While the number of active sites per unit electrode area can be increased via the electrode thickness, this is found to be impossible beyond ≈10 µm due to mechanical instabilities. However, adding carbon nanotubes increases both toughness and conductivity significantly. These enhancements mean that composite electrodes consisting of small Co(OH)₂ nanosheets and 10 wt% nanotubes can be made into freestanding films with thickness of up to 120 µm with no apparent electrical limitations. The presence of diffusion limitations results in an optimum electrode thickness of 70 µm, yielding a current density of 50 mA cm⁻² at an overpotential of 235 mV, close to the state of the art in the field. Applying this procedure to a high‐performance catalyst such as NiFeO_x should significantly surpass the state of the art.

While liquid phase exfoliation can be used to produce nanosheets stabilized in polymer solutions, very little is known about the resultant nanosheet size, thickness, or monolayer content. The present study uses semiquantitative spectroscopic metrics based on extinction, Raman, and photoluminescence (PL) spectroscopy to investigate these parameters for WS₂ nanosheets exfoliated in aqueous poly(vinyl alcohol) (PVA) solutions. By measuring Raman and PL simultaneously, the monolayer content can be tracked via the PL/Raman intensity ratio while varying processing conditions. The PL is found to be maximized for a stabilizing polymer concentration of 2 g L⁻¹. In addition, the monolayer content can be controlled via the centrifugation conditions, exceeding 5% by mass in some cases. These techniques have allowed tracking the ratio of PL/Raman in a droplet of polymer‐stabilized WS₂ nanosheets as the water evaporates during composite formation. No evidence of nanosheet aggregation is found under these conditions although the PL becomes dominated by trion emission as drying proceeds and the balance of doping from PVA/water changes. Finally, bulk PVA/WS₂ composites are produced by freeze drying where >50% of the monolayers remain unaggregated, even at WS₂ volume fractions as high as 10%.

We present, for the first time to our knowledge, WS ₂ photoexcited state dynamics and propose a model that reproduces them.

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.

Recent advances in the liquid-phase exfoliation (LPE) of layered materials have facilitated significant progress in the creation of functional inks. While ethanol/water blends have been shown to yield reasonable nanosheet dispersions with the potential for refinement into printable inks, the exfoliated mass is typically too low for practical use. Here, we show that Irish whiskey can be used as a dispersant for nanosheets of graphene, BN and WS ₂ , yielding stable dispersions at reasonably high concentrations. We see some benefits compared to exfoliation in simple ethanol/water mixtures which we attribute to the presence of organic compounds in the whiskey. Size selection yields nanosheets which are relatively thin, with photoluminescence spectroscopy confirming the presence of monolayer tungsten disulfide (WS ₂ ). We also show that whiskey-dispersed nanosheets of graphene and WS ₂ can be printed into networks. These can be combined in heterostructures to produce thin-film transistors whose current can be modulated using ionic liquid (IL) gating. These devices show on:off ratios up to 340 and mobilities up to 1.5 × 10 ⁻³ cm ² V ⁻¹ s ⁻¹ . The fact that these networks can be gated at all demonstrates the robustness of nanosheet networks against external additives while the mobility reported here should represent a performance-floor for future devices.