N-methyl-2-pyrrolidone (NMP) has been shown to be the most effective solvent for liquid phase exfoliation and dispersion of a range of 2D materials including graphene, molybdenum disulphide (MoS₂) and black phosphorus. However, NMP is also known to be susceptible to sonochemical degradation during exfoliation. We report that this degradation gives rise to strong visible photoluminescence of NMP. Sonochemical modification is shown to influence exfoliation of layered materials in NMP and the optical absorbance of the solvent in the dispersion. The emerging optical properties of the degraded solvent present challenges for spectroscopy of nanomaterial dispersions; most notably the possibility of observing solvent photoluminescence in the spectra of 2D materials such as MoS₂, highlighting the need for stable solvents and exfoliation processes to minimise the influence of solvent degradation on the properties of liquid-exfoliated 2D materials.

Graphene and other graphitic materials are suggested as a route to cheap, high‐performance, environmentally‐sustainable electronic devices owing to their almost unique combination of properties. Liquid‐phase exfoliation is a family of shear‐based techniques that produce dispersions of nanosheets from bulk layered material crystallites. High‐quality nanosheets of graphene can be produced in solvents or surfactant dispersions; however the lateral size of these sheets limits the network transport properties observed in printed films. A high‐throughput, industrially‐scalable aqueous process for the production of graphene and related layered nanomaterials is presented. By considering not only the exfoliation process, but also the size selection and deposition processes, printable graphitic nanoparticulate materials with conductivities up to 50 000 S m⁻¹ are demonstrated. This value is ten times larger than is typically obtained for few‐layer graphene produced by liquid‐phase exfoliation. The size selection process is critical to obtaining the maximum conductivity of deposited films, with an optimized nanographite having greater performance than few‐layer graphene or graphite that is processed and used without size selection. Building on these results a radio‐frequency antenna application is demonstrated, which is competitive with the state‐of‐the‐art, and a route to recycling of such printed short‐lifetime electronic devices to lower the environmental impact is discussed.

There is a growing interest in 2D materials-based devices as the replacement for established materials, such as silicon and metal oxides in microelectronics and sensing, respectively.

Here we present a size selection model for liquid-exfoliated 2D nanosheets. The ability to consistently select exfoliated nanosheets with desired properties is important for development of applications in all areas. The model presented facilitates determination of centrifugation parameters for production of dispersions with controlled size and thickness for different materials, solvents and exfoliation processes. Importantly, after accounting for the influence of viscosity on exfoliation, comparisons of different solvents are shown to be well described by the surface tension and Hansen parameter matching. This suggests that previous analyses may have overestimated the relative performance of more viscous solvents. This understanding can be extended to develop a model based on the force balance of nanosheets falling under viscous drag during centrifugation. By considering the microscopic aspect ratio relationships, this model can be both calibrated for size selection of nanosheets and compare the exfoliation processes themselves.