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Crystalline two-dimensional carbon nitrides with polytriazine imide (PTI) structure are shown to act amphoterically, buffering both HCl and NaOH aqueous solutions, resulting in charged PTI layers that dissolve spontaneously in their aqueous media, particularly for the alkaline solutions. This provides a low energy, green route to their scalable solution processing. Protonation in acid is shown to occur at pyridinic nitrogens, stabilized by adjacent triazines, whereas deprotonation in base occurs primarily at basal plane NH bridges, although NH2 edge deprotonation is competitive. We conclude that mildly acidic or basic pHs are necessary to provide sufficient net charge on the nanosheets to promote dissolution, while avoiding high ion concentrations which screen the repulsion of like-charged PTI sheets in solution. This article is part of the theme issue 'Exploring the length scales, timescales and chemistry of challenging materials (Part 2)'. [ABSTRACT FROM AUTHOR]

The crystalline graphitic carbon nitride, poly-triazine imide (PTI) is highly unusual among layered materials since it is spontaneously soluble in aprotic, polar solvents including dimethylformamide (DMF). The PTI material consists of layers of carbon nitride intercalated with LiBr. When dissolved, the resulting solutions consist of dissolved, luminescent single to multilayer nanosheets of around 60–125 nm in diameter and Li+ and Br− ions originating from the intercalating salt. To understand this unique solubility, the structure of these solutions has been investigated by high-energy X-ray and neutron diffraction. Although the diffraction patterns are dominated by inter-solvent correlations there are clear differences between the X-ray diffraction data of the PTI solution and the solvent in the 4–6 Å−1 range, with real space differences persisting to at least 10 Å. Structural modelling using both neutron and X-ray datasets as a constraint reveal the formation of distinct, dense solvation shells surrounding the nanoparticles with a layer of Br−close to the PTI-solvent interface. This solvent ordering provides a configuration that is energetically favourable underpinning thermodynamically driven PTI dissolution. This article is part of the theme issue 'Exploring the length scales, timescales and chemistry of challenging materials (Part 2)'. [ABSTRACT FROM AUTHOR]

Developing high-performing and scalable electrode materials for supercapacitors and batteries has been of tremendous interest for the world's forthcoming clean and renewable energy transition. As a versatile material, Two-dimensional graphitic carbon nitride (g-CN) has been utilized in electrochemical energy storage (EES) applications due to its nitrogen-rich adsorption sites, cost-effective production, and tunable electronic structure. The electrochemical performance of pristine g-CN has been boosted by forming hybrid architectures with highly conductive carbon-based materials, such as graphene, reduced graphene oxide, carbon nanofibers, carbon nanotubes, and beyond (e.g., MXene). Using such heterogeneous compositions for EES applications has significantly increased in recent years. This study reviews the g-CN/carbon nanomaterial (CNM) hybrids, considering the dimensionality in nanomaterials, and underscores the influence of the material's dimensionality and the synthesis/fabrication routes. The effect of structural and physicochemical changes on the electrode's electrochemical performance after hybridization is presented comparatively. Besides, the comprehensive review outlines challenges and future improvements in g-CN/CNM hybrid materials for outstanding developments in energy storage systems. [Display omitted] • Graphitic carbon nitride (g-CN)/carbon nanomaterial (CNM) hybrids are reviewed for supercapacitor and battery applications. • The impact of the CNM-type on the hybrid electrode's performance is examined through a chemical and physical perspective. • An overview of how hybrid electrode synthesis affects ion/electron transport, surface area, and porosity is provided. • Design-oriented control of the physicochemical properties for enhanced electrochemical performance is exemplified. • g-CN/CNM nanoarchitectures are emphasized as electrode materials with the potential for easy scalability. [ABSTRACT FROM AUTHOR]