Graphite-phase polymeric carbon nitride (GPPCN) has emerged as a promising metal-free material toward optoelectronics and (photo)catalysis. However, the insolubility of GPPCN remains one of the biggest impediments toward its potential applications. Herein, we report that GPPCN could be dissolved in concentrated sulfuric acid, the first feasible solvent so far, due to the synergistic protonation and intercalation. The concentration was up to 300 mg/mL, thousands of time higher than previous reported dispersions. As a result, the first successful liquid-state NMR spectra of GPPCN were obtained, which provides a more feasible method to reveal the finer structure of GPPCN. Moreover, at high concentration, a liquid crystal phase for the carbon nitride family was first observed. The successful dissolution of GPPCN and the formation of highly anisotropic mesophases would greatly pave the potential applications such as GPPCN-based nanocomposites or assembly of marcroscopic, ordered materials.

Responsive assembly of 2D materials is of great interest for a range of applications. In this work, interfacial functionalized carbon nitride (CN) nanofibers were synthesized by hydrolyzing bulk CN in sodium hydroxide solution. The reversible assemble and disassemble behavior of the as-prepared CN nanofibers was investigated by using CO2 as a trigger to form a hydrogel network at first. Compared to the most widespread absorbent materials such as active carbon, graphene and previously reported supramolecular gel, the proposed CN hydrogel not only exhibited a competitive absorbing capacity (maximum absorbing capacity of methylene blue up to 402 mg/g) but also overcame the typical deficiencies such as poor selectivity and high energy-consuming regeneration. This work would provide a strategy to construct a 3D CN network and open an avenue for developing smart assembly for potential applications ranging from environment to selective extraction.

Superior to silica nanoparticles, the easily accessible and removable CaCO3 particles produced porous carbon nitride with photocurrents 7.5-times that of the bulk one.

A heterojunction photocatalyst made up of a single substrate is reported. The heterointerfaces of carbon nitride (CN) are natively compatible due to their very similar chemical and crystalline structures. Moreover, the varieties in the nanostructures of CN led to different energy levels that not only matched well with each other but also enabled a sufficient internal electric field at their interfaces to suppress unwanted recombination of charge carriers in photocatalysis.

No abstract

Polymeric carbon nitride (CN) has recently emerged as a novel metal-free semiconductor due to its unique electronic structure, wide availability, and promising applications in photoelectrochemical solar energy conversion. However, few works regarding CN photoelectrode optimization such as by minimization of unwanted grain boundary effects have been reported, which would greatly influence the photoelectrochemcial conversion efficiency. Herein, three general ways of preparing CN photoelectrode are presented and compared, including drop-casting of CN particles, or further blendeding with Nafion or PEDOT-PSS as the binder. In addition, the influences of CN particle sizes (0.5, 1.1, and 3.2 μm) and the film thickness (i.e., the loading amount) to the overall photoelectrochemcial activity were also evaluated in detail. As a result, when PEDOT-PSS acted as binder, CN particles with size of 0.5 μm and an optimal loading amount (2.4 mg/cm(2)) were adopted; the as-prepared CN photoelectrode had much superior photoelectrochemical activity than all other counterparts. Therefore, this study would pave the way for preparing CN photoelectrode of superior quality so as to promote CN materials to be better applied in solar fuel and sensing applications.

As an emerging metal‐free semiconductor, covalently bonded carbon nitride (CN) has attracted much attention in photocatalysis. However, drawbacks such as a high recombination rate of excited electrons and holes hinder its potential applications. Tailoring the crystallinity of semiconductors is an important way to suppress unwanted charge recombination, but has rarely been applied to CN so far. Herein, a simple method to synthesize CN of high crystallinity by protonation of specific intermediate species during conventional polymerization is reported. Interestingly, the as‐obtained CN exhibited improved photocatalytic activities of up to seven times those of the conventional bulk CN. This approach, with only a slight change to the conventional method, provides a facile way to effectively regulate the crystallinity of bulk CN to improve its photocatalytic activities and sheds light on large‐scale industrial applications of CN with high efficiency for sustainable energy.

Hematite (α-Fe2O3) crystals with uniform size and structure are synthesized through very facile one-pot hydrothermal methods without any additive. The as-synthesized sub-micrometer-sized α-Fe2O3 crystals with small surface areas perform superb visible light photodegradation activities, even much better than most other α-Fe2O3 nanostructures with large surface areas. Profound mechanism analyses reveal that the microwave-assisted hydrothermal (Mic-H) synthesized α-Fe2O3 is enclosed by 12 high-index {2-15} facets. The structure and the low unoccupied molecular orbital (LUMO) of the high-index planes result in the excellent photocatalytic activity. This is the first report on the formation of {2-15} plane group of hematite, and the synthesis of the hematite particles with the {2-15} planes is very simple and no any facet-controlling agent is used. This study may pave the way to further performance enhancement and practical applications of the cheap hematite materials.