Graphitic carbon nitride (g- CN) is a promising heterogeneous metal-free catalyst for organic photosynthesis, solar energy conversion, and photodegradation of pollutants. Its catalytic performance is easily adjustable by modifying texture, optical, and electronic properties via nanocasting, doping, and copolymerization. However, simultaneous optimization has yet to be achieved. Here, a facile synthesis of mesoporous g-CN using molecular cooperative assembly between triazine molecules is reported. Flower-like, layered spherical aggregates of melamine cyanuric acid complex (MCA) are formed by precipitation from equimolecular mixtures in dimethyl sulfoxide (DMSO). Thermal polycondensation of MCA under nitrogen at 550 ° C produces mesoporous hollow spheres comprised of tri-s -triazine based g-CN nanosheets (MCA-CN) with the composition of C 3 N 4.14 H 1.98 . The layered structure succeeded from MCA induces stronger optical absorption, widens the bandgap by 0.16 eV, and increases the lifetime of photoexcited charge carriers by twice compared to that of the bulk g-CN, while the chemical structure remains similar to that of the bulk g-CN. As a result of these simultaneous modifi cations, the photodegradation kinetics of rhodamine B on the catalyst surface can be improved by 10 times.

Ordered mesoporous carbon nitride shows improved photoactivity and is promising as a host semiconductor scaffold for the design of hybrid visible-light-sensitive catalysts, as it enables the co-assembly of chromophoric antenna molecules, water-reduction catalysts (here exemplified by Pt), and/or water-oxidation complexes into the host matrix, thus generating a new type of biomimetic photocatalyst system for water splitting chemistry but also for selective organic synthesis.

A multistep templating procedure is used to prepare graphitic carbon nitride (g‐C3N4) and titanium nitride/carbon composites with ordered, 2D hexagonal porosity. First, the carbon nitride is prepared by nanocasting using a silica (SBA‐15) template. This carbon nitride is then replicated as a metal nitride carbon composite, using a simultaneous templating/conversion scheme (“reactive templating”).

Simple organic cooperative assembly of triazine molecules leads to three-dimensional macroscopic assemblies of low-dimensional graphitic carbon nitrides (g-CNs), for example, nanoparticles, nanotubes, and nanosheets. The approach enables the characterization of the cooperative properties and photocatalytic activities of low-dimensional g-CN materials in hydrogen evolution reactions from water under visible light.