Carbon nitride materials: impact of synthetic method on photocatalysis and immobilization for photocatalytic pollutant degradation

Different synthesis routes for carbon nitride materials (CN) and the resulting products were compared to study the photocatalytic activity (pollutant degradation) in dependence on structure and properties. The CN materials were synthesized by thermal decomposition of dicyandiamide in air and under argon as well as in sealed ampoules with or without the use of a salt melt. The as-prepared materials were characterized by IR spectroscopy, nitrogen adsorption measurement, solid-state NMR spectroscopy, diffuse reflectance UV–Vis spectroscopy, elemental analysis and powder X-ray diffraction (PXRD). The surface polarity of the CN materials was estimated by adsorption of the dicyano-bis(1,10-phenanthroline)-iron(II) complex, which allows an evaluation of the degree of condensation. The CN materials were tested with regard to the photocatalytic degradation of rhodamine B (RhB). It is shown that the photocatalytic activity increases with higher surface polarity. Promising CN materials with high RhB degradation of 85% within 25 min and high surface polarity of 0.89 were selected for an immobilization approach to obtain coatings on a silicone substrate using a high-volume low-pressure (HVLP) spray coating technique. To study the photocatalytic activity of the catalyst coatings, the degradation rates of an aqueous RhB solution and solutions of organic pollutants such as triclosan and ethinyl estradiol were examined. Pollutants are decomposed with up to 63% of the initial concentration. Xenon lamps and different LEDs were used as light sources for comparison. Particularly high degradation efficiencies were obtained using LEDs, and the degradation rates are increased by adjusting the emission spectrum of the lamp to the pollutant and absorption edge of the catalyst, which results in a 40 times higher degradation efficiencies of LEDs compared to a Xe lamp. Graphical abstract