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Graphitic carbon nitride (g-C 3 N 4 ) has aroused intense expectations owing to its outstanding visible-light-response capability for hydrogen generation from water. However, the low-yield, low practical surface area and high photogenerated charge recombination rate severely limits its photocatalytic performance . Here, in this study high-yield synthesis of g-C 3 N 4 with a large surface area has been achieved successfully through an in situ pyrolysis of cyanamide with the assist of the bifunctional urea. During the synthesis process, urea may decompose into a lot of ammonia and carbon dioxide, which acts as the supplementary-nitrogen-source and bubble-generating template respectively. It is found that the surface area and photocatalytic activity can be controlled by adjusting the addition of the environmentally friendly bifunctional urea. The as-prepared g-C 3 N 4 exhibits unique optical activity as well as photoelectriochemical activity for solar-to-chemical conversion, and this simple bifunctional method may open a new pathway for designing and optimizing of photocatalysts. [ABSTRACT FROM AUTHOR]

The search of efficient and stable photocatalysts for the evolution of hydrogen from water using solar energy is of great importance for material science today. Limited by the relatively inferior stability of oxynitrides, the availability of these visible-light-response materials in photocatalysis is still far below what is expected. Here we report a novel oxynitride Ce 0.3 Zr 0.7 O 1.88 N 0.12 as an efficient and stable H 2 -evolving photocatalyst under visible light irradiation, which can further enable overall water splitting by coupling with an O 2 -evolving photocatalyst via Z-scheme. Experimental and theoretical results together reveal that the origin of the excellent activity and stability of Ce 0.3 Zr 0.7 O 1.88 N 0.12 photocatalyst can be attributed to the improved separation rate of photoexcited charge carriers by surface and sub-surface oxygen vacancies. The present study provides a strategy to engineer efficient and stable photocatalysts, and the oxynitride mentioned above could act as a promising candidate of H 2 -evolving photocatalyst for designing a prominent Z-scheme photocatalytic system. [ABSTRACT FROM AUTHOR]

• The carboxyl group with electron-withdrawing effect was grafted on the surface of graphite carbon nitride. • The electron-withdrawing effect can promote the separation and migration of carriers to improve photocatalytic performance. • The performance achieved 52 times enhancement with an apparent quantum yield of 15.7 % at 420 nm. Graphitic carbon nitride (g-C 3 N 4) has recently emerged as a promising candidate for photocatalytic hydrogen evolution, but only showed limited activity owing to its sluggish photogenerated carriers separation and migration. Herein, the carboxyl-functionalized g-C 3 N 4 (O CN) was synthesized by a grafting post-treatment method to alleviate the negative influences from this intrinsic drawback. As a result, the surface carboxyl groups greatly improve charge carrier dynamics to suppress carriers recombination via the driving force originated from its electron-withdrawing effects. The resultant O CN exhibits 52 times higher hydrogen evolution rate than the pristine, and possesses a high apparent quantum yield (AQY) of 15.7 % at 420 ± 15 nm. This work deepens the understanding of the surface group related modifications for photocatalytic materials, further providing a promising approach for rational design of photocatalysts with highly efficient solar energy conversion. [ABSTRACT FROM AUTHOR]