Graphitic
carbon nitride (g-C3N4) offers
a great number of advantages for use as a photocatalyst to facilitate
a wide variety of photocatalytic reactions. However, pristine g-C3N4 suffers from unsatisfactory photocatalytic performance
in actual practice. Nonetheless, as a nitrogen-rich layered material,
g-C3N4 offers abundant opportunities for the
formation of hydrogen bonds between the NH/NH2 groups within
the layers, which can incite proton transfer reactions owing to the
inherent polarity of the proton donor and acceptor in the hydrogen
bond and thereby improve the transport rate of photogenerated carriers,
especially for holes. Yet, relatively little work has been done to
improve the photocatalytic performance of g-C3N4 through efforts to enhance its hydrogen bond network. The present
work addresses this issue by constructing a hydrogen bond network
on g-C3N4 by pressurizing a mixture of pristine
g-C3N4 nanosheets with water at a temperature
of 120 °C for 12 h. The results of nuclear magnetic resonance
spectroscopy and density functional theory demonstrate that the hydrogen
bonds on the g-C3N4 surfaces provide an additional
pathway for the separation of photogenerated electrons and enhanced
hole transfer kinetics. The hydrogen bond network formed between the
g-C3N4 layers effectively suppresses charge
complexation, improves the photocatalytic efficiency of g-C3N4, and increases the selectivity for photocatalytic products.
Our results provide valid insights for designing g-C3N4 photocatalysts with high photocatalytic activity.