Tuning the structural defects of
graphite carbon nitride (g-C3N4) is an effective
strategy to modify its band
structure and promote charge separation, but it is still limited by
complex and harsh preparation processes. Herein, g-C3N4 with nitrogen defects were fabricated by one-pot thermal
polymerization of urea and fumaric acid. The N–(C)3 site, being the active site for photocatalytic hydrogen evolution,
reached at a rate of 94.1 μmol·h–1, which
was approximately 2.64 times that of the original g-C3N4. Nitrogen defective g-C3N4 had more
electrons and stronger H2O molecule adsorption capacity,
identified by systematic experiments and DFT calculations. The carboxyl
group of fumaric acid reacted with amino group of urea to prevent
self-polymerization process of urea and induce nitrogen defects. The
changed band structures promoted the absorption of visible light,
effective separation of charge, and increased hydrogen evolution driving
force. This work will provide a simple and green approach to prepare
nitrogen defective g-C3N4 with tunable band
structures.
The 3D/2D g-C3N4/ZnIn2S4 hollow spherical heterostructure can greatly increase visible light absorption and improve the efficiency of photo-generated electron migration and conversion, resulting in an excellent CO generation rate.
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