Improving the Photocatalytic Activity of Graphitic Carbon Nitride Through Ionic Liquid-Mediated Thermal Annealing

Graphitic carbon nitride (g-C3N4) has shown a great promise in photocatalytic hydrogen evolution. However, the catalytic activity of g-C3N4 derived from nitrogen-rich compounds is still limited by fast charge carrier recombination and slow surface reaction dynamics. Herein, a series of primary g-C3N4 materials were prepared by thermal polymerization of melamine and/or urea, and then thermally treated with the involvement of different ionic liquids under altering heat conditions. Imidazole-containing ionic liquids, such as 1-propyl-3-methylimidazolium chloride ([PMIm]Cl), acted as an effective additive to mediate the thermal annealing behavior of primary g-C3N4, leading to the dissociation of aggregates into porous nanosheets with varying element compositions and with increased surface area. Regardless of little change in optical absorption and electronic structure, the resulting porous g-C3N4 nanosheets promoted the separation and transfer of photogenerated charges and modified surface hydrogen desorption. Hydrogen evolution tests confirmed that the catalytic activity of g-C3N4 from the co-polymerization of melamine and urea was enhanced by ∼3.4 and ∼7.4 times upon [PMIm]Cl-free and -mediated thermal annealing, respectively. This work suggests the potential effect of the additive involvement in the thermal annealing on the photocatalytic activity of g-C3N4.