Holey defective g-C N photocatalysts, which are easily prepared via a novel photoassisted heating process, are reported. The photoassisted treatment not only helps to create abundant holes, endowing g-C N with more exposed catalytic active sites and crossplane diffusion channels to shorten the diffusion distance of both reactants from the surface to bulk and charge carriers from the bulk to surface, but also introduces nitrogen vacancies in the tri-s-triazine repeating units of g-C N , inducing the narrowing of intrinsic bandgap and the formation of defect states within bandgap to extend the visible-light absorption range and suppress the radiative electron-hole recombination. As a result, the holey defective g-C N photocatalysts show much higher photocatalytic activity for H O production with optimized enhancement up to ten times higher than pristine bulk g-C N . The newly developed synthetic strategy adopted here enables the sufficient utilization of solar energy and shows rather promising for the modification of other materials for efficient energy-related applications.

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A simple method is developed to fabricate protonated porous graphitic carbon nitride nanosheets (P-PCNNS) by protonation-exfoliation of bulk graphitic carbon nitride (BCN) with phosphoric acid (H3 PO4 ). The H3 PO4 treatment not only helps to exfoliate the BCN into 2D ultrathin nanosheets with abundant micro- and mesopores, endowing P-PCNNS with more exposed active catalytic sites and cross-plane diffusion channels to facilitate the mass and charge transport, but also induces the protonation of carbon nitride polymer, leading to the moderate removal of the impurities of carbon species in BCN for the optimization of the aromatic π-conjugated system for better charge separation without changing its chemical structure. As a result, the P-PCNNS show much higher photocatalytic performance for hydrogen evolution and CO2 conversion than bare BCN and graphitic carbon nitride nanosheets.

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