3D-crumpled graphitic carbon nitride achieving promoted visible-light-driven molecular oxygen activation for phenol...

Boosting optical absorption and charge transfer of g-C₃N₄ is of great importance but a challenging task for developing metal-free high-performance photocatalyst. Herein, 3D-crumpled g-C₃N₄ (DCN) is synthesized through a direct top-down thermal etching strategy. The thermal exfoliation of layered bulk g-C₃N₄ (BCN) in air atmosphere induces partial distortion of heptazine-based g-C₃N₄ nanosheet, which further self-assemble into 3D-crumpled network structure. Spectroscopic and photoelectrochemical characterization demonstrate that the unique DCN can not only remarkably extend the visible-light response region to 600 nm by awakening the n-π* electron transition, but also significantly promote O₂ activation for selective H₂O₂ generation owing to the intensified electron delocalization and charge transport ability. Thus, DCN catalyst realizes an excellent photocatalytic phenol degradation rate under visible light irradiation (0.690 h^-1), far (4.4-fold) out from the BCN counterparts. This work enables synergistic optimization of optical absorption, charge transport and surface-active sites by constructing a 3D-crumpled structure, which expands the engineering toolbox of metal-free skeleton photocatalyst for developing practical and economical catalysts for environmental remediation.