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The application of solar-driven photocatalytic processes shows considerable potential for renewable energy production and environmental remediation. Graphitic carbon nitride (g-C3N4) has emerged as a highly promising metal-free photocatalyst due to its outstanding electronic structure and physicochemical properties. However, the intrinsic constraints of pristine g-C3N4, such as limited visible light absorption range, high recombination rates of photogenerated charge carriers, and a scarcity of active sites, have significantly hindered its photocatalytic performance and practical implementations. Recent studies have demonstrated that defect engineering can substantially mitigate these issues by enhancing both light absorption and charge separation efficiency, thereby improving photocatalytic performance. This review provides a comprehensive overview of intrinsically defective g-C3N4-based materials, focusing on the types of intrinsic defects, their modification strategies, and the recent advancements in the field. It also highlights the diverse applications of defect-modified g-C3N4, including wastewater remediation, hydrogen evolution, CO2 conversion, NO removal, nitrogen fixation, photocatalytic disinfection, and H2O2 production. Finally, the current challenges and future perspectives are discussed of g-C3N4-based photocatalytic materials, offering insights and practical guidance for the development of advanced g-C3N4-based photocatalysts.
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