<p>The construction of metal-free heterojunctions offers an effective pathway for enhancing photocatalytic degradation of persistent antibiotic. Herein, we report a metal-free 2D/2D polyimide/graphitic carbon nitride (PI/g- C<sub>3</sub>N<sub>4</sub>) heterojunction synthesized through a facile chemical adsorption process, enabling intimate interfacial coupling and efficient visible-light activation. Systematic modulation of the PI:g-C<sub>3</sub>N<sub>4</sub> ratio revealed strong composition, structure and activity relationships, as characterized by XRD, FESEM, HRTEM, UV–Vis DRS, BET, XPS and EIS analysis. Among all formulations, the 1:9 PI/g- C<sub>3</sub>N<sub>4</sub> heterostructure achieved the highest performance, delivering 80% tetracycline degradation under visible light, attributed to its enhanced light-harvesting ability, accelerated charge-carrier separation, and synergistic 2D/2D interfacial interactions. Transient photocurrent and EIS measurements further confirmed the improved charge-transfer kinetics. The photocatalyst demonstrated excellent stability, retaining its activity over four consecutive cycles. Mechanistic studies indicate a type-II charge-transfer pathway, enabling spatially separated redox sites that promote efficient antibiotic mineralization. This work highlights the rational design of 2D/2D metal-free heterojunctions as a sustainable platform for visible-light-driven photocatalysis and provides new insights for developing high-performance photocatalysts for antibiotic removal.</p>

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Construction of metal-free 2D/2D PI/g-C3N4 heterojunction for enhanced photocatalytic degradation of tetracycline: interfacial engineering and charge separation

  • Maode Guo,
  • He Li,
  • Tan Winie,
  • Lim Ying Chin

摘要

The construction of metal-free heterojunctions offers an effective pathway for enhancing photocatalytic degradation of persistent antibiotic. Herein, we report a metal-free 2D/2D polyimide/graphitic carbon nitride (PI/g- C3N4) heterojunction synthesized through a facile chemical adsorption process, enabling intimate interfacial coupling and efficient visible-light activation. Systematic modulation of the PI:g-C3N4 ratio revealed strong composition, structure and activity relationships, as characterized by XRD, FESEM, HRTEM, UV–Vis DRS, BET, XPS and EIS analysis. Among all formulations, the 1:9 PI/g- C3N4 heterostructure achieved the highest performance, delivering 80% tetracycline degradation under visible light, attributed to its enhanced light-harvesting ability, accelerated charge-carrier separation, and synergistic 2D/2D interfacial interactions. Transient photocurrent and EIS measurements further confirmed the improved charge-transfer kinetics. The photocatalyst demonstrated excellent stability, retaining its activity over four consecutive cycles. Mechanistic studies indicate a type-II charge-transfer pathway, enabling spatially separated redox sites that promote efficient antibiotic mineralization. This work highlights the rational design of 2D/2D metal-free heterojunctions as a sustainable platform for visible-light-driven photocatalysis and provides new insights for developing high-performance photocatalysts for antibiotic removal.