Graphitic carbon nitride (g-C3N4) is a promising metal-free photocatalyst, but its efficiency is often limited by rapid charge carrier recombination. We report a scalable, one-step sodium-assisted thermal polycondensation of urea that achieves precise electronic modulation while preserving the structural integrity of the g-C3N4 framework. Urbach energy analysis was employed to quantify band-tail disorder, showing a modest increase of 11.3 meV (71.4 to 82.7 meV). Together with time-resolved fluorescence spectroscopy, this indicates mild band-tail broadening and predominantly shallow electron trapping rather than the formation of a large population of detrimental deep traps. Time-resolved fluorescence spectroscopy confirms enhanced charge carrier separation, as sodium-induced shallow traps suppress radiative recombination and facilitate electron transfer to the surface. Consequently, optimized Na(0.01)–CN nanosheets exhibit exceptional dual-functionality. Under single low-energy 416 nm LED irradiation (3.4 W m−2), the material achieves complete degradation of parent Ofloxacin and Tetracycline (20 ppm) within just 8 min with an apparent quantum yield of 5.83 %. Furthermore, the catalyst demonstrates a remarkable initial hydrogen evolution rate of 8.8 mmol g−1h−1 under simulated solar light. These findings highlight that maintaining low Urbach energy through controlled doping is a superior strategy for developing stable, high-performance photocatalysts for environmental remediation and solar fuel production.

Electron-trap modulated graphitic carbon nitride nanosheets for ultrafast antibiotic degradation and high-rate hydrogen evolution

Fornasiero, Paolo
2026

Abstract

Graphitic carbon nitride (g-C3N4) is a promising metal-free photocatalyst, but its efficiency is often limited by rapid charge carrier recombination. We report a scalable, one-step sodium-assisted thermal polycondensation of urea that achieves precise electronic modulation while preserving the structural integrity of the g-C3N4 framework. Urbach energy analysis was employed to quantify band-tail disorder, showing a modest increase of 11.3 meV (71.4 to 82.7 meV). Together with time-resolved fluorescence spectroscopy, this indicates mild band-tail broadening and predominantly shallow electron trapping rather than the formation of a large population of detrimental deep traps. Time-resolved fluorescence spectroscopy confirms enhanced charge carrier separation, as sodium-induced shallow traps suppress radiative recombination and facilitate electron transfer to the surface. Consequently, optimized Na(0.01)–CN nanosheets exhibit exceptional dual-functionality. Under single low-energy 416 nm LED irradiation (3.4 W m−2), the material achieves complete degradation of parent Ofloxacin and Tetracycline (20 ppm) within just 8 min with an apparent quantum yield of 5.83 %. Furthermore, the catalyst demonstrates a remarkable initial hydrogen evolution rate of 8.8 mmol g−1h−1 under simulated solar light. These findings highlight that maintaining low Urbach energy through controlled doping is a superior strategy for developing stable, high-performance photocatalysts for environmental remediation and solar fuel production.
2026
Istituto di Chimica dei Composti OrganoMetallici - ICCOM -
Antibiotic degradation
g-C3N4
nanosheets
Hydrogen evolution
LED-driven photocatalysis
Shallow trap engineering
Urbach energy
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Utilizza questo identificativo per citare o creare un link a questo documento: https://hdl.handle.net/20.500.14243/574141
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