Addition of Fe<sub>3</sub>O<sub>4</sub> on Carbon Nitride Moves the ROS Formation from HO Radicals to Singlet Oxygen Leading to an Enhanced and Selective Disinfecting Action

Bacterial contamination poses serious challenges for public health in several scenarios, such as in developing antimicrobial surfaces for biomedical applications and clean water availability. To face this, in the current work we have incorporated Fe<sub>3</sub>O<sub>4</sub> domains onto the graphitic carbon nitride framework (g-C<sub>3</sub>N<sub>4</sub>). Therefore, a series of iron-doped nanocomposites (g-C<sub>3</sub>N<sub>4</sub>, g-C<sub>3</sub>N<sub>4</sub>-25, g-C<sub>3</sub>N<sub>4</sub>-50, g-C<sub>3</sub>N<sub>4</sub>-100, and g-C<sub>3</sub>N<sub>4</sub>-500) were synthesized by controlling the adsorption of Fe on bare g-C<sub>3</sub>N<sub>4</sub>. These materials were rigorously characterized by transmission electron microscopy (TEM), X-ray diffraction (XRD), thermogravimetric analysis (TGA), dynamic light scattering (DLS), Fourier transform infrared spectroscopy (FTIR), <i>Z</i>-potential (PZC), fluorescence, electrochemical impedance, and X-ray photoelectron spectroscopy (XPS), confirming the successful formation of Fe<sub>3</sub>O<sub>4</sub> nanoparticles and the creation of abundant surface defects. Photocatalytic experiments using ciprofloxacin (1-cyclopropyl-6-fluoro-4-oxo-7-(piperazin-1-yl)-quinoline-3-carboxylic acid) as probe compound, under UV-Vis irradiation, highlighted the g-C<sub>3</sub>N<sub>4</sub>-25 material as the one having the higher photocatalytic activity. Additional tests using chemical scavengers showed a shift from hydroxyl-radical-driven pathways in bare g-C<sub>3</sub>N<sub>4</sub> to the more selective singlet-oxygen in the Fe-modified material. <i>E. coli</i> disinfection under indoor light produced a 6.0 log<sub>10</sub> CFU/mL reduction with g-C<sub>3</sub>N<sub>4</sub>-25, compared to only 2.8 log<sub>10</sub> with pristine g-C<sub>3</sub>N<sub>4</sub>. Comparative experiments with Co- and Cu-doped analogues further showed superior kinetics and ROS yields of the iron material. Finally, the best-performing Fe-g-C<sub>3</sub>N<sub>4</sub> catalyst was embedded in an alginate matrix to produce a self-disinfecting surface that maintained a 5.9 ± 0.3 log<sub>10</sub> CFU/mL decrease in <i>E. coli</i> after five consecutives 24 h irradiation cycles. These results position Fe-doped g-C<sub>3</sub>N<sub>4</sub> as a versatile platform for the sustainable photocatalytic removal of contaminants and durable antimicrobial coatings.

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Journal
ACS Omega
Published
2025-09-22
DOI
https://doi.org/10.1021/acsomega.5c02329
Citations
1
Primary Topic
Advanced Photocatalysis Techniques
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article
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Addition of Fe3O4 on Carbon Nitride Moves the ROS Formation from HO Radicals to Singlet Oxygen Leading to an Enhanced and Selective Disinfecting Action

Isabel Cristina Ortega-Bedoya, Darwin Augusto Torres-Cerón, Ronald Vargas, Dany S. Monje, D. Fabio Mercado, Gloria Cristina Valencia, Elisabeth Restrepo-Parra, S. Amaya-Roncancio, Ricardo Antonio Torres-Palma
article en
1 citations

Abstract

Bacterial contamination poses serious challenges for public health in several scenarios, such as in developing antimicrobial surfaces for biomedical applications and clean water availability. To face this, in the current work we have incorporated Fe<sub>3</sub>O<sub>4</sub> domains onto the graphitic carbon nitride framework (g-C<sub>3</sub>N<sub>4</sub>). Therefore, a series of iron-doped nanocomposites (g-C<sub>3</sub>N<sub>4</sub>, g-C<sub>3</sub>N<sub>4</sub>-25, g-C<sub>3</sub>N<sub>4</sub>-50, g-C<sub>3</sub>N<sub>4</sub>-100, and g-C<sub>3</sub>N<sub>4</sub>-500) were synthesized by controlling the adsorption of Fe on bare g-C<sub>3</sub>N<sub>4</sub>. These materials were rigorously characterized by transmission electron microscopy (TEM), X-ray diffraction (XRD), thermogravimetric analysis (TGA), dynamic light scattering (DLS), Fourier transform infrared spectroscopy (FTIR), <i>Z</i>-potential (PZC), fluorescence, electrochemical impedance, and X-ray photoelectron spectroscopy (XPS), confirming the successful formation of Fe<sub>3</sub>O<sub>4</sub> nanoparticles and the creation of abundant surface defects. Photocatalytic experiments using ciprofloxacin (1-cyclopropyl-6-fluoro-4-oxo-7-(piperazin-1-yl)-quinoline-3-carboxylic acid) as probe compound, under UV-Vis irradiation, highlighted the g-C<sub>3</sub>N<sub>4</sub>-25 material as the one having the higher photocatalytic activity. Additional tests using chemical scavengers showed a shift from hydroxyl-radical-driven pathways in bare g-C<sub>3</sub>N<sub>4</sub> to the more selective singlet-oxygen in the Fe-modified material. <i>E. coli</i> disinfection under indoor light produced a 6.0 log<sub>10</sub> CFU/mL reduction with g-C<sub>3</sub>N<sub>4</sub>-25, compared to only 2.8 log<sub>10</sub> with pristine g-C<sub>3</sub>N<sub>4</sub>. Comparative experiments with Co- and Cu-doped analogues further showed superior kinetics and ROS yields of the iron material. Finally, the best-performing Fe-g-C<sub>3</sub>N<sub>4</sub> catalyst was embedded in an alginate matrix to produce a self-disinfecting surface that maintained a 5.9 ± 0.3 log<sub>10</sub> CFU/mL decrease in <i>E. coli</i> after five consecutives 24 h irradiation cycles. These results position Fe-doped g-C<sub>3</sub>N<sub>4</sub> as a versatile platform for the sustainable photocatalytic removal of contaminants and durable antimicrobial coatings.

ACS OmegaVol. 10(39)
Universidad Peruana Cayetano Heredia (PE), Pedagogical and Technological University of Colombia (CO), Universidad de Antioquia (CO), Universidad Nacional de Colombia (CO), Institute of Micro and Nanotechnology (ES), Equipos Nucleares (Spain) (ES), Universidad Nacional de San Martín (PE), Institute of Plasma Physics (IT), Clínica CES (CO), Instituto Tecnológico de Chascomús (AR)
Openalex Percentile: Top 38%
Advanced Photocatalysis Techniques
0.36
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