Surface-functionalized g-C3N4/3D-printed alkali-activated materials for the removal of emerging water pollutants

The growing demand for sustainable water treatment technologies has spurred interest in structured photocatalytic materials. Herein, we report the first integration of 3D-printed alkali-activated material (AAM) scaffolds with graphitic carbon nitride (g-C₃N₄) for visible-light-driven degradation of emerging organic contaminants. The scaffolds, fabricated by direct ink writing and subsequently functionalized via a PVA-assisted coating, exhibit preserved mesoporosity and uniform g-C₃N₄ coverage. Structural and spectroscopic analyses confirm the successful anchoring of g-C₃N₄ onto the AAM surface, preventing leaching and ensuring long-term reusability. Nitrogen physisorption revealed a moderate decrease in specific surface area (from 90 to 64 m 2 g −1 ) due to partial pore coverage, while maintaining accessible mesoporosity beneficial for mass transfer and interfacial photocatalysis. Under visible-light irradiation, the hybrid monolith achieved 99 % sulfamethoxazole (SMX) degradation and 72.5 % total organic carbon (TOC) mineralization within 210 min using only 1.6 g L −1 of catalyst—surpassing most powdered systems in efficiency-to-dose ratio. Beyond SMX, tests with a quaternary mixture of carbamazepine, ciprofloxacin, and diclofenac confirmed broad-spectrum photocatalytic activity. Quenching and EPR analyses identified •OH, O ₂ •- , and 1 O ₂ as the main reactive oxygen species. Ecotoxicological assays with freshwater microalgae, rotifers, and zebrafish embryos demonstrated a marked reduction in post-treatment toxicity, validating the environmental safety of the process. This reusable and monolithic photocatalytic platform represents a robust, metal-free, and sustainable solution for real-water purification. • 3D-printed alkali-activated scaffolds with g-C 3 N 4 enable visible-light photocatalysis of emerging pharmaceuticals. • Sulfamethoxazole removal reached 99% and mineralization 72.5% TOC in 210 min using only 1.6 g L -1 catalyst. • Structural and spectroscopic data confirmed uniform g-C 3 N 4 anchoring and a stable AAM matrix with negligible leaching. • •OH, O 2 •− , and 1 O 2 were identified as the principal reactive oxygen species driving pollutant degradation. • Freshwater ecotoxicity assays showed marked post-treatment toxicity reduction, supporting environmental safety.

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Journal
Chemical Engineering Journal
Published
2025-12-31
DOI
https://doi.org/10.1016/j.cej.2025.172457
Primary Topic
Advanced Photocatalysis Techniques
Type
article
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article

Surface-functionalized g-C3N4/3D-printed alkali-activated materials for the removal of emerging water pollutants

Rui M. Novais, Nuno P.F. Gonçalves, J. Labrincha, K. Ben Tayeb et al.
Chemical Engineering Journal
Advanced Photocatalysis Techniques
article

Surface-functionalized g-C3N4/3D-printed alkali-activated materials for the removal of emerging water pollutants

Rui M. Novais, Nuno P.F. Gonçalves, J. Labrincha, K. Ben Tayeb, S. Costa, I. Lopes, J.G. Cuadra, Catia Venancio, T. Trindade
article en

Abstract

The growing demand for sustainable water treatment technologies has spurred interest in structured photocatalytic materials. Herein, we report the first integration of 3D-printed alkali-activated material (AAM) scaffolds with graphitic carbon nitride (g-C₃N₄) for visible-light-driven degradation of emerging organic contaminants. The scaffolds, fabricated by direct ink writing and subsequently functionalized via a PVA-assisted coating, exhibit preserved mesoporosity and uniform g-C₃N₄ coverage. Structural and spectroscopic analyses confirm the successful anchoring of g-C₃N₄ onto the AAM surface, preventing leaching and ensuring long-term reusability. Nitrogen physisorption revealed a moderate decrease in specific surface area (from 90 to 64 m 2 g −1 ) due to partial pore coverage, while maintaining accessible mesoporosity beneficial for mass transfer and interfacial photocatalysis. Under visible-light irradiation, the hybrid monolith achieved 99 % sulfamethoxazole (SMX) degradation and 72.5 % total organic carbon (TOC) mineralization within 210 min using only 1.6 g L −1 of catalyst—surpassing most powdered systems in efficiency-to-dose ratio. Beyond SMX, tests with a quaternary mixture of carbamazepine, ciprofloxacin, and diclofenac confirmed broad-spectrum photocatalytic activity. Quenching and EPR analyses identified •OH, O ₂ •- , and 1 O ₂ as the main reactive oxygen species. Ecotoxicological assays with freshwater microalgae, rotifers, and zebrafish embryos demonstrated a marked reduction in post-treatment toxicity, validating the environmental safety of the process. This reusable and monolithic photocatalytic platform represents a robust, metal-free, and sustainable solution for real-water purification. • 3D-printed alkali-activated scaffolds with g-C 3 N 4 enable visible-light photocatalysis of emerging pharmaceuticals. • Sulfamethoxazole removal reached 99% and mineralization 72.5% TOC in 210 min using only 1.6 g L -1 catalyst. • Structural and spectroscopic data confirmed uniform g-C 3 N 4 anchoring and a stable AAM matrix with negligible leaching. • •OH, O 2 •− , and 1 O 2 were identified as the principal reactive oxygen species driving pollutant degradation. • Freshwater ecotoxicity assays showed marked post-treatment toxicity reduction, supporting environmental safety.

Chemical Engineering JournalVol. 529
Centre National de la Recherche Scientifique (FR), Laboratoire des Sciences de l'Ingénieur pour l'Environnement (FR), University of Aveiro (PT)
Responsible consumption and production
Openalex Percentile: Top 51%
Advanced Photocatalysis Techniques
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