3D printed photopolymer derived carbon catalysts for enhanced wet peroxide oxidation

[Display omitted] •3D printed carbons activated with CO2 reaches BET surface areas up to 884 m2/g.•Urea functionalization improved catalytic activity of carbon monoliths.•The role of adsorption was deeply studied in catalytic wet peroxide oxidation.•Reusability tests demonstrated the stability of th...

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Veröffentlicht in:Chemical engineering journal (Lausanne, Switzerland : 1996) Switzerland : 1996), 2024-11, Vol.499, p.156574, Article 156574
Hauptverfasser: Silva, Adriano S., Diaz de Tuesta, Jose L., Henrique, Adriano, Roman, Fernanda F., Omralinov, Daria, Steldinger, Hendryk, Gläsel, Jan, Etzold, Bastian J.M., Silva, Jose A.C., Silva, Adrián M.T., Pereira, Ana I., Gomes, Helder T.
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Sprache:eng
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Zusammenfassung:[Display omitted] •3D printed carbons activated with CO2 reaches BET surface areas up to 884 m2/g.•Urea functionalization improved catalytic activity of carbon monoliths.•The role of adsorption was deeply studied in catalytic wet peroxide oxidation.•Reusability tests demonstrated the stability of the carbon materials as catalysts.•Carbon monolith kept paracetamol conversions above 85 % for 48 h on stream. In this paper, we explore the application of powdered carbon and 3D-printed carbon monoliths prepared by carbonization of a tailored photopolymer. We demonstrate the efficiency of the developed carbonaceous samples in removing paracetamol (PCM) and sulfamethoxazole (SMX), used as model contaminants. Our results demonstrate that carbon samples are active in CWPO, and their catalytic activity is significantly improved by applying nitric acid and urea functionalization methods. The characterization results showed the pure carbon nature of the material (no ashes), their unique structure defects proven by Raman (D/G > 1.8), textural properties (SBET = 291–884 m2/g) and their surface chemistry, which was addressed by pHPZC (2.5–7.5), acidity (312–2375 µ mol gcat−1) and basicity (117–653 µ mol gcat−1) determination and XPS of highlighted materials (N1s = 0–3.51 at.%, O1s = 7.1–15.3 at.%). Using desorption assays, our study reveals the adsorption role for pollutant degradation by CWPO using carbon monolithic samples. At last, we demonstrated the ability of functionalized 3D-printed carbon monoliths to keep degradation of PCM and total organic carbon (TOC) above 85 % and 80 %, respectively, during 48 h in a continuous flow CWPO system. Sulfamethoxazole degradation in continuous system was also studied to validate the catalyst versatility, achieving 81 % and 79 % pollutant degradation and TOC abatement, respectively, during 48 h on stream. The characterization of the recovered catalyst provides further insights into the absence of structural modifications after the reaction, reinforcing the stability and reusability characteristic of the 3D-printed carbon catalyst.
ISSN:1385-8947
DOI:10.1016/j.cej.2024.156574