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Görünür Işık Altında HKUST-1 ile Peroksimonosülfat Aktivasyonu Yoluyla Parasetamolün Fotokatalitik Bozunumu

Year 2026, Volume: 21 Issue: 1 , 195 - 205 , 30.03.2026
https://doi.org/10.55525/tjst.1775116
https://izlik.org/JA65GF97CU

Abstract

Parasetamol, su ortamlarında giderek daha sık tespit edilen ve üreme, hormonal denge ve ekosistem güvenliği üzerinde potansiyel riskler oluşturabilen yeni ortaya çıkan kirleticilerden biridir. Bu nedenle, parasetamolün giderimi için etkili ve sürdürülebilir yöntemlerin geliştirilmesi büyük önem taşımaktadır. Bu çalışmada bakır tabanlı metal-organik kafes yapısı HKUST-1, görünür ışık altında peroksimonosülfat (PMS) aktivasyonu için bir fotokatalizör olarak kullanılmış ve parasetamolün bozunumu incelenmiştir. HKUST-1/PMS/görünür ışık sistemi 150 dakika içerisinde %90’ın üzerinde giderim sağlayarak yalnızca PMS veya yalnızca görünür ışık kullanılan sistemlere kıyasla önemli ölçüde daha yüksek performans göstermiştir. Radikal yakalama deneyleri sülfat radikallerinin (SO4•⁻) başlıca aktif tür olduğunu, hidroksil radikallerinin (•OH) ise sürece katkı sağladığını göstermiştir. PMS/görünür ışık sistemine kıyasla HKUST-1’in varlığı bozunma hızını belirgin şekilde artırmış ve fotokataliz ile PMS aktivasyonu arasında güçlü bir sinerjik etki olduğunu ortaya koymuştur. Ayrıca HKUST-1’in yapısal bozulma göstermeden birden fazla döngü boyunca yüksek kararlılık ve yeniden kullanılabilirlik sergilediği PXRD analizleri ile doğrulanmıştır. Bu çalışma, saf HKUST-1’in farmasötik kirleticilerin gideriminde etkili ve geri kazanılabilir bir fotokatalizör olarak kullanılabileceğini ve görünür ışık altında MOF tabanlı PMS aktivasyonu hakkında yeni bilgiler sunduğunu göstermektedir.

Ethical Statement

Bu çalışma tüm etik kurallara uygun olarak yürütülmüş olup, insan veya hayvan denek kullanılmamıştır.

Thanks

Sürekli destekleri ve katkılarından dolayı danışmanım Prof. Dr. Yunus Zorlu’ya ve onun liderliğindeki Nanoyapılı Fonksiyonel Retiküler Malzemeler Araştırma Grubu – NanoFrames Lab ekibine özel teşekkürlerimi sunarım. Ayrıca, fotokataliz çalışmaları sırasında değerli rehberliği ve danışmanlığı için Prof. Dr. Cengiz Yatmaz’a teşekkür ederim.

References

  • Mingmongkol Y., Polnok A., Phuinthiang P., Channei D., Ratananikom K., Nakaruk A., Khanitchaidecha W. Photocatalytic degradation mechanism of the pharmaceutical agent salbutamol using the Mn-doped TiO2 nanoparticles under visible light irradiation. ACS Omega. 2023;8(19):17254-17263.
  • Zulfiqar N., Nadeem R., Al Musaimi O. Photocatalytic degradation of antibiotics via exploitation of a magnetic nanocomposite: a green nanotechnology approach toward drug-contaminated wastewater reclamation. ACS Omega. 2024;9(7):7986-8004.
  • Ruziwa D.T., Oluwalana A.E., Mupa M., Meili L., Selvasembian R., Nindi M.M., Sillanpaa M., Gwenzi W., Chaukura N. Pharmaceuticals in wastewater and their photocatalytic degradation using nano-enabled photocatalysts. J. Water Process Eng. 2023;54:103880.
  • Zia J., Riaz U. Microwave-assisted degradation of paracetamol drug using polythiophene-sensitized Ag–Ag₂O heterogeneous photocatalyst derived from plant extract. ACS Omega. 2020;5(27):16386-16394.
  • Brillas E., Peralta-Hernández J.M. Removal of paracetamol (acetaminophen) by photocatalysis and photoelectrocatalysis: a critical review. Sep. Purif. Technol. 2023;309:122982.
  • D’Alessio M., Ray C. Pharmaceuticals and groundwater resources. In: Fares A., ed. Emerg. Issues Groundw. Resour. Cham: Springer; 2016:101-144.
  • Madesh S., Gopi S., Sau A., Rajagopal R., Namasivayam S.K.R., Arockiaraj J. Chemical contaminants and environmental stressors induced teratogenic effect in aquatic ecosystem: a comprehensive review. Toxicol. Rep. 2024;13:101819.
  • Okuthe G.E., Dube E., Mafunda P.S. Effects of pharmaceuticals and endocrine-disrupting chemicals on reproductive biology of aquatic fauna: penguins as sentinel species. J. Xenobiot. 2025;15(4):110.
  • Mansouri F., Chouchene K., Roche N., Ksibi M. Removal of pharmaceuticals from water by adsorption and advanced oxidation processes: state of the art and trends. Appl. Sci. 2021;11(14):6659.
  • Loganathan P., Vigneswaran S., Kandasamy J., Cuprys A.K., Maletskyi Z., Ratnaweera H. Treatment trends and combined methods in removing pharmaceuticals and personal care products from wastewater: a review. Membranes. 2023;13(2):158.
  • Titchou F.E., Zazou H., Afanga H., El Gaayda J., Ait Akbour R., Nidheesh P.V., Hamdani M. Removal of organic pollutants from wastewater by advanced oxidation processes and its combination with membrane processes. Chem. Eng. Process. Process Intensif. 2021;169:108631.
  • Roslan N., Lau H.L.H., Suhaimi N.A.A., Shahri N.M.N., Verinda S.B., Nur M., Lim J.W., Usman A. Recent advances in advanced oxidation processes for degrading pharmaceuticals in wastewater: a review. Catalysts. 2024;14(3):189.
  • Zhang L., Chen J., Song L.B., Pan J.J., Luo Q. MOF-derived La/ZnO–TiO₂ composite with enhanced photocatalytic ability for degradation of tetracycline. Prog. Nat. Sci. Mater. Int. 2023;33(4):544-550.
  • Hou X., Stanley S.L., Zhao M., Zhang J., Zhou H., Cai Y., Huang F., Wei Q. MOF-based C-doped coupled TiO2/ZnO nanofibrous membrane with crossed network connection for enhanced photocatalytic activity. J. Alloys Compd. 2019;777:982-990.
  • Chi H., Wang Z., He X., Zhang J., Wang D., Ma J. Activation of peroxymonosulfate system by copper-based catalyst for degradation of naproxen: mechanisms and pathways. Chemosphere. 2019;228:54-64.
  • Chen R., Zhang H., Dong Y., Shi H. Dual metal ions/BNQDs boost PMS activation over copper tungstate photocatalyst for antibiotic removal: intermediate, toxicity assessment and mechanism. J. Mater. Sci. Technol. 2024;170:11-24.
  • Soleimani Z., Absalan Y., Gholizadeh M., Asadimanesh M., Utenishev A.N., Galeev R., Souri K. Unveiling the mechanisms of enhanced photocatalysis: a comprehensive study on metal–organic framework encapsulation strategies and the synthesis of Pt@MOF for efficient C–N coupling reactions. ACS Appl. Energy Mater. 2024;7(9):3787-3805.
  • Navalón S., Dhakshinamoorthy A., Álvaro M., Ferrer B., García H. Metal–organic frameworks as photocatalysts for solar-driven overall water splitting. Chem. Rev. 2023;123(1):445-490.
  • Abou-Elyazed A.S., Ftooh A.I., Sun Y., Ashry A.G., Shaban A.K.F., El-Nahas A.M., Yousif A.M. Solvent-free synthesis of HKUST-1 with abundant defect sites and its catalytic performance in the esterification reaction of oleic acid. ACS Omega. 2024;9(36):37662-37671.
  • Jagódka P., Matus K., Łamacz A. On the HKUST-1/GO and HKUST-1/rGO composites: the impact of synthesis method on physicochemical properties. Molecules. 2022;27(20):7082.
  • Yañez-Aulestia A., Trejos V.M., Esparza-Schulz J.M., Ibarra I.A., Sánchez-González E. Chemically modified HKUST-1(Cu) for gas adsorption and separation: mixed-metal and hierarchical porosity. ACS Appl. Mater. Interfaces. 2024;16(47):65581-65591.
  • Grande C.A., Kaiser A., Andreassen K.A. Methane storage in metal-organic framework HKUST-1 with enhanced heat management using 3D printed metal lattices. Chem. Eng. Res. Des. 2023;192:362-370.
  • Zhang J., Su C., Xie X., Liu P., Huq M.E. Enhanced visible light photocatalytic degradation of dyes in aqueous solution activated by HKUST-1: performance and mechanism. RSC Adv. 2020;10:37028-37038.
  • Zhuo Y., Meng H., Zhang Y., Chen Y., Cui J. Peroxymonosulfate activation by Fe/C composites for paracetamol degradation: Performance evaluation and mechanism insight. Catalysts. 2025;15(3):217.
  • Wu Q., Zhang Y., Meng H., Wu X., Liu Y., Li L. Cu/N co-doped biochar activating PMS for selective degrading paracetamol via a non-radical pathway dominated by singlet oxygen and electron transfer. Chemosphere. 2024;357:141858.
  • Shen Y., Martín de Vidales M.J., Espíndola J.C., Gómez-Herrero A., Dos Santos-García A.J. Paracetamol degradation by photo-assisted activation of peroxymonosulfate over ZnxNi1−xFe2O4@BiOBr heterojunctions. J. Environ. Chem. Eng. 2021;9(5):106797. Lin Y., Mo X., Zhang Y., Nie M., Yan C., Wu L. Selective degradation of acetaminophen from hydrolyzed urine by peroxymonosulfate alone: performances and mechanisms. RSC Adv. 2021;11:40022-40032.
  • Jagannathan M., Grieser F., Ashokkumar M. Sonophotocatalytic degradation of paracetamol using TiO2 and Fe3+. Sep. Purif. Technol. 2013;103:114-118.
  • Lin K.Y.A., Hsieh Y.T. Copper-based metal organic framework (MOF), HKUST-1, as an efficient adsorbent to remove p-nitrophenol from water. J. Taiwan Inst. Chem. Eng. 2015;50:223-228.

Paracetamol Degradation via Visible-Light-Assisted Peroxymonosulfate Activation on HKUST-1 MOF

Year 2026, Volume: 21 Issue: 1 , 195 - 205 , 30.03.2026
https://doi.org/10.55525/tjst.1775116
https://izlik.org/JA65GF97CU

Abstract

Paracetamol, increasingly detected in aquatic environments, is an emerging contaminant with potential risks to reproduction, hormonal balance, and ecosystem safety. Developing efficient and sustainable removal strategies is therefore essential. In this study, the copper-based metal–organic framework HKUST-1 was utilized as a photocatalyst to activate peroxymonosulfate (PMS) under visible-light irradiation for the degradation of paracetamol. The combined HKUST-1/PMS/Vis system demonstrated remarkable catalytic activity, achieving more than 90% removal of paracetamol within 150 minutes. This performance was significantly higher than that obtained using PMS or visible light individually, highlighting the strong synergistic interaction between the catalyst and PMS activation under visible light. Radical quenching experiments identified sulfate radicals (SO4•–) as the primary active species, with hydroxyl radicals (•OH) also contributing. Compared to PMS/Vis, the presence of HKUST-1 markedly accelerated the degradation rate, confirming a strong synergistic effect between photocatalysis and PMS activation. Moreover, HKUST-1 exhibited high stability and reusability, retaining performance over multiple cycles without structural degradation, as confirmed by PXRD. This study demonstrates that pristine HKUST-1 can serve as an effective and recyclable photocatalyst for pharmaceutical pollutant removal, offering new insights into MOF-based PMS activation under visible light.

Ethical Statement

This study complies with all ethical standards and does not involve human or animal subjects.

Thanks

The author would like to extend special thanks to Prof. Dr. Yunus Zorlu and the Nanostructured Functional Reticular Materials Research Lab – NanoFrames Lab research team under his leadership for their continuous support and contributions. The author also thanks Prof. Dr. Cengiz Yatmaz for his guidance and consultancy during the photocatalysis studies.

References

  • Mingmongkol Y., Polnok A., Phuinthiang P., Channei D., Ratananikom K., Nakaruk A., Khanitchaidecha W. Photocatalytic degradation mechanism of the pharmaceutical agent salbutamol using the Mn-doped TiO2 nanoparticles under visible light irradiation. ACS Omega. 2023;8(19):17254-17263.
  • Zulfiqar N., Nadeem R., Al Musaimi O. Photocatalytic degradation of antibiotics via exploitation of a magnetic nanocomposite: a green nanotechnology approach toward drug-contaminated wastewater reclamation. ACS Omega. 2024;9(7):7986-8004.
  • Ruziwa D.T., Oluwalana A.E., Mupa M., Meili L., Selvasembian R., Nindi M.M., Sillanpaa M., Gwenzi W., Chaukura N. Pharmaceuticals in wastewater and their photocatalytic degradation using nano-enabled photocatalysts. J. Water Process Eng. 2023;54:103880.
  • Zia J., Riaz U. Microwave-assisted degradation of paracetamol drug using polythiophene-sensitized Ag–Ag₂O heterogeneous photocatalyst derived from plant extract. ACS Omega. 2020;5(27):16386-16394.
  • Brillas E., Peralta-Hernández J.M. Removal of paracetamol (acetaminophen) by photocatalysis and photoelectrocatalysis: a critical review. Sep. Purif. Technol. 2023;309:122982.
  • D’Alessio M., Ray C. Pharmaceuticals and groundwater resources. In: Fares A., ed. Emerg. Issues Groundw. Resour. Cham: Springer; 2016:101-144.
  • Madesh S., Gopi S., Sau A., Rajagopal R., Namasivayam S.K.R., Arockiaraj J. Chemical contaminants and environmental stressors induced teratogenic effect in aquatic ecosystem: a comprehensive review. Toxicol. Rep. 2024;13:101819.
  • Okuthe G.E., Dube E., Mafunda P.S. Effects of pharmaceuticals and endocrine-disrupting chemicals on reproductive biology of aquatic fauna: penguins as sentinel species. J. Xenobiot. 2025;15(4):110.
  • Mansouri F., Chouchene K., Roche N., Ksibi M. Removal of pharmaceuticals from water by adsorption and advanced oxidation processes: state of the art and trends. Appl. Sci. 2021;11(14):6659.
  • Loganathan P., Vigneswaran S., Kandasamy J., Cuprys A.K., Maletskyi Z., Ratnaweera H. Treatment trends and combined methods in removing pharmaceuticals and personal care products from wastewater: a review. Membranes. 2023;13(2):158.
  • Titchou F.E., Zazou H., Afanga H., El Gaayda J., Ait Akbour R., Nidheesh P.V., Hamdani M. Removal of organic pollutants from wastewater by advanced oxidation processes and its combination with membrane processes. Chem. Eng. Process. Process Intensif. 2021;169:108631.
  • Roslan N., Lau H.L.H., Suhaimi N.A.A., Shahri N.M.N., Verinda S.B., Nur M., Lim J.W., Usman A. Recent advances in advanced oxidation processes for degrading pharmaceuticals in wastewater: a review. Catalysts. 2024;14(3):189.
  • Zhang L., Chen J., Song L.B., Pan J.J., Luo Q. MOF-derived La/ZnO–TiO₂ composite with enhanced photocatalytic ability for degradation of tetracycline. Prog. Nat. Sci. Mater. Int. 2023;33(4):544-550.
  • Hou X., Stanley S.L., Zhao M., Zhang J., Zhou H., Cai Y., Huang F., Wei Q. MOF-based C-doped coupled TiO2/ZnO nanofibrous membrane with crossed network connection for enhanced photocatalytic activity. J. Alloys Compd. 2019;777:982-990.
  • Chi H., Wang Z., He X., Zhang J., Wang D., Ma J. Activation of peroxymonosulfate system by copper-based catalyst for degradation of naproxen: mechanisms and pathways. Chemosphere. 2019;228:54-64.
  • Chen R., Zhang H., Dong Y., Shi H. Dual metal ions/BNQDs boost PMS activation over copper tungstate photocatalyst for antibiotic removal: intermediate, toxicity assessment and mechanism. J. Mater. Sci. Technol. 2024;170:11-24.
  • Soleimani Z., Absalan Y., Gholizadeh M., Asadimanesh M., Utenishev A.N., Galeev R., Souri K. Unveiling the mechanisms of enhanced photocatalysis: a comprehensive study on metal–organic framework encapsulation strategies and the synthesis of Pt@MOF for efficient C–N coupling reactions. ACS Appl. Energy Mater. 2024;7(9):3787-3805.
  • Navalón S., Dhakshinamoorthy A., Álvaro M., Ferrer B., García H. Metal–organic frameworks as photocatalysts for solar-driven overall water splitting. Chem. Rev. 2023;123(1):445-490.
  • Abou-Elyazed A.S., Ftooh A.I., Sun Y., Ashry A.G., Shaban A.K.F., El-Nahas A.M., Yousif A.M. Solvent-free synthesis of HKUST-1 with abundant defect sites and its catalytic performance in the esterification reaction of oleic acid. ACS Omega. 2024;9(36):37662-37671.
  • Jagódka P., Matus K., Łamacz A. On the HKUST-1/GO and HKUST-1/rGO composites: the impact of synthesis method on physicochemical properties. Molecules. 2022;27(20):7082.
  • Yañez-Aulestia A., Trejos V.M., Esparza-Schulz J.M., Ibarra I.A., Sánchez-González E. Chemically modified HKUST-1(Cu) for gas adsorption and separation: mixed-metal and hierarchical porosity. ACS Appl. Mater. Interfaces. 2024;16(47):65581-65591.
  • Grande C.A., Kaiser A., Andreassen K.A. Methane storage in metal-organic framework HKUST-1 with enhanced heat management using 3D printed metal lattices. Chem. Eng. Res. Des. 2023;192:362-370.
  • Zhang J., Su C., Xie X., Liu P., Huq M.E. Enhanced visible light photocatalytic degradation of dyes in aqueous solution activated by HKUST-1: performance and mechanism. RSC Adv. 2020;10:37028-37038.
  • Zhuo Y., Meng H., Zhang Y., Chen Y., Cui J. Peroxymonosulfate activation by Fe/C composites for paracetamol degradation: Performance evaluation and mechanism insight. Catalysts. 2025;15(3):217.
  • Wu Q., Zhang Y., Meng H., Wu X., Liu Y., Li L. Cu/N co-doped biochar activating PMS for selective degrading paracetamol via a non-radical pathway dominated by singlet oxygen and electron transfer. Chemosphere. 2024;357:141858.
  • Shen Y., Martín de Vidales M.J., Espíndola J.C., Gómez-Herrero A., Dos Santos-García A.J. Paracetamol degradation by photo-assisted activation of peroxymonosulfate over ZnxNi1−xFe2O4@BiOBr heterojunctions. J. Environ. Chem. Eng. 2021;9(5):106797. Lin Y., Mo X., Zhang Y., Nie M., Yan C., Wu L. Selective degradation of acetaminophen from hydrolyzed urine by peroxymonosulfate alone: performances and mechanisms. RSC Adv. 2021;11:40022-40032.
  • Jagannathan M., Grieser F., Ashokkumar M. Sonophotocatalytic degradation of paracetamol using TiO2 and Fe3+. Sep. Purif. Technol. 2013;103:114-118.
  • Lin K.Y.A., Hsieh Y.T. Copper-based metal organic framework (MOF), HKUST-1, as an efficient adsorbent to remove p-nitrophenol from water. J. Taiwan Inst. Chem. Eng. 2015;50:223-228.
There are 28 citations in total.

Details

Primary Language English
Subjects Metal Organic Frameworks, Catalytic Activity, Materials Science and Technologies, Water Treatment Processes
Journal Section Research Article
Authors

Elif Özcan 0000-0002-4375-2320

Submission Date August 31, 2025
Acceptance Date October 24, 2025
Publication Date March 30, 2026
DOI https://doi.org/10.55525/tjst.1775116
IZ https://izlik.org/JA65GF97CU
Published in Issue Year 2026 Volume: 21 Issue: 1

Cite

APA Özcan, E. (2026). Paracetamol Degradation via Visible-Light-Assisted Peroxymonosulfate Activation on HKUST-1 MOF. Turkish Journal of Science and Technology, 21(1), 195-205. https://doi.org/10.55525/tjst.1775116
AMA 1.Özcan E. Paracetamol Degradation via Visible-Light-Assisted Peroxymonosulfate Activation on HKUST-1 MOF. TJST. 2026;21(1):195-205. doi:10.55525/tjst.1775116
Chicago Özcan, Elif. 2026. “Paracetamol Degradation via Visible-Light-Assisted Peroxymonosulfate Activation on HKUST-1 MOF”. Turkish Journal of Science and Technology 21 (1): 195-205. https://doi.org/10.55525/tjst.1775116.
EndNote Özcan E (March 1, 2026) Paracetamol Degradation via Visible-Light-Assisted Peroxymonosulfate Activation on HKUST-1 MOF. Turkish Journal of Science and Technology 21 1 195–205.
IEEE [1]E. Özcan, “Paracetamol Degradation via Visible-Light-Assisted Peroxymonosulfate Activation on HKUST-1 MOF”, TJST, vol. 21, no. 1, pp. 195–205, Mar. 2026, doi: 10.55525/tjst.1775116.
ISNAD Özcan, Elif. “Paracetamol Degradation via Visible-Light-Assisted Peroxymonosulfate Activation on HKUST-1 MOF”. Turkish Journal of Science and Technology 21/1 (March 1, 2026): 195-205. https://doi.org/10.55525/tjst.1775116.
JAMA 1.Özcan E. Paracetamol Degradation via Visible-Light-Assisted Peroxymonosulfate Activation on HKUST-1 MOF. TJST. 2026;21:195–205.
MLA Özcan, Elif. “Paracetamol Degradation via Visible-Light-Assisted Peroxymonosulfate Activation on HKUST-1 MOF”. Turkish Journal of Science and Technology, vol. 21, no. 1, Mar. 2026, pp. 195-0, doi:10.55525/tjst.1775116.
Vancouver 1.Elif Özcan. Paracetamol Degradation via Visible-Light-Assisted Peroxymonosulfate Activation on HKUST-1 MOF. TJST. 2026 Mar. 1;21(1):195-20. doi:10.55525/tjst.1775116