Advanced technology for photocatalytic degradation of thiophanate-methyl: Degradation pathways, DFT calculations and embryotoxic potential
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2023
Authors
Jovanović, AleksandarStevanović, Marija
Barudžija, Tanja
Cvijetić, Ilija
Lazarević, Slavica
Tomašević, Anđelka
Marinković, Aleksandar
Article (Published version)
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This study focuses on establishing an efficient two-step technology, which includes: (1) consecutive adsorption-desorption, using cellulose-based membranes, bCells, and (2) photocatalytic degradation of the fungicide thiophanate-methyl (TPM), using synthesized Ag-P25 and Ce-P25 catalysts. The catalysts, obtained by controlled deposition of Ag2O/Ag and CeO2 onto P25 TiO2 carrier (Degussa), were characterized using ATR-FTIR, XRPD, BET, FESEM, HRTEM, HAADF-EDS and UV–DRS techniques. In order to establish a feasible purification technology, preconcentration of TPM was performed by adsorption, achieving 75.5 and 92.9 mg/g of TPM removal using bCell-EpL and bCell–EpL–TA membranes, respectively, followed by efficient desorption (> 95%) that provided acceptable TPM concentration for photodegradation experiments. Under optimal conditions (0.07 g/L of both catalysts), complete degradation of TPM (5 mg/L) occurred within 2 h, compared to 4 h for the base TiO2 P25. Measurements of quantum yield an...d the results of HPLC-MS analysis, alongside DFT calculation, assisted in understanding the TPM degradation pathways. New degradation products were detected and proposed from HPLC–MS analysis. Embryotoxic assays, performed on zebrafish (Danio rerio), applied to estimate the toxicity evolution of time-dependent generated TPM degradation products, showed low embryotoxic potential. Chemical oxygen demand (26 mg O2/L) confirmed low ecotoxicological pressure of effluent water.
Keywords:
Ag-P25 and Ce-P25 photocatalyst / bCells / Danio rerio embryos / Quantum chemical calculations / Thiophanate-methylSource:
Process Safety and Environmental Protection, 2023, 178, 423-443Publisher:
- Institution of Chemical Engineers
Funding / projects:
- Ministry of Science, Technological Development and Innovation of the Republic of Serbia, institutional funding - 200023 (Institute of Technology of Nuclear and Other Mineral Row Materials - ITNMS, Belgrade) (RS-MESTD-inst-2020-200023)
- Ministry of Science, Technological Development and Innovation of the Republic of Serbia, institutional funding - 200214 (Institue of Pesticides and Environmental Protection, Belgrade) (RS-MESTD-inst-2020-200214)
- Ministry of Science, Technological Development and Innovation of the Republic of Serbia, institutional funding - 200017 (University of Belgrade, Institute of Nuclear Sciences 'Vinča', Belgrade-Vinča) (RS-MESTD-inst-2020-200017)
- Ministry of Science, Technological Development and Innovation of the Republic of Serbia, institutional funding - 200168 (University of Belgrade, Faculty of Chemistry) (RS-MESTD-inst-2020-200168)
- Ministry of Science, Technological Development and Innovation of the Republic of Serbia, institutional funding - 200135 (University of Belgrade, Faculty of Technology and Metallurgy) (RS-MESTD-inst-2020-200135)
Institution/Community
Tehnološko-metalurški fakultetTY - JOUR AU - Jovanović, Aleksandar AU - Stevanović, Marija AU - Barudžija, Tanja AU - Cvijetić, Ilija AU - Lazarević, Slavica AU - Tomašević, Anđelka AU - Marinković, Aleksandar PY - 2023 UR - http://TechnoRep.tmf.bg.ac.rs/handle/123456789/6611 AB - This study focuses on establishing an efficient two-step technology, which includes: (1) consecutive adsorption-desorption, using cellulose-based membranes, bCells, and (2) photocatalytic degradation of the fungicide thiophanate-methyl (TPM), using synthesized Ag-P25 and Ce-P25 catalysts. The catalysts, obtained by controlled deposition of Ag2O/Ag and CeO2 onto P25 TiO2 carrier (Degussa), were characterized using ATR-FTIR, XRPD, BET, FESEM, HRTEM, HAADF-EDS and UV–DRS techniques. In order to establish a feasible purification technology, preconcentration of TPM was performed by adsorption, achieving 75.5 and 92.9 mg/g of TPM removal using bCell-EpL and bCell–EpL–TA membranes, respectively, followed by efficient desorption (> 95%) that provided acceptable TPM concentration for photodegradation experiments. Under optimal conditions (0.07 g/L of both catalysts), complete degradation of TPM (5 mg/L) occurred within 2 h, compared to 4 h for the base TiO2 P25. Measurements of quantum yield and the results of HPLC-MS analysis, alongside DFT calculation, assisted in understanding the TPM degradation pathways. New degradation products were detected and proposed from HPLC–MS analysis. Embryotoxic assays, performed on zebrafish (Danio rerio), applied to estimate the toxicity evolution of time-dependent generated TPM degradation products, showed low embryotoxic potential. Chemical oxygen demand (26 mg O2/L) confirmed low ecotoxicological pressure of effluent water. PB - Institution of Chemical Engineers T2 - Process Safety and Environmental Protection T1 - Advanced technology for photocatalytic degradation of thiophanate-methyl: Degradation pathways, DFT calculations and embryotoxic potential EP - 443 SP - 423 VL - 178 DO - 10.1016/j.psep.2023.08.054 ER -
@article{ author = "Jovanović, Aleksandar and Stevanović, Marija and Barudžija, Tanja and Cvijetić, Ilija and Lazarević, Slavica and Tomašević, Anđelka and Marinković, Aleksandar", year = "2023", abstract = "This study focuses on establishing an efficient two-step technology, which includes: (1) consecutive adsorption-desorption, using cellulose-based membranes, bCells, and (2) photocatalytic degradation of the fungicide thiophanate-methyl (TPM), using synthesized Ag-P25 and Ce-P25 catalysts. The catalysts, obtained by controlled deposition of Ag2O/Ag and CeO2 onto P25 TiO2 carrier (Degussa), were characterized using ATR-FTIR, XRPD, BET, FESEM, HRTEM, HAADF-EDS and UV–DRS techniques. In order to establish a feasible purification technology, preconcentration of TPM was performed by adsorption, achieving 75.5 and 92.9 mg/g of TPM removal using bCell-EpL and bCell–EpL–TA membranes, respectively, followed by efficient desorption (> 95%) that provided acceptable TPM concentration for photodegradation experiments. Under optimal conditions (0.07 g/L of both catalysts), complete degradation of TPM (5 mg/L) occurred within 2 h, compared to 4 h for the base TiO2 P25. Measurements of quantum yield and the results of HPLC-MS analysis, alongside DFT calculation, assisted in understanding the TPM degradation pathways. New degradation products were detected and proposed from HPLC–MS analysis. Embryotoxic assays, performed on zebrafish (Danio rerio), applied to estimate the toxicity evolution of time-dependent generated TPM degradation products, showed low embryotoxic potential. Chemical oxygen demand (26 mg O2/L) confirmed low ecotoxicological pressure of effluent water.", publisher = "Institution of Chemical Engineers", journal = "Process Safety and Environmental Protection", title = "Advanced technology for photocatalytic degradation of thiophanate-methyl: Degradation pathways, DFT calculations and embryotoxic potential", pages = "443-423", volume = "178", doi = "10.1016/j.psep.2023.08.054" }
Jovanović, A., Stevanović, M., Barudžija, T., Cvijetić, I., Lazarević, S., Tomašević, A.,& Marinković, A.. (2023). Advanced technology for photocatalytic degradation of thiophanate-methyl: Degradation pathways, DFT calculations and embryotoxic potential. in Process Safety and Environmental Protection Institution of Chemical Engineers., 178, 423-443. https://doi.org/10.1016/j.psep.2023.08.054
Jovanović A, Stevanović M, Barudžija T, Cvijetić I, Lazarević S, Tomašević A, Marinković A. Advanced technology for photocatalytic degradation of thiophanate-methyl: Degradation pathways, DFT calculations and embryotoxic potential. in Process Safety and Environmental Protection. 2023;178:423-443. doi:10.1016/j.psep.2023.08.054 .
Jovanović, Aleksandar, Stevanović, Marija, Barudžija, Tanja, Cvijetić, Ilija, Lazarević, Slavica, Tomašević, Anđelka, Marinković, Aleksandar, "Advanced technology for photocatalytic degradation of thiophanate-methyl: Degradation pathways, DFT calculations and embryotoxic potential" in Process Safety and Environmental Protection, 178 (2023):423-443, https://doi.org/10.1016/j.psep.2023.08.054 . .