SA'ADAH, Fatkhiyatus and Sutanto, Heri and Hadiyanto, Hadiyanto (2025) PHARMACEUTICAL WASTEWATER TREATMENT USING BISMUTH OXIDE-BASED PHOTOCATALYTIC METHOD. Doctoral thesis, UNIVERSITAS DIPONEGORO.

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Abstract

The growing presence of antibiotic residues in pharmaceutical wastewater poses a critical environmental and public health concern, as conventional treatment systems often fail to fully remove these micropollutants. The research focuses on both the current state of pharmaceutical wastewater effluents and the development of advanced photocatalytic materials for antibiotic degradation. Field studies at pharmaceutical wastewater treatment plants (WWTPs) in Indonesia showed that although COD, BOD, and TSS removal efficiencies reached 82.15%, 82.71%, and 66.27% respectively at Company XX, the final effluent still exceeded national discharge limits, COD and BOD were 22.74 and 2.38 times above the threshold. High levels of oxytetracycline (3.887 mg/L), ciprofloxacin (2.849 mg/L), amoxicillin (2.1207 mg/L), and cefadroxil (2.3871 mg/L) were detected in Company XX's effluent, underscoring the inadequacy of current treatment practices. To address this issue, a bibliometric analysis of 1,033 Scopus-indexed articles from 2013–2023 confirmed a rising global research focus on Bi2O3 thin films for antibiotic degradation. Experimentally, Bi2O3 thin films were synthesized using sol-gel and precipitation-assisted microwave methods and modified with Cu, Zn, Co, and Fe to enhance photocatalytic activity. Cu-Bi2O3 (4%) achieved notable removal efficiencies of 52.06% for amoxicillin, 61.72% for ciprofloxacin, and 69.44% for tetracycline, with a band gap of 2.32 eV and crystal size of 37.04 nm.Cu-Bi2O3 thin films showed up to 85.95% levofloxacin degradation, with a pseudo-second-order rate constant of 0.00676 min-1. Further, Fe-Bi2O3 thin films showed moderate doxycycline degradation rates (62.46%), while Co-Bi2O3 lowered degradation efficiency (62.46%). Zn-Bi2O3 films demonstrated superior performance in degrading doxycycline, achieving 87.28% degradation, 65.45% mineralization, a rate constant of 0.0951 min-1, and a TOF of 4.35 h-1. Additionally, toxicity assessments using T.E.S.T. and bacterial inhibition assays (S. aureus and E. coli) confirmed reduced environmental risks post-degradation. Finally, Zn–α-Bi2O3 thin films were optimized for amoxicillin degradation using Response Surface Methodology (RSM), with the best-performing catalyst (Zn-αBO-357-3.19-25) achieving 70.06% AMX degradation and 49.28% TOC removal under visible light. The films also demonstrated 64.23% COD, 51.52% BOD, and 57.58% TSS removal when applied to real pharmaceutical wastewater. The research highlights the environmental risks of pharmaceutical effluents and presents Bi2O3 based photocatalysts, particularly metal-doped thin films, as an effective and sustainable strategy for antibiotic remediation in wastewater systems.
Keywords: Pharmaceutical waste, bismuth oxide, photocatalyst, antibiotic pollution

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