The tapping of municipal wastewater for potable reuse significantly enhances drinking water supply in drought-stricken regions worldwide. Membrane-based potable reuse treatment trains commonly employ ultraviolet-based advanced oxidation processes (UV-AOPs) to degrade trace organic contaminants in water to produce high-quality recycled water. Hydrogen peroxide (H 2 O 2 ) is used as the default photo-oxidant. Meanwhile, chloramines, which are added to prevent biofouling, pass through the membranes and impact the treatment efficiency of UV-AOP. Water reuse facilities therefore face the dilemma of optimizing H 2 O 2 (an added photo-oxidant) and chloramines (a carry-over photooxidant) doses. Utilizing a uniquely designed pilot-scale reactor and real-time recycled water, we evaluated treatment efficiencies of UV-AOP on six important indicator contaminants, with monochloramine (NH 2 Cl) and H 2 O 2 as photo-oxidants. Hydroxyl radical (HO • ) and reactive chlorine species, such as the chlorine atom (Cl • ) and chlorine dimer (Cl 2•− ), were the major reactive species. Overall, radicals generated from photolysis of NH 2 Cl alone achieved removal of indicator compounds, which can be further improved by optimizing UV fluence, i.e., the UV dose. Furthermore, the addition of H 2 O 2 enhanced HO • formation and improved contaminant removal. However, the addition of H 2 O 2 , when the background NH 2 Cl level was above 2 mg L −1 (as Cl 2 ), provided limited improvement in treatment efficiency. These trade-offs between chloramine and H 2 O 2 as oxidants, and the recommended optimization of the associated effective UV fluence, are critical for energy-efficient and costeffective potable reuse to address the challenges of global water scarcity.
Three fluoroquinolone-to-fluoroquinolone antibiotic transformations were monitored during UV-C irradiation processes. In particular, the following reactions were observed: enrofloxacin-to-ciprofloxacin, difloxacin-to-sarafloxacin, and pefloxacin-to-norfloxacin. The apparent molar absorptivity and fluence-based pseudo-first-order rate constants for transformation of the six fluoroquinolones by direct photolysis at 253.7 nm were determined for the pH 2-12 range. These parameters were deconvoluted to calculate specific molar absorptivity and fluence-based rate constants for cationic, zwitterionic, and anionic fluoroquinolone species. For a typical disinfection fluence of 40 mJ/cm(2), the apparent transformation efficiencies were inflated by 2-8% when fluoroquinolone products were not considered; moreover, the overall transformation efficiencies at 400 mJ/cm(2) varied by up to 40% depending on pH. The three product antibiotics, namely ciprofloxacin, sarafloxacin, and norfloxacin, were found to be equally or more potent than the parent fluoroquinolones using an Escherichia coli-based assay. UV treatment of a solution containing difloxacin was found to increase antimicrobial activity due to formation of sarafloxacin. These results highlight the importance of considering antibiotic-to-antibiotic transformations in UV-based processes.
This study examined the photolytic fate of the chlortetracycline (CTC), ciprofloxacin (CIP), roxarsone (ROX), and sulfamethoxazole (SMX) antibiotics in agriculturally relevant matrices. The observed photodegradation kinetics for antibiotics in solutions containing dissolved organic matter (DOM) from three poultry litter extracts was modeled to identify contributions from direct and indirect photolysis. Suwannee River natural organic matter (SRN) was used as a surrogate DOM standard. Poultry litter-derived DOM generated lower concentrations of reactive species compared to SRN. Direct photolysis was the dominant transformation mechanism for CIP, whereas CTC, ROX, and SMX were sensitized by DOM* andO. The impacts of agricultural DOM on photodegradation of antibiotics were identified in terms of pseudo-first-order rate constants for formation of reactive species and second-order rate constants for reaction of reactive species with DOM. Solutions containing poultry litter-derived DOM generated similar levels of DOM* andO, enhancing degradation of CTC, ROX, and SMX. The reactivity of SMX was markedly different in solutions containing poultry litter DOM compared to solutions with SRN, indicating that the photolytic fate of select antibiotics varies for agricultural and surface water matrices. As the majority of antibiotics are consumed by animals, these findings provide new insight into agriculturally relevant transformation mechanisms and kinetics.
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