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Ball milled biochar effectively removes sulfamethoxazole and sulfapyridine antibiotics from water and wastewater
2020
Wong, Kam Sing | Zimmerman, Andrew R. | Chen, Hao | Gao, Bin
Release of antibiotics into the environment, which often occurs downstream of wastewater treatment plants, poses a human health threat due to the potential development of bacterial antibiotic resistance. In this study, laboratory experiments were conducted to evaluate the performance of ball milled biochar on the removal of two sulfonamide antibiotics, sulfamethoxazole (SMX) and sulfapyridine (SPY) from water and wastewater. Aqueous batch sorption experiment using both pristine and ball milled biochar derived from bagasse (BG), bamboo (BB) and hickory chips (HC), made at three pyrolysis temperatures (300, 450, 600 °C), showed that ball milling greatly enhanced the SMX and SPY adsorption. The 450 °C ball milled HC biochar and BB biochar exhibited the best removal efficiency for SMX (83.3%) and SPY (89.6%), respectively. A range of functional groups were produced by ball milling, leading to the conclusion that the adsorption of sulfonamides on the biochars was controlled by multiple mechanisms including hydrophobic interaction, π–π interaction, hydrogen bonding, and electrostatic interaction. Due to the importance of electrostatic interaction, SMX and SPY adsorption was pH dependent. In laboratory water solutions, the Langmuir maximum adsorption capacities of SMX and SPY reached 100.3 mg/g and 57.9 mg/g, respectively. When tested in real wastewater solution, the 450 °C ball milled biochar still performed well, especially in the removal of SPY. The maximum adsorption capacities of SMX and SPY in wastewater were 25.7 mg/g and 58.6 mg/g, respectively. Thus, ball milled biochar has great potential for SMX and SPY removal from aqueous solutions including wastewater.
Mostrar más [+] Menos [-]Fate and risk assessment of sulfonamides and metabolites in urban groundwater
2020
Jurado, Anna | Margareto, Alejandro | Pujades, Estanislao | Vázquez-Suñé, Enric | Díaz-Cruz, M. Silvia
Antibiotics, such as sulfonamides (SAs), have recently raised concern as wastewater treatment plants (WWTPs) partly remove them, and thus, SAs continuously enter the aquifers. In this context, the aims of this work are to (1) investigate the temporal evolution of SAs and metabolites in an urban aquifer recharged by a polluted river; (2) identify the potential geochemical processes that might affect SAs in the river-groundwater interface and (3) evaluate the ecological and human health risk assessment of SAs. To this end, 14 SAs and 4 metabolites were analyzed in river and urban groundwater from the metropolitan area of Barcelona (NE, Spain) in three different sampling campaigns. These substances had a distinct behavior when river water, which is the main recharge source, infiltrates the aquifer. Mixing of the river water recharge into the aquifer drives several redox reactions such as aerobic respiration and denitrification. This reducing character of the aquifer seemed to favor the natural attenuation of some SAs as sulfamethoxazole, sulfapyridine, and sulfamethizole. However, most of the SAs detected were not likely to undergo degradation and adsorption because their concentrations were constant along groundwater flow path. In fact, the intensity of SAs adsorption is low as the retardation factors are close to 1 at average groundwater pH of 7.2 for most SAs.Finally, risk quotients (RQs) are used to evaluate the ecological and human health risks posed by single and mixture of SAs in river water and groundwater, respectively. Life-stage RQs of the SAs detected in groundwater for the 8 age intervals were low, indicating that SAs and their mixture do not pose any risk to human beings. Concerning the environmental risk assessment, SAs do not pose any risk for algae, fish and crustaceans as the RQs evaluated are further lower than 0.1.
Mostrar más [+] Menos [-]Adsorption of sulfonamides to demineralized pine wood biochars prepared under different thermochemical conditions
2014
Xie, Mengxing | Chen, Wei | Xu, Zhaoyi | Zheng, Shourong | Zhu, Dongqiang
The main objective of this study was to understand the key factors and mechanisms controlling adsorption of sulfonamides to biochars. Batch adsorption experiments were performed for sulfamethoxazole and sulfapyridine to three pine-wood biochars prepared under different thermochemical conditions: pyrolysis at 400 °C (C400) and 500 °C (C500), and pyrolysis at 500 °C followed with hydrogenation (C500-H). For both sulfonamides, the adsorbent surface area-normalized adsorption was stronger to C500 than to C400. This is attributable to the enhanced π–π electron-donor–acceptor interaction with the carbon surface of C500 due to the higher degree of graphitization. Despite the relatively large difference in surface O-functionality content between C500 (12.2%) and C500-H (6.6%), the two biochars exhibited nearly identical adsorbent surface area-normalized adsorption, indicating negligible role of surface O-functionalities in the adsorption to these adsorbents. Effects of solution chemistry conditions (pH, Cu2+, and dissolved soil humic acid) on adsorption were examined.
Mostrar más [+] Menos [-]Antibiotics in the surface water of the Yangtze Estuary: Occurrence, distribution and risk assessment
2013
Yan, Caixia | Yang, Yi | Zhou, Junliang | Liu, Min | Nie, Minghua | Shi, Hao | Gu, Lijun
The occurrence and distribution of five groups of antibiotics were investigated in the surface water of Yangtze Estuary over four seasons. Of the 20 antibiotics, only sulfamerazine was not detected at all sampling sites, indicating widespread occurrence of antibiotic residues in the study area. Detection frequencies and concentrations of antibiotics were generally higher in January, indicating that low flow conditions and low temperature might enhance the persistence of antibiotics in water. Antibiotic levels varied with location, with the highest concentrations being observed around river discharge and sewage outfall. Furthermore, a positive correlation between total antibiotic and DOC concentrations revealed the significant role played by DOC. Risk assessment based on single compound exposure showed that sulfapyridine and sulfamethoxazole could cause medium risk to daphnid in the Yangtze Estuary.
Mostrar más [+] Menos [-]Investigation of antibiotics in mollusks from coastal waters in the Bohai Sea of China
2012
Li, Wenhui | Shi, Yali | Gao, Lihong | Liu, Jiemin | Cai, Yaqi
This study focused on the presence and distribution of 22 antibiotics, including eight quinolones, nine sulfonamides and five macrolides in mollusks from the Bohai Sea of China. 190 samples of eleven species were collected in 2006, 2007 and 2009. Laboratory analyses revealed that antibiotics were widely distributed in the mollusks with quinolones as the major compounds with concentrations of 0.71∼1575.10 μg/kg, which were up to two orders of magnitude higher than those of sulfonamides (0∼76.75 μg/kg) and macrolides (0∼36.21 μg/kg). The contents of quinolones and macrolides did not show significant changes from 2006, 2007 to 2009, while sulfonamides decreased significantly from 2006 to 2009. Compared with other sites, the city of Dalian was more polluted with quinolones, while Beidaihe was more contaminated with erythromycin and sulfapyridine. In addition, Mactra veneriformis and Meretrix merehjgntrix Linnaeus contained higher concentrations of quinolones and sulfamonomethoxine, while Mytilus edulis had higher levels of erythromycin and sulfapyridine.
Mostrar más [+] Menos [-]Adsorption of sulfamethoxazole and sulfapyridine antibiotics in high organic content soils
2017
Chen, Kuen-Lin | Liu, Li-Chun | Chen, Wan-Ru
Many antibiotics, including sulfonamides, are being frequently detected in soil and groundwater. Livestock waste is an important source of antibiotic pollution, and sulfonamides may be present along with organic-rich substances. This study aims to investigate the sorption reaction of two sulfonamides, sulfamethoxazole (SMZ) and sulfapyridine (SPY) in two organic-rich sorbents: a commercial peat soil (38.41% carbon content) and a composted manure (24.33% carbon content). Batch reactions were conducted to evaluate the impacts of pH (4.5–9.5) and background ions (0.001 M–0.1 M CaCl2) on their sorption. Both linear partitioning and Freundlich sorption isotherms fit the reaction well. The n values of Freundlich isotherm were close to 1 in most conditions suggesting that the hydrophobic partition is the major adsorption mechanism. In terms of SMZ, Kd declined with increases in the pH. SPY has a pyridine group that is responsible for adsorption at high pH values, and thus, no significant trend between Kd and pH was observed. At high pH ranges, SPY sorption deviated significantly from linear partitioning. The results suggested the sorption mechanism of these two sulfonamide antibiotics tended to be hydrophobic partitioning under most of the experimental conditions, especially at pH values lower than their corresponding pKa2. The fluorescence excitation emission matrix and dissolved organic carbon leaching test suggested composted manure has higher fulvic acid organics and that peat soil has higher humus-like organics. Small organic molecules showed stronger affinity toward sulfonamide antibiotics and cause the composted manure to exhibit higher sorption capacity. Overall, this study suggests that the chemical structure and properties of sulfonamides antibiotics and the type of organic matter in soils will greatly influence the fate and transport of these contaminants into the environment.
Mostrar más [+] Menos [-]Enhanced removal of sulfonamide antibiotics by KOH-activated anthracite coal: Batch and fixed-bed studies
2016
Zuo, Linzi | Ai, Jing | Fu, Heyun | Chen, Wei | Zheng, Shourong | Xu, Zhaoyi | Zhu, Dongqiang
The presence of sulfonamide antibiotics in aquatic environments poses potential risks to human health and ecosystems. In the present study, a highly porous activated carbon was prepared by KOH activation of an anthracite coal (Anth-KOH), and its adsorption properties toward two sulfonamides (sulfamethoxazole and sulfapyridine) and three smaller-sized monoaromatics (phenol, 4-nitrophenol and 1,3-dinitrobenzene) were examined in both batch and fixed-bed adsorption experiments to probe the interplay between adsorbate molecular size and adsorbent pore structure. A commercial powder microporous activated carbon (PAC) and a commercial mesoporous carbon (CMK-3) possessing distinct pore properties were included as comparative adsorbents. Among the three adsorbents Anth-KOH exhibited the largest adsorption capacities for all test adsorbates (especially the two sulfonamides) in both batch mode and fixed-bed mode. After being normalized by the adsorbent surface area, the batch adsorption isotherms of sulfonamides on PAC and Anth-KOH were displaced upward relative to the isotherms on CMK-3, likely due to the micropore-filling effect facilitated by the microporosity of adsorbents. In the fixed-bed mode, the surface area-normalized adsorption capacities of Anth-KOH for sulfonamides were close to that of CMK-3, and higher than that of PAC. The irregular, closed micropores of PAC might impede the diffusion of the relatively large-sized sulfonamide molecules and in turn led to lowered fixed-bed adsorption capacities. The overall superior adsorption of sulfonamides on Anth-KOH can be attributed to its large specific surface area (2514 m²/g), high pore volume (1.23 cm³/g) and large micropore sizes (centered at 2.0 nm). These findings imply that KOH-activated anthracite coal is a promising adsorbent for the removal of sulfonamide antibiotics from aqueous solution.
Mostrar más [+] Menos [-]Peroxymonosulfate activation using heterogeneous catalyst Sr2FeO4 coated on SBA-15 for efficient degradation of antibiotic sulfapyridine
2022
Zhao, Zheng-Yin | Xiong, Jun | Wang, Yuan | Cui, Caixi
It is significant to explore the advanced oxidation process (AOP) for antibiotic degradation. Herein, a peroxymonosulfate (PMS) activator, Sr₂FeO₄/SBA-15 (SFS) heterogeneous catalyst, was synthesized by in situ growth of Sr₂FeO₄ on the surface of SBA-15. In SFS/PMS catalytic system, Sr atom provided electrons to Fe(II) ↔Fe(III) ↔Fe(II) redox cycle through Sr-O-Fe bonds for PMS activation. The SFS catalyst could activate PMS to generate a free radical coexistence system, including sulfate radical (SO₄∙⁻) and hydroxyl radicals (∙OH). The catalyst possessed high catalytic activity and high stability. The degradation efficiency of sulfapyridine (SAD) over the SFS/PMS catalytic system could reach 99.0% after 90 min reaction. After the 5th reuse, the degradation efficiency of SAD was still more than 94.0%, and the phase structure of the catalyst did not alter. The low ion leaching concentration would be more conducive to reuse and avoiding secondary pollution, in comparison to homogeneous catalysts. This catalyst can be widely applied to organic wastewater treatment.-->
Mostrar más [+] Menos [-]Presence of Pharmaceuticals and Hormones in Waters from Sewage Treatment Plants
2011
Pedrouzo, Marta | Borrull, Francesc | Pocurull, Eva | Marcé, Rosa Maria
This paper describes the presence of 33 pharmaceuticals and hormones in waters from two sewage treatment plants (STPs) situated in Catalonia, in northeastern Spain. The target compounds were one psychoactive stimulant, one antiepileptic, four analgesics and non-steroidal anti-inflammatories, one lipid regulators, two anti-ulcer agents, nine antibiotics (sulfonamides and macrolides), two beta-blockers, two metabolites, and 11 hormones (free and conjugates). The determination was performed using liquid chromatography coupled to tandem mass spectrometry after enrichment by solid-phase extraction with Oasis HLB sorbent. Most of the pharmaceuticals were found in both influent and effluent samples from the two STPs. The most frequently detected were caffeine, acetaminophen, carbamazepine, diclofenac, ibuprofen, naproxen, sulfamethoxazole, sulfapyridine, sulfathiazole, ranitidine, omeprazole, estrone 3-sulfate, and estradiol 17-glucuronide. Specifically, the highest concentrations found in influents were 19,850Â ng/L (acetaminophen), 9,945Â ng/L (caffeine), 4,215Â ng/L (ibuprofen), 5,695Â ng/L (sulfamethoxazole), and 5,140Â ng/L (sulfathiazole). Most of the pharmaceuticals present in influent waters were found in effluents at lower concentrations. The highest concentrations in effluents were 970Â ng/L (caffeine), 670Â ng/L (sulfamethoxazole), 510Â ng/L (bezafibrate), and 1,032Â ng/L (diclofenac).
Mostrar más [+] Menos [-]Antibiotics in the surface water of Shanghai, China: screening, distribution, and indicator selecting
2021
Zhu, Feng | Wang, Siqi | Liu, Yujie | Wu, Minghong | Wang, Hongyong | Xu, Gang
The widespread existence of antibiotics has caused inevitable influence on ecology and humans. In this study, we screened the most commonly used antibiotics, and 64 antibiotics were detected in Shanghai, an international metropolis. Most of the target substances were detected in all 46 water samples including main rivers and districts in Shanghai, with concentrations ranging from 0.02 to 502.43 ng L⁻¹. In particular, sulfadiazine (502.43 ng L⁻¹) had the highest maximum concentration. Besides, risk quotients based on fish suggested that sulfonamides had a medium risk (0.12) in Shanghai. Correlation studies had shown that most compounds with frequencies exceeding 60% were significantly positively correlated with the total concentration. Based on further analysis, sulfadiazine, sulfamerazine, and sulfapyridine were screened as indicators to reflect the pollution status of antibiotics in Shanghai for a long time. The screening conditions for these indicators include detection rate (> 60%), maximum concentration (> 100 ng L⁻¹), RQ (> 0.01), and correlation (> 0). In addition, population density may be the main factor for antibiotic pollution through regional comparison. In a word, this work can systematically reflect the overall situation of Shanghai antibiotics and provide support for global data comparison in the future. Meanwhile, we provided the potential indicators that can be applied in the long term and economical monitoring of antibiotics.
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