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[Display omitted] • Non-antibiotic pharmaceuticals have higher risk than antibiotics in landfill leachates. • Population size contributed to the regional differences of pharmaceuticals in leachates. • Solid waste composition and loading affect pharmaceutical concentrations in leachate. • High level of pharmaceuticals was observed in the leachate of residual/food waste. Municipal solid waste (MSW) landfill sites have been identified as a significant source of pharmaceuticals in the environment because unused or expired pharmaceuticals are discarded into MSW, which eventually percolate into leachates. However, the contamination of pharmaceuticals in landfill leachate in China is not comprehensively understood. Previous research into factors influencing pharmaceutical concentrations focused on a limited number and type of target pollutants or restricted study area. In the present study, 66 pharmaceuticals were analyzed (including 45 antibiotic and 21 non-antibiotic pharmaceuticals, also categorized as 59 prescription and 7 non-prescription pharmaceuticals) in leachate samples from landfill sites with various characteristics in different regions of China. The results indicated that non-antibiotic pollutants were present at significantly higher concentrations than antibiotic pollutants, with median concentrations of 1.74 μg/L and 527 ng/L, respectively. Non-antibiotic pollutants also presented a higher environmental risk than antibiotic pollutants, by 2 to 4 orders of magnitude, highlighting that non-antibiotic pharmaceuticals should not be overlooked during the assessment of landfill leachate. Pharmaceutical concentrations in landfill leachate samples exhibited regional differences; the population size served by the landfills was the dominant factor contributing to the observed differences. In addition, landfill characteristics such as the solid waste composition and MSW loading can also affect pharmaceutical concentrations in landfill leachate. Despite the implementation of the classification and disposal policy of MSW in Shanghai, China since July 2019, specifying that unused or expired pharmaceuticals should be discarded as hazardous waste, high levels of pharmaceutical contaminations were detected in leachate from the main components of classified MSW (i.e., residual and food waste). These findings emphasize the importance of pharmaceutical management in solid waste systems. [ABSTRACT FROM AUTHOR]

Highlights • PPCPs in a typical urban river of megacity Shanghai were investigated. • Untreated wastewater was proposed as a major source of PPCPs in Huangpu River. • Higher concentrations of PPCPs were detected in the lower reach and dry seasons. • Overflow of untreated wastewater led to higher PPCPs load after rainfall. Abstract Occurrence of eleven pharmaceuticals and personal care products (PPCPs) along Huangpu River, a representative urban river of megacity Shanghai, was investigated in four sampling campaigns. The overall concentrations of PPCPs ranged from

• PPCPs in the aquatic environment near the largest landfill in China was studied. • Concentration of PPCPs in groundwater decreased with the distance from landfill. • Composition of PPCPs in groundwater was similar to that in raw landfill leachate. • Impacts of studied landfill on PPCPs in the surface water were negligible. Landfill leachates are identified as a significant source of pharmaceutical and personal care products (PPCPs), which might pose a threat to groundwater and surface water nearby the landfill. However, knowledge of PPCP contamination in the surrounding water environment of landfills is very limited. Here we investigated eighteen PPCPs in water environment near the largest landfill in China, focusing on their occurrences and spatial distribution, as well as the environmental risks. The results showed the concentration of target PPCPs was below the limit of quantification (

Pharmaceuticals have been detected at high concentrations in municipal solid waste (MSW) landfill leachates, which are recognized as an underestimated source of pharmaceutical residues in the environment. However, limited efforts have been made to characterize pharmaceuticals in MSW landfill refuse, which is also of significant concern given the potential long-term environmental impact. Herein, we excavated landfill refuse from six cells with landfill ages of 7-27 years in the largest MSW landfill in Shanghai (in each cell, landfill refuse was collected from different depths of 2-8 m) and analyzed samples for the presence of 55 pharmaceuticals, including antibiotics and non-antibiotics. The results reveal the presence of 42 pharmaceuticals in landfill refuse, with median concentrations ranging from 0.30 to 116 μg/kg. Antibiotic and non-antibiotic pharmaceuticals exhibited diverse concentration trends with age, related to changes in policy intervention and consumption over time. Different concentration variations of individual pharmaceuticals were observed in refuse samples excavated at different depths and positively correlated to their sorption ability. The mass of pharmaceuticals in the investigated landfill was estimated from the obtained concentrations to be 80-220 tons with 95% probability, based on Monte Carlo analysis. To the best of our knowledge, this study provides the first estimate of pharmaceutical mass in an MSW landfill. The results will be helpful for understanding the potential long-term environmental impact of pharmaceuticals in landfills.

During the temporal storage of municipal solid wastes (MSWs), pharmaceutically contained in MSWs may percolate into leachates and migrate into receiving waters via surface runoff. However, knowledge of their intra-event variations during the rainfall is quite limited. To fill in this gap, we collected runoff samples in a typical MSW transfer station over the full length of a rainfall event to comprehensively characterize the pharmaceutical contamination profiles. The results showed that 18 pharmaceuticals were detected in the runoff samples with high frequencies and concentrations ranging from below MQL to 18.6 μg/L. During the rainfall event, pharmaceuticals exhibited discrepant leachabilities as a result of different sorption capacities; two concentration peaks of each pharmaceutical were observed, suggesting the leaching effect by rainwater and the potential influence of human-related rinse. A further sampling campaign for one-week-long runoff samples generated by diurnal rinse water was conducted, and the results indicated comparable mass loads of pharmaceuticals in surface runoff receiving rinse water (0.37-8250 μg) to those in rainfall runoff (0.58-1754 μg), suggesting the similar discharge of pharmaceuticals from MSW transfer stations despite the weather. The estimated per capita discharge load of caffeine, one of the typical Pharmaceuticals, from MSW transfer stations was 4383 ng capita -1 d -1 , higher than that in other emission sources, e.g. municipal wastewater effluent, indicating an overlooked influence of MSW transfer stations on its contamination in the surface waters in Shanghai., Competing Interests: Declaration of competing interest The authors declare that they have no known competing financial interests or personal relationships that could have appeared to influence the work reported in this paper., (Copyright © 2022 Elsevier B.V. All rights reserved.)

Recognizing the main sources of pharmaceutically active compounds (PhACs) found in surface waters has been a challenge to the effective control of PhAC contamination from the sources. In the present study, a novel method based on Characteristic Matrix (ChaMa) model of indicator PhACs to quantitatively identify the contribution of multiple emission sources was developed, verified, and applied in Huangpu River, Shanghai. Carbamazepine (CBZ), caffeine (CF) and sulfadiazine (SDZ) were proposed as indicators. Their occurrence patterns in the corresponding emission sources and the factor analysis of their composition in the surface water samples were employed to construct the ChaMa model and develop the source apportionment method. Samples from typical emission sources were collected and analyzed as hypothetical surface water samples, to verify the method proposed. The results showed that the calculated contribution proportions of emission sources to the corresponding source samples were 45%-85%, proving the feasibility of the method. Finally, the method was applied to different sections in Huangpu River, and the results showed that livestock wastewater was the dominant emission source, accounting for 55%-73% in the upper reach of Huangpu River. Untreated municipal wastewater was dominant in the middle and lower reaches of Huangpu River, accounting for 76%-94%. This novel source apportionment method allows the quantitative identification of the contribution of multiple PhAC emission sources. It can be replicated in other regions where the occurrence of localized indicators was available, and will be helpful to control the contamination of PhACs in the water environment from the major sources., Competing Interests: Declaration of competing interest The authors declare that they have no known competing financial interests or personal relationships that could have appeared to influence the work reported in this paper., (Copyright © 2022 Elsevier B.V. All rights reserved.)

The source apportionment of pharmaceuticals and personal care products (PPCPs) in the water environment based on indicators (i-PPCPs) requires a comprehensive characterization of various emission sources using reliable analytical methods for a wide spectrum of PPCPs. In this study, a robust and sensitive method based on solid phase extraction (SPE) and ultra-high performance liquid chromatography coupled with tandem mass spectrometry (UHPLC-MS/MS) for analyzing 70 PPCPs belonging to 17 therapeutic classes in landfill leachates and livestock wastewaters was developed. The SPE cartridges, sample pH, elution solvents and chelating agent additions were optimized, and acceptable recoveries (60- 130% for 67 target compounds), low method quantification limits (landfill leachate: 3- 1309 ng/L; livestock wastewater: 3- 686 ng/L) and high precisions (repeatability: 0- 20% for over 99% injections; reproducibility: 0- 20% for over 90% injections) were obtained. Using the optimized analytical method to characterize PPCPs in the typical landfill leachate and livestock wastewater in Yangtze River Delta, China, we found anthelmintics, which were first reported in landfill leachates globally, exhibited the highest concentration (albendazole, maximum concentration of 61.6 μg/L), and therefore proposed albendazole as one of the promising i-PPCP candidates in landfill leachates. In livestock wastewaters, antibiotics lincomycin was the most abundant PPCP (maximum concentration: 735 μg/L) and identified as an i-PPCP candidate for livestock-originated contamination. In addition, 15 non-antibiotic PPCPs were first investigated in the livestock wastewater in China and some non-steroidal anti-inflammatory drugs, acetaminophen, diclofenac and naproxen, were detected at similar concentration level (1.16- 91.1 μg/L) to antibiotics, highlighting the necessity to include representative non-antibiotic PPCPs in the studies of emerging contaminants in livestock wastewaters. The developed method provides a tool to comprehensively investigate PPCPs in high-strength wastewater, and the preliminary findings in the characterization of typical landfill leachates and livestock wastewaters are helpful to select i-PPCPs for the source apportionment of PPCPs in Yangtze River Delta, China., Competing Interests: Declaration of competing interest The authors declare that they have no known competing financial interests or personal relationships that could have appeared to influence the work reported in this paper., (Copyright © 2020 Elsevier B.V. All rights reserved.)

The strict environmental management has been implemented in Taihu Basin to reduce the surface water contamination; however, the effectiveness of the management actions has not been comprehensively evaluated. In the present study, 364 samples were collected during four campaigns over a span of one year from surface water, municipal wastewater treatment plants (MWWTPs), industrial wastewater treatment plants (IWWTPs), industrial enterprises, and aquaculture in a typical region in the Upper Taihu Basin. Overall concentration, temporal variation and spatial distribution of 16 PAHs in surface water and various pollution sources were evaluated and the potential pollution sources were identified. Results showed that concentrations of individual PAHs in the surface water ranged from less than the limit of quantification (LOQ) to 949 ng L -1 , indicating a reduction of PAH contamination level after the implementation of environmental management actions. Influent of MWWTPs and wastewater from industrial enterprises exhibited relatively high ∑PAHs concentrations (mean: 880 ng L -1 and 642 ng L -1 , respectively); these samples also exhibited a similar seasonal variation as well as composition of PAH congeners to those found in surface water, and therefore were designated as the main emission sources of PAHs in the studied region. Additional source apportionment using principal component analysis was also conducted to verify the proposed sources and diagnose other pollution sources. The findings provided a thorough understanding of PAH pollution, especially its major emission sources, in a typical region with pollution-intensive industries after the implementation of strict environmental management., Competing Interests: Declaration of competing interest The authors declare that they have no known competing financial interests or personal relationships that could have appeared to influence the work reported in this paper., (Copyright © 2020 Elsevier Ltd. All rights reserved.)