Bikram Subedi

Occurrence of Pharmaceuticals and Personal Care Products in German Fish Tissue: A National Study

German Environment Specimen Bank (GESB) fish tissue samples, collected from 14 different GESB locations, were analyzed for 15 pharmaceuticals, 2 pharmaceutical metabolites, and 12 personal care products. Only 2 pharmaceuticals, diphenhydramine and desmethylsertraline, were measured above MDL. Diphenhydramine (0.04-0.07 ng g(-1) ww) and desmethylsertraline (1.65-3.28 ng g(-1) ww) were measured at 4 and 2 locations, respectively. The maximum concentrations of galaxolide (HHCB) (447 ng g(-1) ww) and tonalide (AHTN) (15 ng g(-1) ww) were measured at the Rehlingen sampling site in the Saar River. A significant decrease in HHCB and AHTN fish tissue concentrations was observed from 1995 to 2008 at select GESB sampling sites (r(2) = 0.69-0.89 for galaxolide and 0.89-0.97 for tonalide with p < 0.003). Galaxolide and tonalide fish tissue concentrations in Germany were ∼19× and ∼28× lower, respectively, as compared to fish tissue concentrations measured in a United States nationwide PPCP study conducted in 2006. Proximity of the sampling locations to the upstream wastewater treatment plant discharging point and mean annual flow at the sampling location were found to significantly predict galaxolide and tonalide fish tissue concentrations (HHCB: r(2) = 0.79, p = 0.021 and AHTN: r(2) = 0.81, p = 0.037) in Germany.

Mass Loading and Removal of Select Illicit Drugs in Two Wastewater Treatment Plants in New York State and Estimation of Illicit Drug Usage in Communities through Wastewater Analysis

Sewage epidemiology is a rapidly expanding field that can provide information on illicit drug usage in communities, based on the measured concentrations in samples from wastewater treatment plants (WWTPs). In this study, select illicit drugs (six drugs and eight metabolites) were determined on a daily basis for a week in wastewater, suspended particulate matter (SPM), and sludge from two WWTPs in the Albany area in New York State. The WWTP that served a larger population (∼100 000, with a flow rate of 83 300 m(3)/d) showed 3.2 (methadone) to 51 (3,4-methylenedioxyamphetamine; MDA) times higher mass flows of illicit drugs than did the WWTP that served a smaller population (∼15 000, with a flow rate of 6850 m(3)/d). The consumption rate of target illicit drugs in the communities served by the two WWTPs was estimated to range from 1.67 to 3510 mg/d/1000 people. Between the dissolved and particulate phases, the fraction of methadone, 2-ethylidene-1,5-dimethyl-3,3-diphenylpyrrolidine (EDDP), amphetamine, and MDA sorbed to SPM ranged from 34.3% to 41.1% of the total mass in the waste stream. The removal efficiencies of illicit drugs from the two WWTPs ranged from 4% (norcocaine) to 99% (cocaine); however, methamphetamine, methadone, and EDDP showed a negative removal in WWTPs. The environmental emission of illicit drugs from WWTP discharges was calculated to range from 0.38 (MDEA) to 67.5 (EDDP) mg/d/1000 people. Other markers such as caffeine, paraxanthine, nicotine, and cotinine were found to predict the concentrations of select illicit drugs in raw wastewater (r(2) = 0.20-0.79; p ≤ 0.029).

Occurrence and fate of select psychoactive pharmaceuticals and antihypertensives in two wastewater treatment plants in New York State, USA.

The fates of psychoactive pharmaceuticals, including two antischizophrenics, six sedative-hypnotic-anxiolytics, four antidepressants, four antihypertensives, and their select metabolites, were determined in two wastewater treatment plants (WWTPs) in the Albany area of New York. All target psychoactive pharmaceuticals and their metabolites were found at a mean concentration that ranged from 0.98 (quetiapine) to 1220 ng/L (atenolol) in wastewater and from 0.26 (lorazepam) to 1490 ng/g dry weight (sertraline) in sludge. In this study, the fraction of psychoactive pharmaceuticals that was sorbed to suspended particulate matter (SPM) was calculated for the first time. Over 50% of the total mass of aripiprazole, norquetiapine, norsertraline, citalopram, desmethyl citalopram, propranolol, verapamil, and norverapamil was found sorbed to SPM in the influent. The mass loadings, i.e., influx, of target psychoactive pharmaceuticals in WWTPs ranged from 0.91 (diazepam) to 347 mg/d/1000 inhabitants (atenolol), whereas the environmental emissions ranged from 0.01 (dehydro-aripiprazole) to 316 mg/d/1000 inhabitants (atenolol). The highest calculated removal efficiencies were found for antischizophrenics (quetiapine=88%; aripiprazole=71%). However, the removal of some psychoactive pharmaceuticals through adsorption onto sludge was minimal (<1% of the initial mass load), which suggests that bio-degradation and/or chemical-transformation are the dominant mechanisms of removal of these pharmaceuticals in WWTPs.

Fate of artificial sweeteners in wastewater treatment plants in New York State, U.S.A.

Very few studies describe the fate of artificial sweeteners (ASWs) in wastewater treatment plants (WWTPs). In this study, mass loadings, removal efficiencies, and environmental emission of sucralose, saccharin, aspartame, and acesulfame were determined based on the concentrations measured in wastewater influent, primary effluent, effluent, suspended particulate matter (SPM), and sludge collected from two WWTPs in the Albany area of New York State, U.S.A. All ASWs were detected at a mean concentration that ranged from 0.13 (aspartame) to 29.4 μg/L (sucralose) in wastewater influent, 0.49 (aspartame) to 27.7 μg/L (sucralose) in primary influent, 0.11 (aspartame) to 29.6 μg/L (sucralose) in effluent, and from 0.08 (aspartame) to 0.65 μg/g dw (sucralose) in sludge. Aspartame was found in 92% of influent SPM samples at a mean concentration of 444 ng/g dw, followed by acesulfame (92 ng/g) and saccharin (49 ng/g). The fraction of the total mass of ASWs sorbed to SPM was in the rank order: aspartame (50.4%) > acesulfame (10.9%) > saccharin and sucralose (0.8%). The sorption coefficients of ASWs ranged from 4.10 (saccharin) to 4540 L/kg (aspartame). Significant removal of aspartame (68.2%) and saccharin (90.3%) was found in WWTPs; however, sucralose and acesulfame were less efficiently removed (<2.0%). The total mass loading of sucralose, saccharin, and acesulfame in the WWTP that served a smaller population (∼15,000) was 1.3-1.5 times lower than that in another WWTP that served a larger population (∼100,000). The average daily loading of sucralose in both WWTPs (18.5 g/d/1000 people) was ∼2 times higher than the average loading of saccharin. The daily discharge of sucralose from the WWTPs was the highest (17.6 g/d/1000 people), followed by acesulfame (1.22 g/d/1000 people), and saccharin (1.07 g/d/1000 people). Approximately, 1180 g of saccharin and 291 g of acesulfame were transformed in or removed daily from the two WWTPs. This is the first study to describe the fate of ASWs, including the fraction found in SPM and in sludge, in addition to the aqueous portion of wastewater in WWTPs.

Simultaneous analysis of select pharmaceuticals and personal care products in fish tissue using pressurized liquid extraction combined with silica gel cleanup

Analytical improvements were developed and validated for measuring select personal care products (PCPs) and two pharmaceuticals in fish tissue. The method was validated using fortified fillet tissue for twelve PCPs including fragrance materials, alkylphenols, photo initiators, and triclosan as well as two pharmaceuticals including carbamazepine (anti-seizure) and diazepam (anti-convulsant). The analytical method utilized pressurized liquid extraction (PLE) combined with silica gel cleanup, gel permeation chromatography, and gas chromatography ion-trap tandem mass spectrometry. Silica gel cleanup was combined with the PLE to produce one automated extraction/cleanup technique. This analytical improvement served to reduce the incurred cost, time, and loss of potential target analytes associated with independent cleanup steps. The combined extraction/cleanup technique resulted in an average increase of 10% in analyte recoveries. Average triplicate recoveries and relative standard deviations for the entire method, using 2.5 g of fish fillet tissue, were 92 ± 9% (recoveries ranged from 64 to 131%). The sensitivity of the analytical methods was improved by optimizing the resonant collision induced dissociation energy to the hundredths place (0.01 V). Improvements in ion production range from 24 to 122% for six of the 12 PCPs. Statistically derived method detection limits (MDLs) were also lowered on average by a factor of 8 and ranged from 1.2 to 38 ng/g wet weight. MDLs for carbamazepine and diazepam were 18 and 3.7 ng/g wet weight, respectively. Galaxolide and tonalide were measured in an environmental sample at concentrations of 81 and 5.5 ng/g wet weight, respectively.

Emission of artificial sweeteners, select pharmaceuticals, and personal care products through sewage sludge from wastewater treatment plants in Korea.

Concern over the occurrence of artificial sweeteners (ASWs) as well as pharmaceuticals and personal care products (PPCPs) in the environment is growing, due to their high use and potential adverse effects on non-target organisms. The data for this study are drawn from a nationwide survey of ASWs in sewage sludge from 40 representative wastewater treatment plants (WWTPs) that receive domestic (WWTPD), industrial (WWTPI), or mixed (domestic plus industrial; WWTPM) wastewaters in Korea. Five ASWs (concentrations ranged from 7.08 to 5220 ng/g dry weight [dw]) and ten PPCPs (4.95-6930 ng/g dw) were determined in sludge. Aspartame (concentrations ranged from 28.4 to 5220 ng/g dw) was determined for the first time in sewage sludge. The median concentrations of ASWs and PPCPs in sludge from domestic WWTPs were 0.8-2.5 and 1.0-3.4 times, respectively, the concentrations found in WWTPs that receive combined domestic and industrial wastewaters. Among the five ASWs analyzed, the median environmental emission rates of aspartame through domestic WWTPs (both sludge and effluent discharges combined) were calculated to be 417 μg/capita/day, followed by sucralose (117 μg/capita/day), acesulfame (90 μg/capita/day), and saccharin (66μg/capita/day). The per-capita emission rates of select PPCPs, such as antimicrobials (triclocarban: 158 μg/capita/day) and analgesics (acetaminophen: 59 μg/capita/day), were an order of magnitude higher than those calculated for antimycotic (miconazole) and anthelmintic (thiabendazole) drugs analyzed in this study. Multiple linear regression analysis of measured concentrations of ASWs and PPCPs in sludge revealed that several WWTP parameters, such as treatment capacity, population-served, sludge production rate, and hydraulic retention time could influence the concentrations found in sludge.

Psychoactive Pharmaceuticals in Sludge and Their Emission from Wastewater Treatment Facilities in Korea

Concern over the occurrence of pharmaceuticals and their metabolites in the environment is mounting due to the potential adverse effects on nontarget organisms. This study draws upon a nationwide survey of psychoactive pharmaceuticals (i.e., antischizophrenics, anxiolytics, and antidepressants) in sludge from 40 representative wastewater treatment plants (WWTPs) that receive domestic, industrial, or mixed (domestic plus industrial) wastewaters in Korea. A total of 16 psychoactive pharmaceuticals (0.12-460 ng/g dry weight) and nine of their metabolites (0.97-276 ng/g dry weight) were determined in sludge. The median concentrations of psychoactive drugs in sludge from domestic WWTPs were 1.2-3.2 times higher than the concentrations found in WWTPs that receive combined domestic and industrial wastewaters. Among the psychoactive drugs analyzed, the median environmental emission rates of alprazolam (APZ) and carbamazepine (CBZ) through domestic WWTPs (both sludge and effluent discharges combined) were calculated to be ≥ 15.5 μg/capita/day, followed by quetiapine (QTP; 8.51 μg/capita/day), citalopram (CLP; 5.45 μg/capita/day), and venlafaxine (VLF; 3.59 μg/capita/day). The per-capita emission rates of some of the metabolites of psychoactive drugs through WWTP discharges were higher than those calculated for parent compounds. Significant correlations (ρ = 0.432-0.780, p < 0.05) were found between the concentrations of typically coprescribed antischizophrenics and antidepressants in sludge. Multiple linear regression analysis of measured concentrations of drugs in sludge revealed that several WWTP parameters such as treatment capacity, population-served, sludge production rate, composition of wastewater (domestic versus industrial), and hydraulic retention time can affect the concentrations of psychoactive drugs in sludge.

A review of the occurrence of pharmaceuticals and personal care products in Indian water bodies

Little information exists on the occurrence and the ultimate fate of pharmaceuticals in the water bodies in India despite being one of the world leaders in pharmaceutical production and consumption. This paper has reviewed 19 published reports of pharmaceutical occurrence in the aquatic environment in India [conventional activated sludge wastewater treatment plants (WTPs), hospital WTPs, rivers, and groundwater]. Carbamazepine (antipsychoactive), atenolol (antihypertensive), triclocarban and triclosan (antimicrobials), trimethoprim and sulfamethoxazole (antibacterials), ibuprofen and acetaminophen (analgesics), and caffeine (stimulant) are the most commonly detected at higher concentrations in Indian WTPs that treat predominantly the domestic sewage. The concentration of ciprofloxacin, sulfamethoxazole, amoxicillin, norfloxacin, and ofloxacin in Indian WTPs were up to 40 times higher than that in other countries in Europe, Australia, Asia, and North America. A very few studies in Indian rivers reported the presence of ciprofloxacin, enoxacin, ketoprofen, erythromycin, naproxen, ibuprofen, diclofenac and enrofloxacin. Similar compounds were reported in rivers in China, indicating a similar usage pattern in both of these developing countries. In a study reported from an open well in southern India, the groundwater showed the presence of cetirizine, ciprofloxacin, enoxacin, citalopram and terbinafine, which was close to a WTP receiving effluents from pharmaceutical production.

The Occurrence of Bisphenol A, Phthalates, Parabens and Other Environmental Phenolic Compounds in House Dust: A Review

Dust from indoor environments can contain significant amounts environmental contaminants and is an important source of human exposure to several toxicants. In this article, studies on the occurrence of several emerging environmental contaminants, namely bisphenol A (BPA), tetrabromobisphenol A (TBBPA), phthalates, parabens, and other environmental phenolic compounds in indoor dust from various countries, were reviewed. Issues associated with sampling of dust and the uncertainties introduced in the analytical proce- dures were also summarized. Finally, exposure to environmental phenolic compounds through dust ingestion was evaluated, and the contribution of indoor dust to the total daily exposure of toxicants was estimated. Overall, the reported concentrations of target chemicals in dust were found, in decreasing order, as phthalates (overall mean: 949 ± 669 μg/g, range: 0.9-10,900 μg/g) >>> nonylphenol (8.9 ± 6.8 μg/g, 2.6-29.2 μg/g) > BPA (3.6 ± 4.5 μg/g, 0.35-16.6 μg/g) > � parabens (1.53 ± 0.52 μg/g, 0.03-125 μg/g) > pentachlorophenol (1.39 ± 2.31 μg/g, 0.050- 5.76 μg/g) > triclosan (0.65 ± 0.23 μg/g, 0.38-0.93 μg/g) > TBBPA (0.18 ± 0.14 μg/g, 0.049-0.505 μg/g). Despite the elevated levels of the target phenolic compounds reported in indoor dust, exposure of humans through dust ingestion was minor. Never- theless, dust can be a significant source of exposure to phenolic compounds for infants and toddlers. Elevated levels of phenolic com- pounds were found in dust collected from certain microenvironments such as offices and laboratories.

Enhanced pressurized liquid extraction technique capable of analyzing polychlorodibenzo-p-dioxins, polychlorodibenzofurans, and polychlorobiphenyls in fish tissue

A high-throughput enhanced pressurized liquid extraction technique was developed by incorporating pressurized liquid extraction and multiple cleanup techniques. USEPA methods of polychlorodibenzo-p-dioxins, polychlorodibenzofurans (PCDD/Fs) and dioxin-like polychlorobiphenyls (dl-PCBs) analysis in fish tissue include independent silica gel, florisil, alumina, and carbopack/celite column cleanup techniques following extraction. Under the improved method, fish composites (~10 g) were extracted and cleaned simultaneously using alumina (~10 g), florisil (~10 g), silica gel (~5 g), celite (~5 g), and carbopack (~0.5 g). Clean extracts were concentrated and then analyzed by high resolution gas chromatography coupled with electron capture negative ionization mass spectrometry. Carbopack/celite within the extraction cell provided the analytical separation of dl-PCBs from PCDD/Fs, reducing potential molecular interferences. The average recoveries (n=3) of dl-PCBs in dichloromethane:hexane (1:1, v/v) extracts were 93±2.4% and PCDD/Fs in toluene extracts were 85±3.0%. The developed method was applied to measure the PCDD/Fs and dl-PCBs in catfish from San Jacinto River Waste Pits, a Superfund site in Houston, TX. The dl-PCBs were measured at 5.0-17,000 pg g(-1) ww. Sample preparation time and solvents were reduced as much as 95% and 65%, respectively, as compared to USEPA method 1613.