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Di(2-ethylhexyl)phthalate (DEHP) is a widely used plasticizer to render poly(vinyl chloride) (PVC) soft and malleable. Plasticized PVC is used in hospital equipment, food wrapping, and numerous other commercial and industrial products. Unfortunately, plasticizers can migrate within the material and leach out of it over time, ending up in the environment and, frequently, the human body. DEHP has come under increased scrutiny as its breakdown products are believed to be endocrine disruptors and more toxic than DEHP itself. DEHP and its breakdown products have been identified as ubiquitous environmental contaminants, and daily human exposure is estimated to be in the microgram per kilogram level. The objective of this review is to summarize and comment on published sources of DEHP exposure and to give an overview of its environmental fate. Exposure through bottled water was examined specifically, as this concern is raised frequently, yet only little exposure to DEHP occurs through bottled water, and DEHP exposure is unlikely to stem from the packaging material itself. Packaged food was also examined and showed higher levels of DEHP contamination compared to bottled water. Exposure to DEHP also occurs in hospital environments, where DEHP leaches directly into liquids that passed through PVC/DEHP tubing and equipment. The latter exposure is at considerably higher levels compared to food and bottled water, specifically putting patients with chronic illnesses at risk. Overall, levels of DEHP in food and bottled water were below current tolerable daily intake (TDI) values. However, our understanding of the risks of DEHP exposure is still evolving. Given the prevalence of DEHP in our atmosphere and environment, and the uncertainty revolving around it, the precautionary principle would suggest its phaseout and replacement. Increased efforts to develop viable replacement compounds, which necessarily includes rigorous leaching, toxicity, and impact assessment studies, are needed before alternative plasticizers can be adopted as viable replacements.

Phthalate plasticizers are incorporated into plastics to make them soft and malleable, but are known to leach out of the final product into their surroundings with potential detrimental effects to human and ecological health. The replacement of widely-used phthalate plasticizers, such as di-ethylhexyl phthalate (DEHP), that are of known toxicity, by the commercially-available alternative Tris(2-ethylhexyl) tri-mellitate (TOTM) is increasing. Additionally, several newly designed “green” plasticizers, including di-heptyl succinate (DHPS) and di-octyl succinate (DOS) have been identified as potential replacements. However, the impact of plasticizer exposure from medical devices on patient recovery is unknown and, moreover, the safety of TOTM, DHPS, and DOS is not well established in the context of patient recovery. To study the direct effect of clinically based chemical exposures, we exposed C57bl/6 N male and female mice to DEHP, TOTM, DOS, and DHPS during recovery from cardiac surgery and assessed survival, cardiac structure and function, immune cell infiltration into the cardiac wound and activation of the NLRP3 inflammasome. Male, but not female, mice treated in vivo with DEHP and TOTM had greater cardiac dilation, reduced cardiac function, increased infiltration of neutrophils, monocytes, and macrophages and increased expression of inflammasome receptors and effectors, thereby suggesting impaired recovery in exposed mice. In contrast, no impact was detected in female mice and male mice exposed to DOS and DHPS. To examine the direct effects in cells involved in wound healing, we treated human THP-1 macrophages with the plasticizers in vitro and found DEHP induced greater NLRP3 expression and activation. These results suggest that replacing current plasticizers with non-phthalate-based plasticizers may improve patient recovery, especially in the male population. In our assessment, DHPS is a promising possibility for a non-toxic biocompatible plasticizer.

The main objective of wastewater treatment plants (WWTPs) is to remove pathogens, nutrients, organics, and other pollutants from wastewater. After these contaminants are partially or fully removed through physical, biological, and/or chemical processes, the treated effluents are discharged into receiving waterbodies. However, since WWTPs cannot remove all contaminants, especially those of emerging concern, they inevitably represent concentrated point sources of residual contaminant loads into surface waters. To understand the severity and extent of the impact of treated-wastewater discharges from such facilities into rivers and lakes, as well as to identify opportunities of improved management, detailed information about WWTPs is required, including (1) their explicit geospatial locations to identify the waterbodies affected and (2) individual plant characteristics such as the population served, flow rate of effluents, and level of treatment of processed wastewater. These characteristics are especially important for contaminant fate models that are designed to assess the distribution of substances that are not typically included in environmental monitoring programs. Although there are several regional datasets that provide information on WWTP locations and characteristics, data are still lacking at a global scale, especially in developing countries. Here we introduce a spatially explicit global database, termed HydroWASTE, containing 58 502 WWTPs and their characteristics. This database was developed by combining national and regional datasets with auxiliary information to derive or complete missing WWTP characteristics, including the number of people served. A high-resolution river network with streamflow estimates was used to georeference WWTP outfall locations and calculate each plant's dilution factor (i.e., the ratio of the natural discharge of the receiving waterbody to the WWTP effluent discharge). The utility of this information was demonstrated in an assessment of the distribution of treated wastewater at a global scale. Results show that 1 200 000 km of the global river network receives wastewater input from upstream WWTPs, of which more than 90 000 km is downstream of WWTPs that offer only primary treatment. Wastewater ratios originating from WWTPs exceed 10 % in over 72 000 km of rivers, mostly in areas of high population densities in Europe, the USA, China, India, and South Africa. In addition, 2533 plants show a dilution factor of less than 10, which represents a common threshold for environmental concern. HydroWASTE can be accessed at https://doi.org/10.6084/m9.figshare.14847786.v1 (Ehalt Macedo et al., 2021).

This work explores the relationships between a user's choice of a given contraceptive option and the load of steroidal estrogens that can be associated with that choice. Family planning data for the USA served as a basis for the analysis. The results showed that collectively the use of contraception in the USA conservatively averts the release of approximately 4.8 tonnes of estradiol equivalents to the environment. 35% of the estrogenic load released over the course of all experienced pregnancies events and 34% the estrogenic load represented by all resultant legacies are a result of contraception failure and the non-use of contraception. A scenario analysis conducted to explore the impacts of discontinuing the use of ethinylestradiol-based oral contraceptives revealed that this would not only result in a 1.7-fold increase in the estrogenic loading of the users, but the users would also be expected to experience undesired family planning outcomes at a rate that is 3.3 times higher. Additional scenario analyses in which ethinylestradiol-based oral contraceptive users were modeled as having switched entirely to the use of male condoms, diaphragms or copper IUDs suggested that whether a higher or lower estrogenic load can be associated with the switching population depends on the typical failure rates of the options adopted following discontinuation. And, finally, it was estimated that, in the USA, at most 13% of the annual estrogenic load can be averted by fully meeting the contraceptive needs of the population. Therefore, while the issue of estrogen impacts on the environment cannot be addressed solely by meeting the population's contraceptive needs, a significant fraction of the estrogenic mass released to environment can be averted by improving the level with which their contraceptive needs are met.

The presence of antibiotics in surface waters poses risks to aquatic ecosystems and human health due to their toxicity and influence on antimicrobial resistance. After human consumption and partial metabolism, antibiotic residues are excreted and undergo complex accumulation and decay processes along their pathway from wastewater to natural river systems. Here, we use a global contaminant fate model to estimate that of the annual human consumption of the 40 most used antibiotics (30,300 tonnes), 9,500 tonnes (31%) are released into the river system and 3,250 tonnes (11%) reach the world's oceans or inland sinks. Even when only domestic sources are considered (i.e. not including veterinary or industrial sources), we estimate that 6 million km of rivers worldwide are subject to total antibiotic concentrations in excess of thresholds that are protective of ecosystems and resistance promotion during low streamflow conditions, with the dominant contributors being amoxicillin, ceftriaxone, and cefixime. Therefore, it is of concern that human consumption alone represents a significant risk for rivers across all continents, with the largest extents found in Southeast Asia. Global antibiotic consumption has grown rapidly over the last 15 years and continues to increase, particularly in low- and middle-income countries, requiring new strategies to safeguard water quality and protect human and ecosystem health.

Several linear alkyl diol dibenzoate compounds, ranging from C3 to C6 in central diol length, were evaluated for their plasticizing effectiveness in blends with poly(vinyl chloride) (PVC). The results were compared to blends of PVC/di(2-ethylhexyl) phthalate (DEHP), the most commonly used commercial plasticizer. DEHP has come under scrutiny, due to its suspected endocrine-disrupting behaviour, and the proposed diol dibenzoates have previously been shown to have the potential to be green, safe candidates for DEHP replacement. The thermal and mechanical properties of PVC/dibenzoate blends were determined, and include glass transition temperature (Tg), the elongation at break, maximum stress, apparent moduli, torsional modulus, and surface hardness. The C3, C5, and C6 dibenzoates performed as well as or better than DEHP, with the exception of torsional modulus, further supporting their use as green plasticizers. For blends with 1,4-butanediol dibenzoate, differential scanning calorimetry and torsional temperature sweeps suggested that the compound partly crystallizes within PVC blends over the course of two days, thereby losing the ability to effectively plasticize PVC. However, upon heating to temperatures above 60 °C, effective plasticization was again observed. 1,4-Butanediol dibenzoate is thereby a reversible heat-activated plasticizer or processing aid with excellent plasticizer properties at mildly elevated temperatures.

Di(2-ethylhexyl)phthalate (DEHP) is a widely used plasticizer to render poly(vinyl chloride) (PVC) soft and malleable. Plasticized PVC is used in hospital equipment, food wrapping, and numerous other commercial and industrial products. Unfortunately, plasticizers can migrate within the material and leach out of it over time, ending up in the environment and, frequently, the human body. DEHP has come under increased scrutiny as its breakdown products are believed to be endocrine disruptors and more toxic than DEHP itself. DEHP and its breakdown products have been identified as ubiquitous environmental contaminants, and daily human exposure is estimated to be in the microgram per kilogram level. The objective of this review is to summarize and comment on published sources of DEHP exposure and to give an overview of its environmental fate. Exposure through bottled water was examined specifically, as this concern is raised frequently, yet only little exposure to DEHP occurs through bottled water, and DEHP exposure is unlikely to stem from the packaging material itself. Packaged food was also examined and showed higher levels of DEHP contamination compared to bottled water. Exposure to DEHP also occurs in hospital environments, where DEHP leaches directly into liquids that passed through PVC/DEHP tubing and equipment. The latter exposure is at considerably higher levels compared to food and bottled water, specifically putting patients with chronic illnesses at risk. Overall, levels of DEHP in food and bottled water were below current tolerable daily intake (TDI) values. However, our understanding of the risks of DEHP exposure is still evolving. Given the prevalence of DEHP in our atmosphere and environment, and the uncertainty revolving around it, the precautionary principle would suggest its phaseout and replacement. Increased efforts to develop viable replacement compounds, which necessarily includes rigorous leaching, toxicity, and impact assessment studies, are needed before alternative plasticizers can be adopted as viable replacements.

It has been proposed that Trametes versicolor laccase can be used to detoxify wastewaters that are contaminated with phenolic pollutants. However, the oxidation of phenols at low concentrations may be impacted if other substrates tend to interfere with or enhance the oxidation of the target substrate. To test this, experiments were conducted to evaluate effects arising from the simultaneous presence of mixed substrates including phenol (P), estradiol (E2), cumylphenol (CP), and triclosan (TCL), each of which are characterized by different rates of oxidation and tendencies to inactivate laccase. Slower and faster substrates were found to have only minor negative impacts upon the rate of conversion of targeted substrates, except where they tended to cause inactivation. No enhancements in substrate oxidation were observed. A multi-substrate kinetic model was shown to be able to accurately predict the time course of reactions of mixed substrates over extended periods at micromolar and sub-micromolar concentrations, except when estradiol and triclosan were simultaneously present. In this case, more enzyme inactivation was observed than would be expected from the oxidation of individual substrates alone. The utility of the model for providing insights into the reaction phenomenon and for evaluating the feasibility of oxidizing targeted substrates in the presence of other substrates is demonstrated.

Pharmaceuticals and household chemicals are neither fully consumed nor fully metabolized when routinely used by humans, thereby resulting in the emission of residues down household drains and into wastewater collection systems. Since treatment systems cannot entirely remove these substances from wastewaters, the contaminants from many households connected to sewer systems are continually released into surface waters. Furthermore, diffuse contributions of wastewaters from populations that are not connected to treatment systems can directly (i.e., through surface runoff) or indirectly (i.e., through soils and groundwater) contribute to contaminant concentrations in rivers and lakes. The unplanned and unmonitored release of such contaminants can pose important risks to aquatic ecosystems and ultimately human health. In this work, the contaminant fate model HydroFATE is presented, which is designed to estimate the surface-water concentrations of domestically used substances for virtually any river in the world. The emission of compounds is calculated based on per capita consumption rates and population density. A global database of wastewater treatment plants is used to separate the effluent pathways from populations into treated and untreated and to incorporate the contaminant pathways into the river network. The transport in the river system is simulated while accounting for processes of environmental decay in streams and in lakes. To serve as a preliminary performance evaluation and proof of concept of the model, the antibiotic sulfamethoxazole (SMX) was chosen, due to its widespread use and the availability of input and validation data. The comparison of modelled concentrations against a compilation of reported SMX measurements in surface waters revealed reasonable results despite inherent model uncertainties. A total of 409 000 km of rivers were predicted to have SMX concentrations that exceed environmental risk thresholds. Given the high spatial resolution of predictions, HydroFATE is particularly useful as a screening tool to identify areas of potentially elevated contaminant exposure and to guide where local monitoring and mitigation strategies should be prioritized.

The biodegradation of plasticizers has been previously shown to result in the accumulation of metabolites that are more toxic than the initial compound. The present work shows that the pattern of degradation of di-2-ethylhexyl adipate by Bacillus subtilis can be significantly altered by the presence of biosurfactants, such as surfactin, or synthetic surfactants, such as Pluronic L122. In particular, this work confirms that the monoester, mono-2-ethylhexyl adipate, is a metabolite in the breakdown of the plasticizer. This metabolite was proposed but not observed in earlier studies. Toxicity measurements showed it to be significantly more toxic than the plasticizer. Thus, the effect of the surfactants was to significantly increase the accumulation of one or both of the two most toxic metabolites; i.e., the monoester and 2-ethylhexanol. It was proposed that the most likely cause of the effect of the surfactants was the sequestering of these two metabolites into mixed micelles, resulting in their reduced availability for further degradation.