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To date, the toxicity of organophosphate esters has primarily been studied regarding their use as pesticides and their effects on the neurotransmitter acetylcholinesterase (AChE). Currently, flame retardants and plasticizers are the two largest market segments for organophosphate esters and they are found in a wide variety of products, including electronics, building materials, vehicles, furniture, car seats, plastics, and textiles. As a result, organophosphate esters and their metabolites are routinely found in human urine, blood, placental tissue, and breast milk across the globe. It has been asserted that their neurological effects are minimal given that they do not act on AChE in precisely the same way as organophosphate ester pesticides. This commentary describes research on the non-AChE neurodevelopmental toxicity of organophosphate esters used as flame retardants and plasticizers (OPEs). Studies in humans, mammalian, nonmammalian, and models are presented, and relevant neurodevelopmental pathways, including adverse outcome pathways, are described. By highlighting this scientific evidence, we hope to elevate the level of concern for widespread human exposure to these OPEs and to provide recommendations for how to better protect public health. Collectively, the findings presented demonstrate that OPEs can alter neurodevelopmental processes by interfering with noncholinergic pathways at environmentally relevant doses. Application of a pathways framework indicates several specific mechanisms of action, including perturbation of glutamate and gamma-aminobutyric acid and disruption of the endocrine system. The effects may have implications for the development of cognitive and social skills in children. Our conclusion is that concern is warranted for the developmental neurotoxicity of OPE exposure. We thus describe important considerations for reducing harm and to provide recommendations for government and industry decision makers. https://doi.org/10.1289/EHP9285.

BackgroundMany phthalates are environmental pollutants and toxic to humans. Following phthalate regulations, human exposure to phthalates has globally decreased with time in European countries, the US and Korea. Conversely, exposure to their substitutes DEHT and/or DINCH has increased. In other countries, including China, little is known on the time-trends in human exposure to these plasticizers.ObjectiveWe aimed to estimate time-trends in the urinary concentrations of phthalates, DEHT, and DINCH metabolites, in general population from non-European countries, in the last decade.MethodsWe compiled human biomonitoring (HBM) data from 123 studies worldwide in a database termed “PhthaLit”. We analyzed time-trends in the urinary concentrations of the excreted metabolites of various phthalates as well as DEHT and DINCH per metabolite, age group, and country/region, in 2009–2019. Additionally, we compared urinary metabolites levels between continents.ResultsWe found solid time-trends in adults and/or children from the US, Canada, China and Taiwan. DEHP metabolites decreased in the US and Canada. Conversely in Asia, 5oxo- and 5OH-MEHP (DEHP metabolites) increased in Chinese children. For low-weight phthalates, the trends showed a mixed picture between metabolites and countries. Notably, MnBP (a DnBP metabolite) increased in China. The phthalate substitutes DEHT and DINCH markedly increased in the US.SignificanceWe addressed the major question of time-trends in human exposure to phthalates and their substitutes and compared the results in different countries worldwide.ImpactPhthalates account for more than 50% of the plasticizer world market. Because of their toxicity, some phthalates have been regulated. In turn, the consumption of non-phthalate substitutes, such as DEHT and DINCH, is growing. Currently, phthalates and their substitutes show high detection percentages in human urine. Concerning time-trends, several studies, mainly in Europe, show a global decrease in phthalate exposure, and an increase in the exposure to phthalate substitutes in the last decade. In this study, we address the important question of time-trends in human exposure to phthalates and their substitutes and compare the results in different countries worldwide.

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.

Non-targeted analysis (NTA) and suspect screening analysis (SSA) are powerful techniques that rely on high-resolution mass spectrometry (HRMS) and computational tools to detect and identify unknown or suspected chemicals in the exposome. Fully understanding the chemical exposome requires characterization of both environmental media and human specimens. As such, we conducted a review to examine the use of different NTA and SSA methods in various exposure media and human samples, including the results and chemicals detected. The literature review was conducted by searching literature databases, such as PubMed and Web of Science, for keywords, such as “non-targeted analysis”, “suspect screening analysis” and the exposure media. Sources of human exposure to environmental chemicals discussed in this review include water, air, soil/sediment, dust, and food and consumer products. The use of NTA for exposure discovery in human biospecimen is also reviewed. The chemical space that has been captured using NTA varies by media analyzed and analytical platform. In each media the chemicals that were frequently detected using NTA were: per- and polyfluoroalkyl substances (PFAS) and pharmaceuticals in water, pesticides and polyaromatic hydrocarbons (PAHs) in soil and sediment, volatile and semi-volatile organic compounds in air, flame retardants in dust, plasticizers in consumer products, and plasticizers, pesticides, and halogenated compounds in human samples. Some studies reviewed herein used both liquid chromatography (LC) and gas chromatography (GC) HRMS to increase the detected chemical space (16%); however, the majority (51%) only used LC-HRMS and fewer used GC-HRMS (32%). Finally, we identify knowledge and technology gaps that must be overcome to fully assess potential chemical exposures using NTA. Understanding the chemical space is essential to identifying and prioritizing gaps in our understanding of exposure sources and prior exposures.Impact statementThis review examines the results and chemicals detected by analyzing exposure media and human samples using high-resolution mass spectrometry based non-targeted analysis (NTA) and suspect screening analysis (SSA).

Plasticizers are added to diverse consumer products including children’s products. Owing to their potential for endocrine disruption, the use of phthalate plasticizers is restricted in many children’s products. In this study, exposure to five phthalate esters (dibutylphthalate, di(2-ethylhexyl) phthalate (DEHP), diethyl phthalate, di-isobutyl phthalate, and diisononyl phthalate (DINP)) and an alternative (di-ethylhexyl adipate) was assessed by the use of children’s products based on chemical analysis of 3345 products purchased during 2017 and 2019 in Korea. Plasticizers were found above the detection limits in 387 products, and DEHP and DINP were the two most predominantly detected plasticizers. Deterministic and probabilistic estimation of the margin of exposure at a screening level revealed that the use of children’s products might be an important risk factor. However, it is also highly likely that the exposure could be overestimated, because the migration rate was estimated based solely on the content of plasticizers in children’s products. Chemical migration is a key process determining the absorption of plasticizers from products; thus, further refinements in experimental determination or model estimation of the migration rate are required.

The development of methodologies for the determination of plasticizers is essential for assessing the environmental and human impact resulting from the use of plastics. A fast analytical method with on-line purification based on turbulent flow chromatography (TFC) coupled to tandem mass spectrometry (MS–MS) has been developed for the analysis of ten phthalates, four alternative plasticizers (including adipates and citrates), and 20 organophosphate esters (OPEs). The method has been validated for the determination of plasticizers across different matrices. Analytical parameters showed acceptable recoveries ranging between 50 and 125%, RSDs lower than 20%, and mLODs of 0.001–2.08 ng g−1 wet weight (ww), 0.002–0.30 ng g−1, and 0.001–0.93 ng m−3 for foodstuffs, face masks, and ambient air, respectively. These methodologies were applied to foodstuff samples purchased in grocery stores, reusable and self-filtering masks, and indoor air measured in different locations. Plasticizers were detected in all the analyzed samples, with values up to 22.0 μg g−1 ww, 6.78 μg g−1, and 572 ng m−3 for foodstuffs, face masks, and indoor air, respectively. The contribution of each family to the total plasticizer content varied between 1.3 and 87%, 0.5 and 98%, and 0.5 and 65% for phthalates, alternative plasticizers, and OPEs, respectively. These findings highlighted the need for analytical methodologies capable of simultaneously assessing a wide number of plasticizers with minimal extraction steps. This capability is crucial in order to obtain more conclusive insights into the impact of these pollutants on both the environment and human health, arising from different sources of exposure such as foodstuffs, plastic materials, and atmospheric air.

Due to their formulation and/or processing, plastics contain additives and impurities that may leach out under conditions of use and accumulate in the environment. To evaluate their role as vectors of chemical contaminants in marine environment, plastic debris ( n  = 19) collected from coastal beaches along with new plastics ( n  = 25; same or same brand) bought from local markets were screened by gas chromatography–mass spectrometry in full scan mode. Detected peaks were identified using NIST library in different polymers (polypropylene (PP) > polyethylene (PE) > PP + PE > polyethyl terephthalate > poly(acylene:styrene) with different use (food, fishery, and general use). A database on the presence of 231 different chemicals were grouped into hydrocarbons, ultra-violet (UV)-stabilizers, antioxidants, plasticizers, lubricants, intermediates, compounds for dyes and inks, flame retardants, etc. The UV326, UV327, UV328, UV320, UvinualMC80, irganox 1076, DEHP, antioxidant no 33, di- n -octylisophthalate, diisooctyl phthalate, hexanoic acid 2-ethyl-hexadecyl ester, and hydrocarbons were most frequently detected. Finding of toxic phthalates and UV stabilizers in those products having moisture contact (like bottles with short use) raised concern to humans and indicated their irregular use. The comparison between new and debris plastics clearly indicated the leaching and absorption of chemicals and supports our assumption of plastic as media for transferring these additives in marine environment.

Babassu ( Atallea sp. ), a native palm tree from South America’s Amazon produces bio-oil and biochar with significant potential for industrial applications. Babassu oil as a bio-based plasticizer is reported here for the first time to replace petrochemical alternatives in the production of conductive filaments for additive manufacturing purposes. The newly developed filament, consisting of 30 wt.% carbon black (CB), 60 wt.% polylactic acid (PLA), and 10 wt.% Babassu oil, demonstrates enhanced thermal stability, improved printability, and superior electrochemical performance. 3D-printed electrodes made from this Babassu-CB/PLA filament outperform those made from commercial CB/PLA filaments, exhibiting better voltammetric responses (e.g., lower peak-to-peak separation and higher current intensity) for inner-sphere redox probes. As a proof-of-concept, these bio-based electrodes were successfully used to detect cocaine in real-world street samples, with a limit of detection (LOD) of 1.2 µmol L −1 . The Babassu-CB/PLA electrodes provided reliable cocaine quantification without interference from common adulterants such as caffeine, paracetamol, and phenacetin and showed no matrix effects, as confirmed by recovery values ranging from 88 to 102%. Notably, the use of Babassu oil eliminates the need for laborious post-treatment protocols to achieve optimal electrochemical performance. In this study, only mechanical polishing on the electrode surface is required. This study highlights the potential of Babassu oil as a sustainable alternative in the fabrication of conductive filaments for electrochemical applications, advancing the field of environmentally friendly and efficient 3D-printed sensors. Graphical Abstract

Purpose of Review Organophosphate esters (OPEs) are applied to a variety of consumer products, primarily as flame retardants and plasticizers. OPEs can leach out of products over time and are consequently prevalent in the environment and frequently detected in human biomonitoring studies. Exposure during pregnancy is of particular concern as OPEs have recently been detected in placental tissues, suggesting they may be transferred to the developing infant. Also, studies have now shown that children typically experience higher exposure to several OPEs compared with adults, indicating they may be disproportionately impacted by these compounds. This review summarizes the current literature on reproductive and child health outcomes of OPE exposures and highlights areas for future research. Recent Findings Experimental animal studies demonstrate potential for OPEs to adversely impact health, and a limited number of epidemiologic studies conducted in adult cohorts suggest that OPEs may interfere with the endocrine system. Neurodevelopment is perhaps the most well studied of children’s health endpoints, and several studies indicate that prenatal and early life OPE exposures impact both cognitive and behavioral development. Associations have also been reported with reproductive outcomes (e.g., fertilization and pregnancy loss) and with the timing of parturition and preterm birth. Cross-sectional studies also demonstrate associations between OPEs and respiratory health outcomes, allergic disease, and measures of adiposity. Summary An expanding body of research demonstrates that OPEs are associated with adverse reproductive health and birth outcomes, asthma and allergic disease, early growth and adiposity, and neurodevelopment. Still, additional research is urgently needed to elucidate the full impact of OPEs on children’s health.

Phthalate esters are commonly included in the formulations of cosmetics and related products in order to retain fragrance, enhance flexibility (i.e., by acting as plasticizers), facilitate the dissolution and dispersion of other ingredients, and improve the overall texture and sensory experience of the products. This study aimed to assess the presence and concentrations of phthalates in cosmetics by analyzing a comprehensive set of samples collected over a period of five years (2016–2020). The concentrations of nine different phthalate esters (BBP, DEHP, DNOP, DPP, DBP, DIPP, DMEP, DMP and PIPP) in 1110 cosmetics samples from France and Spain were determined by gas chromatography–mass spectrometry. The samples were included in five categories: soaps and shampoos; hand and body creams; lip gloss and lipsticks; nail polish; and facial makeup and skincare products. Some of the samples (4.86%) contained at least one phthalate at concentrations above the threshold limit (1 µg mL−1). Variable concentrations of different phthalates were determined in the 54 positive samples identified. DEHP was the most frequently detected phthalate, followed by DBP. The findings revealed different profiles according to the different categories of cosmetics and the phthalates detected in each. The results were critically compared with those obtained in various previous studies.