A review on organophosphate Ester (OPE) flame retardants and plasticizers in foodstuffs: Levels, distribution, human dietary exposure, and future directions

Given the ongoing studies on the adverse effects of organophosphate ester (OPE) flame retardants and plasticizers on human health, there is an increasing scientific interest in the risk of exposure to OPEs via dietary intake. Using peer-reviewed literature published up to 2018, this review surveyed and compiled the available and reported data on the concentrations and distributions of 30 OPEs based on their occurrence in various food samples from around the world. Regardless of sampling locations or food categories, 22 OPEs were detectable in at least one of analyzed sample, and there were clear variations in OPE levels among samples from different locations or food categories. For instance, cereals and fats/oils were the most contaminated by OPEs in China and Belgium, whereas fats/oils and desserts were the main polluted products in Sweden. In contrast, vegetables, fruits, fluid dairy products, and cereals were reported as the primary categories of food polluted by OPEs in Australia. Animal-based food categories such as eggs, fish and meat were the least contaminated, whereas the highest median OPE concentrations were found in meat and fish from the United State. The levels and distribution patterns of OPEs in foodstuffs demonstrated a tremendous difference even when collected from the same country and the same food item. Rice from China had the highest tris(2‑chloroethyl) phosphate (TCEP, mean: 29.8 ng/g dw) levels, whereas 2‑ethylhexyl‑diphenyl phosphate (EHDPP, mean: 4.17 ng/g ww), triphenyl phosphate (TPHP, mean: 26.14 ng/g ww), tris(2-chloroisopropyl) phosphate (TCIPP, mean: 0.87 ng/g ww) and tributyl phosphate (TNBP, median: 0.55 ng/g ww) concentrations were the highest in the same food category from Sweden, Belgium, Australia, and the United States, respectively. These discrepancies may be due to a variety of reasons such as differences in OPE physico-chemical properties, extent of usage, uptake, metabolic pathways, industrial food manufacturing processes, OPE level differences as a function of habitat, and accumulation and degradability of OPEs in different species. It is worth noting that, due to its worldwide usage in food packaging materials, EHDPP was more prominently found in processed food compared to non-processed food. Based on reported OPE levels in various foods, this review conducted a preliminary assessment of human exposure to OPEs through dietary intake, which suggested that the OPE estimated daily intake (EDI) for humans was around 880 ng/kg bw/day (95th percentile). This value was well below the corresponding OPE health reference dose given by the U.S. EPA (≥15,000 ng/kg bw/day). Even so, dietary exposure to OPEs via food intake may be not negligible based on some important factors such as dilution effects, cooking processes, and the contribution of as yet unknown means of OPE exposure. Overall, this review highlights several gaps in our understanding of OPEs in foodstuffs: 1) the investigation of contamination levels of OPEs in foodstuffs should be extended to other regions, especially North America and European countries, where OPEs are widely used and frequently detected in environmental samples, and 2) newly identified OPE derivatives/by-products, e.g., OP diesters and hydroxylated metabolites, which have been reported as end-products of OPE enzymatic metabolism or degradation through aqueous hydrolysis, and which may co-exist with parent OPEs, could also be screened with precursor OPEs in foodstuffs in future studies.