Organophosphate Esters in Foodstuffs from Multiple Provinces in China: Possible Sources during Food Processing and Implications for Human Exposure

Abstract

With increasing application of organophosphate esters (OPEs) as flame retardants and plasticizers in the world, the health and ecological risks posed by these chemicals have raised people's concern over the years. Despite the fact that dietary intake is an important pathway for human exposure to OPEs, monitoring on OPEs in foodstuffs is scarce. In this study, we measured 14 OPEs in both packaged (n = 229) and fresh (n = 58) foodstuffs collected across China with a new method that was developed by two-stage solid-phase extraction. The total concentrations of OPEs (ΣOPEs) in 12 categories of packaged foodstuffs and 5 categories of fresh foodstuffs were in the range of 0.212−273 ng/g wet weight (ww) [geometric mean (GM): 5.06 ng/g ww] and 0.189−2.82 ng/g ww (GM: 0.618 ng/g ww), respectively. Significantly higher levels of ΣOPEs were found in packaged food categories of fruits and meat than those in the corresponding fresh ones, implying the extra introduction of OPEs during the processing and storage of foodstuffs. Correlation analysis showed that the GM concentrations of individual OPEs in animal-derived foods with few industrial processing were positively correlated with their annual production volumes in China in 2020, emphasizing the significance of natural sources of OPEs in these food samples. Elevated levels of ΣOPEs (range: 8.94−4120 and GM: 274 ng/g) were found in foodpackaging materials, and the predominant OPE analogues were consistent with those found in packaged food samples. The result implies that the food-packaging material can be an important contamination source of OPEs in packaged foodstuffs, which is in particular true for triphenyl phosphate, tris(2-chloroisopropyl) phosphate, tris(2-chloroethyl) phosphate, and 2-ethylhexyl diphenyl phosphate. The median daily intake of ΣOPEs via food was estimated as 65.4 ng/kg bw/day for adults in China, and the category of cereals was the major contributor (72.7%) of the dietary exposure to OPEs. The exposure risk of OPEs via food intake was generally low for the Chinese population. Overall, this study establishes a baseline concentration for OPEs in Chinese foodstuffs and uncovers food contact material as a potential source of OPEs in foods. It is expected that the research in terms of food safety and OPE contamination will benefit from this work.

Establishment of an Integrated Nontarget and Suspect Screening Workflow for Organophosphate Diesters (Di-OPEs) and Identification of Seven Previously Unknown Di-OPEs in Food Contact Plastics

“…Recent studies have identified the presence of both tri-OPEs and several di-OPEs in foodstuffs. ,, It has been suspected by numerous researchers that food packaging could be an important source of tri-OPE contamination in food. − This is corroborated by our previous study, which found 28 tri-OPEs in food contact materials and further demonstrated the migration of some tri-OPEs into food simulants . Given the information from the PubChem database, which suggests that certain di-OPEs can be used directly as additives in polymeric materials or can result from the degradation of tri-OPEs, there exists the potential for di-OPE contamination during food packaging processes .…”

Organophosphate Flame Retardants in Pregnant Women: Sources, Occurrence, and Potential Risks to Pregnancy Outcomes

“…OPFRs can be detected in agricultural products such as grains (rice, corn), vegetables (potatoes, cereals, tomatoes, cabbage, rape, carrots, broccoli, onions, and celery), fruits (apples, bananas, oranges, pears, peaches, citrus, strawberries, and grapes), meat, dairy products, and eggs around the world. ,− Pregnant women and mothers have a higher daily consumption of OPFRs than other adults, perhaps due to their specialized prenatal and postnatal diets. , Throughout the pregnancy and breastfeeding period, women should have a well-balanced diet and refuel frequently in order to obtain sufficient calories and nutrients. , They may consume more food rich in protein, vitamins, and healthy fats, which maybe contribute to a relative increase in their body burdens of OPFRs . OPFRs can be frequently detected in cereals and meat. − For example, China has the highest levels of ∑OPFRs in rice worldwide, as high as 802 ng/g dry weight (dw) . The median concentration of OPFRs in meats and fish collected from a local market in America was higher than those in dairy and cereal products .…”

Convenient Self-Heating Instant Food Causes Significant Increasing Human Exposure to Organophosphate Esters

“…The concentration of the total OPEs ranged from 14.9 to 588 ng/g ww (average, 96.9 ± 97.9; median, 73.9; geometric mean (GM), 75.1) in HF, and the eight most abundant analogues were TCEP (average, 32.3 ng/g ww), TEP (27.5), CDPP (20.5), TPhP (5.90), TCIPP (4.80), TDCIPP (1.61), EHDPP (0.63), and TnBP (0.62), respectively. The OPE concentrations in HF were at least 1 order of magnitude higher than those reported in packaged food from China (GM, 5.06 ng/g ww) 19 and the United States (<10 ng/g ww) 24 and 5 times higher than stock food from Belgium. 18 In comparison to fresh food, HF showed remarkably higher OPE levels than meat (GM,1.07 ng/g ww), aquatic products (1.18), and eggs (0.62) from China, 19 as well as meat (median, 6.76 ng/g ww), fish/seafood (7.11), dairy products (1.22), and cereal (1.94) from the United States 24 and meat and fish from Sweden (1.01−2.46 ng/g ww) 22 and Canada (0.26−3.20 ng/g ww).…”

“…19 Wang et al examined 16 food additives as potential OPE sources but found that their concentrations accounted for only 9.0% of the processed food, implying their limited contributions. 19 Therefore, there might be other OPE sources in the processed food. As known, processed food is usually fried to minimize water content for preservation purposes, and oils and fats are typically one of the most OPE-contaminated food categories.…”

“…Several studies have found higher OPE concentrations in packaged foods than in raw food materials. 19,24 Investigations into paper and plastic packages indicated that these packing materials had high levels of OPEs. 18,25 Migration studies have confirmed that OPEs can release from single-use food packaging into food simulants, suggesting it to be an important contamination source.…”