Effects of Speciation, Cooking and Changes in Bioaccessibility on Methylmercury Exposure Assessment for Contrasting Diets of Fish and Marine Mammals.

Uptake of the neurotoxicant monomethylmercury (MeHg) from fish and marine mammals continues to present a public health concern in Canada and elsewhere. However, fish and marine mammals are key diet items contributing to food security for some Indigenous populations in Canada. Mercury (Hg) exposure is estimated assuming that 100% of Hg is methylated, that 100% will be absorbed by the consumer and that cooking does not affect MeHg concentrations. Some of these assumptions do not correspond to our current state of knowledge. The aim of this study was to assess the impact of additional variables on Hg exposure equation using probabilistic risk analysis. New variables tested were (1) the proportion of methylated Hg compared to total Hg (pMeHg, %), (2) the relative absorption factor (RAF, %) expressed as bioaccessibility and (3) the mass loss factor (MLF, unitless) that represents the loss of moisture during cooking, known to increase MeHg concentration in fish and mammals. For the new variables, data from literature were used in order to set point estimate values that were further used in the probabilistic risk analysis. Modelling results for both fish and marine mammals indicate that adding these new variables significantly influenced estimates of MeHg exposure (Mood's median test, p < 0.05). This study highlights that the evaluation of exposure to MeHg is sensitive to pMeHg, RAF and MLF, and the inclusion of these variables in risk assessment should be considered with care. Further research is needed to provide better food-dependent, population-specific estimates of RAF and MLF before formal inclusion in exposure estimates.

Assessment of In Vitro Bioaccessibility and In Vivo Oral Bioavailability as Complementary Tools to Better Understand the Effect of Cooking on Methylmercury, Arsenic, and Selenium in Tuna.

Fish consumption is the main exposure pathway of the neurotoxicant methylmercury (MeHg) in humans. The risk associated with exposure to MeHg may be modified by its interactions with selenium (Se) and arsenic (As). In vitro bioaccessibility studies have demonstrated that cooking the fish muscle decreases MeHg solubility markedly and, as a consequence, its potential absorption by the consumer. However, this phenomenon has yet to be validated by in vivo models. Our study aimed to test whether MeHg bioaccessibility can be used as a surrogate to assess the effect of cooking on MeHg in vivo availability. We fed pigs raw and cooked tuna meals and collected blood samples from catheters in the portal vein and carotid artery at: 0, 30, 60, 90, 120, 180, 240, 300, 360, 420, 480 and 540 min post-meal. In contrast to in vitro models, pig oral bioavailability of MeHg was not affected by cooking, although the MeHg kinetics of absorption was faster for the cooked meal than for the raw meal. We conclude that bioaccessibility should not be readily used as a direct surrogate for in vivo studies and that, in contrast with the in vitro results, the cooking of fish muscle did not decrease the exposure of the consumer to MeHg.

Mapping metal (Hg, As, Se), lipid and protein levels within fish muscular system in two fish species (Striped Bass and Northern Pike).

Current guidelines tend to limit fish consumption based on mercury (Hg) or monomethylmercury (MeHg) content in fish flesh, without considering the presence of antagonist chemical elements that could modulate Hg toxicity. However, it is difficult to assess the potential for antagonistic interactions of these elements since their covariation within muscle tissues is poorly known. Here we present the first study simultaneously mapping multiple metal(oid)s (Hg, As and Se), lipids and proteins in fish fillets in order to assess the magnitude of intra-organ variability of metals and the potential for antagonistic interactions. We mapped two fish species (Striped Bass and Northern Pike) with contrasting muscular structure with respect to the presence of white, intermediate and red muscles. In individual Striped Bass muscle tissues, metals varied on average by 2.2-fold. Methylmercury and selenium covaried strongly and were related to protein content as assessed by % N; arsenic was inversely related to these elements and was associated with the lipid fraction of the muscle. In Pike, no such relationship was found because the contents in proteins and lipids were less variable. Arsenic speciation revealed that arsenobetaine and arsenolipids were the only As species in those fish species, whereas the toxic inorganic As species (As3+) was under the detection limit. Arsenobetaine was related to % N, whereas arsenolipids covaried with % lipids. Elemental associations found with muscle lipids and proteins could help explain changes in bioaccumulation patterns within and between individuals with potential implications on fish toxicology, biomonitoring and human consumption guidelines.

Cooking and co-ingested polyphenols reduce in vitro methylmercury bioaccessibility from fish and may alter exposure in humans.

Fish consumption is a major pathway for mercury exposure in humans. Current guidelines and risk assessments assume that 100% of methylmercury (MeHg) in fish is absorbed by the human body after ingestion. However, a growing body of literature suggests that this absorption rate may be overestimated. We used an in vitro digestion method to measure MeHg bioaccessibility in commercially-purchased fish, and investigated the effects of dietary practices on MeHg bioaccessibility. Cooking had the greatest effect, decreasing bioaccessibility on average to 12.5±5.6%. Polyphenol-rich beverages also significantly reduced bioaccessibility to 22.7±3.8% and 28.6±13.9%, for green and black tea respectively. We confirmed the suspected role of polyphenols in tea as being a driver of MeHg's reduced bioaccessibility, and found that epicatechin, epigallocatechin gallate, rutin and cafeic acid could individually decrease MeHg bioaccessibility by up to 55%. When both cooking and polyphenol-rich beverage treatments were combined, only 1% of MeHg remained bioaccessible. These results call for in vivo validation, and suggest that dietary practices should be considered when setting consumer guidelines for MeHg. More realistic risk assessments could promote consumption of fish as a source of fatty acids, which can play a protective role against cardiovascular disease.