Refining health risk assessment of arsenic in wild edible boletus from typical high geochemical background areas: The role of As species, bioavailability, and enterotoxicity.

Arsenic (As) is easily accumulated in wild Boletus. However, the accurate health risks and adverse effects of As on humans were largely unknown. In this study, we analyzed the total concentration, bioavailability, and speciation of As in dried wild boletus from some typical high geochemical background areas using an in vitro digestion/Caco-2 model. The health risk assessment, enterotoxicity, and risk prevention strategy after consumption of As-contaminated wild Boletus were further investigated. The results showed that the average concentration of As was 3.41-95.87 mg/kg dw, being 1.29-56.3 folds of the Chinese food safety standard limit. DMA and MMA were the dominant chemical forms in raw and cooked boletus, while their total (3.76-281 mg/kg) and bioaccessible (0.69-153 mg/kg) concentrations decreased to 0.05-9.27 mg/kg and 0.01-2.38 mg/kg after cooking. The EDI value of total As was higher than the WHO/FAO limit value, while the bioaccessible or bioavailable EDI suggested no health risks. However, the intestinal extracts of raw wild boletus triggered cytotoxicity, inflammation, cell apoptosis, and DNA damage in Caco-2 cells, indicating existing health risk assessment models based on total, bioaccessible, or bioavailable As may be not accurate enough. Given that, the bioavailability, species, and cytotoxicity should be systematically considered in accurate risk assessment. In addition, cooking mitigated the enterotoxicity along with decreasing the total and bioavailable DMA and MMA in wild boletus, suggesting that cooking could be a simple and effective way to decrease the health risks of consumption of As-contaminated wild boletus.

Heavy metal(loid)s in agriculture soils, rice, and wheat across China: Status assessment and spatiotemporal analysis.

Heavy metal(loid)s (HMs) accumulation in agricultural soils, rice, and wheat is of particular concern in China, while the status and spatio-temporal distribution of HMs in the soil-crops system have been rarely reported at the national scale. This study aimed to summarize the overall pollution status, spatiotemporal patterns, and drivers of HMs in agricultural soil, rice, and wheat nationwide. The metal-polluted data from 1030 agricultural soils, rice, and wheat in China were collected from the literature published from 2000 to 2022. The results showed that Cd was the most prevailing contaminant in soils based on its spatiotemporal distribution and accumulation. The pollution cases and severe pollution percentage of Cd (103 %) and Hg (128 %) show an increasing trend pattern. Mining activities are the main anthropogenic sources of agricultural soil HMs in China. Cd and Pb had the highest exceedance rate in rice (33.5 and 32.2 %) and wheat (25.8 and 30.3 %). The rice from Hunan, Fujian, and Guangxi showed the highest average concentration of Cd and Pb, respectively, while wheat samples from Hubei had the greatest exceedance rate of Pb. Besides, HMs in crops was not usually corresponding to soil HMs but increased gradually from north to south areas. Several mitigation strategies and accurate health risk assessments model of HMs based on bioavailability were also proposed and recommended. Collectively, this review provides valuable information to improve the management of farmland nationwide, optimize the accurate risk assessment, and reduce HMs pollution.

Total and bioaccessible heavy metals in cabbage from major producing cities in Southwest China: health risk assessment and cytotoxicity.

Green leafy vegetables are economical and nutritious, but they may be contaminated with heavy metals. In this study, we assessed the total and bioaccessible concentrations of As, Cd, Pb and Cr in a popular vegetable cabbage (Brassica oleracea) from four major producing cities in Yunnan, Southwest China. With the mean concentrations of As, Cd, Pb and Cr being 0.24, 0.20, 0.32 and 1.28 mg kg-1, the As, Cd and Pb concentrations were within the limits of 0.2-0.5 mg kg-1 based on Chinese National Standards and the WHO/FAO, but Cr concentration was 2.6-times greater than the limit of 0.5 mg kg-1. Based on an in vitro bioaccessibility assay of the Solubility Bioaccessibility Research Consortium (SBRC), As bioaccessibility was the lowest at 11% while those of Cd, Pb and Cr were much greater at 68-87%. The estimated daily intake (EDI) of metals through cabbage ingestion was similar for children and adults. Among the four metals, only Cr's EDI at 2.29-1.87 exceeded 1 based on total and bioaccessible concentrations. The high Cr concentration at 1.28 mg kg-1 coupled with its high bioaccessibility at 67.5% makes Cr of concern in cabbage. However, human gastrointestinal cells exposed to the gastric digesta with high bioaccessible heavy metals and risky EDI, showed no obvious cytotoxicity, indicating that existing models based on total or bioaccessible heavy metals may overestimate their human health risk. Taken together, to accurately assess the human health risk of heavy metals in cabbage, both total/bioaccessible concentrations and the gastrointestinal cell responses should be considered.

Geogenic nickel exposure from food consumption and soil ingestion: A bioavailability based assessment.

Accumulation and oral bioavailability of nickel (Ni) were rarely assessed for staple crops grown in high geogenic Ni soils. To assess exposure risk of geogenic Ni, soil, wheat, and rice samples were collected from a naturally high background Ni area and measured for Ni oral relative bioavailability (RBA, relative to NiSO4) using a newly developed mouse urinary Ni excretion bioassay. Results showed that soils were enriched with Ni (80.5 ± 23.0 mg kg-1, n = 58), while high Ni contents were observed in rice (2.66 ± 1.46 mg kg-1) and wheat (1.32 ± 0.78 mg kg-1) grains, with rice containing ∼2-fold higher Ni content than wheat. Ni-RBA was low in soil (14.8 ± 7.79%, n = 18), but high in wheat and rice with rice Ni-RBA (85.9 ± 19.1%, n = 9) being ∼2-fold higher than wheat (46.1 ± 21.2%, n = 16). A negative correlation (r = 0.61) was observed between Ni-RBA and iron content in rice and wheat, suggesting the low iron status of rice drives its high Ni bioavailability. The higher Ni accumulation and bioavailability for rice highlights that rice consumption was a more important contributor to daily Ni intake compared to wheat, while Ni intake from direct soil ingestion was negligible. This study suggests a potential health risk of staple crops especially rice when grown in high geogenic Ni areas.

Linking elevated blood lead level in urban school-aged children with bioaccessible lead in neighborhood soil.

Lead (Pb) exposure is known to affect the health of children while soil Pb is an important contributor to human Pb exposure. To analyze the effects of both environmental and other factors, especially total and bioaccessible Pb in neighborhood soil, on school-aged urban children's blood lead level (BLL), 75 children (6-11 years old) were recruited from an industry city in eastern China for BLL measurement and questionnaire survey. Soil samples were collected from their living neighborhoods and measured for total and bioaccessible Pb. The mean BLL was 4.82 µg dL-1, with 42 out of 75 children having BLL exceeding the international guideline of 5 µg dL-1. Low Pb contamination was observed in soil with total Pb ranging from 12.5 to 271 mg kg-1 (mean 34.3 mg kg-1). Based on the in vitro Solubility Bioaccessibility Research Consortium (SBRC) gastric fluid extraction, bioaccessible Pb in soil ranged from 0.40 to 79.1 mg kg-1 (mean 7.58 mg kg-1) with Pb bioaccessibility ranging from 1.74 to 68.1 (mean 19.9%). When BLL was correlated with total Pb in soil, insignificant linear relationship was observed (P > 0.05, correlation coefficient 95%CI = -0.047-0.40, R2 = 0.07). However, when BLL was correlated with soil bioaccessible Pb or Pb bioaccessibility, much stronger linear relationships were observed (P < 0.01, correlation coefficient 95%CI = 0.28-0.64, R2 = 0.16-0.20), suggesting that bioaccessible Pb was a much stronger predictor of BLL. In addition, strong associations were also observed between BLL and social factors such as house decoration, residence time, and personal habits, suggesting that both soil Pb contamination and social factors play important roles in elevating BLL for city children.

Inhalation bioaccessibility of PAHs in PM2.5: Implications for risk assessment and toxicity prediction.

In this study, 46 PM2.5 samples collected from Nanjing, China were analyzed for total PAH concentration, with 14 samples assessed for PAH inhalation bioaccessibility and dioxin toxicity. The concentration of 19 PAH compounds in PM2.5 ranged from 4.03 to 102 ng m-3. When PAH inhalation bioaccessibility was assessed using simulated epithelial lung fluid, mean bioaccessibility values ranged from 3.21% (Benzo(c)fluorene) to 44.2% (Acenaphthylene). Benzo(a)pyrene concentration in 50% of the PM2.5 samples exceeded the Chinese air quality standard of 2.5 ng m-3, however, when bioaccessibility was considered, all samples were below the criterion. Similarly, the cancer risk probability for all PM2.5 samples was >10-4 incidences on the basis of total PAH concentration, while only 37% of samples posed a risk >10-4 after incorporation of bioaccessibility. Dioxin toxicity of PM2.5-bound PAHs was also investigated by characterizing mRNA expression of cytochrome P450 superfamily members in human lung cells (A549 cell). Compared to total PAH concentration, the use of bioaccessible concentration was better at predicting dioxin toxicity of PM2.5-associated PAHs (correlation coefficient R2 = 0.40-0.83 with p < 0.05). This study indicates that PAH inhalation bioaccessibility is an important consideration when assessing and predicting the risk posed by PM2.5 particles, which is particularly important for countries with deteriorating air quality.

Assessment of trace metals in five most-consumed vegetables in the US: Conventional vs. organic.

Metal concentrations (As, Cd, Pb, Cr, Ba, Co, Ni, Cu, and Zn) in conventional and organic produce were assessed, specifically, five most-consumed vegetables from the US including potato, lettuce, tomato, carrot and onion. They were from four representative supermarkets in a college town in Florida. All vegetables contained detectable metals, while As, Cd, Pb, Cr, and Ba are toxic metals, Co, Ni, Cu, and Zn are nutrients for humans. The mean concentrations of As, Cd, Pb, Cr and Ba in five vegetables were 7.86, 9.17, 12.1, 44.8 and 410 µg/kg for organic produce, slightly lower than conventional produce at 7.29, 15.3, 17.9, 46.3 and 423 µg/kg. The mean concentrations of Co, Ni, Cu, and Zn in five vegetables were 3.86, 58.5, 632, and 2528 µg/kg for organic produce, comparable to conventional produce at 5.94, 68.2, 577, and 2354 µg/kg. For toxic metals, the order followed tomato < lettuce < onion < carrot < potato, with root vegetables being the highest. All metals in vegetables were lower than the allowable concentrations by FAO/WHO. Health risks associated with vegetable consumption based on daily intake and non-carcinogenic risk based on hazard quotient were lower than allowable limits. For the five most-consumed vegetables in the US, metal contents in conventional produce were slightly greater than organic produce, especially for Cd and Pb.

Fluoride concentrations in traditional and herbal teas: Health risk assessment.

Traditional tea (Camellia sinensis) and herbal tea are being consumed across the world. However, long term consumption of tea can increase the chances of fluorosis owing to the presence of fluoride (F) in teas. Therefore, it is imperative to assess the health risk associated with tea consumption. The main objectives of this study were to: 1) estimate total F in 47 popular teas, including traditional and herbal teas and F concentrations in 1% (w/v) infusion of 5 min, and 2) assess the exposure risks of F from tea consumption in children and adults. The data showed that total F was the least in herbal teas (33-102 mg/kg) and their infusions (0.06-0.69 mg/L) compared to traditional teas (296-1112 mg/kg) and their infusions (1.47-6.9 mg/L). During tea infusion, 6-96% and 18-99% of the F was released into the water from herbal and traditional teas, respectively. Ten samples of traditional teas, including five green teas had chronic daily intake (CDI) values of F > 0.05 mg/d/kg bw, the stipulated permissible limits of F intake from all sources. Although the F from teas posed no immediate health hazards with hazard quotient <1, some tea samples could potentially contribute >4 mg F/d, thereby adding to the overall F burden. Therefore, together with F from food and water sources, daily F consumptions from teas might increase its health risks to humans. So, caution should be excised when drinking teas containing high F.

A diffusive gradients in thin-films technique for the assessment of bisphenols desorption from soils.

Desorption/adsorption of bisphenols (BPs) in soils affects their mobility and availability. However, the kinetics of these processes have not been well studied, due to the lack of appropriate means of measurement. Diffusive gradients in thin-films (DGT) technique can assess kinetic processes in soils and have recently been developed for measuring three BPs (BPA, BPB and BPF). DGT was deployed for 2.5h to 20 d in five soils with different soil properties. Non-linear increase in mass accumulation by DGT with time indicated poor resupply of BPs from soil solid to solution phase. By fitting the data with DIFS (DGT-induced fluxes in soils) model, values for the labile partition coefficient (Kdl), response time (tc) and rates of exchange (k1 and k-1) of BPs between soil solid and solution phases were obtained. The derived values of Kdl showed that most of the BPs in the soil could participate in labile exchange. Average response times of 1-2h implied that the supply of BPs to DGT was limited by their desorption rate. Soils with more binding sites (higher DOM, CEC and Fe oxides) could resupply BPs more quickly, highlighting the danger of just considering partition effects.

Assessment of cadmium bioaccessibility to predict its bioavailability in contaminated soils.

In vitro assays have been developed to determine metal bioaccessibility in contaminated soils; however, their application to Cd is limited. To assess their suitability to determine Cd relative bioavailability (RBA), Cd-RBA in 12 contaminated soils containing 3.00-296mgkg(-1) Cd were determined using a mouse model and compared with Cd bioaccessibility data based on four assays including the UBM, SBRC, IVG, and PBET. After being administered feed amended with soil or CdCl2 for 10-day, the Cd concentrations in the mouse liver and/or kidneys were used as biomarkers to estimate Cd-RBA. Cd-RBA was comparable at 34-90% and 40-78% based on mouse liver and kidneys with RSD of 7.10-8.99%, and 37-84% based on mouse liver plus kidneys with lower RSD of 5.8%. Cadmium bioaccessibility in soils varied with assays, with 61-99, 59-103, 54-107, and 35-97% in the gastric phase and 20-56, 38-77, 42-88, and 19-64% in the intestinal phase of the UBM, SBRC, IVG and PBET assays. Based on the combined biomarker of liver plus kidneys, better correlation was observed for PBET (r(2)=0.61-0.70) than those for IVG, UBM and SBRC assays (0.12-0.52). The monthly Cd intake in children was 0.24-23.9µgkg(-1) using total Cd concentration in soils, which was reduced by 43% to 0.18-12.3µgkg(-1) using bioavailable Cd. Our data suggest it is important to consider Cd-RBA to assess risk associated with contaminated soils and the PBET may have potential to predict Cd-RBA in contaminated soils.

Organophosphorus flame retardants and phthalate esters in indoor dust from different microenvironments: Bioaccessibility and risk assessment.

Incidental ingestion of indoor dust is an important pathway for human exposure to organophosphorus flame retardants (OPFRs) and phthalate esters (PAEs). However, little is known about their bioaccessibility in indoor dust. In this study, indoor dust samples were collected from houses, offices, public microenvironments (PMEs), and university dorms, and physiologically based extraction test (PBET) was used to measure the bioaccessibility of OPFRs and PAEs in these dust samples. Total concentrations of OPFRs in dust samples ranged from 0.01 to 63.2 µg g(-1), with significantly lower concentrations in dorm dust (median = 0.30 µg g(-1)) than those in houses (3.12), offices (5.94), and PMEs (11.6). Total PAEs ranged from 5.49 to 2161 µg g(-1) with significantly lower concentrations in dorm dust (379 µg g(-1)) than those in the other three types of dust (767, 515, and 731 µg g(-1)). When subject to PBET, the bioaccessibility of OPFRs ranged from 8.18% (triphenyl phosphate) to 54.5% (Tris(2-chloroisopropyl) phosphate) for OPFRs, and from 1.21% (di-2-ethylhexyl phthalate, DEHP) to 81.1% (dimethyl phthalate) for PAEs. Estimated exposure doses for adults and infants to OPFRs via dust ingestion were much lower than the reference doses (RfD), but intake dose of DEHP for infants was higher than the RfD of 20 µg kg(-1) d(-1). However, the DEHP intake dose did not exceed the RfD after incorporating bioaccessibility into risk assessment. Our data indicated the importance of considering contaminant bioaccessibility during risk assessment of indoor dust.

Toxic metals in children's toys and jewelry: coupling bioaccessibility with risk assessment.

A total of 45 children's toys and jewelry were tested for total and bioaccessible metal concentrations. Total As, Cd, Sb, Cr, Ni, and Pb concentrations were 0.22-19, 0.01-139, 0.1-189, 0.06-846, 0.14-2894 and 0.08-860,000 mg kg(-1). Metallic products had the highest concentrations, with 3-7 out of 13 samples exceeding the European Union safety limit for Cd, Pb, Cr, or Ni. However, assessment based on hazard index >1 and bioaccessible metal showed different trends. Under saliva mobilization or gastric ingestion, 11 out of 45 samples showed HI >1 for As, Cd, Sb, Cr, or Ni. Pb with the highest total concentration showed HI <1 for all samples while Ni showed the most hazard with HI up to 113. Our data suggest the importance of using bioaccessibility to evaluate health hazard of metals in children's toys and jewelry, and besides Pb and Cd, As, Ni, Cr, and Sb in children's products also deserve attention.

Correlation of in vivo relative bioavailability to in vitro bioaccessibility for arsenic in household dust from China and its implication for human exposure assessment.

Incidental ingestion of household dust is an important arsenic (As) exposure pathway for children. However, compared to soils, assessment of As relative bioavailability (RBA) in household dust is limited. In this study, As-RBA in 12 household dust samples (7­38 mg kg(­1)) was measured using an in vivo mouse model and compared to As bioaccessibility determined using 4 assays [Solubility Bioaccessibility Research Consortium method (SBRC), in vitro gastrointestinal method (IVG), Deutsches Institut für Normunge.V. method (DIN), and physiologically based extraction test (PBET)]. Arsenic RBA ranged from 21.8 ± 1.6 to 85.6 ± 7.2% with samples containing low Fe and high total organic carbon content having higher As-RBA. Strong in vivo­in vitro correlations (IVIVC) were found between As-RBA and As bioaccessibility for SBRC and DIN (r2 = 0.63­0.85), but weaker ones were obtained for IVG and PBET (r2 = 0.29­0.55). The developed IVIVC for SBRC and DIN were used to calculate As-RBA based on As bioaccessibility for an additional 12 household dust samples. Although As bioaccessibility differed significantly (up to 7.7-fold) based on in vitro methods, predicted As-RBA was less variable (up to 3.0-fold) when calculated using As bioaccessibility data and the corresponding IVIVC. Our data suggested that both SBRC and DIN had potential to assess As bioavailability in household dust samples; however, additional research is needed.

Assessment of in vitro lead bioaccessibility in house dust and its relationship to in vivo lead relative bioavailability.

House dust samples containing 25-738 mg of Pb kg(-1) from 15 cities in China were assessed for in vitro Pb bioaccessibility and in vivo Pb relative bioavailability. On the basis of stable Pb isotope ratios, the Pb in dust samples mainly originated from coal combustion. Lead bioaccessibility was determined using gastric (GP) and intestinal phase (IP) of solubility bioaccessibility research consortium (SBRC), in vitro gastrointestinal (IVG), Deutsches Institut für Normunge.V. (DIN), and physiologically based extraction test methods (PBET), while Pb relative bioavailability (RBA) was determined using a mouse blood model. Lead bioaccessibility in 24 house dust samples varied significantly (23-99%) depending on the methods. Values from the IP were considerably lower than those from the GP because of the co-precipitation of Pb with iron and re-adsorption onto the dust matrix. The SBRC assay with lower GP pH produced higher Pb bioaccessibility because of enhanced Pb dissolution. When compared to mouse blood data using 12 dust samples (29-60%), SBRC-GP and DIN-GP data were correlated with Pb RBA with r(2) values of 0.68 and 0.85 and intercepts 3.15 and 17.4, respectively. Overall, SBRC-GP had potential to predict Pb RBA in dust samples. However, our data suggested that more research is needed to develop a valid in vitro method for predicting Pb RBA in house dust.

Assessment of children's exposure to arsenic from CCA-wood staircases at apartment complexes in Florida.

Arsenic exposure from wood treated with chromated copper arsenate (CCA) remains a concern due to its presence around homes. This study evaluated children's exposure to As from CCA-treated staircases through determination of bioaccessible soil As and measurements of dislodgeable As on hand railings, steps and surfaces of household objects impacted by CCA-wood leachate. Total As concentrations in 84 soil samples from 4 apartment complexes were elevated at 1.2-66.6 mg/kg with bioaccessible As at 17-84%. Deterministic risk equations were used to estimate daily doses of As in children with estimates ranging from 0.41-54.9 µg/day from ingestion of dislodgeable As. Lifetime average daily doses from ingestion of dislodgeable As and soil ranged from 8.1×10(-6) to 3.0×10(-5) mg/kg/day, with estimated cancer risks being 1.2-4.5×10(-5). Collectively, these results highlight potential health risks in children who have near-daily exposure to As from CCA-wood and are consistent with estimates generated by USEPA's SHEDS-Wood probabilistic exposure model.

Source, distribution, and health risk assessment of polycyclic aromatic hydrocarbons in urban street dust from Tianjin, China.

To better assess and understand potential health risk of urban residents exposed to urban street dust, the total concentration, sources, and distribution of 16 polycyclic aromatic hydrocarbons (PAHs) in 87 urban street dust samples from Tianjin as a Chinese megacity that has undergone rapid urbanization were investigated. In the meantime, potential sources of PAHs were identified using the principal component analysis (PCA), and the risk of residents' exposure to PAHs via urban street dust was calculated using the Incremental Lifetime Cancer Risk (ILCR) model. The results showed that the total PAHs (∑PAHs) in urban street dust from Tianjin ranged from 538 µg kg(-1) to 34.3 mg kg(-1), averaging 7.99 mg kg(-1). According to PCA, the two to three- and four to six-ring PAHs contributed 10.3 and 89.7 % of ∑PAHs, respectively. The ratio of the sum of major combustion specific compounds (ΣCOMB) / ∑PAHs varied from 0.57 to 0.79, averaging 0.64. The ratio of Ant/(Ant + Phe) varied from 0.05 to 0.41, averaging 0.10; Fla/(Fla + Pyr) from 0.40 to 0.68, averaging 0.60; BaA/(BaA + Chry) from 0.29 to 0.51, averaging 0.38; and IcdP/(IcdP + BghiP) from 0.07 to 0.37, averaging 0.22. The biomass combustion, coal combustion, and traffic emission were the main sources of PAHs in urban street dust with the similar proportion. According to the ILCR model, the total cancer risk for children and adults was up to 2.55 × 10(-5) and 9.33 × 10(-5), respectively.

Field assessment of lead immobilization in a contaminated soil after phosphate application.

A pilot-scale field demonstration was conducted at a Pb-contaminated site to assess the effectiveness of Pb immobilization using P amendments. The test site was contaminated by past battery recycling activities, with average soil Pb concentration of 1.16%. Phosphate amendments were applied at a 4.0 molar ratio of P/Pb with three treatments: T1, 100% P from H(3)PO(4); T2, 50% from H(3)PO(4)+50% from Ca(H(2)PO(4))(2); and T3, 50% from H(3)PO(4)+5% phosphate rock. Soil samples were collected and characterized 220 days after P application. Surface soil pH was reduced from 6.45 to 5.05 in T1, to 5.22 in T2, and to 5.71 in T3. Phosphate treatments effectively transformed up to 60% of total soil Pb from the non-residual fraction (sum of water soluble and exchangeable, carbonate, Fe-Mn oxide, and organic fractions) to the residual fraction relative to the control. In addition, P treatments reduced Toxicity Characteristic Leaching Procedure (TCLP) Pb from 82 mg l(-1) to below EPA's regulatory level of 5 mg l(-1) in the surface soil. Scanning electron microscopy-energy dispersive X-ray elemental analysis and X-ray diffraction analysis indicated formation of insoluble chloropyromorphite [Pb(5)(PO(4))(3)Cl] mineral in the P-treated soils. Although H(3)PO(4) is necessary to dissolve meta-stable Pb in soil for further lead immobilization, it should be used with caution due to its potential secondary contamination. A mixture of H(3)PO(4) and Ca(H(2)PO(4))(2) or phosphate rock was effective in immobilizing Pb with minimum adverse impacts associated with pH reduction.