Periodic floods and ebb tides driven by seawater affect arsenic (As) behavior in coastal wetlands, which is not fully understood. In this study, we combined DGT, high-throughput sequencing, and real-time quantitative polymerase chain reaction (qPCR) techniques for the first time to investigate the effects of flood and ebb tide on As transformation and mobility in a typical coastal tidal flat wetland by laboratory experiments. In the flood-tide stage, more As was released into the water solution, and As(III) concentration in water solution was notably higher (51 μg/L) than in the ebb-tide stage, especially in SA (sodium acetate addition) treatment. As-methylation also occurred in this stage. The release of As was attributed to the reductive dissolution of amorphous and crystalline Fe oxides bound As induced by microbes. Fusibacter, Sva1033, Bradyrhizobium, Ralstonia, and Desulfobacter were primarily involved in the reduction of As, Fe, and S. The copy numbers of arsC were 20–148 times higher than arrA, suggesting that the detoxification reduction pathway was the primary mechanism of direct As-reduction in the flood-tide stage. However, 2-D high-resolution DGT techniques revealed that the concentrations of As(III) and total As in pore water of sediments in the ebb-tide stage were higher than those in the flood-tide stage. The detected aioA gene indicated that As was oxidized in the sediment surface, resulting in As stabilization by crystalline iron minerals, whereas more As(III) were accumulated in pore water. The reduction pathway mediated by arrA may play a prominent role in the ebb-tide stage. This study provides new insights into As release processes in coastal wetlands in seawater environments, which further deepens our understanding of As biogeochemical cycling behavior in different natural environments.
Lead (Pb) contamination is one of the most significant exposure hazards to human health. Contaminated soil particles may be eroded and transferred either to the atmosphere (<10 μm) or to streams; or they may be incidentally ingested (<200 μm). Among strategies for the long-term management of this risk, one of the most cost-effective is the reduction of Pb mobility and bioavailability via amendment with phosphorus-containing materials. To clarify the effectiveness of P amendment in reducing Pb mobility and bioaccessibility in different soil size fractions, an experiment was performed by adding a soluble P compound to a historically contaminated urban soil (RO), a mining soil (MI), and an uncontaminated spiked soil (SP) at different P:Pb molar ratios (2.5:1, 5:1, and 15:1). In the <10 μm fraction of soils, P addition reduced bioaccessible Pb only in the SP soil at the highest dose, with little to no effect on RO and MI soils. Similarly, in the coarse fraction, Pb was immobilized only in the SP soil with all three P doses. These results were probably due to the higher stability of Pb in historically contaminated soils, where Pb dissolution is the limiting factor to the formation of insoluble Pb compounds. The bioaccessible proportion of Pb (using SBET method) was higher than 70 % of the total Pb in all soils and was similar in both fine and coarse particle fractions. Due to the enrichment of Pb in finer particles, this implies possible adverse effects to the environment or to human health if these particles escape from the soil. These results call for increasing attention to the effect of remediation activities on fine soil particles, considering their significant environmental role especially in urban and in historically low or moderately contaminated areas.
Perchlorate is a kind of persistent pollutant which occurs widely in the environment. The news of “high content of perchlorate detected in tea exported from China to Europe” has aroused public concerns on perchlorate in tea. However, limited data on its occurrence in tea and health risks for the tea consumers are available. To this end, this study explored the occurrence and spatial distribution of perchlorate based on 747 tea samples collected from the 13 major tea producing regions in China. Perchlorate was detected in 100% of tea samples. The average concentration of perchlorate was 163 μg/kg with the range from 1.2 μg/kg to 3132 μg/kg. From the perspective of spatial distribution, a remarkable difference was observed for perchlorate concentrations in tea samples between different regions (p < 0.0001), and the average concentration of perchlorate from the central China (409 μg/kg) was higher than that from the eastern (90.7 μg/kg) and western (140 μg/kg) regions. However, this study cannot obtain the difference of perchlorate concentrations between different tea categories. Furthermore, a human exposure assessment of perchlorate intake through tea consumption was performed by deterministic and probabilistic risk assessment. The average chronic daily intake (CDI) to perchlorate of Chinese tea consumers was 0.0183 μg/kg bw/day, however, CDI for high tea consumers (99% and 99.9%) was 0.1514–0.4675 μg/kg bw/day. The health risk assessment conducted with a hazard quotient showed that perchlorate exposure through tea consumption was under a safety threshold. Nevertheless, if other dietary exposure pathways were considered, health risks to perchlorate for high tea consumers would be paid attention to.
Effects of vitamin C supplementation on the oral bioaccessibility of lead (Pb) present in contaminated soils were examined using a number of in vitro assays (PBET, SBRC, UBM and IVG). In the presence of vitamin C, an increase in Pb bioaccessibility was observed in the gastric phase by 1.3-fold (30.5%−85.5%) and in the intestinal phase by 3.1-fold (0.9%−58.9%). Lead mobilization was regulated by reductive dissolution of Fe(III) and sequestration of Pb on secondary Fe minerals. Sequential extraction by the Bureau Community of Reference (BCR) provided more evidence that reducible fraction and residual fraction were major contributor of gastric Pb bioaccessibility, as well as reduced fractions in intestinal Pb bioaccessibility. In addition, higher non-carcinogenic risks may occur based on target hazard quotient (THQ ≥ 1). For people exposed to Pb present in soil, the management of vitamin C supplements is of serious concern.
Flue gas desulfurization (FGD) wastewater is a terminal wastewater in power plant which seriously restricts the realization of zero-liquid discharge.Bipolar membrane electrodialysis (BMED) is a sustainable and eco-friendly technology widely applied in wastewater treatment.In this study, response surface methodology is employed to optimize the three key independent operating parameters: feed concentration, current density and initial acid and base concentration in order to increase desalination rate and by-product yield.The optimum condition was obtained as feed concentration 0.675 mol/L, current density 25 mA/cm 2 and initial acid and base concentration 0 mol/L.In this optimum condition, the mean value of alkali conversion rate could be higher than 89.99%.The process cost for the regeneration of 1 kg NaOH from the FGD wastewater was $0.84.Increasing current density is an effective method to enhance by-product yield and shorten operation time, but it can cause a higher energy consumption, which means that the performance of the BMED system should be improved by optimizing operational conditions.Therefore, BMED is a new technology to realize the resource utilization and reuse of FGD wastewater.
Incidental oral ingestion is considered to be an important exposure route for humans to soil contaminants, such as fluoride (F). For 25 soil samples containing 4000 mg F/kg from aluminium smelting site in southwestern China, this study investigated F bioaccessibility in the human gastrointestinal tract in vitro. Fluoride bioaccessibility (2.4-48.8%) in the gastric phase was primarily caused by the dissolution of F-Ca and F-Al compounds (assigned to residual phase), identified by X-ray photoelectron spectroscopy and sequential extraction. Following modification to the small intestinal phase, the variation in F bioaccessibility (2.5-38.8%) should be the result of concurrent processes, including the formation of F complexes and competitive adsorption, and inversely the precipitation of fluorite and surface adsorption of formed F-Al complexes. The colon incubation with human gut microbiota yielded a 1.3-fold increase in F bioaccessibility (3.9-45.7%), probably due to the dissolution of F bound to Fe (hydr)oxides. Bioaccessibility adjustment can reduce hazard quotient of fluoride, and noncarcinogenic risk for children should be noted that soil F intake contributed 21.7% on average, up to 76.6% of oral reference dose. This will result in better understanding of human health risk assessment associated with F exposures.
Potentially Toxic Elements (PTE) are common soil contaminants and pose a significant risk to human health. In this study, ingestion (<150 μm) and inhalation (<10 μm) bioaccessibility and human health risk due to PTE were investigated in soils of the urban and peri-urban area of Torino. Lead, Cd, Cu, and Zn were observed to be the most soluble elements in simulated gastric and lung fluids. Higher bioaccessible concentrations of Pb, Ni, Co and Sb were observed in the inhalable size fraction (<10 μm) compared to ingestible one probably because of the higher concentration in fine soil size fraction. Conversely, the relative bioaccessibility of Pb, Cu, Cd, Zn and As was lower, due to the different extracting conditions and to the presumable different elemental speciation. Average values suggested that PTE would be more bioavailable if ingested than inhaled, particularly in urban areas, were the bioaccessible percentages were always higher than in peri-urban sites. Health risk assessment was conducted using bioaccessible concentrations and their corresponding toxicities via ingestion and inhalation exposures. Unacceptable non-carcinogenic risk (HQ > 1) was found through ingestion exposure for children in some urban sites and Pb was the most hazardous elements. Carcinogenic risks were under the threshold levels for every soil (CR < 10−4), with Cr and As being the dominant contributors to risk. Therefore, necessary soil remediation activities are needed to reduce the risks of human, especially for children, exposure to Pb.
In the last decade, extensive studies have been conducted to quantify the influence of different factors on potentially toxic elements (PTE) bioaccessibility in soil; one of the most important is soil size fraction. However, there is no agreement about the size fraction and the methods to investigate bioaccessibility, as very few review articles are available on soil PTE bioaccessibility and none addressed the influence of particle size on PTE bioaccessibility. This study provides a review of the relations between PTE bioaccessibility and soil particle size fractions. The available research indicates that PTE bioaccessibility distribution across different size fractions varies widely in soil, but a general trend of higher bioaccessibility in finer size fraction was found. The different elements may exhibit different relationships between bioaccessibility and soil size fraction and, in some cases, their bioaccessibility seems to be more related to the source and to the chemico-physical form of PTE in soil. Often, soil pollution and related health risk are assessed based on PTE total concentration rather than their bioaccessible fraction, but from the available studies it appears that consensus must be pursued on the methods to determine PTE bioaccessibility in the fine soil size fractions to achieve a more accurate human health risk assessment.
Soil arsenic (As) contamination is an important environmental problem, and chemical stabilization is one of the major techniques used to remediate soil As contamination. Iron and iron nanoparticle materials are widely used for soil As stabilization because they have one or more of the following advantages: high adsorption capacity, high reduction capacity, cost effectiveness and environmental friendliness. Therefore, this review introduces the stabilization of soil As with iron and iron nanoparticles, including zero-valent iron, iron oxides/hydroxides, some iron salts and Fe-based binary oxides and the nanoparticles of these iron materials. The mechanism of chemical soil As stabilization, which involves adsorption and the coprecipitation process, is discussed. The factors affecting the chemical stabilization process are presented, and challenges to overcome in the future are also discussed in this review.
Presently, the potential health risks of neonicotinoid insecticides (neonics) are now receiving much attention, but no data regarding the exposure of infants to neonics via human breast milk intake have been reported. In this study, a nationwide survey was conducted during the period of 2017-2019, wherein 97 pooled breast milk samples were collected from 3570 lactating women of 23 provinces in China. Nationally, acetamiprid-N-desmethyl was the most predominant compound, accounting for 61.2% of the total amount of neonics, followed by imidacloprid (15.6%). The concentration of the sum of acetamiprid and its metabolite acetamiprid-N-desmethyl in breast milk was positively correlated with corresponding dietary exposure, while no statistically significant association between the other neonic levels in breast milk and dietary exposure was found. The cumulative daily intakes of neonics (9.40-249 ng kg(-1) of body weight day(-1)) were estimated for breastfed infants, indicating a minuscule risk to Chinese infants from neonic exposure via breastfeeding.
Rice bran, a super food or health food supplement, contains high arsenic (As) levels. However, the evaluation of relative bioavailability (RBA) or bioaccessibility (BA) is limited in the rice bran. In this study, the As-RBA in rice bran was determined based on mice model and compared to As-BA using in vitro methods. The As-BA from rice bran-amended feed in the gastric, small intestinal, and colon phases were 33.1-56.4%, 50.5-75.6%, and 35.5-71.4%, respectively. The As-BA was adversely associated with bioaccessible Ca and Fe concentrations in the gastrointestinal phases. Similarly, the As-RBA was significant negative relative with Ca, Fe, and Zn concentrations. The As-RBA values were 37.9-65.5%, 41.5-75.6% and 38.7-71.5% based on liver, kidneys, and combined endpoint (liver plus kidneys), respectively. The in vitro-in vivo correlations (IVIVCs) in the gastric (R-2 = 0.392) and colon (R-2 = 0.362) phases were weak. While the IVIVC (R-2 = 0.544) in the small intestinal phase was stronger than those of the gastric and colon phases. In addition, there was no significant difference in As speciation between colonic residual solids and faeces (p > 0.05). This work provides a better view of human health risk evaluation on rice bran As consumption in humans. (C) 2020 Elsevier Ltd. All rights reserved.
To better understand the risk assessment of Lead (Pb) in contaminated soils, 78 soil samples were collected from different locations in China and Pb bioaccessibility was assessed using the PBET (The Physiologically Based Extraction Test) method combined with SHIME (The Simulator of the Human Intestinal Microbial Ecosystem), and Pb bioaccessibility data from the PBET method on 88 soil samples that found in the literature were also used for the assessment. For all the soils, the mean Pb bioaccessibility was as follows: the gastric phase (31.25%) > colon phase (17.78%) > small intestinal phase (10.13%). The values of Pb bioaccessibility in most soils were lower than 60%, which is the typical default assumption for Pb (RBA, relatively bioavailability) by the US EPA. Mean Pb bioaccessibility (41.10% and 14.00% for gastric and small intestinal phases, respectively) in the present study was slightly higher than the values from the literature (24.80% and 8.68% for gastric and small intestinal phases, respectively) in the gastrointestinal tract. Mean Pb bioaccessibility was lower in acidic soil during the small intestinal phase, while the values for the alkaline soil were higher in the small intestinal and colon phases. In the gastric and small intestinal phases, mean Pb bioaccessibility in farming soils was slightly lower than it was in mining soils. However, the mean Pb bioaccessibility from farming soils was increased compared with mining soils in the colon phase given the action of human gut microbiota. Soil pH and type are important factors for predicting soil Pb bioaccessibility and health risk. (C) 2019 Elsevier B.V. All rights reserved.
Organic matter (OM) was proved to have a high affinity for arsenic (As) in the presence of ferric iron (Fe(III)), the formed ternary complex OM-Fe(III)-As(V) were frequently studied before; however, the mobilization and transformation of As from OM-Fe(III)-As(V) in the presence of As(V)-reducing bacteria remains unclear. Two different strains (Desulfitobacterium sp. DJ-3, Exiguobacterium sp. DJ-4) were incubated with OM-Fe(III)-As(V) to assess the biotransformation of As and Fe. Results showed that Desulfitobacterium sp. DJ-3 could substantially stimulate the reduction and release of OM-Fe complexed As(V) and resulted in notable As(III) release (30 mg/L). The linear combination fitting result of k3-weighted As K-edge EXAFS spectra showed that 56% of OM-Fe-As(V) was transformed to OM-Fe-As(III) after 144 h. Besides, strain DJ-3 could also reduce OM complexed Fe(III), which lead to the decomposition of ternary complex and the release of 11.8 mg/g Fe(II), this microbial Fe(III) reduction process has resulted in 11% more As liberation from OM-Fe(III)-As(V) than without bacteria. In contrast, Exiguobacterium sp. DJ-4 could only reduce free As(V) but cannot stimulate As release from the complex. Our study provides the first evidence for microbial As reduction and release from ternary complex OM-Fe(III)-As(V), which could be of great importance in As geochemical circulation.