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Phytoremediation is a cost-effective and eco-friendly alternative method for arsenic (As) contaminated water treatment. This study conducted a two-year year-round field study (cycle1 and cycle2) in a temperate area (Sendai, Japan) using small As-hyperaccumulator Pteris vittata seedlings to reduce pre-cultivation time and associated costs. The number of seedlings was changed from 256 in the cycle1 period to 165 in the cycle2 period to evaluate the As removal efficiency of P. vittata for As-contaminated water in field conditions with different plant densities. Before the winter season, with continuously increasing fronds, rhizomes, and roots growth, this reduction did not affect the plant's As removal efficiency for As-contaminated water to decrease the As concentration from 30 μg/L to the environmental quality standard for As in water, set at 10 μg/L in Japan. During the winter season, we found that cold weather caused P. vittata to wither and release the accumulated As into water without a greenhouse (cycle1). In the meantime, the bioaccumulation factor (BAF) and the translocation factor (TF) values for fronds of P. vittata decreased (BAF for fronds: from 66,089 to 8,460; TF for fronds: from 13.4 to 3.4). On the other hand, with greenhouse protection (cycle2), P. vittata did not severely wither and kept accumulating As. Moreover, BAF and TF values for fronds of P. vittata increased (BAF for fronds: from 24,372 to 36,740; TF for fronds: from 5.2 to 17.2). Maintaining the air temperature inside the greenhouse, particularly around the rhizomes, above 0 °C may be the reason why P. vittata remained alive and functional during the cold winter. These results indicate that a single-layer polyethylene greenhouse was sufficient for the tropical-subtropical As-hyperaccumulator fern P. vittata to survive the cold winter and snow in the temperate area, enabling year-round phytoremediation treatment of As-contaminated water in the open field., Competing Interests: Declaration of competing interest The authors declare that they have no known competing financial interests or personal relationships that could have appeared to influence the work reported in this paper., (Copyright © 2024 Elsevier Ltd. All rights reserved.)

In this study, the phytoremediation potential of tropical and subtropical arsenic (As) hyperaccumulating fern Pteris vittata in an As contaminated farmland field near an abandoned goldmine was investigated. The tested field is located in a subarctic area of northeast Japan. This study was aimed at decreasing the risk of As in the soil (water-soluble As) with nurturing the soil and respecting the plant life cycle for the sustainable phytoremediation for 8 years. The field was tilled and planted with new seedlings of the fern every spring and the grown fern was harvested every autumn. The biomass and As concentration in fronds, rhizomes and roots of the fern were analyzed separately after harvesting each year. The biomass of the fronds of P. vittata was significantly affected by the yearly change of the weather condition, but As concentration in fronds was kept at 100-150 mg/kg dry weight. The accumulated As in P. vittata was higher than that of As-hyperaccumulator fern Pteris cretica, the native fern in the field trial area. Harvested biomass of P. vittata per plant was also higher than that of P. cretica. More than 43.5 g As/154 m 2 (convertible to 2.82 kg of As per hectare) was removed from the farmland field by P. vittata phytoremediation at the end of the 8-year experiment. Because of the short-term plant growth period and soil tilling process, total As in soil did not show significant depletion. However, the water-soluble As in the surface and deeper soil, which is phytoavailable and easily taken in cultivated plants, decreased to 10 μg/L (Japan Environmental Quality Standard for water-soluble As in soil) by the 8-year phytoremediation using P. vittata. These research data elucidate that the tropical and subtropical As hyperaccumulating fern, P. vittata, is applicable for As phytoremediation in the subarctic climate area., Competing Interests: Declaration of competing interest The authors declare that they have no known competing financial interests or personal relationships that could have appeared to influence the work reported in this paper., (Copyright © 2022 Elsevier B.V. All rights reserved.)

Pteris vittata is an arsenic (As) hyperaccumulator plant that accumulates a large amount of As into fronds and rhizomes (around 16,000 mg/kg in both after 16 weeks hydroponic cultivation with 30 mg/L arsenate). However, the sequence of long-distance transport of As in this hyperaccumulator plant is unclear. In this study, we used a positron-emitting tracer imaging system (PETIS) for the first time to obtain noninvasive serial images of As behavior in living plants with positron-emitting 74 As-labeled tracer. We found that As kept accumulating in rhizomes as in fronds of P. vittata, whereas As was retained in roots of a non-accumulator plant Arabidopsis thaliana. Autoradiograph results of As distribution in P. vittata showed that with low As exposure, As was predominantly accumulated in young fronds and the midrib and rachis of mature fronds. Under high As exposure, As accumulation shifted from young fronds to mature fronds, especially in the margin of pinna, which resulted in necrotic symptoms, turning the marginal color to gray and then brown. Our results indicated that the function of rhizomes in P. vittata was As accumulation and the regulation of As translocation to the mature fronds to protect the young fronds under high As exposure.

Objectives: The sum of urinary inorganic arsenic (iAs), monomethylarsonic acid (MMA), and dimethylarsinic acid (DMA) concentrations is used for the biological monitoring of occupational iAs exposure. Although DMA is a major metabolite of iAs, it is an inadequate index because high DMA levels are present in urine after seafood consumption. We estimated the urinary iAs+MMA concentration corresponding to iAs exposure., Methods: We used data from two arsenic speciation analyses of urine samples from 330 Bangladeshi with oral iAs exposure and 172 Japanese workers without occupational iAs exposure using high-performance liquid chromatography with inductively coupled plasma mass spectrometry., Results: iAs, MMA, and DMA, but not arsenobetaine (AsBe), were detected in the urine of the Bangladeshi subjects. The correlation between iAs+MMA+DMA and iAs+MMA was obtained as log (iAs+MMA) = 1.038 log (iAs+MMA+DMA) -0.658. Using the regression formula, the iAs+MMA value was calculated as 2.15 and 7.5 μg As/l, corresponding to 3 and 10 μg As/m(3) of exposures, respectively. In the urine of the Japanese workers, arsenic was mostly excreted as AsBe. We used the 95th percentile of iAs+MMA (12.6 μg As/l) as the background value. The sum of the calculated and background values can be used as a biological indicator of iAs exposure., Conclusion: We propose 14.8 and 20.1 μg As/l of urinary iAs+MMA as the biological indicators of 3 and 10 μg As/m(3) iAs exposure, respectively.

In this study, we found that high-performance hydroponics of arsenic hyperaccumulator fern Pteris vittata is possible without any mechanical aeration system, if rhizomes of the ferns are kept over the water surface level. It was also found that very low-nutrition condition is better for root elongation of P. vittata that is an important factor of the arsenic removal from contaminated water. By the non-aeration and low-nutrition hydroponics for four months, roots of P. vittata were elongated more than 500 mm. The results of arsenate phytofiltration experiments showed that arsenic concentrations in water declined from the initial concentrations (50 μg/L, 500 μg/L, and 1000 μg/L) to lower than the detection limit (0.1 μg/L) and about 80% of arsenic removed was accumulated in the fern fronds. The improved hydroponics method for P. vittata developed in this study enables low-cost phytoremediation of arsenic-contaminated water and high-affinity removal of arsenic from water.

On March 11, 2011, one of the negative effects of the tsunami phenomenon that devastated the Pacific coast of the Tohoku district in Japan was the deposition of a wide range of arsenic (As) contamination to the soil. To remediate such a huge area of contamination, phytoremediation by Pteris vittata, an As-hyperaccumulator, was considered. To evaluate the efficacy of applying P. vittata to the area, the salt tolerance of P. vittata and the phytoextraction of As from soil samples were investigated. For the salt tolerance test, spore germination was considerably decreased at an NaCl level of more than 100 mM. At 200 mM, the gametophytes exhibited a morphological defect. Furthermore, the growth inhibition of P. vittata was observed with a salinity that corresponded to 66.2 mS/m of electric conductivity (EC) in the soil. A laboratory phytoremediation experiment was conducted using As-contaminated soils for 166 days. P. vittata grew and accumulated As at 264 mg/kg-DW into the shoots. Consequently, the soluble As in the soil was evidently decreased. These results showed that P. vittata was applicable to the phytoremediation of As-contaminated soil with low salinity as with the contamination caused by the 2011 tsunami.

Objectives: Chronic inorganic arsenic (iAs) exposure currently affects tens of millions of people worldwide. To accurately determine the proportion of urinary arsenic metabolites in residents continuously exposed to iAs, we performed arsenic speciation analysis of the urine of these individuals and determined whether a correlation exists between the concentration of iAs in drinking water and the urinary arsenic species content., Methods: The subjects were 165 married couples who had lived in the Pabna District in Bangladesh for more than 5 years. Arsenic species were measured using high-performance liquid chromatography and inductively coupled plasma mass spectrometry., Results: The median iAs concentration in drinking water was 55 μgAs/L (range <0.5-332 μgAs/L). Speciation analysis revealed the presence of arsenite, arsenate, monomethylarsonic acid (MMA), and dimethylarsinic acid in urine samples with medians (range) of 16.8 (7.7-32.3), 1.8 (<0.5-3.3), 13.7 (5.6-25.0), and 88.6 μgAs/L (47.9-153.4 μgAs/L), respectively. No arsenobetaine or arsenocholine was detected. The concentrations of the 4 urinary arsenic species were significantly and linearly related to each other. The urinary concentrations of total arsenic and each species were significantly correlated with the iAs concentration of drinking water., Conclusions: All urinary arsenic species are well correlated with each other and with iAs in drinking water. The most significant linear relationship existed between the iAs concentration in drinking water and urinary iAs + MMA concentration. From these results, combined with the effects of seafood ingestion, the best biomarker of iAs exposure is urinary iAs + MMA concentration.

Background: Arsenic in drinking water remains a major public problem in Bangladesh, although arsenic mitigation programs began there a decade ago. The purpose of this study was to examine the effectiveness of this program by determining the relationship between current arsenic levels in well water and the high level of urinary arsenic excretion., Methods: A community-based cross-sectional study was conducted in the Pabna district of Bangladesh between May and July 2005. We included 174 married couples and collected their drinking water from 138 wells. The allowable limit for arsenic in drinking water is 50 microg/L in Bangladesh, while the normal level of urinary arsenic is < or =40 microg x 1.5 L(-1) x day(-1) by Dhaka Community Hospital., Results: Of 348 subjects, 304 exceeded the urinary arsenic level of 40 microg x 1.5 L(-1) x day(-1). Of all wells, 44.2% had arsenic levels >50 microg/L. Multiple-adjusted odds ratios of urinary arsenic level >40 microg x 1.5 L(-1) x day(-1) were 8.90 (95% CI: 3.31-23.93) for the arsenic level in well water of 11-50 microg/L, and 53.07 (11.91-236.46) for that of 51-332 microg/L, compared with < or =10 microg/L. When the Bangladeshi standard arsenic level in drinking water of 50 microg/L was used, the sensitivity in detecting subjects with a urinary arsenic level >40 microg x 1.5 L(-1) x day(-1) was 50%, although when the World Health Organization (WHO) guideline value of 10 microg/L was used, it was 76.3%., Conclusions: Green marked wells, which the Bangladesh government regards as safe, are not always safe. The mitigation programs should use the WHO guideline arsenic level to determine the safety of well water for drinking.

The toxicity and carcinogenicity of arsenic depend on its species. Individuals living in Japan consume much seafood that contains high levels of organoarsenics. Speciation analysis of urinary arsenic is required to clarify the health risks of arsenic intake. There has been no report of urinary arsenic analysis in Japan using high performance liquid chromatography with inductively coupled plasma mass spectrometry (HPLC-ICP-MS). We performed speciation analysis of urinary arsenic for 210 Japanese male subjects without occupational exposure using HPLC-ICP-MS. The median values of urinary arsenics were as follows: sodium arsenite (AsIII), 3.5; sodium arsenate (AsV), 0.1; monomethylarsonic acid (MMA), 3.1; dimethylarsinic acid (DMA), 42.6; arsenobetaine (AsBe), 61.3; arsenocholine, trimethylarsine oxide, and unidentified arsenics (others), 5.2; and total arsenic (total As), 141.3 microgAs/l. The median creatinine-adjusted values were as follows: AsIII, 3.0; AsV, 0.1; MMA, 2.6; DMA, 35.9; AsBe, 52.1; others 3.5; and total As, 114.9 microgAs/g creatinine. Our findings indicate that DMA and AsBe levels in Japan are much higher than those found in Italian and American studies. It appears that the high levels of DMA and AsBe observed in Japan may be due in part to seafood intake. ACGIH and DFG set the BEI and BAT values for occupational arsenic exposure as 35 microgAs/l and 50 microgAs/l, respectively, using the sum of inorganic arsenic (iAs), MMA, and DMA. In the general Japanese population, the sums of these were above 50 microgAs/l in 115 (55%) samples. We therefore recommend excluding DMA concentration in monitoring of iAs exposure.

The metabolism of arsenic compounds in rats was studied by comparing urinary metabolites of arsenic compounds administered for 1 wk or 7 mo. Male F344/DuCrj rats were given 100 mg As/L as monomethylarsonic acid (MMA), dimethylarsinic acid (DMA), trimethylarsine oxide (TMAO), or arsenobetaine (AsBe), or 10 mg As/L as arsenite [As(III)] via drinking water for 7 mo. Urine was collected by forced urination after 1 wk or 7 mo. Arsenic metabolites in urine were analyzed by ion chromatography with inductively coupled plasma mass spectrometry. In the case of As(III) ingestion, a small portion of all arsenic excreted in urine (about 6%) was excreted in inorganic form, while most arsenic was excreted as methylated arsenic metabolites. Following MMA treatments for 1 wk or 7 mo, the predominant products excreted were unchanged MMA and DMA accompanied by small amounts of TMAO and tetramethylarsonium (TeMA). In the case of DMA treatment the urinary compounds found were mainly the parent DMA and TMAO with minute amounts of TeMA. TMAO was methylated to TeMA to a slight extent after 1 wk and 7 mo of administration, although most TMAO was excreted in the form of unchanged TMAO. AsBe was predominantly eliminated in urine without any transformation. Two unidentified metabolites were detected in urine after 7 mo of arsenic species exposure; the amounts of these metabolites increased in the order DMA > MMA > TMAO with only small quantities of these detected in the As(III)-treated group. These results suggest that these unidentified metabolites are formed during a demethylation process, and not during methylation. Our findings indicate that long-term exposure to As(III), MMA, or DMA decreases the proportion of TMAO elimination in urine and increases that of DMA, M-1, and M-2, and that further methylation to TMAO to TeMA does occur to a slight extent following long-term exposure to arsenical compounds in rats.

The biotransformation following oral administration of dimethylarsinic acid (DMA), an organoarsenical herbicide and the main metabolite of inorganic arsenic in mammals, was studied in rats. Male F344/DuCrj rats were administered a single dose of DMA (50 mg/kg) orally. Urine was collected at 0, 2, 4, 8, 10, 24, and 48 h after administration by forced urination. Arsenic metabolites in urine were analyzed by ion chromatography with inductively coupled plasma mass spectrometry (IC-ICP-MS). The proportions of urinary elimination of DMA, trimethylarsine oxide (TMAO), methylarsonic acid (MMA), an unidentified arsenic metabolite, and arsenite were determined at various timepoints after administration. Unmetabolized DMA was the most common form excreted during the first 4 h. Thereafter, a gradual decrease in the proportion of DMA was observed, while progressive increases in those of TMAO, the unidentified metabolite, and arsenite occurred. The proportion of TMAO excreted amounted to over 50% of all arsenic in urine between 6 and 24 h. The proportion of the unidentified metabolite and arsenite were each approximately 10% at 10 and 24 h after administration. The findings indicate that DMA administered to rats was initially excreted as unchanged DMA, and later as the methylated metabolite, TMAO. Arsenite, a demethylated metabolite of DMA, also was excreted later than elimination of DMA and TMAO. The hypothesis of demethylation by intestinal microorganisms can be supported by comparing the metabolites following oral and intraperitoneal administration. The unidentified metabolite was readily decomposed by HCl but was left unchanged by NaOH; these findings suggest that it was present in a complexed form in urine.

The toxic effects of arsenic compounds on cell divisionwere studied, using Chinese hamster V79 cells. Seven arsenic compounds weretested. Inorganic arsenic compounds (arsenite and arsenate), which have beenfound in drinking water, inhibited cell growth at very low concentrations. Monomethylarsonic acid (MMA), dimethylarsinic acid (DMA), and trimethylarsineoxide (TMAO), which are methylated metabolites of inorganic arsenics, wereless cytotoxic than the inorganic arsenics themselves. The cytotoxicity ofthe three methylated metabolites decreased as the number of methyl groupsincreased. Arsenobetaine (AsBe) and arsenocholine (AsC), which have beenfound in some marine products, did not show any cytotoxicity. Threemethylated metabolites; MMA, DMA and TMAO induced mitotic arrest. Tetraploidyproduction was observed in cells exposed to DMA or TMAO. Arsenite, arsenate,AsBe and AsC did not induce mitotic arrest or tetraploids. These resultssuggest that MMA, DMA and TMAO exert some effect on cell division inmetaphase and may thereby give some clue as to the carcinogenic mechanism ofarsenic.