Toxic Organic Form Research Articles

Rhizophagus intraradices mediated mitigation of arsenic toxicity in wheat involves differential distribution of arsenic in subcellular fractions and modulated expression of Phts and ABCCs

Biomagnification of arsenic in food chain through wheat consumption poses a serious threat to human health. Therefore, it is necessary to elucidate mechanism of arsenic tolerance and detoxification in wheat. The study aimed to unravel the strategies adopted by arbuscular mycorrhizal fungi to alleviate arsenic toxicity in wheat. To accomplish this, independent and interactive effects of arsenic and Rhizophagus intraradices were assessed. Colonization by R. intraradices resulted in lower expression of high-affinity phosphate transporters (Phts) in comparison with non-mycorrhizal (NM) plants, thereby lowering arsenic concentrations in mycorrhizal (M) plants. Additionally, the subcellular fractionation analysis indicated differential distribution of arsenic. In NM plants, arsenic accumulated primarily in cell wall and organelle fractions. Conversely, in M plants arsenic was more concentrated in the cell wall and vacuolar fractions. This was related to higher levels of hydroxyl and aldehyde groups in cell wall fraction of root along with increased expression of C-type ATP-binding cassette transporters in root and leaves. These factors enabled effective sequestration of arsenic in the cell wall and vacuoles of M plants, thereby reducing its toxicity. Furthermore, the proportion of inorganic arsenic was lower in M plant, as it transformed it into less toxic organic forms.

Hazardous Elements in the Edible Portion of Perna perna Mussels: Relation with the COVID-19 Pandemic Period and Assessment of the Risk to Human Health.

In this work, the concentrations of hazardous elements (As, Cd and Pb) in the edible portion of the Perna perna mussel from Southeast Brazil were analyzed to understand the effects of the COVID-19 pandemic on the coastal environment and to evaluate the quality of this fishery resource. Decreases in anthropogenic chemical outputs to the environment were expected to occur during the COVID-19 pandemic, with decreases in element concentrations in mussels. The ranges of median concentrations (µgg-1dw) in the pre- and pandemic periods were 5.4-16.1 and 2.2-10.6 for As; 0.2-0.6 and 0.1-0.5 for Cd; and 1.2-3.2 and 0.7-1.8 for Pb, respectively. Temporal variations (prepandemic x pandemic) were more significant than spatial variations (five sampling sites). The relationships between the concentrations of hazardous elements and isotopic ratios (δ15N and δ13C) suggested that food sources were more diverse across the sampling sites during the pandemic period, when individuals exhibited less efficient trophic transfer. The concentrations of Cd and Pb were below the tolerable maximum limit, whereas for As, they were above the limit; however, these concentrations are not a risk to human health, as most As was present in the least toxic organic form. The intake estimates were below the tolerable intake limits, and only Pb concentrations are at risk of causing concern if the intake of mussels increases. This is the first study in Brazil that presents a spatial-temporal comparison of hazardous elements in marine fauna considering COVID-19 as a temporal landmark. The results are of interest for both public health and environmental health management in a post-COVID-19 scenario.

Total mercury and methylmercury in garfish (Belone belone) of different body weights, sizes, ages, and sexes

BackgroundGarfish, (Belone belone) is a migratory pelagic fish that inhabits the waters of coastal Europe, North Africa, the North Sea, the Mediterranean Sea. Little information about garfish has been disseminated mainly because of its low abundance and its brief occurrence in various water bodies. Data is lacking on mercury compounds, particularly dangerous the toxic organic form of methylmercury (MeHg), which endangers the health of fish and their consumers. MethodsThe research material was garfish caught off the southern Baltic Sea coast in Puck Bay during the spawning period. Total mercury (THg) content was assayed with the cold vapour atomic absorption method in an AMA 254 mercury analyser. The MeHg extraction procedure was based on three-step sequential extraction method: hydrolysis using of hydrochloric acid, extract by toluene, bind the MeHg by L-cysteine. ResultsThe concentrations of THg and MeHg was determined in the muscle of garfish. The highest concentrations of THg (0.210 mg kg-1) and MeHg (0154 mg kg-1) were detected in the longest specimens (80 cm). The THg and MeHg concentrations in garfish muscles increased with specimens length, weight and age, which was confirmed by positive correlations. Differences were also noted depending on sex. Males accumulated more THg and MeHg than did females. The mercury in garfish from the southern Baltic Sea occurred mainly in its organic form MeHg and accounted for 84.7% of the THg. ConclusionSignificant differences were noted in mercury concentrations depends on length, weight, age and sex. Concentration of MeHg in garfish must be done by length class, and fish sex when selecting this fish for contamination studies and risk assessment. The toxic MeHg in garfish tissues did not pose a threat to the health of consumers, as indicated by the low values of EDI, TWI and THQ indices.

Se-enrichment of Chlorella vulgaris grown under different trophic states for food supplementation

Most European countries, including Portugal, have soils with low selenium (Se) concentrations. This mineral has antioxidant and chemoprotective functions essential for the human immune system. Despite Se being mostly supplied in the diet in the inorganic form, organic Se is more rapidly assimilated by the organism, presenting lower toxicity. Microalgae can incorporate inorganic Se and metabolize it into less toxic organic forms. In this context, Chlorella vulgaris biomass was tested as a biological carrier for organic Se. For this purpose, C. vulgaris was cultivated under two trophic regimes (auto- and heterotrophic) supplied with sodium selenate. The optimal Na2SeO4 concentration for autotrophic cultivation was 20 mg.L−1. From the total Se absorbed by the biomass, 81 % was organic. The biochemical composition of Se-enriched biomass compared with the non-supplemented was similar (41 vs 42 % proteins, and 5.3 vs 6.2 % lipids, respectively), except for carbohydrates (0.64 vs 2.6 %, respectively). C18:1 and C18:0 were the major fatty acids present, but different profiles were observed. The same was observed for monosaccharides, being glucose the main monosaccharide. Pigments (Chl a, Chl b, and total carotenoids) were similar for both conditions. All potential toxic metals were below the limits regulated by the European Union. Under the optimal Se concentration for autotrophic C. vulgaris growth, most Se was converted into an organic form and 0.72 g biomass would be enough to satisfy human daily Se requirements. C. vulgaris showed a high potential to be used as a biofortified food to correct or prevent Se deficiency-related diseases.

Regional and Global Scale Challenges for Controlling Arsenic Contamination in Agricultural Soil, Water Supplies, Foods and Ayurvedic Medicines

Arsenic is naturally present at high concentration levels in aquifers adversely affecting the life of some 200 million people in a number of countries on four continents. Human exposure to As from dietary sources such as marine fish, seafood, poultry, cereals is generally much lower compared to exposure through drinking contaminated water, using contaminated water in food preparation and irrigation of crops. Arsenic toxicity depends on its four valences [As(-III), As0, As(III) and As(V)] and chemical compounds. Thus, in seafood, As is mainly found in its less toxic organic forms. The qualitative and quantitative determinations of individual As species are crucial to understand the environmental fate and behavior of As. The aim of the present review is to give a brief overview on the main As speciation methods and to present how to control As contamination at local and global scales in several environmental (soil, waters) and biological (crops, basic and processed food) samples, as well as complementary and alternative medicinal products marketed as food supplements. In terms of chromatographic separation, emphasis is placed on separation by thin layer chromatography and solid phase extraction. Some approaches to address As contamination (e.g., stabilization in soil, provision of a safe water supply in affected communities) at global and regional scales are also presented.

Poaching of endangered species in Mediterranean Sea: Alopias vulpinus

A thresher shark poached by fishermen in the stretch of sea between the island of Ponza and the coast of Terracina (Lazio, Central Italy, Mediterranean Sea) and confiscated by the Italian health authorities was evaluated for the presence of chemical contaminants. Hg mean concentration of 2.1 mg kg−1 was found in muscle; speciation analysis confirmed it was almost in the toxic organic form of MeHg (2.0 mg kg−1). The Se:Hg molar ratio was <1 not protective against the toxic effect of Hg. 137Cs was detected at a mean concentration of 0.53 Bq kg−1, and 40K, radioisotope of natural origin was found at 91 Bq kg−1. Dioxins and PCBs were found in the common thresher shark at mean concentrations of 0.012 and 0.088 pg TEQ-WHO g−1 w.w. while NDL PCBs at 4.5 ng g−1 w.w., lower than limits set by European Regulation. The major concern is constituted by the presence of Hg twice the maximum limit set by EU Regulation, then the consumption of thresher shark flesh should be strongly discouraged.

Concentration of folic acid (FA) in serum of Japanese pregnant women.

Objectives Exposure to inorganic arsenic (iAs) is a world-wide health concern. We reported that Japanese children and pregnant women are exposed to moderate levels of iAs through food. Reducing iAs contamination from foods of high iAs is an important issue unique in Japan. Integrated iAs is methylated to less toxic organic forms, and S-adenosyl-L-methyonine (SAM), a common methyl-donor of DNA and histones, is utilized in this process. Chronic consumption of SAM by iAs metabolism due to exposure to iAs might alter the epigenetic modification of genome. The SAM biosynthesis pathway is dependent on folate cycle, and it is possible that ingestion of sufficient folic acid (FA) is protective to iAs induced toxicity. Methods In the course of our cross-sectional body burden analyses of Pb and iAs in Japanese children and pregnant women, termed "PbAs study", FA concentration in serum of 104 pregnant women was measured. Results Mean (±SEM) of serum FA concentration was 15.8 ± 1.3 (ng/mL). There are significant number of people showing very high FA (>30 ng/ mL), and large fraction of them were taking supplements daily. Conclusions These results suggested that level of FA ingestion of Japanese pregnant women is high for supporting normal fetal development.

Evaluation of claws as an alternative route of mercury elimination from the herring gull (Larus argentatus)

Abstract Mercury enters the body of seabirds in its most toxic organic form, i.e. methylmercury, mainly via the alimentary tract. Inside the body, mercury is transformed into less toxic forms and accumulates in the internal organs. The process of mercury removal from the body, most effective during the formation of new feathers and claws, is beneficial for the bird. The presented research was undertaken on account of the high affinity of mercury to keratin – a protein that forms feathers and claws – to compare the concentration levels (HgTOT) in these structures and to assess their contribution to the purification of the body of herring gulls (Larus argentatus) Bird feathers are the only epidermal structure that is extensively described in the literature, whereas the claws have so far been poorly researched. The study has shown that mercury in claws is built in as effectively as in feathers, and the obtained concentrations were within a wide range of 127.2–5341.5 ng HgTOT g–1 of dry weight. In addition, the concentrations of total mercury accumulated in the claws were a better reflection of Hg levels in internal organs compared to feathers.

Spatial Variation in Mercury Bioaccumulation and Magnification in a Temperate Estuarine Food Web

Estuaries are renown sinks or repositories of contaminants and reflect historical pollution of persistent compounds. In particular, mercury (Hg) contamination is widespread in coastal environments and occurs in both inorganic (THg) and highly toxic organic forms (OHg) with high bioaccumulation potential. Trophic magnification factors have been increasingly used to quantify biomagnification and represent the average rate of change in contaminant concentration throughout a food web. Here, we assessed small-scale spatial variation in THg and OHg concentrations, as well as variations in local trophic magnification factors in three segregated areas of the Tejo estuary. Selected sites covered a gradient of contamination from industrial Hg hotspots to a natural reserve area, and are key nursery areas for multiple fishes. We analyzed concentrations in sediment and biota, representing the entire local food webs. Samples included sediments, primary producers (salt marsh plants), primary consumers (macrobenthic invertebrates) and top consumers (fish muscle and liver), and the trophic web structure was characterized via SIAR mixed-modeling of nitrogen and carbon isotopic ratios. Spatial variation in Hg concentrations was observed in sediment and biota (but not for all species), with highest concentrations in the area near historical mercury input. Hg concentrations increased with trophic level, and so did the OHg fraction (% of OHg relative to THg), with mean maximum values up to 48.7% and 94.9% in invertebrates and fish, respectively. Trophic magnification factors were positive for all sites (p<0.05 for all regressions), ranging between 1.56 to 1.76 and 1.78 to 2.47 for THg and OHg, respectively. Overall, rates of mercury bioaccumulation were similar across sites with variations in biota´s Hg concentrations reflecting baseline differences in site environmental levels. Understanding mercury bioaccumulation and magnification in estuarine biota is critical to safeguard the multiple ecologic functions and economic benefits estuaries provide.

Risk estimation to human health caused by the mercury content of Sushi and Sashimi sold in Japanese restaurants in Brazil

ABSTRACTAlthough fish is a healthy alternative for meat, it can be a vehicle for mercury (Hg), including in its most toxic organic form, methylmercury (MeHg). The objective of the present study was to estimate the risk to human health caused by the consumption of sushi and sashimi as commercialized by Japanese food restaurants in the city of Campinas (SP, Brazil). The total Hg content was determined by atomic absorption spectrometry with thermal decomposition and amalgamation, and the MeHg content calculated considering that 90% of the total Hg is in the organic form. The health risk was estimated from the values for the provisional tolerable weekly ingestion (PTWI) by both adults and children. The mean concentrations for total Hg were: 147.99, 6.13, and 3.42 µg kg−1 in the tuna, kani, and salmon sushi samples, respectively, and 589.09, 85.09, and 11.38 µg kg−1 in the tuna, octopus and salmon sashimi samples, respectively. The tuna samples showed the highest Hg concentrations. One portion of tuna sashimi exceeded the PTWI value for MeHg established for children and adults. The estimate of risk for human health indicated that the level of toxicity depended on the type of fish and size of the portion consumed.

Arbuscular mycorrhizal fungi reduced the ratios of inorganic/organic arsenic in rice grains.

Arbuscular mycorrhizal fungi (AMF) - Rhizophagus intraradices was inoculated to rice to investigate its effects on arsenic (As) uptake, grain As speciation, and rhizospheric As concentration of six rice cultivars grown in As-amended soil (60 mg As kg(-1) soil). The AMF inoculation induced either positive, neutral or negative responses in rice grown in As contaminated soil, suggesting that functional diversity may exist in AMF symbiosis when As is taken up and transferred. The ratios of inorganic/organic As concentrations in rice grains of all cultivars were significantly reduced by AMF, that involved the transformation of inorganic As into less toxic organic form dimethylarsinic acid (DMA) in rice. AMF decreased significantly total As and inorganic As concentrations in rice grains of Handao 3. Positive correlations (R(2) = 0.30-0.56, P < 0.05) between As in the rhizospheric soil solution and As in rice grain at different periods were observed. This inferred that the As survey of soil solution can be an effective measure for evaluating As in grains.

Biotransformation and detoxification of inorganic arsenic in Bombay oyster Saccostrea cucullata

Arsenic (As) exists as the toxic inorganic forms in marine water and sediment, while marine oysters usually accumulate high As contents mostly as the less toxic organic forms. It has not yet been clear that how As is biotransformed in marine oysters. This study therefore investigated the biotransformation and detoxification of two inorganic As forms (As(III) and As(V)) in Bombay oyster Saccostrea cucullata after waterborne exposures for 30 days. Seven treatments of dissolved As exposure (clean seawater, 1, 5, 20mg/L As(III), and 1, 5, 20mg/L As(V)) were performed. Body As concentration increased significantly after all As exposure treatments except 1mg/L As(V). Total As, As(III), and As(V) concentration were positive correlated with glutathione-S-transferases (GST) activities, suggesting GST might play an important role in the As biotransformation and detoxification process. Organic As species were predominant in control and the low As exposed oysters, whereas a large fraction of As was remained as the inorganic forms in the high As exposed oysters, suggesting As could be biotransformed efficiently in the oysters in clean or light contaminated environment. The results of As speciation demonstrated the As biotransformation in the oysters included As(V) reduction, methylation to monomethylarsonic acid (MMA) and dimethylarsinic acid (DMA), and subsequent conversion to arsenobetaine (AsB). More As was distributed in the subcellular metallothionein-like proteins fraction (MTLP) functioning sequestration and detoxification in the inorganic As exposed oysters, suggesting it was also a strategy for oysters against As stress. In summary, this study elucidated that marine oysters had high ability to accumulate, biotransform, and detoxify inorganic As.

Species-level study on arsenic availability from dietary components

Arsenic (As) contaminated water and foodstuffs are of major concern. Samples of drinking–cooking water (n = 50), raw rice (n = 50), common vegetables (eight types), and common pulses (three types) were collected from households in the endemic region. The study found up to 70% As reduction by using safe water for cooking of rice and vegetables. Speciation study reflected more arsenate than arsenite and other organic arsenicals in all the types of samples. Male intake of 293 μg As through drinking water contained 38 μg arsenite and 246 μg arsenate, and female intake of 199 μg As contained 167 μg arsenate and 25 μg arsenite. In cooked rice, 108 μg As contained 69 μg arsenate and 17 μg arsenite with 9 μg dimethylarsonic acid (DMA). Total As consumption from cooked vegetables was 45 μg with 34 and 4 μg of arsenite and arsenate, respectively, and 5 μg of DMA. Data indicate that cooking with As-free water removes arsenic in already contaminated foodstuffs but without interconversion of the As species, from toxic inorganic to less toxic organic forms.

Assessment of solid phase microfiber extraction fibers for the monitoring of volatile organoarsinicals emitted from a plant–soil system

Phytoremediation, the use of plants and microbes to clean up inorganic and organic pollutants, has shown great promise as an inexpensive and feasible form of remediation. More recently, studies have shown that some plants have an amazing capacity to volatilize contaminants and can be an effective remediation strategy if the chemicals released are non-toxic. Arsenic contamination and remediation has drawn great attention in the scientific community. However, its toxicity also varies depending on its form. We evaluated, optimized, and then utilized a solid phase microfiber extraction (SPME) head space sampling technique to characterize the organoarsinical emissions from rabbitfoot grass (Polypogon monspeliensis) in arsenic treated soils to determine if the potentially more toxic organic forms of arsenic (AsH3, AsH2CH3, AsH(CH3)2, and As(CH3)3) were being emitted from the plant–soil system. The SPME fiber that proved best fitted for this application was the DVB/CAR/PDMS fiber with a 45min sampling period. We did detect and confirm the emissions of dimethylchloroarsine (AsCl(CH3)2) and pentamethylarsine (As(CH3)5). However, it was determined that the more toxic organic forms of arsenic were not released during phytovolatilization.

Biotransformation and detoxification of inorganic arsenic in a marine juvenile fish Terapon jarbua after waterborne and dietborne exposure

Arsenic (As) is a major hazardous metalloid in many aquatic environments. This study quantified the biotransformation of two inorganic As species [As(III) and As(V)] in a marine juvenile grunt Terapon jarbua following waterborne and dietborne exposures for 10d. The fish were fed As contaminated artificial diets at nominal concentrations of 50, 150, and 500μg As(III) and As(V)/g (dry weight), and their transformation and growth responses were compared to those exposed to 100μg/L waterborne As(III) and As(V). Within the 10d exposure period, waterborne and dietborne inorganic As exposure had no significant effect on the fish growth performance. The bioaccumulation of As was very low and not proportional to the inorganic As exposure concentration. We demonstrated that both inorganic As(III) and As(V) in the dietborne and waterborne phases were rapidly biotransformed to the less toxic arsenobetaine (AsB, 89–97%). After exposure to inorganic As, T. jarbua developed correspondingly detoxified strategies, such as the reduction of As(V) to As(III) followed by methylation to less toxic organic forms, as well as the synthesis of metal-binding proteins such as metallothionein-like proteins. This study elucidated that As(III) and As(V) had little potential toxicity on marine fish.

Hair mercury levels in Amazonian populations: spatial distribution and trends.

BackgroundMercury is present in the Amazonian aquatic environments from both natural and anthropogenic sources. As a consequence, many riverside populations are exposed to methylmercury, a highly toxic organic form of mercury, because of their intense fish consumption. Many studies have analysed this exposure from different approaches since the early nineties. This review aims to systematize the information in spatial distribution, comparing hair mercury levels by studied population and Amazonian river basin, looking for exposure trends.MethodsThe reviewed papers were selected from scientific databases and online libraries. We included studies with a direct measure of hair mercury concentrations in a sample size larger than 10 people, without considering the objectives, approach of the study or mercury speciation. The results are presented in tables and maps by river basin, displaying hair mercury levels and specifying the studied population and health impact, if any.ResultsThe majority of the studies have been carried out in communities from the central Amazonian regions, particularly on the Tapajós River basin. The results seem quite variable; hair mercury means range from 1.1 to 34.2 μg/g. Most studies did not show any significant difference in hair mercury levels by gender or age. Overall, authors emphasized fish consumption frequency as the main risk factor of exposure. The most studied adverse health effect is by far the neurological performance, especially motricity. However, it is not possible to conclude on the relation between hair mercury levels and health impact in the Amazonian situation because of the relatively small number of studies.ConclusionsHair mercury levels in the Amazonian regions seem to be very heterogenic, depending on several factors. There is no obvious spatial trend and there are many areas that have never been studied. Taking into account the low mercury levels currently handled as acceptable, the majority of the Amazonian populations can be considered exposed to methylmercury contamination. The situation for many of these traditional communities is very complex because of their high dependence on fish nutrients. It remains difficult to conclude on the Public Health implication of mercury exposure in this context.

Ecotoxicology of Methylmercury: A Transdisciplinary Challenge

Ecotoxicology of Methylmercury: A Transdisciplinary Challenge

Effect of mercury on the human health and environment: an overview

This article aims to review and to demonstrate the effect of mercury on the human health and environment. Mercury is one of the 12 toxic pollutants identified by the US Environmental Protection Agency and can be toxic at low levels in the environment. Mercury can stay in the atmosphere for up to a year. When released to the air, mercury is transported and deposited globally. Mercury ultimately accumulates in lake's bottom sediments, where it is transformed into its more toxic organic form, methyl mercury, which accumulates in fish tissue. Mercury is expected to have serious risks for human health, because it bio accumulates and persists in the environment. There are several ways to expose to mercury, such as breathing contaminated air, drinking contaminated water, consuming contaminated fishes, touching polluted subjects in home and job medias and other ways. Acute and chronic exposures have different effects on the human health. The polluting effect of mercury on the environment and human as a result of agricultural, medical, dental and industrial operations, is the main concern of this paper. Multiple sclerosis is a condition of the central nervous system that usually starts in early adult life. Mercury pollution must be considered globally but controlled locally. The polluting effect of mercury on the environment and humans as a result of agricultural, medical, dental, and industrial operations, is the main concern of this paper.

Effects of arbuscular mycorrhiza and phosphorus application on arsenic toxicity in sunflower (Helianthus annuus L.) and on the transformation of arsenic in the rhizosphere

Effects of arbuscular mycorrhiza (AM) and phosphorus (P) application on arsenic (As) toxicity were studied in a rhizobox system with As-contaminated soil collected from Shimane Prefecture, Japan. The treatments consisted of a combination of two levels of AM (Glomus aggregatum) inoculation (−AM and +AM) and two levels of P application (−P and +P at 30 mg P kg−1). Sunflower (Helianthus annuus L.) seedlings were cultured in rhizoboxes for 6 weeks. Rates of root AM infection in +AM treatments were about 40% regardless of P application. AM inoculation as well as P application reduced As toxicity symptoms, most clearly so in the +AM−P treatment. Plant growth was highest in the +AM + P treatment. Shoot As concentrations were slightly reduced by AM inoculation but enhanced by P application. Shoot P concentration in the +AM−P treatment was similar to that of +P treatments and was higher than in −AM−P. Analyses of rhizosphere soils at the end of the cultivation period indicated that P application increased water-soluble As (WS−As) in all compartments while AM inoculation increased WS−As in the central compartment only. Both the WS−arsenite [WS−As(III)] and the dominant form, arsenate [WS−As(V)], showed gradients toward the root surface. Dimethylarsine (DMAA) was detected in the +AM treatments only. To our knowledge, this is the first report of the occurrence of DMAA in the mycorrhizosphere. AM inoculation increased WS−P similarly as +P treatments did and promoted acid phosphatase activity in the soil. In conclusion, AM inoculation alleviated the effects of As toxicity by improving P nutrition without increasing As concentrations in the shoots. Moreover, AM appeared to be involved in the transformation of soil inorganic As into less toxic organic forms.

Chemical response of lakes in the Adirondack Region of New York to declines in acidic deposition.

Long-term changes in the chemistry of wet deposition and lake water were investigated in the Adirondack Region of New York. Marked decreases in concentrations of SO4(2-) and H+ in wet deposition have occurred at two sites since the late 1970s. These decreases are consistent with long-term declines in emissions of sulfur dioxide (SO2) in the eastern United States. Changes in wet NO3- deposition and nitrogen oxides (NOx) emissions have been minor over the same interval. Virtually all Adirondack Lakes have shown marked decreases in concentrations of SO4(2-), which coincide with decreases in atmospheric S deposition. Concentrations of NO3- have also decreased in several Adirondack lakes. As atmospheric N deposition has not changed over this period, the mechanism contributing to this apparent increase in lake/watershed N retention is not evident. Decreases in concentrations of SO4(2-) + NO3- have resulted in increases in acid-neutralizing capacity (ANC) and pH and resulted in a shift in the speciation of monomeric Al from toxic inorganic species toward less toxic organic forms in some lakes. Nevertheless, many lakes continue to exhibit pH values and concentrations of inorganic monomeric Al that are critical to aquatic biota. Extrapolation of rates of ANC increase suggests that the time frame of chemical recovery of Adirondack Lakes will be several decades if current decreases in acidic deposition are maintained.