Tracing organic matter composition and distribution and its role on arsenic release in shallow Cambodian groundwaters

Biogeochemical processes that utilize dissolved organic carbon are widely thought to be responsible for the liberation of arsenic from sediments to shallow groundwater in south and southeast Asia. The accumulation of this known carcinogen to hazardously high concentrations has occurred in the primary source of drinking water in large parts of densely populated countries in this region. Both surface and sedimentary sources of organic matter have been suggested to contribute dissolved organic carbon in these aquifers. However, identification of the source of organic carbon responsible for driving arsenic release remains enigmatic and even controversial. Here, we provide the most extensive interrogation to date of the isotopic signature of ground and surface waters at a known arsenic hotspot in Cambodia. We present tritium and radiocarbon data that demonstrates that recharge through ponds and/or clay windows can transport young, surface derived organic matter in to groundwater to depths of 44 m under natural flow conditions. Young organic matter dominates the dissolved organic carbon pool in groundwater that is in close proximity to these surface water sources and we suggest this is likely a regional relationship. In locations distal to surface water contact, dissolved organic carbon represents a mixture of both young surface and older sedimentary derived organic matter. Ground-surface water interaction therefore strongly influences the average dissolved organic carbon age and how this is distributed spatially across the field site. Arsenic mobilization rates appear to be controlled by the age of dissolved organic matter present in these groundwaters. Arsenic concentrations in shallow groundwaters (< 20 m) increase by 1 μg/l for every year increase in dissolved organic carbon age compared to only 0.25 μg/l for every year increase in dissolved organic carbon age in deeper (> 20 m) groundwaters. We suggest that, while the rate of arsenic release is greatest in shallow aquifer sediments, arsenic release also occurs in deeper aquifer sediments and as such remains an important process in controlling the spatial distribution of arsenic in the groundwaters of SE Asia. Our findings suggest that any anthropogenic activities that alter the source of groundwater recharge or the timescales over which recharge takes place may also drive changes in the natural composition of dissolved organic carbon in these groundwaters. Such changes have the potential to influence both the spatial and temporal evolution of the current groundwater arsenic hazard in this region

Exploratory study of the association in the United Kingdom between hypertension and inorganic arsenic (iAs) intake from rice and rice products

From Springer Nature via Jisc Publications RouterHistory: received 2019-12-13, accepted 2020-04-10, registration 2020-04-10, pub-electronic 2020-04-28, online 2020-04-28, pub-print 2021-07Publication status: PublishedFunder: University of Manchester; Grant(s): Presidents Doctoral ScholarshipAbstract: Hypertension risks arising from chronic exposure to inorganic arsenic (iAs) are well documented. Consumption of rice is a major iAs exposure route for over 3 billion people; however, there is a lack of epidemiological evidence demonstrating an association of hypertension risks with iAs intake from rice, especially in areas where there is little exposure from drinking water but a growing demand for rice intake. To address this, we conducted an individual-level cross-sectional analysis to quantify the extent to which daily iAs intake from rice and rice products (E-iAsing,rice) modifies the association between hypertension risks and previously well-established risk factors. The analysis was based on secondary dietary, socio-demographic and health status data of 598 participants recorded in the UK National Diet and Nutrition Survey 2014–2016. E-iAsing,rice and five blood pressure endpoints were derived with potential associations explored through generalized linear models. According to the results, a negative but not significant relationship was found between hypertension risks and E-iAsing,rice after adjusting for major risk factors, notably age, gender, diabetes and obesity, with relatively higher risks being observed for male, middle-aged, overweight, alcohol consumer or Asian or Asian British, Black or Black British and mixed ethnic groups. Though inconclusive and mainly limited by potential incomplete adjustment for major confounders and intrinsic disadvantages of a cross-sectional design, this study was the first quantifying the individual level dose–response relationship between E-iAsing,rice and hypertension risks and is consistent with previous studies on the limited associations of hypertension with low-level arsenic exposure from drinking water. Larger scale cohort studies are indicated to quantify the association but in any event it is likely to be weak

Electrical resistivity tomography determines the spatial distribution of clay layer thickness and aquifer vulnerability, Kandal Province, Cambodia

Despite being rich in water resources, many areas of South East Asia face difficulties in securing clean water supply. This is particularly problematic in regions with a rapidly growing population. In this study, the spatial variability of the thickness of a clay layer, controlling surface – groundwater interactions that affect aquifer vulnerability, was investigated using electrical resistivity tomography (ERT). Data were acquired along two transects, showing significant differences in the imaged resistivities. Borehole samples were analyzed regarding particle density and composition, and linked to their resistivity. The obtained relationships were used to translate the field electrical resistivities into lithologies. Those revealed considerable variations in the thickness of the clay layer, ranging from 0 m up to 25 m. Geochemical data, highlighting zones of increased ingress of surface water into the groundwater, confirmed areas of discontinuities in the clay layer, which act as preferential flow paths. The results may guide urban planning of the Phnom Penh city expansion, in order to supply the growing population with safe water. The presented approach of using geophysics to estimate groundwater availability, accessibility, and vulnerability is not only applicable to Kandal Province, Cambodia, but also to many other areas of fast urbanization in South East Asia and beyond

Use of lithium tracers to quantify drilling fluid contamination for groundwater monitoring in Southeast Asia

Drilling is widely used in groundwater monitoring and many other applications but has the inherent problem of introducing some degree of external contamination into the natural systems being monitored. Contamination from drilling fluid is particularly problematic for (i) wells with relatively low water flow rates which are difficult to flush; and for (ii) hydrogeochemical research studies of groundwaters hosted by incompletely consolidated shallow sediments, which are widely utilized as sources of drinking water and irrigation water across many parts of Asia. Here, we develop and evaluate a method that can be simply used to quantify the extent of drilling fluid contribution to a water sample either to optimize sample collection for reduced contamination, or to allow a correction for contamination to be made. We report the utility of lithium chloride tracers using both field and laboratory analytical techniques to quantitatively evaluate and correct for drilling fluid contamination of casing waters through an investigation of 15 sites in Kandal Province, Cambodia. High analytical errors limit the practicality and resolution of field-based lithium ion selective electrode measurements for purposes other than broad estimates of gross contamination. However, when laboratory analysis is integrated with the method (e.g. via inductively coupled plasma atomic emission spectrometry analysis), lithium tracers can provide a robust and accurate method for evaluating drilling-related contamination if appropriate samples are collected. Casing water is susceptible to contamination from drilling fluid which was shown to be significantly reduced within two to three well volumes of flushing but can still persist above background for greater than seven well volumes of flushing. A waiting period after drilling and prior to water sampling was shown to further decrease contamination due to dilution from the surrounding aquifer, particularly in more permeable wells. Contamination values were generally <3% for 34 monitoring wells across 15 sites after flushing a mean of 4.6 ± 3.8 well volumes, even when lithium-spiked water was directly injected during flushing to remove settled mud/debris. Operational issues can be encountered which can (i) lead to contamination being much higher than the mean if wells are highly unproductive and clay-dominated or (ii) lead to higher flushing volumes than the mean particularly in sandy areas where fine sand may enter the well screening. General correction factors have been provided for typical monitoring wells in poorly consolidated shallow aquifers in Southeast Asia, and examples provided for how to correct other groundwater data for contamination. For most analytes such as sodium or dissolved organic carbon (DOC), specific corrections may not be necessary for the typical magnitude of contamination encountered, particularly when the differences in concentrations between the drilling fluid and groundwater are relatively small. In the particular circumstance where drilling fluid may have much higher DOC than groundwaters, or vice versa with drilling fluid having much lower DOC than groundwaters in organic-rich alluvial sediments, corrections may still be necessary and significant. Similarly, for highly sensitive parameters such as 14C model age or other age-related parameters (such as tritium, chlorofluorocarbons (CFCs) or sulfur hexafluoride (SF6)), corrections can be significant in typical field scenarios particularly when contamination values are high and/or there is a large difference in age between groundwater and drilling fluid. The lithium method was verified with comparison to changes in concentration of a suite of representative and naturally occurring groundwater constituents as a function of well flushing from relatively low and high permeability groundwater monitoring wells to further illustrate the technique

Groundwater Arsenic-Attributable Cardiovascular Disease (CVD) Mortality Risks in India

From MDPI via Jisc Publications RouterHistory: accepted 2021-08-12, pub-electronic 2021-08-17Publication status: PublishedFunder: Natural Environment Research Council; Grant(s): NE/R003386/1Funder: Department of Science and Technology (India); Grant(s): DST/TM/INDO-UK/2K17/55(C) & 55(G)Cardiovascular diseases (CVDs) have been recognized as the most serious non-carcinogenic detrimental health outcome arising from chronic exposure to arsenic. Drinking arsenic contaminated groundwaters is a critical and common exposure pathway for arsenic, notably in India and other countries in the circum-Himalayan region. Notwithstanding this, there has hitherto been a dearth of data on the likely impacts of this exposure on CVD in India. In this study, CVD mortality risks arising from drinking groundwater with high arsenic (>10 μg/L) in India and its constituent states, territories, and districts were quantified using the population-attributable fraction (PAF) approach. Using a novel pseudo-contouring approach, we estimate that between 58 and 64 million people are exposed to arsenic exceeding 10 μg/L in groundwater-derived drinking water in India. On an all-India basis, we estimate that 0.3–0.6% of CVD mortality is attributable to exposure to high arsenic groundwaters, corresponding to annual avoidable premature CVD-related deaths attributable to chronic exposure to groundwater arsenic in India of between around 6500 and 13,000. Based on the reported reduction in life of 12 to 28 years per death due to heart disease, we calculate value of statistical life (VSL) based annual costs to India of arsenic-attributable CVD mortality of between USD 750 million and USD 3400 million

Geochemical compositional controls on DNA strand breaks induced in in vitro cell-free assays by crushed rock powders from the Panasqueira mine area, Portugal

From Springer Nature via Jisc Publications RouterHistory: received 2019-12-15, accepted 2020-06-24, registration 2020-06-24, pub-electronic 2020-07-09, online 2020-07-09, pub-print 2021-07Publication status: PublishedFunder: Saudi Arabia Cultural Bureau in London; doi: http://dx.doi.org/10.13039/100012363Abstract: DNA strand breaks are a common form of DNA damage that can contribute to chromosomal instability or gene mutations. Such strand breaks may be caused by exposure to heavy metals. The aim of this study was to assess the level of DNA strand breaks caused by µm-scale solid particles of known chemical composition with elevated heavy metals/metalloids, notably arsenic, using an in vitro cell-free DNA plasmid scission assay. These samples were incubated with and without H2O2 to see whether damage occurs directly or indirectly through the Fenton reaction. Levels of DNA damage in the absence of H2O2 were < 10%, but in the presence of H2O2, all samples showed higher levels of damage ranging from 10 to 100% suggesting that damage was being incurred through the Fenton reaction. Using bivariate correlation analysis and multiple linear regression, manganese oxide (MnO), sulphur (S), copper (Cu), and zinc (Zn) concentrations in the particulates were found to be the most significant predictors of DNA damage. The mechanism of this DNA damage formation has yet to be thoroughly investigated but is hypothesised to be due to reactive oxygen species formation. Further work is required to assess the extent of contribution of reactive oxygen species to this DNA damage, but this study highlights the potential role of chemistry and/or mineralogy to the extent and/or nature of DNA damage caused by particulates

A comparative assessment of dilution correction methods for spot urinary analyte concentrations in a UK population exposed to arsenic in drinking water

Spot urinary concentrations of environmental exposure biomarkers require correction for dilution. There is no consensus on the most appropriate method, with creatinine used by default despite lacking theoretical robustness. We comparatively assessed the efficacy of creatinine; specific gravity (SG); osmolality and modifications of all three for dilution correcting urinary arsenic. For 202 participants with urinary arsenic, creatinine, osmolality and SG measurements paired to drinking water As, we compared the performance corrections against two independent criteria: primarily, (A) correlations of corrected urinary As and the dilution measurements used to correct them - weak correlations indicating good performance and (B) correlations of corrected urinary As and drinking water As - strong correlations indicating good performance. More than a third of variation in spot urinary As concentrations was attributable to dilution. Conventional SG and osmolality correction removed significant dilution variation from As concentrations, whereas conventional creatinine over-corrected, and modifications of all three removed measurable dilution variation. Modified creatinine and both methods of SG and osmolality generated stronger correlations of urinary and drinking water As concentrations than conventional creatinine, which gave weaker correlations than uncorrected values. A disparity in optima between performance criteria was observed, with much smaller improvements possible for Criterion B relative to A. Conventional corrections – particularly creatinine - limit the utility spot urine samples, whereas a modified technique outlined here may allow substantial improvement and can be readily retrospectively applied to existing datasets. More studies are needed to optimize urinary dilution correction methods. Covariates of urinary dilution measurements still warrant consideration

Geostatistical model of the spatial distribution of arsenic in groundwaters in Gujarat State, India

From Springer Nature via Jisc Publications RouterHistory: received 2019-12-15, accepted 2020-06-24, registration 2020-06-24, pub-electronic 2020-07-11, online 2020-07-11, pub-print 2021-07Publication status: PublishedFunder: Engineering and Physical Sciences Research Council; doi: http://dx.doi.org/10.13039/501100000266; Grant(s): IAA Impact AwardAbstract: Geogenic arsenic contamination in groundwaters poses a severe health risk to hundreds of millions of people globally. Notwithstanding the particular risks to exposed populations in the Indian sub-continent, at the time of writing, there was a paucity of geostatistically based models of the spatial distribution of groundwater hazard in India. In this study, we used logistic regression models of secondary groundwater arsenic data with research-informed secondary soil, climate and topographic variables as principal predictors generate hazard and risk maps of groundwater arsenic at a resolution of 1 km across Gujarat State. By combining models based on different arsenic concentrations, we have generated a pseudo-contour map of groundwater arsenic concentrations, which indicates greater arsenic hazard (> 10 μg/L) in the northwest, northeast and south-east parts of Kachchh District as well as northwest and southwest Banas Kantha District. The total number of people living in areas in Gujarat with groundwater arsenic concentration exceeding 10 μg/L is estimated to be around 122,000, of which we estimate approximately 49,000 people consume groundwater exceeding 10 µg/L. Using simple previously published dose–response relationships, this is estimated to have given rise to 700 (prevalence) cases of skin cancer and around 10 cases of premature avoidable mortality/annum from internal (lung, liver, bladder) cancers—that latter value is on the order of just 0.001% of internal cancers in Gujarat, reflecting the relative low groundwater arsenic hazard in Gujarat State

Tritium tracers of rapid surface water ingression into arsenic-bearing aquifers in the Lower Mekong Basin, Cambodia

Arsenic (As) contamination of groundwaters in South and Southeast Asia is a major threat to public health in these areas. Understanding the source and age of the groundwaters is critically important to understanding the controls on As mobilization in these aquifers. Using tritium (3H) and noble gas (He and Ne) signatures, model groundwater ages and dominant hydrological controls were identified in a transect oriented broadly parallel to inferred groundwater flowpaths in Kandal Province, Cambodia in the lower Mekong Basin. Apparent 3H-3He ages showed that most groundwaters are modern (< 55 years), indicating relatively fast recharge even in the absence of large-scale groundwater abstraction. The age-depth relationship indicates a strong vertical component of groundwater flow and allows for recharge rates to be estimated. Vertical and horizontal flow velocities are heterogeneous and site-specific. The conceptual framework will be used to better understand As mobilization and subsequent transport with these and similar aquifers

EJVES vol 34, issue 2 (August 2007) - Spanish Translated Abstracts

Chronic exposure to arsenic (As) through the consumption of contaminated groundwaters is a major threat to public health in South and Southeast Asia. The source of As-affected groundwaters is important to the fundamental understanding of the controls on As mobilization and subsequent transport throughout shallow aquifers. Using the stable isotopes of hydrogen and oxygen, the source of groundwater and the interactions between various water bodies were investigated in Cambodia’s Kandal Province, an area which is heavily affected by As and typical of many circum-Himalayan shallow aquifers. Two-point mixing models based on δD and δ18O allowed the relative extent of evaporation of groundwater sources to be estimated and allowed various water bodies to be broadly distinguished within the aquifer system. Model limitations are discussed, including the spatial and temporal variation in end member compositions. The conservative tracer Cl/Br is used to further discriminate between groundwater bodies. The stable isotopic signatures of groundwaters containing high As and/or high dissolved organic carbon plot both near the local meteoric water line and near more evaporative lines. The varying degrees of evaporation of high As groundwater sources are indicative of differing recharge contributions (and thus indirectly inferred associated organic matter contributions). The presence of high As groundwaters with recharge derived from both local precipitation and relatively evaporated surface water sources, such as ponds or flooded wetlands, are consistent with (but do not provide direct evidence for) models of a potential dual role of surface-derived and sedimentary organic matter in As mobilization