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Drinking Water Criteria for Arsenic in High-Income, Low-Dose Countries: The Effect of Legislation on Public Health

  • Loren Ramsay
    Loren Ramsay
    Research Center for Built Environment, Energy, Water and Climate, VIA University College, 8700 Horsens, Denmark
    More by Loren Ramsay
  • , 
  • Mette M. Petersen
    Mette M. Petersen
    Research Center for Built Environment, Energy, Water and Climate, VIA University College, 8700 Horsens, Denmark
    Department of Geoscience, Aarhus University, 8000 Aarhus, Denmark
    More by Mette M. Petersen
  • , 
  • Birgitte Hansen
    Birgitte Hansen
    Geological Survey of Denmark and Greenland, 8000 Aarhus, Denmark
    More by Birgitte Hansen
  • , 
  • Jörg Schullehner
    Jörg Schullehner
    Geological Survey of Denmark and Greenland, 8000 Aarhus, Denmark
    Department of Public Health, Aarhus University, 8000 Aarhus, Denmark
    More by Jörg Schullehner
  • , 
  • Patrick van der Wens
    Patrick van der Wens
    Brabant Water, 5223 MA Hertogenbosch, The Netherlands
    More by Patrick van der Wens
  • , 
  • Denitza Voutchkova
    Denitza Voutchkova
    Geological Survey of Denmark and Greenland, 8000 Aarhus, Denmark
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  • , and 
  • Søren M. Kristiansen*
    Søren M. Kristiansen
    Department of Geoscience, Aarhus University, 8000 Aarhus, Denmark
    *Email for S.M.K.: [email protected]
    More by Søren M. Kristiansen
    Orcidhttp://orcid.org/0000-0003-3128-4061
Cite this: Environ. Sci. Technol. 2021, 55, 6, 3483–3493
Publication Date (Web):February 26, 2021
https://doi.org/10.1021/acs.est.0c03974
Copyright © 2021 American Chemical Society
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Abstract

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Due to the potential health risks at very low concentrations, the criterion for arsenic in drinking water has been debated. High-income, low-dose countries are uniquely positioned to follow WHO’s recommendation of keeping concentrations “as low as reasonably possible.” In this policy analysis, 47646 arsenic analyses from Denmark are used to follow the effect of lowering the national criterion from 50 to 5 μg/L. The first 3 years (2002–2004) following the criterion change, 106 waterworks were identified as noncompliant. An additional 64 waterworks were identified as noncompliant in the next 12 years (2005–2016). Of the 106 waterworks initially (2002–2004) aware of the violation, an average concentration drop from 6 to 3 μg/L was observed during a 6 year period following a lag time of 1 year. After this point, no further improvements were observed. Thirteen years after regulation was imposed, 25 of 170 waterworks were still in violation. The results suggest that legislation alone is insufficient to ensure better drinking water quality at some waterworks and that stakeholders’ drivers and barriers to change also play an important role. In an exploration of five legislation scenarios, this study showed that a criterion of 1 μg/L would require action by more than 500 Danish waterworks, with treatment costs from 0.06 to 0.70 €/m3. These scenarios illustrate that it can be technically feasible and affordable to lower the arsenic criterion below 5 μg/L in low-dose, high-income countries. However, more information is needed to apply a cost–benefit model, and comparative studies from other counties are warranted.

This publication is licensed for personal use by The American Chemical Society.

1. Introduction

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Globally, inorganic arsenic (As) in groundwater-based drinking water is a major public health risk. (1,2) Numerous epidemiological studies from all over the world confirm that high concentrations of As in drinking water increase the risk of lung, bladder, and skin cancer as well as other undesirable health effects. (3−8) As the body of evidence of negative health effects has grown, the World Health Organization (WHO) has lowered its guideline value accordingly, from 200 to 50 μg/L in 1963 and from 50 to 10 μg/L in 1993. (9) WHO designates the current value of 10 μg/L as provisional, recognizing that lower values may be difficult to achieve in areas where water treatment methods or analytical capabilities are limited. Therefore, WHO recommends that As concentrations in drinking water should be kept “as low as reasonably possible.” (7) This recommendation adheres to the precautionary principle, given the lack of knowledge regarding the mode of action for As-associated health outcomes (10) and the controversy over the shape of the dose–response curve at low concentrations and the existence of a dose threshold for inorganic As, below which exposures are not harmful. (11)
Many countries are currently in alignment with the provisional WHO guideline. Some countries, however, have a criterion below 10 μg As/L, referring to the precautionary principle. Examples include Denmark since 2003 (12) and New Jersey, USA, since 2006, (13) which have a criterion of 5 μg/L, and the water sector in The Netherlands since 2016, which pledged a voluntary limit of 1 μg/L on the basis of a societal cost–benefit analysis. (14,15) Other countries retain a criterion of 50 μg/L (if lower As source waters are not available) to discourage replacing noncompliant well water with contaminated surface water, which may present far greater health risks due to the presence of pathogens. (16)
Research often focuses on regions with high As levels and/or low income. (17−19) However, there are also health concerns about As in drinking water in regions with high income and low As levels. In these regions, two important questions may be raised. First, since lowering As concentrations below 10 μg/L may bring public health benefits, at what level should the reasonable (sensu WHO) As criterion for drinking water be set? Second, is there evidence that lowering the drinking water criterion through legislation actually results in a reduction of As concentrations at the tap or are other actions necessary to supplement the legislation?
Several studies in high-income, low-dose areas have previously shed light on the effect of regulatory intervention on water quality. As an example Nigra et al. (20) found that in users of public water in the US, urinary As levels decreased after the implementation of the current US maximum contamination level (10 μg/L), while no such decrease was found in unregulated private well users, suggesting a crucial role of drinking water regulation in reducing toxic exposures. A major barrier for reducing As in private well water in the USA has been the lack of legislation requiring testing. (21) The New Jersey Private Well Testing Act (PWTA) from 2002 requires well testing for As prior to real estate transactions and is especially interesting as New Jersey, like Denmark, has an As criterion of 5 μg/L. A survey with 670 New Jersey respondents (22) suggests that the PWTA did lead to significantly higher well testing rates, as intended. However, post-PWTA households were no more likely to take protective action. The authors suggest that future public health efforts will need to shift the emphasis from well testing to the actual behaviors that protect health (such as water treatment) and that real elimination of As exposure is elusive, due to deficiencies in technology and behavior in practice.
In 2006, the maximum contaminant level for As in the USA was lowered from 50 to 10 μg/L. A recent case study from the USA identified trends in the number of As violations for the period 2006–2017. (23) The results showed a maximum of 883 systems in violation in 2008, and this number dropped to 348 violations in 2017, suggesting that regulatory intervention may be a major factor in reducing human As exposure. None of the temporal decline, however, could be explained by documented water treatment, although under-reporting of treatment was a potential cause of this result. Interestingly, 1.8% of those systems in violation remained in violation for 12 years.
In The Netherlands, water quality data have shown complete compliance with the As guideline for drinking water (10 μg/L) for some time. (14) Since the voluntary lowering of the As guideline to 1 μg/L in 2016 by the governing board of VEWIN (the national association of water companies) no formal evaluation has taken place on the developments. However, waterworks at several utilities have made improvements, lowering As to <1 μg/L. The treatment methods of advanced oxidation and coprecipitation with iron salts were used. (14) In addition, research has been conducted on treatment methods and ways to enhance regular treatment processes to improve As removal. (14,24) The Dutch situation indicates the possibility of lowering As levels in high-income countries even without formal legislation but purely through decision making based on the precautionary principle.
The work presented here is a policy analysis of As in drinking water, based on a case study from Denmark, a high-income, low-dose country. In a longitudinal study of waterworks with As challenges, the work examines the effect of legislative intervention (i.e., lowering the criterion from 50 to 5 μg/L in 2003) as well as the role of other prerequisites for change with regard to water quality. In addition, this analysis uses scenarios to determine whether lowering the As criterion below the current 5 μg/L can be technically feasible and affordable in high-income, low-dose countries.

2. Case Study: Denmark

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For several reasons, Denmark is well-suited for a case study of lowering exposure to As in a high-income, low-dose country. First, more than a decade has passed since the As drinking water criterion was lowered, giving adequate time for a follow-up study. Second, 100% of the drinking water in the country comes from groundwater sources, which are more susceptible to natural As contamination than surface waters. Third, 97% of the Danish population are served by public waterworks. (25) Finally, a very comprehensive set of water quality monitoring data is available for all public waterworks and public supply wells. (26)
In Denmark, natural, geogenic sources are the origin of As contamination in groundwater. Often, aquifers used for drinking water are in a chemically reduced state, which causes the dissolution of iron oxides in the sediments and the release of the As that is bound to the oxides. (27) The three most prolific drinking water aquifer types are composed of quaternary sand, tertiary sand, and Paleogene or Cretaceous limestone. Concentrations of As above the 5 μg/L criterion are found in all three aquifer types in some geographical areas. (28)
Figure 1 shows the spatial distribution of public waterworks with As analyses of finished water from the study period (2002–2016), as well as the location of public water supply wells with As analyses of groundwater. Private wells and private waterworks supplying less than 10 houses are not included in this study and are not shown on Figure 1. Public waterworks identified as noncompliant during the first part of the study period (2002–2004) are shown in red and were followed over time in this study.

Figure 1

Figure 1. Location of public waterworks and public water supply wells with As data for the study period 2002–2016. Waterworks identified during the 2002–2004 period as noncompliant were used in the follow-up study and are shown here as red triangles.

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2.1. Danish Policy Decisions

On September 21, 2001, Danish legislation announced the lowering of the drinking water criterion for As. (29) The new criterion was to be 5 μg/L for water leaving the waterworks and 10 μg/L for water at the consumer tap. This unusual double criterion was chosen due to uncertainty as to whether additional As may be released by housing installations such as water faucets, as had been shown to be the case for nickel. The criterion of 5 μg/L is below the WHO provisional guideline of 10 μg/L and follows the appeal by WHO to obtain concentrations “as low as reasonably possible”. Waterworks were allowed 27 months to prepare for needed changes before the new criterion became enforceable December 25, 2003. In 2018, a single criterion of 5 μg/L at the consumer tap replaced the former double criterion. (12)
In December 2005, the Danish EPA adopted the gold standard (30) for acceptable excess lifetime cancer risk of one per million for drinking water, which is more stringent than the WHO standard. (31) In addition, it was decided that precautionary protection should be extended to particularly vulnerable persons. (32,33) Clearly, the Danish As criterion of 5 μg/L does not align with the adopted gold standard.

2.2. Monitoring

The monitoring of As concentrations in Danish groundwater and drinking water has been mandatory since January 1, 2002. (34) Wells are generally purged with submersible pumps prior to sampling unless they are already in operation. Chemical analyses were performed by accredited laboratories, and the analytical method used was almost exclusively ICP-MS during the study period. The results were confirmed by data owners prior to entry into a national database. Groundwater from water supply wells must be sampled at least once every 4 years, while the produced drinking water must be sampled at least every other year at waterworks serving 10 or more households.
Groundwater and drinking water analyses are publicly available in the national well database named “Jupiter”, which is the Danish warehouse for information regarding borehole lithology, well construction logs, waterworks information, chemical and microbiological analyses, etc. (26) For all As measurements from the study period, the data were downloaded from Jupiter and underwent a rigorous quality control procedure. Erroneous and potentially erroneous results were removed due to the following problems: (1) groundwater or backwash water samples mislabeled as drinking water samples, (2) lacking or improper concentration units, (3) detection limits above the criterion or above the actual measurement, and (4) clear outliers as judged from a time series graph.
This resulted in a total of 47646 As analyses, including samples of both the finished drinking water (n = 25827) and groundwater (n = 21819), nationwide within the study period of 2002–2016. These drinking water analyses stem from 3125 public waterworks, while the groundwater analyses stem from 6133 public wells used by these waterworks to abstract groundwater for drinking water purposes (Figure 1), a number of which were closed during the study period. This large number of waterworks for a relatively small country illustrates that Denmark has a decentralized water supply structure. It should be noted that drinking water for about 3% of the population comes from approximately 50000 private wells, each supplying <10 households. (35,36) Although the risk caused by As in these wells is of concern, they are excluded from this study (hence, not shown on Figure 1) due to the paucity of monitoring data for As.
Figure 2 shows the concentration distribution as a frequency plot of these 47646 As analyses in samples from both Danish groundwater supply wells and finished drinking water for the period 2002–2016. Concentrations in the groundwater samples range up to 170 μg/L, while concentrations in the drinking water samples range up to 36 μg/L. Median values for groundwater and drinking water are only 0.96 and 0.54 μg/L, respectively. However, a total of 31% of the drinking water samples from the study period are above 1 μg/L and 3% are above the 5 μg/L criterion. Although concentrations above 1 μg/L may be of concern, these results place Denmark in the category of “low-dose” countries. The separation between the curves for groundwater and drinking water (Figure 2) indicates that some As is removed in the water treatment process and that supply wells with lower As concentrations are favored for drinking water production.

Figure 2

Figure 2. Arsenic concentrations in Danish groundwater (n = 21819) and drinking water (n = 25827) from the Danish national database Jupiter. All results are from samples collected in the period 2002–2016 from active supply wells (n = 6133) and active waterworks (n = 3125), respectively. Waterworks serving <10 households are excluded (ca. 3% of the population).

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3. In the Wake of Legislation

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This section looks at changes that occurred at Danish waterworks in the wake of legislation which lowered the drinking water criterion from 50 to 5 μg/L in 2003.

3.1. Identification of Noncompliant Waterworks

Waterworks were flagged as noncompliant if one or more drinking water samples collected during the 15 year study period (January 1, 2002–December 31, 2016) showed As >5 μg/L. In this way, all waterworks even occasionally above the criterion were identified, regardless of whether or not noncompliance was apparent at the beginning of the study period. This definition may differ somewhat from the waterworks’ own interpretation.
This exercise identified 883 drinking water samples with As >5 μg/L during the study period. These samples represented 170 waterworks which were flagged as noncompliant. During the first 3 years of the study period (2002–2004), 106 of the 170 had been identified as noncompliant, while the remaining 66 waterworks were not in violation until later in the study period (2005–2016). In this study, the 106 waterworks which were in violation early were followed over time to determine the effect of the legislative intervention. This large number of waterworks presents an excellent opportunity to analyze the varied responses of the utilities to the noncompliance situation and to understand the mechanisms in play.

3.2. Effect of Legislation on As Concentration

In the wake of the new criterion going into effect, one would expect concentrations of As in drinking water to drop over time. Such a drop has previously been observed with, for example, As in the US and nitrate worldwide. (23,36,37)Figure 3 shows a time series for the 106 noncompliant waterworks that were in violation early in the study period. The figure highlights the mean annual arsenic concentrations for each waterwork (Y1 axis and blue points) as well as the number of noncompliant waterworks (Y2 axis and red points).

Figure 3

Figure 3. Mean annual arsenic concentrations in drinking water for each waterworks (blue points) and number of waterworks identified as noncompliant (red points), on the basis of the 106 waterworks initially in violation for the study period 2002–2016. Boxplot: fifth and 95th percentile (lower and upper whiskers), 25th and 75th percentile (bottom and top of box), median (thick line), with a color change on the bars that follows the boxplots. The horizontal displacement of As concentration data points within each bar plot is for visualization purposes only. Below the bars: n1, number of the 106 noncompliant waterworks reporting at least one As concentration that year; n2, number of the 106 waterworks identified as noncompliant that year.

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A visual inspection of Figure 3 shows that the median of As concentrations (thick line) drops from approximately 6 μg/L to 3 μg/L during the study period. The individual annual mean As concentrations (blue points) also show a decrease. This is supported by linear regression, which shows a slope of –0.38 μg/L per year (95% confidence interval from −0.43 to −0.33). It should be noted that waterworks do not necessarily report As concentrations annually and that annual means may be calculated from different numbers of As analyses.
Likewise, the number of waterworks that reported noncompliant results (red points) dropped during the study period from a high of 76 in 2004 to a low of 6 in 2015. This is also supported by linear regression, which shows a slope of −4.3 waterworks per year (95% confidence interval from −5.4 to −3.2). Using Local polynomial regression fitting, (38,39) a higher rate of change is observed in the middle part of the study period (see Figure 3). This sigmoidal curve indicates that the response at the utilities began to bear fruit only after a lag time (in addition to the 27 month grace period between the announcement and the new criterion going into effect) of about 1 year (2004), that improvements were made exclusively during a 6 year period, 1 to 7 years after legislation went into effect (2005–2010), and that no further improvements were made when most individual waterworks had become compliant (2011–2016). A time series such as this in which a trend is interrupted by an intervention that separates a preintervention from a postintervention period is referred to as an interrupted time series. (40)

3.3. Measures Implemented to Improve Water Quality

Corrective measures implemented at the noncompliant waterworks to improve the drinking water quality with respect to As were determined in this study by interviewing the utilities by telephone. The results showed that a variety of measures have been implemented (see Figure 4).

Figure 4

Figure 4. Corrective measures implemented in the period 2002–2016 to improve drinking water quality for As. The figure includes the 106 waterworks that were noncompliant in 2002–2004. “Other actions” include abolishing the reaction basin between aeration and filtration steps, changing the screen depth in the well, and changing the aeration method.

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The most frequently chosen corrective measure was abandonment. In this measure, a well or wells with high As concentrations are closed. In most cases, this meant closing the treatment plant (26.4%). A prerequisite for closing a treatment plant is a neighboring waterworks with the capacity to step in and produce the needed quantity of water. In the final 1.9% of the abandonment category, a well is closed, with other wells in the wellfield taking up the slack. The second most frequently chosen corrective measure was implementation of advanced water treatment (19.8%).
The simplest corrective measure is wellfield management, which may be implemented in wellfields with multiple wells. This measure was chosen by 7.5% of the noncompliant waterworks. It includes several variations: (1) simple dilution in which water from wells with high and low As are abstracted simultaneously to allow for mixing, (2) abstraction that favors—if capacity concerns allow it—wells with lower As over wells with higher As, and (3) abstraction that gives preference to well combinations in which wells with high As are paired with wells with high iron. Wellfield management can typically be applied immediately for insignificant costs. However, the flexibility of the wellfield may be compromised by these variations, especially if other constraints with respect to water quality, water quantity, or energy use are already in existence. Abstraction changes may also change flow patterns in the aquifer, mobilizing As or other contaminants from one part of the aquifer to another. It should be noted that using a simple dilution approach does not necessarily reduce the mass of As sent to consumers but simply redistributes it, resulting in even concentrations rather than concentrations that are higher at times and lower at other times. If a linear dose–response relationship is assumed, simple dilution will not make an overall difference in the number of adverse outcomes, although recent studies have suggested that assuming a linear nonthreshold carcinogenic response may be inappropriate for inorganic As. (41,42) Although inexpensive, simple dilution is therefore not fully in line with WHO’s recommendation of achieving concentrations as low as possible. Finally, 3.8% of the noncompliant waterworks chose to improve drinking water quality by finding a new groundwater source with lower As levels or higher iron levels. This often requires hydrogeological investigations, well drilling, and the laying of new raw water pipelines.

4. Exposure Reduction

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To assess the health benefits of lower As exposures, one must select the most sensitive toxicological end point. Since inorganic As in drinking water is a multisite human carcinogen, there are several end point candidates, where lung and bladder cancer are best characterized and are currently thought to be the most sensitive. (3,5) Due to the lack of studies in low-dose settings, high-dose epidemiological data must be extrapolated to the low doses that are relevant for this study. To do this, the shape of the dose–response curve (linear, sublinear, or supralinear) at low doses must be assumed and a decision must be made whether to include a threshold value below which no detrimental effects develop. In lack of evidence to the contrary, one could follow environmental custom by invoking the precautionary principle and assume a linear dose–response curve with no lower threshold value. (5) Using the linear dose–effect model and the accepted level of risk of one per million due to the consumption of drinking water as mentioned in section 2.1, the maximum level of As should be 0.004 μg/L. (15) Under these assumptions, any reduction in As concentrations will lead to a smaller risk. However, it should be emphasized that this approach is based on conservative modeling because of the lack of proven safe threshold values for exposure to inorganic As.
It should be noted that exposure to inorganic As comes from food as well as drinking water, and a risk assessment of drinking water criteria must take this into account. Meacher et al. (43) found that food was the greatest source of inorganic As intake in the adult US population, while drinking water was the second greatest source. Thus, at increasingly lower As concentrations in drinking water, exposure from drinking water becomes less important to the total exposure while the diet becomes increasingly important. (44) Therefore, no scenarios in which the drinking water criterion is lowered below 1 μg/L are explored in this policy analysis paper.
Several approaches for estimating the potential health benefits of lowering As exposure are possible, such as a three-step approach described by van der Wens et al. (15) In the Danish case described here, an estimation of potential health benefits could be composed of determining exposure patterns in the population before and after As concentrations are lowered, converting exposure to annual incidence: i.e., the risk of becoming ill with a selected end point during a given year. However, several links in this chain are weak due to limitations of the data set. Quantifying potential health benefits and health-related economic benefits of lower exposures is in our view dubious, as long as the shape of the relationship between As and adverse health outcomes in the lower range has not been established. (11)
To illustrate the effects of lowering the As drinking water criterion, five scenarios were defined for the purpose of estimating the health benefits using drinking water analyses from 2015 to 2016. Scenario A assumes that all waterworks that were noncompliant in the last 2 years of the study period reach 100% compliance with the current 5 μg/L criterion. Scenarios B–E assume that waterworks lower their As levels to obtain compliance with new drinking water criteria of 4, 3, 2, and 1 μg/L, respectively (see Table 1). Waterworks were flagged as noncompliant if one or more drinking water samples collected during the study period (January 1, 2002–December 31, 2016) showed an As concentration greater than the criterion of the scenario in question. Table 1 gives the number of noncompliant waterworks according to the different scenarios. Scenario E shows that 26.7% of all Danish waterworks would be noncompliant if the criteria were lowered to 1 μg/L.
Table 1. Scenarios Showing the Number of Waterworks in Violation According to Different Scenarios for Lowering the Drinking Water Criterion for Arsenic
  noncompliant waterworks 
 scenario: from 2015–2016 level down to (μg As/L)N%avolume (1000 m3/year)population exposed above criterion: no. (in 1000)
A5251.2210054
B4562.74000103
C31135.59300240
D223711.628500735
E154626.7581001500
a

Based on the total number of waterworks with As measurements in 2015–2016 (N = 2045).

The size of each noncompliant waterworks was then taken into account. To this end, the abstracted volume for the noncompliant waterworks was summed in m3/year (see Table 1). We estimated the number of exposed persons by assuming the population served by each waterworks is proportional to the waterworks’ abstraction volumes. Clearly, this straightforward approach ignores the fact that the production/population ratio naturally varies somewhat between waterworks, depending on variations in water used by industry etc. in the service area of the utility. Notably, in scenario A one single waterworks accounts for approximately 33% of the abstracted volume. This waterworks had one noncompliant As analysis in the period 2015–2016 but three compliant analyses. Table 1 shows that the number of people potentially affected by noncompliant water increases exponentially for each μg/L that the criterion is lowered and that ∼1.5 million (27%) of the Danish population in 2015–2016 received drinking water ≥1 μg As/L.

5. Drinking Water Treatment

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Drinking water treatment is one measure that can be used to ensure lower As concentrations in drinking water. According to Larsen et al., (45) however, treatment should only be considered after exhausting all possibilities for obtaining a better source of water.

5.1. Treatment Methods in Denmark

Internationally, a variety of treatment methods are commercially available for the removal of arsenic from drinking water (24,46) and additional methods are being developed. The method selection depends on factors such as system size, raw water quality, treatment goals, method experience, and costs. Twenty of the 106 noncompliant waterworks followed in this study reported advanced water treatment as the corrective measure. These waterworks were relatively small, ranging in size from 9000–300000 m3/year with a median of 65000 m3/year. Only two treatment methods were used in Denmark. (47)
In one method used by 13 systems, dissolved Fe(II) or Fe(III) salt solutions (IS) are dosed just prior to biofiltration. (24) Since these solutions are extremely acidic, care must be taken in handling the chemicals to prevent personal injury and corrosion. Therefore, this method is more suitable for larger systems (for example >100000 m3/year) with trained personnel. In Denmark, heterogeneous iron removal on media grains (48) is used rather than coagulation prior to filtration. Oxidation and removal of As and iron occur simultaneously on the biofilters. It should be noted that iron dosage and As removal do not have a linear relationship. Approximately 50% of a low inlet As concentration is removed by 1 mg/L iron, while only an additional 20% of As is removed by doubling the iron dosage. (45) This means that systems with naturally low concentrations of iron in the raw water stand to gain the most when they use the IS method.
In the other method used by 6 systems, granular iron oxide adsorption media (AM) is placed in a pressure filter as a final polishing step just prior to the clearwater tank. This step is preceded by biofiltration, which typically removes iron, manganese, ammonium, and some As as well as oxidizes the remaining As(III) to As(V) even though no chemical oxidants other than oxygen are added. This method is suitable for smaller systems (for example <300000 m3/year), due to the ease of operation. Once the AM is in place, only infrequent backwashes are required until the AM must be replaced or regenerated. (49) This method results in very low initial As concentrations in the treated water, followed by increasing concentrations until the target is reached, at which point the AM must be replaced. The higher the raw water concentration and the lower the drinking water target, the shorter the lifespan of the AM, which is measured in bed volumes.
Including the first permits from 2004, more than 40 permits regarding water treatment for As have been issued in Denmark. (50) In connection with permitting, authorities may be faced with the conflict of maintaining a decentralized water supply and ensuring utilization of the cleanest water sources available. In one case, a permit application was refused, with the authority citing that the utility could be abandoned and connected to a neighboring utility with better water quality. (50)

5.2. Estimation of Treatment Costs

In the study period, introduction of arsenic treatment at the waterworks was often based on a rough estimate from a single contractor for a single method or even handled by the utility internally. Cost information from the small waterworks of this study was of poor quality or was misleading (for example due to overly optimiztic estimates of AM lifespan). Therefore, a cost estimation tool was utilized to estimate treatment costs for scenarios in which As is removed from 5 μg/L to lower target values at a fictive waterworks producing 100000 m3/yr. Background material for the tool included more recent contractor offers and calculation of AM bed volumes from waterworks with frequent monitoring and 10 years of operational data.
Capital costs included pressure filters, chemical feed systems (IS method), installation, and running-in. Costs for constructing additional building space at the waterworks, was excluded as this has generally not been required in Denmark. An additional filter in series just prior to the clearwater tank was assumed to be necessary (IS method) to a achieve low target concentration. Capital costs were amortized over 15 years. Operation and maintenance (O&M) costs included media replacement (AM method), chemical costs (IS method), additional monitoring, and labor/maintenance. Minor costs for any additional backwashing were excluded.
Calculations using the cost estimation tool show that the AM method costs 0.20–0.70 €/m3. Of these costs, 80% or more were due to the expense of AM replacement. The range in costs was due to the range in the number of treated bed volumes prior to media replacement. Bed volumes were seen to decrease nearly linearly from 120000 (for reducing As concentrations to 5 μg/L from slightly higher concentrations) to 24000 (for reducing As concentrations from 5 to 1 μg/L). The IS method costs were 0.06–0.10 €/m3. Here, the range was largely due to capital costs and whether an additional pressure filter for dosing iron was required.
A cost study from the USA (51) for the period 2004–2010 included 28 small AM systems. This study showed that O&M costs for the 15 systems that replaced their exhausted media during the study period ranged from 0.61 to 22.05 USD/1000 gal (approximately 0.11–4.31 €/m3) for raw water with 13–88 μg/L As. The AM costs in our paper are within this range, even though the two studies varied with respect to inlet and target As concentrations. Both the American study and our study show that O&M costs for AM far outweigh capital costs when capital costs are spread over 15 years.

5.3. Affordability

In comparison to other countries, drinking water costs in Denmark are high, partly because there are no subsidies and all related costs including groundwater protection costs and taxes are paid for by the consumer. Households pay an average of 259 €/yr for drinking water, assuming a per capita consumption of 105 L per day, 2.15 persons per household, and a cost of 3.14 €/m3. (52) The most common metric for determining household affordability for drinking water is to compare the cost of water to the median household income (MHI). Despite its shortcomings, such as its binary nature (affordable or not affordable) and the disregard of households with incomes below the median, this metric was chosen for our study. The MHI for Denmark is 37000 €/yr, (53) whereby typical water costs are approximately 0.7% of the MHI, well below the widely used threshold of 2% or 2.5%. (54)
The maximum cost for advanced water treatment for As was previously estimated in this study to be 0.70 €/m3. This equals approximately 58 €/yr per household, which is 21% of the total water costs or an incremental increase of just 0.16% of the MHI metric. On the basis of the above assumptions, it can be concluded that utilizing advanced water treatment to remove As from drinking water to a criterion below 5 μg/L is technically feasible and affordable in Denmark.

6. Discussion

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The data set behind this policy analysis has some limitations: analyses of drinking water from private wells are not included, the monitoring frequency is generally less than annual, no Danish studies of health outcomes related to the <10 μg/L level of exposure have been made, and information on the cost of As treatment methods at individual utilities is not available in this study. Strengths of the data set include that monitoring results are available at the individual waterworks level, that there is no under-reporting since reporting to the database is automated (in a study by Foster et al. (23) it was estimated that 26–38% of health-based violations were not reported or were inaccurately reported), and that we have a high response from violating waterworks regarding corrective measures (75.5%) (see Figure 4).
The data set shows that quality improvements occurred over a 6 year period (see Figure 3). It is possible that this period involves two different sets of corrective measures used by the waterworks: i.e., the easy measure of wellfield management in the early part of the period and more difficult measures such as advanced water treatment or even closing the waterworks that require investment and/or permission by authorities in the later part of the period. The water quality improvement period may also be separated into two parts, due to a major structural reform of Danish municipalities in January 2007 which changed the permitting authority for advanced water treatment applications. It is hence possible that water treatment projects were simply put on hold for long periods prior to and after this change. At the end of the study period, a triennial data window from 2015 and 2016 showed that 25 waterworks across Denmark were noncompliant, 13 years after the new criteria went into effect. It should be noted that many of these waterworks were not among the 106 who were in violation from 2002 to 2004 and were included in our longitudinal study. As the waterworks in the Danish data set have different monitoring frequencies, with a 4 year interval as a maximum for smaller waterworks, a narrower time window would exclude potential violators among the smaller waterworks in this follow-up study, while a broader window would have biased comparisons with Foster et al., (23) who also used triennial data from the US.

6.1. Precautionary Principle

As awareness of the public health risk from As grew, the desire to improve drinking water quality arose. However, effectuating an improvement in water quality on a national scale is by no means a trivial exercise. To understand how the As concentrations in Danish drinking water were improved in the past and may be further improved in the future, it is instructive to look at the precautionary principle.
Since the inclusion of the precautionary principle in the Rio Declaration, (55) it has become customary to take action to reduce health risks, even when scientific uncertainty exists. European Union policy on the environment is explicitly based on the precautionary principle, while Danish legislation is not as explicit. Denmark has incorporated the precautionary principle through terms (translated from the Danish) such as “likelihood” and “suspicion” of risk. (50)

6.2. Leaders and Laggards

The new Danish drinking water criterion for As of ≤5 μg/L went into effect on December 25, 2003. Total compliance, however, was not immediately achieved nor is it achieved at the present. An adequate response to more stringent legislation requires the will and ability to transform regulation into implementation. This regulation to implementation process has previously been the object of studies. The wide variety of responses from different water utilities seen in this work gives us a clue that more is going on here than simple attempts at compliance and that some utilities likely face much greater challenges than others. As observed by Gunningham et al. (56) in their book Shades of Green, there will always be leaders and laggards. In other words, some utilities will quickly comply to more stringent criteria and may actually exhibit “overcompliance”: i.e., achieve As concentrations even lower than those required by law. Laggards, on the other hand, have a tendency only to respond when threatened by sanctions, only after a significant time lag and by barely meeting the legal criteria with no overcompliance. In some instances, laggards are hampered by circumstances beyond their control, such as a widespread, poor-quality groundwater resource.

6.3. Stakeholders’ Drivers and Barriers

To understand these different responses to the same legislation, it is valuable to focus separately on the individual stakeholders engaged in the goal of improving drinking water quality. These stakeholders are composed of undercharacterized flesh and blood individuals, each with their own ethics, drive, and experience, set in a context of family, friends, colleagues, and a need for job satisfaction. (57) Regulations are therefore never simply “impersonally implemented or blindly executed” by organizations. (58) Below, three categories of stakeholders are discussed.
First, the “regulated party” is the water utility. Before implementation can begin, individuals in the utility must have an awareness not only of the new criteria but also of its importance so that the implementation task can be prioritized above other tasks calling for attention. Dialogue with utilities through more than a decade of teaching professional training courses on water quality indicates a general change in attitude during the study period (59) from indifference to serious awareness of the new As regulations, a recognition of the geogenic source of As in groundwater, and an understanding of the potential health consequences of As in drinking water. Once prioritized, the knowledge level of various solutions had to be increased through investigation and training. This presupposes that mature treatment technologies were available, which was not the case. Technology was further developed, and experience was collected in guidance manuals. Armed with awareness, mature technology and ethics, the “regulated party” then had to balance costs with risks to decide whether to use an overly compliant or barely compliant approach. Although waterworks in Denmark enjoy a natural monopoly and are not-for-profit organizations by law, water prices are nonetheless regulated. Therefore, there are limits to the use of expensive water treatment measures and a reluctance to increase consumer costs constitutes a barrier to compliance with drinking water criteria (56) and can reduce or delay the effect of legislation that lowers drinking water criteria.
Second, the “regulators” are governmental legislators and their enforcement agencies. In Denmark, the enforcement of drinking water quality regulations is assigned to the municipalities. (12) The regulation of drinking water criteria is based on so-called “command-and-control legislation” rather than regulation through incentives. Utilities are required to monitor As concentrations, and municipalities are required to follow up in noncompliance situations, wielding powerful tools including the legal framework to ultimately close the waterworks. Kasdorp (60) explored the realm of enforcement efforts that are not directly dictated by the letter of the law. These so-called “Regulatory Interventions Beyond the Law” (RIBL) were placed in a typology based on a range of “increasingly expansive discretionary attitudes of regulators towards their enforcement mandate”. These varying parallel attitudes among regulators contribute to defining the leaders and the laggards. The authors’ own experience from the period in question was a frequent reluctance on the part of the enforcing party to push for implementation, including dragging out the permitting process for advanced water treatment.
Third, the “third-party stakeholders” include the news media, consumers, nongovernmental agencies, and any other interest group related to drinking water quality. In 2009, the Danish trade magazine “Ingeniøren” wrote a watchdog journalism article about waterworks not yet in compliance with the new criteria for As in drinking water, 5 years after the legislation went into effect. (61) This article—along with follow-ups in various national media (62)—likely raised consumer awareness and public awareness in general. This put public pressure on the collective set of expectations or the social license of waterworks. Gaining attention in the past two decades, social license is an unpredictable, dynamic, and subjective force, which may also function as a powerful driver for going beyond compliance. (63)
The above discussion exemplifies that numerous drivers (which prompt corrective action) and barriers (which hinder corrective action) may exist for the different stakeholders. A nonexhaustive list of these is given in Table 2. Further studies would be needed to determine the relative importance of each of these.
Table 2. Potential Corrective Action Drivers and Barriers in Regard to Lowering As Concentrations in Drinking Water
stakeholderdrivers (D)/barriers (B)description
all partiesawareness (D)awareness of drinking water criteria and health risks associated with inorganic arsenic
regulated partypride in product (D)desire to conduct the business of drinking water production according to principles of right and wrong
 training (B)lack of knowledge of advanced water treatment methods to remove arsenic from drinking water
 maturity of technology (B)lack of commercial availability of components and service; experience with operational practices regarding drinking water treatment for arsenic
 costs (B)costs of implementing advanced water treatment must not exceed price ceilings and must be included in considering a course of action
regulatorcommand-and-control legislation (D)lowering the drinking water criteria through legislation reduces public health risks if the legislation results in waterworks out of compliance; if a new criterion does not require action, it is sham legislation
 regulatory intervention beyond the law (RIBL) (D)regulators take an expansive view of their enforcement mandate, putting effort into areas that are not strictly enforceable
third-party stakeholderwatchdog journalism (D)informs the public of topics in a manner that invokes a sense of dissatisfaction and a desire for change.
 social license (D)public pressure to improve water quality through organizations and the media

6.4. Looking Ahead

This Danish case study shows that the existing Danish policy regarding the acceptable level of risk is not upheld by the current concentrations of As in drinking water. The study also shows that lowering the criterion coincided with a significant reduction in As concentrations among the noncompliant waterworks, even though a 1–7 year lag time was required for the response and even though the response did not result in 100% compliance.
In the Introduction, the question of whether the As criteria in drinking water should be lowered further was raised. This type of question separates us from the descriptive realm of science to the prescriptive realm of the decision maker. Decisions involve complex interactions among academic disciplines such as natural sciences (geology, chemistry), social sciences (economics, education), and humanities (politics, ethics). Each discipline is encumbered with its own uncertainties. Multiple conflicting criteria must be examined before a course of action can be selected, as this global threat demands multisector solutions. (16)
Scenarios of future legislation lowering the As criterion even further suggest that significant public health advantages are only gained if the criterion is lowered to a level which throws a large percentage of waterworks into noncompliance. Costs of this action appear to be affordable in a Danish context, and the necessary water treatment appears to be technically feasible.
This study provides input to other countries with high income and low As concentrations in drinking water. We speculate that, whether a new criterion is adopted through legislation or on a voluntary basis in the industry, leaders and laggards will be present and an implementation period will be necessary. We speculate further that, to achieve a successful risk reduction, multiple drivers and barriers must be addressed as a supplement to promulgating stricter legislation, in both low- and high-income countries.

Author Information

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  • Corresponding Author
  • Authors
    • Loren Ramsay - Research Center for Built Environment, Energy, Water and Climate, VIA University College, 8700 Horsens, Denmark
    • Mette M. Petersen - Research Center for Built Environment, Energy, Water and Climate, VIA University College, 8700 Horsens, Denmark;  Department of Geoscience, Aarhus University, 8000 Aarhus, Denmark
    • Birgitte Hansen - Geological Survey of Denmark and Greenland, 8000 Aarhus, Denmark
    • Jörg Schullehner - Geological Survey of Denmark and Greenland, 8000 Aarhus, Denmark;  Department of Public Health, Aarhus University, 8000 Aarhus, Denmark
    • Patrick van der Wens - Brabant Water, 5223 MA Hertogenbosch, The Netherlands
    • Denitza Voutchkova - Geological Survey of Denmark and Greenland, 8000 Aarhus, Denmark
  • Notes
    The authors declare no competing financial interest.

Acknowledgments

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The authors acknowledge Silhorko Eurowater, Stilling, Denmark, for supplying data regarding the cost of water treatment for arsenic. Four anonymous reviewers and James Mihelcic (Associate Editor) are thanked for their constructive comments.

References

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    Regularly ingesting water with elevated As increases adverse health risks. Since Sept. 2002, the NJ Private Well Testing Act (PWTA) has required testing untreated well water for As during real estate transactions in 12 counties. Its implementation provides an opportunity to study the effects of policy intervention on well testing and treatment behavior. We analyze results of a survey mailed to 1943 random addresses (37% response), including responses from 502 private well households who purchased their homes prior to PWTA commencement and 168 who purchased after. We find the PWTA has significantly increased arsenic testing rates in an area where 21% of wells contain As above the 5 μg/L NJ drinking water std. The PWTA has allowed identification of more wells with As (20% of post-PWTA vs. 4% of pre-PWTA households) and more treatment for As (19% of post-PWTA vs. 3% of pre-PWTA households). Such an Act is a partial answer to significant socioeconomic disparities in testing obsd. among households for whom it is not required. Addnl. residents purchasing homes since 2002 are younger and disproportionately more likely to have children in their household (60 vs. 32%), a priority group given their particular vulnerability to effects of As. Despite more wells tested under the PWTA, post-PWTA well owners forget or misremember As test results more often, are more likely to report not knowing what kind of treatment they are using, and are not reporting better maintenance or monitoring of their treatment systems than pre-PWTA households. This suggests serious challenges to reducing As exposure remain even when testing is a requirement. Only a fraction of wells have been tested under the PWTA due to the slow pace of housing turnover. We recommend more public resources be made available to support private well testing among socially and biol. vulnerable groups.
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    Foster, S. A.; Pennino, M. J.; Compton, J. E.; Leibowitz, S. G.; Kile, M. L. Arsenic Drinking Water Violations Decreased across the United States Following Revision of the Maximum Contaminant Level. Environ. Sci. Technol. 2019, 53 (19), 11478– 11485,  DOI: 10.1021/acs.est.9b02358
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    Arsenic Drinking Water Violations Decreased across the United States Following Revision of the Maximum Contaminant Level
    Foster, Stephanie A.; Pennino, Michael J.; Compton, Jana E.; Leibowitz, Scott G.; Kile, Molly L.
    Environmental Science & Technology (2019), 53 (19), 11478-11485CODEN: ESTHAG; ISSN:0013-936X. (American Chemical Society)
    Arsenic poses a threat to public health due to widespread environmental prevalence and known carcinogenic effects. In 2001, the US EPA published the Final Arsenic Rule (FAR) for public drinking water, reducing the max. contaminant level (MCL) from 50 to 10 μg/L. We studied impacts of the FAR on drinking water violations temporally and geog. using the Safe Drinking Water Information System. Violations exceeding the MCL and the population served by violating systems were analyzed across the conterminous US from 2006 (onset of FAR enforcement) to 2017. The public water system violations declined from 1.3% in 2008 to 0.55% in 2017 (p <0.001, slope = -0.070), and the population served decreased by over 1 million (p <0.001, slope = -106 886). Geog. anal. demonstrated higher mean violations and populations served in certain counties rather than evenly distributed across states. The decline in violations is likely due to the adoption of documented and undocumented treatment methods and possibly from reduced environmental releases. Considering other studies that have shown decreased urinary arsenic levels in the population served by public water systems since the new std., it may be inferred that the FAR is facilitating the redn. of arsenic exposure in the US.
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    Gude, J. C. J.; Rietveld, L. C.; van Halem, D. As(III) removal in rapid filters: Effect of pH, Fe(II)/Fe(III), filtration velocity and media size. Water Res. 2018, 147, 342– 349,  DOI: 10.1016/j.watres.2018.10.005
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    As(III) removal in rapid filters: Effect of pH, Fe(II)/Fe(III), filtration velocity and media size
    Gude, J. C. J.; Rietveld, L. C.; van Halem, D.
    Water Research (2018), 147 (), 342-349CODEN: WATRAG; ISSN:0043-1354. (Elsevier Ltd.)
    In the top layer of aerated rapid sand filtration systems, uncharged As(III) is biol. converted to charged As(V). Subsequently, the main removal mechanism for As(V) is adsorption onto oxidised, flocculated Fe(III) (hydrous ferric hydroxides; HFO). The aim of this research was to understand the interactions between As and Fe in biol. active rapid filter columns and investigate the effect of different operational modes on Fe removal to subsequently promote As removal. For this purpose, different filter media column expts. were performed using natural, aerated groundwater contg. 3.4μg/l As(III). Results show that independent of the filter media size, complete (biol.) conversion of As(III), manganese, ammonium and nitrite was achieved in approx. 70 days. After ripening, enhanced As removal was achieved with a top layer of coarse media or by dosing addnl. Fe(III). Addn. of Fe(II) did not have the same effect on As removal, potentially due to heterogeneous Fe(II) oxidn. in the upper layer of the filter, attaching rapidly to the filter grain surface and thereby preventing HFO flocs to penetrate deeper into the bed. Increasing the flow rate from 1 to 4 m/h did not improve As removal and lowering the pH from 8 to 7.4, resulted in an 55% increased removal of dissolved As. Altogether it is concluded that As removal in biol. active rapid sand filters can be improved by applying coarser filter media on top, in combination with dosing Fe(III) and/or pH correction.
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    Schullehner, J.; Hansen, B.; Thygesen, M.; Pedersen, C. B.; Sigsgaard, T. Nitrate in drinking water and colorectal cancer risk: A nationwide population-based cohort study. Int. J. Cancer 2018, 143 (1), 73– 79,  DOI: 10.1002/ijc.31306
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    Nitrate in drinking water and colorectal cancer risk: A nationwide population-based cohort study
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    International Journal of Cancer (2018), 143 (1), 73-79CODEN: IJCNAW; ISSN:0020-7136. (John Wiley & Sons, Inc.)
    Nitrate in drinking water may increase risk of colorectal cancer due to endogenous transformation into carcinogenic N-nitroso compds. Epidemiol. studies are few and often challenged by their limited ability of estg. long-term exposure on a detailed individual level. We exploited population-based health register data, linked in time and space with longitudinal drinking water quality data, on an individual level to study the assocn. between long-term drinking water nitrate exposure and colorectal cancer (CRC) risk. Individual nitrate exposure was calcd. for 2.7 million adults based on drinking water quality analyses at public waterworks and private wells between 1978 and 2011. For the main analyses, 1.7 million individuals with highest exposure assessment quality were included. Follow-up started at age 35. We identified 5,944 incident CRC cases during 23 million person-years at risk. We used Cox proportional hazards models to est. hazard ratios (HRs) of nitrate exposure on the risk of CRC, colon and rectal cancer. Persons exposed to the highest level of drinking water nitrate had an HR of 1.16 (95% CI: 1.08-1.25) for CRC compared with persons exposed to the lowest level. We found statistically significant increased risks at drinking water levels above 3.87 mg/L, well below the current drinking water std. of 50 mg/L. Our results add to the existing evidence suggesting increased CRC risk at drinking water nitrate concns. below the current drinking water std. A discussion on the adequacy of the drinking water std. in regards to chronic effects is warranted.
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    Nitrate exposure from drinking water in Denmark over the last 35 years
    Schullehner, Jorg; Hansen, Birgitte
    Environmental Research Letters (2014), 9 (9), 095001/1-095001/9, 9 pp.CODEN: ERLNAL; ISSN:1748-9326. (IOP Publishing Ltd.)
    In Denmark, drinking water quality data covering the entire country for over 35 years are registered in a publicly-accessible database. These data were analyzed to det. the fraction of population exposed to elevated nitrate concns. Data from 2,852 water supply areas from the 98 Danish municipalities were collected in one dataset. Public water supplies are extensively registered; private wells supplying only few households are neither monitored nor registered sufficiently. The study showed that 5.1% of the Danish population was exposed to nitrate concns. >25 mg L-1 in 2012. Private well users were far more prone to exposure to elevated nitrate concns. than consumers connected to public supplies. While the fraction exposed to elevated nitrate concns. amongst public supply users has been decreasing since the 1970s, it has been increasing amongst private well users, leading to the hypothesis that the decrease in nitrate concns. in drinking water is mainly due to structural changes and not improvement of the groundwater quality. A combination of this new drinking water quality map with extensive Danish health registers would permit an epidemiol. study on health effects of nitrate, as long as the lack of data on private well users is addressed.
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    Pennino, M. J.; Compton, J. E.; Leibowitz, S. G. Trends in Drinking Water Nitrate Violations Across the United States. Environ. Sci. Technol. 2017, 51 (22), 13450– 13460,  DOI: 10.1021/acs.est.7b04269
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    Trends in Drinking Water Nitrate Violations Across the United States
    Pennino, Michael J.; Compton, Jana E.; Leibowitz, Scott G.
    Environmental Science & Technology (2017), 51 (22), 13450-13460CODEN: ESTHAG; ISSN:0013-936X. (American Chemical Society)
    Drinking water max. contaminant levels (MCL) are established by the U.S.EPA to protect human health. Since 1975, U.S. public water suppliers have reported MCL violations to the national Safe Drinking Water Information System (SDWIS). This study assessed temporal and geog. trends for violations of the 10 mg nitrate-N L-1 MCL in the conterminous U.S. We found that the proportion of systems in violation for nitrate significantly increased from 0.28% to 0.42% of all systems between 1994 and 2009 and then decreased to 0.32% by 2016. The no. of people served by systems in violation decreased from 1.5 million in 1997 to 200,000 in 2014. Periodic spikes in people served were often driven by just one large system in violation. On av., Nebraska and Delaware had the greatest proportion of systems in violation (2.7% and 2.4%, resp.), while Ohio and California had the greatest av. annual no. of people served by systems in violation (278,374 and 139,149 people, resp.). Even though surface water systems that serve more people have been improving over time, groundwater systems in violation and av. duration of violations are increasing, indicating persistent nitrate problems in drinking water.
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    Bernal, J. L.; Cummins, S.; Gasparrini, A. Interrupted time series regression for the evaluation of public health interventions: a tutorial. Int. J. Epidemiol 2020, 49 (4), 1414– 1414,  DOI: 10.1093/ije/dyaa118
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    Corrigendum to: Interrupted time series regression for the evaluation of public health interventions: a tutorial
    Bernal James Lopez; Cummins Steven; Gasparrini Antonio
    International journal of epidemiology (2020), 49 (4), 1414 ISSN:.
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    Lamm, S. H.; Engel, A.; Penn, C. A.; Chen, R.; Feinleib, M. Arsenic cancer risk confounder in southwest Taiwan data set. Environ. Health Perspect. 2006, 114 (7), 1077– 1082,  DOI: 10.1289/ehp.8704
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    Arsenic cancer risk confounder in southwest Taiwan data set
    Lamm, Steven H.; Engel, Arnold; Penn, Cecilia A.; Chen, Rusan; Feinleib, Manning
    Environmental Health Perspectives (2006), 114 (7), 1077-1082CODEN: EVHPAZ; ISSN:0091-6765. (U. S. Department of Health and Human Services, Public Health Services)
    Quant. anal. for the risk of human cancer from the ingestion of inorg. arsenic has been based on the reported cancer mortality experience in the blackfoot disease (BFD)-endemic area of southwest Taiwan. Linear regression anal. shows that arsenic as the sole etiol. factor accounts for only 21% of the variance in the village standardized mortality ratios for bladder and lung cancer. A previous study had reported the influence of confounders (township, BFD prevalence, and artesian well dependency) qual., but they have not been introduced into a quant. assessment. In this six-township study, only three townships (2, 4, and 6) showed a significant pos. dose-response relationship with arsenic exposure. The other three townships (0, 3, and 5) demonstrated significant bladder and lung cancer risks that were independent of arsenic exposure. The data for bladder and lung cancer mortality for townships 2, 4, and 6 fit an inverse linear regression model (p < 0.001) with an estd. threshold at 151 μg/L (95% confidence interval, 42 to 229 μg/L). Such a model is consistent with epidemiol. and toxicol. literature for bladder cancer. Exploration of the southwest Taiwan cancer mortality data set has clarified the dose-response relationship with arsenic exposure by sepg. out township as a confounding factor.
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    Tsuji, J. S.; Chang, E. T.; Gentry, P. R.; Clewell, H. J.; Boffetta, P.; Cohen, S. M. Dose-response for assessing the cancer risk of inorganic arsenic in drinking water: the scientific basis for use of a threshold approach. Crit. Rev. Toxicol. 2019, 49 (1), 36– 84,  DOI: 10.1080/10408444.2019.1573804
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    Dose-response for assessing the cancer risk of inorganic arsenic in drinking water: the scientific basis for use of a threshold approach
    Tsuji, Joyce S.; Chang, Ellen T.; Gentry, P. Robinan; Clewell, Harvey J.; Boffetta, Paolo; Cohen, Samuel M.
    Critical Reviews in Toxicology (2019), 49 (1), 36-84CODEN: CRTXB2; ISSN:1040-8444. (Taylor & Francis Ltd.)
    A review. The biol. effects of inorg. arsenic predominantly involve reaction of the trivalent forms with sulfhydryl groups in crit. proteins in target cells, potentially leading to various toxicol. events including cancer. This mode of action is a threshold process, requiring sufficient concns. of trivalent arsenic to disrupt normal cellular function. Nevertheless, cancer risk assessments for inorg. arsenic have traditionally utilized various dose-response models that extrapolate risks from high doses assuming low-dose linearity without a threshold. We present here an approach for a cancer risk assessment for inorg. arsenic in drinking water that involves considerations of this threshold process. Extensive investigations in mode of action anal., in vitro studies (>0.1 μM), and in animal studies (>2 mg/L in drinking water or 2 mg/kg of diet), collectively indicate a threshold basis for inorg. arsenic-related cancers. These studies support a threshold for the effects of arsenic in humans of 50-100 μg/L in drinking water (about 65 μg/L). We then evaluate the epidemiol. of cancers of the urinary bladder, lung, and skin and non-cancer skin changes for consistency with this calcd. value, focusing on studies involving low-level exposures to inorg. arsenic primarily in drinking water (approx. <150 μg/L). Based on the relevant epidemiol. studies with individual-level data, a threshold level for inorg. arsenic in the drinking water for these cancers is estd. to be around 100 μg/L, with strong evidence that it is between 50 and 150 μg/L, consistent with the value calcd. based on mechanistic, in vitro and in vivo investigations. This evaluation provides an alternative mode of action-based approach for assessing health-protective levels for oral arsenic exposure based on the collective in vitro, in vivo, and human evidence rather than the use of a linear low-dose extrapolation based on default assumptions and theories.
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    Human and Ecological Risk Assessment (2002), 8 (7), 1697-1721CODEN: HERAFR; ISSN:1080-7039. (CRC Press LLC)
    Arsenic is widely distributed in the environment by natural and human means. The potential for adverse health effects from inorg. arsenic depends on the level and route of exposure. To est. potential health risks of inorg. arsenic, the apportionment of exposure among sources of inorg. arsenic is crit. In this study, daily inorg. arsenic intake of U.S. adults from food, water, and soil ingestion and from airborne particle inhalation was estd. To account for variations in exposure across the U.S., a Monte Carlo approach was taken using simulations for 100,000 individuals representing the age, gender, and county of residence of the U.S. population based on census data. The present anal. found that food is the greatest source of inorg. arsenic intake and that drinking water is the next highest contributor. Inhalation of airborne arsenic-contg. particles and ingestion of arsenic-contg. soils were negligible contributors. The exposure is best represented by the ranges of inorg. arsenic intake (at the 10th and 90th percentiles), which were 1.8 to 11.4 μg/day for males and 1.3 to 9.4 μg/day for females. Regional differences in inorg. arsenic exposure were due mostly to consumption of drinking water contg. differing inorg. arsenic content rather than to food preferences.
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    This paper examines the implications of arsenic chem., occurrence, and routes of exposure for risk assessment. In order to illustrate the relative importance of exposure through consumption of food and drinking water, the contribution of dietary intake to human exposure to inorg. arsenic was estd. as 2 μg/d. This est. is based on a total dietary intake of arsenic of 40 μg/d and a 5% contribution of inorg. arsenic to the total dietary intake. This estd. value for dietary intake of inorg. arsenic (2 μg/d) is comparable to the exposure that would result from consumption of 2L/d of drinking water contg. 1 μg/L inorg. arsenic. At lower concns. of arsenic in drinking water, daily intake of inorg. arsenic becomes increasingly dominated by the dietary contribution. Evaluation of stds. for arsenic in drinking water should include careful consideration of exposure through other routes, particularly food consumption.
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  • Abstract

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    Figure 1

    Figure 1. Location of public waterworks and public water supply wells with As data for the study period 2002–2016. Waterworks identified during the 2002–2004 period as noncompliant were used in the follow-up study and are shown here as red triangles.

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    Figure 2

    Figure 2. Arsenic concentrations in Danish groundwater (n = 21819) and drinking water (n = 25827) from the Danish national database Jupiter. All results are from samples collected in the period 2002–2016 from active supply wells (n = 6133) and active waterworks (n = 3125), respectively. Waterworks serving <10 households are excluded (ca. 3% of the population).

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    Figure 3

    Figure 3. Mean annual arsenic concentrations in drinking water for each waterworks (blue points) and number of waterworks identified as noncompliant (red points), on the basis of the 106 waterworks initially in violation for the study period 2002–2016. Boxplot: fifth and 95th percentile (lower and upper whiskers), 25th and 75th percentile (bottom and top of box), median (thick line), with a color change on the bars that follows the boxplots. The horizontal displacement of As concentration data points within each bar plot is for visualization purposes only. Below the bars: n1, number of the 106 noncompliant waterworks reporting at least one As concentration that year; n2, number of the 106 waterworks identified as noncompliant that year.

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    Figure 4

    Figure 4. Corrective measures implemented in the period 2002–2016 to improve drinking water quality for As. The figure includes the 106 waterworks that were noncompliant in 2002–2004. “Other actions” include abolishing the reaction basin between aeration and filtration steps, changing the screen depth in the well, and changing the aeration method.

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  • References

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      At present one of the greatest barriers to reducing exposure to naturally occurring arsenic from unregulated private well water is a lack of well testing. The New Jersey Private Well Testing Act (PWTA) has since 2002 required testing during real estate transactions. Due to limitations in relying on individual well owners to take protective actions, such state-wide testing regulations have been shown to make a significant contribution towards exposure redn. This study examines the New Jersey PWTA as a case of testing requirements successfully adopted into law, and failed attempts to pass equiv. requirements in Maine for comparison. Although New Jersey's long history of drinking water quality problems due to population d., an industrial past, and vulnerable aquifers was the root of the PWTA and earlier local testing ordinances, several high-profile events immediately prior focused public and legislator attention and mobilized environmental advocacy groups to gain political support statewide. Viewed through Kingdon's Multiple Streams framework, the PWTA was the result of problem, policy, and politics streams successfully aligned during a significant and unique political window of opportunity. In Maine, where naturally occurring arsenic, not industrial contamination, is the primary concern, private sector opposition and a conservative administration resistant to government involvement in "private" well water, all played a role in blocking legislative attempts to require testing. A modest education and outreach bill without testing mandates passed in 2017 after compromise among stakeholders. For policy to be an effective tool to achieve universal well water screening, a philosophical evolution on the role of government in private water may be necessary.
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    22. 22
      Flanagan, S. V.; Spayd, S. E.; Procopio, N. A.; Chillrud, S. N.; Braman, S.; Zheng, Y. Arsenic in private well water part 1 of 3: Impact of the New Jersey Private Well Testing Act on household testing and mitigation behavior. Sci. Total Environ. 2016, 562, 999– 1009,  DOI: 10.1016/j.scitotenv.2016.03.196
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      Arsenic in private well water part 1 of 3: Impact of the New Jersey Private Well Testing Act on household testing and mitigation behavior
      Flanagan, Sara V.; Spayd, Steven E.; Procopio, Nicholas A.; Chillrud, Steven N.; Braman, Stuart; Zheng, Yan
      Science of the Total Environment (2016), 562 (), 999-1009CODEN: STENDL; ISSN:0048-9697. (Elsevier B.V.)
      Regularly ingesting water with elevated As increases adverse health risks. Since Sept. 2002, the NJ Private Well Testing Act (PWTA) has required testing untreated well water for As during real estate transactions in 12 counties. Its implementation provides an opportunity to study the effects of policy intervention on well testing and treatment behavior. We analyze results of a survey mailed to 1943 random addresses (37% response), including responses from 502 private well households who purchased their homes prior to PWTA commencement and 168 who purchased after. We find the PWTA has significantly increased arsenic testing rates in an area where 21% of wells contain As above the 5 μg/L NJ drinking water std. The PWTA has allowed identification of more wells with As (20% of post-PWTA vs. 4% of pre-PWTA households) and more treatment for As (19% of post-PWTA vs. 3% of pre-PWTA households). Such an Act is a partial answer to significant socioeconomic disparities in testing obsd. among households for whom it is not required. Addnl. residents purchasing homes since 2002 are younger and disproportionately more likely to have children in their household (60 vs. 32%), a priority group given their particular vulnerability to effects of As. Despite more wells tested under the PWTA, post-PWTA well owners forget or misremember As test results more often, are more likely to report not knowing what kind of treatment they are using, and are not reporting better maintenance or monitoring of their treatment systems than pre-PWTA households. This suggests serious challenges to reducing As exposure remain even when testing is a requirement. Only a fraction of wells have been tested under the PWTA due to the slow pace of housing turnover. We recommend more public resources be made available to support private well testing among socially and biol. vulnerable groups.
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    23. 23
      Foster, S. A.; Pennino, M. J.; Compton, J. E.; Leibowitz, S. G.; Kile, M. L. Arsenic Drinking Water Violations Decreased across the United States Following Revision of the Maximum Contaminant Level. Environ. Sci. Technol. 2019, 53 (19), 11478– 11485,  DOI: 10.1021/acs.est.9b02358
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      Arsenic Drinking Water Violations Decreased across the United States Following Revision of the Maximum Contaminant Level
      Foster, Stephanie A.; Pennino, Michael J.; Compton, Jana E.; Leibowitz, Scott G.; Kile, Molly L.
      Environmental Science & Technology (2019), 53 (19), 11478-11485CODEN: ESTHAG; ISSN:0013-936X. (American Chemical Society)
      Arsenic poses a threat to public health due to widespread environmental prevalence and known carcinogenic effects. In 2001, the US EPA published the Final Arsenic Rule (FAR) for public drinking water, reducing the max. contaminant level (MCL) from 50 to 10 μg/L. We studied impacts of the FAR on drinking water violations temporally and geog. using the Safe Drinking Water Information System. Violations exceeding the MCL and the population served by violating systems were analyzed across the conterminous US from 2006 (onset of FAR enforcement) to 2017. The public water system violations declined from 1.3% in 2008 to 0.55% in 2017 (p <0.001, slope = -0.070), and the population served decreased by over 1 million (p <0.001, slope = -106 886). Geog. anal. demonstrated higher mean violations and populations served in certain counties rather than evenly distributed across states. The decline in violations is likely due to the adoption of documented and undocumented treatment methods and possibly from reduced environmental releases. Considering other studies that have shown decreased urinary arsenic levels in the population served by public water systems since the new std., it may be inferred that the FAR is facilitating the redn. of arsenic exposure in the US.
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      Gude, J. C. J.; Rietveld, L. C.; van Halem, D. As(III) removal in rapid filters: Effect of pH, Fe(II)/Fe(III), filtration velocity and media size. Water Res. 2018, 147, 342– 349,  DOI: 10.1016/j.watres.2018.10.005
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      As(III) removal in rapid filters: Effect of pH, Fe(II)/Fe(III), filtration velocity and media size
      Gude, J. C. J.; Rietveld, L. C.; van Halem, D.
      Water Research (2018), 147 (), 342-349CODEN: WATRAG; ISSN:0043-1354. (Elsevier Ltd.)
      In the top layer of aerated rapid sand filtration systems, uncharged As(III) is biol. converted to charged As(V). Subsequently, the main removal mechanism for As(V) is adsorption onto oxidised, flocculated Fe(III) (hydrous ferric hydroxides; HFO). The aim of this research was to understand the interactions between As and Fe in biol. active rapid filter columns and investigate the effect of different operational modes on Fe removal to subsequently promote As removal. For this purpose, different filter media column expts. were performed using natural, aerated groundwater contg. 3.4μg/l As(III). Results show that independent of the filter media size, complete (biol.) conversion of As(III), manganese, ammonium and nitrite was achieved in approx. 70 days. After ripening, enhanced As removal was achieved with a top layer of coarse media or by dosing addnl. Fe(III). Addn. of Fe(II) did not have the same effect on As removal, potentially due to heterogeneous Fe(II) oxidn. in the upper layer of the filter, attaching rapidly to the filter grain surface and thereby preventing HFO flocs to penetrate deeper into the bed. Increasing the flow rate from 1 to 4 m/h did not improve As removal and lowering the pH from 8 to 7.4, resulted in an 55% increased removal of dissolved As. Altogether it is concluded that As removal in biol. active rapid sand filters can be improved by applying coarser filter media on top, in combination with dosing Fe(III) and/or pH correction.
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      Schullehner, J.; Hansen, B.; Thygesen, M.; Pedersen, C. B.; Sigsgaard, T. Nitrate in drinking water and colorectal cancer risk: A nationwide population-based cohort study. Int. J. Cancer 2018, 143 (1), 73– 79,  DOI: 10.1002/ijc.31306
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      Nitrate in drinking water and colorectal cancer risk: A nationwide population-based cohort study
      Schullehner, Joerg; Hansen, Birgitte; Thygesen, Malene; Pedersen, Carsten B.; Sigsgaard, Torben
      International Journal of Cancer (2018), 143 (1), 73-79CODEN: IJCNAW; ISSN:0020-7136. (John Wiley & Sons, Inc.)
      Nitrate in drinking water may increase risk of colorectal cancer due to endogenous transformation into carcinogenic N-nitroso compds. Epidemiol. studies are few and often challenged by their limited ability of estg. long-term exposure on a detailed individual level. We exploited population-based health register data, linked in time and space with longitudinal drinking water quality data, on an individual level to study the assocn. between long-term drinking water nitrate exposure and colorectal cancer (CRC) risk. Individual nitrate exposure was calcd. for 2.7 million adults based on drinking water quality analyses at public waterworks and private wells between 1978 and 2011. For the main analyses, 1.7 million individuals with highest exposure assessment quality were included. Follow-up started at age 35. We identified 5,944 incident CRC cases during 23 million person-years at risk. We used Cox proportional hazards models to est. hazard ratios (HRs) of nitrate exposure on the risk of CRC, colon and rectal cancer. Persons exposed to the highest level of drinking water nitrate had an HR of 1.16 (95% CI: 1.08-1.25) for CRC compared with persons exposed to the lowest level. We found statistically significant increased risks at drinking water levels above 3.87 mg/L, well below the current drinking water std. of 50 mg/L. Our results add to the existing evidence suggesting increased CRC risk at drinking water nitrate concns. below the current drinking water std. A discussion on the adequacy of the drinking water std. in regards to chronic effects is warranted.
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      Schullehner, J.; Hansen, B. Nitrate exposure from drinking water in Denmark over the last 35 years. Environ. Res. Lett. 2014, 9 (9), 095001,  DOI: 10.1088/1748-9326/9/9/095001
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      Nitrate exposure from drinking water in Denmark over the last 35 years
      Schullehner, Jorg; Hansen, Birgitte
      Environmental Research Letters (2014), 9 (9), 095001/1-095001/9, 9 pp.CODEN: ERLNAL; ISSN:1748-9326. (IOP Publishing Ltd.)
      In Denmark, drinking water quality data covering the entire country for over 35 years are registered in a publicly-accessible database. These data were analyzed to det. the fraction of population exposed to elevated nitrate concns. Data from 2,852 water supply areas from the 98 Danish municipalities were collected in one dataset. Public water supplies are extensively registered; private wells supplying only few households are neither monitored nor registered sufficiently. The study showed that 5.1% of the Danish population was exposed to nitrate concns. >25 mg L-1 in 2012. Private well users were far more prone to exposure to elevated nitrate concns. than consumers connected to public supplies. While the fraction exposed to elevated nitrate concns. amongst public supply users has been decreasing since the 1970s, it has been increasing amongst private well users, leading to the hypothesis that the decrease in nitrate concns. in drinking water is mainly due to structural changes and not improvement of the groundwater quality. A combination of this new drinking water quality map with extensive Danish health registers would permit an epidemiol. study on health effects of nitrate, as long as the lack of data on private well users is addressed.
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      Pennino, M. J.; Compton, J. E.; Leibowitz, S. G. Trends in Drinking Water Nitrate Violations Across the United States. Environ. Sci. Technol. 2017, 51 (22), 13450– 13460,  DOI: 10.1021/acs.est.7b04269
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      Trends in Drinking Water Nitrate Violations Across the United States
      Pennino, Michael J.; Compton, Jana E.; Leibowitz, Scott G.
      Environmental Science & Technology (2017), 51 (22), 13450-13460CODEN: ESTHAG; ISSN:0013-936X. (American Chemical Society)
      Drinking water max. contaminant levels (MCL) are established by the U.S.EPA to protect human health. Since 1975, U.S. public water suppliers have reported MCL violations to the national Safe Drinking Water Information System (SDWIS). This study assessed temporal and geog. trends for violations of the 10 mg nitrate-N L-1 MCL in the conterminous U.S. We found that the proportion of systems in violation for nitrate significantly increased from 0.28% to 0.42% of all systems between 1994 and 2009 and then decreased to 0.32% by 2016. The no. of people served by systems in violation decreased from 1.5 million in 1997 to 200,000 in 2014. Periodic spikes in people served were often driven by just one large system in violation. On av., Nebraska and Delaware had the greatest proportion of systems in violation (2.7% and 2.4%, resp.), while Ohio and California had the greatest av. annual no. of people served by systems in violation (278,374 and 139,149 people, resp.). Even though surface water systems that serve more people have been improving over time, groundwater systems in violation and av. duration of violations are increasing, indicating persistent nitrate problems in drinking water.
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      Bernal, J. L.; Cummins, S.; Gasparrini, A. Interrupted time series regression for the evaluation of public health interventions: a tutorial. Int. J. Epidemiol 2020, 49 (4), 1414– 1414,  DOI: 10.1093/ije/dyaa118
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      Corrigendum to: Interrupted time series regression for the evaluation of public health interventions: a tutorial
      Bernal James Lopez; Cummins Steven; Gasparrini Antonio
      International journal of epidemiology (2020), 49 (4), 1414 ISSN:.
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      Lamm, S. H.; Engel, A.; Penn, C. A.; Chen, R.; Feinleib, M. Arsenic cancer risk confounder in southwest Taiwan data set. Environ. Health Perspect. 2006, 114 (7), 1077– 1082,  DOI: 10.1289/ehp.8704
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      Arsenic cancer risk confounder in southwest Taiwan data set
      Lamm, Steven H.; Engel, Arnold; Penn, Cecilia A.; Chen, Rusan; Feinleib, Manning
      Environmental Health Perspectives (2006), 114 (7), 1077-1082CODEN: EVHPAZ; ISSN:0091-6765. (U. S. Department of Health and Human Services, Public Health Services)
      Quant. anal. for the risk of human cancer from the ingestion of inorg. arsenic has been based on the reported cancer mortality experience in the blackfoot disease (BFD)-endemic area of southwest Taiwan. Linear regression anal. shows that arsenic as the sole etiol. factor accounts for only 21% of the variance in the village standardized mortality ratios for bladder and lung cancer. A previous study had reported the influence of confounders (township, BFD prevalence, and artesian well dependency) qual., but they have not been introduced into a quant. assessment. In this six-township study, only three townships (2, 4, and 6) showed a significant pos. dose-response relationship with arsenic exposure. The other three townships (0, 3, and 5) demonstrated significant bladder and lung cancer risks that were independent of arsenic exposure. The data for bladder and lung cancer mortality for townships 2, 4, and 6 fit an inverse linear regression model (p < 0.001) with an estd. threshold at 151 μg/L (95% confidence interval, 42 to 229 μg/L). Such a model is consistent with epidemiol. and toxicol. literature for bladder cancer. Exploration of the southwest Taiwan cancer mortality data set has clarified the dose-response relationship with arsenic exposure by sepg. out township as a confounding factor.
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      Tsuji, J. S.; Chang, E. T.; Gentry, P. R.; Clewell, H. J.; Boffetta, P.; Cohen, S. M. Dose-response for assessing the cancer risk of inorganic arsenic in drinking water: the scientific basis for use of a threshold approach. Crit. Rev. Toxicol. 2019, 49 (1), 36– 84,  DOI: 10.1080/10408444.2019.1573804
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      Dose-response for assessing the cancer risk of inorganic arsenic in drinking water: the scientific basis for use of a threshold approach
      Tsuji, Joyce S.; Chang, Ellen T.; Gentry, P. Robinan; Clewell, Harvey J.; Boffetta, Paolo; Cohen, Samuel M.
      Critical Reviews in Toxicology (2019), 49 (1), 36-84CODEN: CRTXB2; ISSN:1040-8444. (Taylor & Francis Ltd.)
      A review. The biol. effects of inorg. arsenic predominantly involve reaction of the trivalent forms with sulfhydryl groups in crit. proteins in target cells, potentially leading to various toxicol. events including cancer. This mode of action is a threshold process, requiring sufficient concns. of trivalent arsenic to disrupt normal cellular function. Nevertheless, cancer risk assessments for inorg. arsenic have traditionally utilized various dose-response models that extrapolate risks from high doses assuming low-dose linearity without a threshold. We present here an approach for a cancer risk assessment for inorg. arsenic in drinking water that involves considerations of this threshold process. Extensive investigations in mode of action anal., in vitro studies (>0.1 μM), and in animal studies (>2 mg/L in drinking water or 2 mg/kg of diet), collectively indicate a threshold basis for inorg. arsenic-related cancers. These studies support a threshold for the effects of arsenic in humans of 50-100 μg/L in drinking water (about 65 μg/L). We then evaluate the epidemiol. of cancers of the urinary bladder, lung, and skin and non-cancer skin changes for consistency with this calcd. value, focusing on studies involving low-level exposures to inorg. arsenic primarily in drinking water (approx. <150 μg/L). Based on the relevant epidemiol. studies with individual-level data, a threshold level for inorg. arsenic in the drinking water for these cancers is estd. to be around 100 μg/L, with strong evidence that it is between 50 and 150 μg/L, consistent with the value calcd. based on mechanistic, in vitro and in vivo investigations. This evaluation provides an alternative mode of action-based approach for assessing health-protective levels for oral arsenic exposure based on the collective in vitro, in vivo, and human evidence rather than the use of a linear low-dose extrapolation based on default assumptions and theories.
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      Meacher, D. M.; Menzel, D. B.; Dillencourt, M. D.; Bic, L. F.; Schoof, R. A.; Yost, L. J.; Eickhoff, J. C.; Farr, C. H. Estimation of multimedia inorganic arsenic intake in the US population. Hum. Ecol. Risk Assess. 2002, 8 (7), 1697– 1721,  DOI: 10.1080/20028091057565
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      Estimation of multimedia inorganic arsenic intake in the U.S. Population
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      Human and Ecological Risk Assessment (2002), 8 (7), 1697-1721CODEN: HERAFR; ISSN:1080-7039. (CRC Press LLC)
      Arsenic is widely distributed in the environment by natural and human means. The potential for adverse health effects from inorg. arsenic depends on the level and route of exposure. To est. potential health risks of inorg. arsenic, the apportionment of exposure among sources of inorg. arsenic is crit. In this study, daily inorg. arsenic intake of U.S. adults from food, water, and soil ingestion and from airborne particle inhalation was estd. To account for variations in exposure across the U.S., a Monte Carlo approach was taken using simulations for 100,000 individuals representing the age, gender, and county of residence of the U.S. population based on census data. The present anal. found that food is the greatest source of inorg. arsenic intake and that drinking water is the next highest contributor. Inhalation of airborne arsenic-contg. particles and ingestion of arsenic-contg. soils were negligible contributors. The exposure is best represented by the ranges of inorg. arsenic intake (at the 10th and 90th percentiles), which were 1.8 to 11.4 μg/day for males and 1.3 to 9.4 μg/day for females. Regional differences in inorg. arsenic exposure were due mostly to consumption of drinking water contg. differing inorg. arsenic content rather than to food preferences.
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      This paper examines the implications of arsenic chem., occurrence, and routes of exposure for risk assessment. In order to illustrate the relative importance of exposure through consumption of food and drinking water, the contribution of dietary intake to human exposure to inorg. arsenic was estd. as 2 μg/d. This est. is based on a total dietary intake of arsenic of 40 μg/d and a 5% contribution of inorg. arsenic to the total dietary intake. This estd. value for dietary intake of inorg. arsenic (2 μg/d) is comparable to the exposure that would result from consumption of 2L/d of drinking water contg. 1 μg/L inorg. arsenic. At lower concns. of arsenic in drinking water, daily intake of inorg. arsenic becomes increasingly dominated by the dietary contribution. Evaluation of stds. for arsenic in drinking water should include careful consideration of exposure through other routes, particularly food consumption.
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