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. 2016 May 9:6:25656.
doi: 10.1038/srep25656.

Urinary arsenic profiles reveal exposures to inorganic arsenic from private drinking water supplies in Cornwall, UK

D R S Middleton  1   2   3 , M J Watts  2 , E M Hamilton  2 , E L Ander  2 , R M Close  3 , K S Exley  3 , H Crabbe  3 , G S Leonardi  3 , T Fletcher  3 , D A Polya  1
Affiliations

Urinary arsenic profiles reveal exposures to inorganic arsenic from private drinking water supplies in Cornwall, UK

D R S Middleton et al. Sci Rep. .

Abstract

Private water supplies (PWS) in Cornwall, South West England exceeded the current WHO guidance value and UK prescribed concentration or value (PCV) for arsenic of 10 μg/L in 5% of properties surveyed (n = 497). In this follow-up study, the first of its kind in the UK, volunteers (n = 207) from 127 households who used their PWS for drinking, provided urine and drinking water samples for total As determination by inductively coupled plasma mass spectrometry (ICP-MS) and urinary As speciation by high performance liquid chromatography ICP-MS (HPLC-ICP-MS). Arsenic concentrations exceeding 10 μg/L were found in the PWS of 10% of the volunteers. Unadjusted total urinary As concentrations were poorly correlated (Spearman's ρ = 0.36 (P < 0.001)) with PWS As largely due to the use of spot urine samples and the dominance of arsenobetaine (AB) from seafood sources. However, the osmolality adjusted sum, U-As(IMM), of urinary inorganic As species, arsenite (As(III)) and arsenate (As(V)), and their metabolites, methylarsonate (MA) and dimethylarsinate (DMA), was found to strongly correlate (Spearman's ρ: 0.62 (P < 0.001)) with PWS As, indicating private water supplies as the dominant source of inorganic As exposure in the study population of PWS users.

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Figures

Figure 1
Figure 1. Spatial distribution of sampled households.
Compiled using ArcMap 10.1.
Figure 2
Figure 2. Study group age and gender distribution.
While population risk assessment is not the focus of this aspect of the study, it is noted for future reference that the present sample is not wholly representative of the underlying population of rural Cornwall. *Office for National Statistics (ONS) Rural-urban classification 2011 (RUC11) was used to determine the underlying population (see supplementary information). Adapted from data from the Office for National Statistics licensed under the Open Government Licence v.3.0.
Figure 3
Figure 3. Box and whisker plots of private water supply (PWS) drinking water and urinary As.
(a) Total As in drinking water samples plotted with its analytical limit of detection (LOD) (lower dashed line) and the UK As PCV (upper solid line). (b) Individual urinary As species plotted with their respective LODs (dashed lines). (c) Urinary total As and urinary sum of species excluding AB (U-AsIMM). Boxes range from 1st to 3rd quartiles with a median line, lower and upper whiskers are the lowest and highest datum within 1.5 inter quartile range (IQR) of the lowest and upper quartile respectively and circles are outliers. For plotting purposes, speciation data were censored by replacing <LOD values with ½ LOD.
Figure 4
Figure 4. Unadjusted and adjusted urinary As – PWS drinking water As.
(a) Unadjusted urinary total As. (b) Unadjusted U-AsIMM (adjusted for AB). (c) Osmolality adjusted U-AsIMM. Linear regression lines are for reference only. A poor relationship between drinking water total As and unadjusted urinary total As is evident (a) due to seafood intake and the large contribution of AB on urinary total As results. This is illustrated by the red dashed line showing high urinary total As results at low drinking water As exposure.
Figure 5
Figure 5. Comparison of alternative U-AsIMM adjustment methods.
The comparison between unadjusted results (a), creatinine adjusted results (b) and osmolality adjusted results (c). The Spearman correlation is stronger in osmolality adjusted results than both alternatives.
Figure 6
Figure 6. Log-log plot of U-AsIMM vs PWS drinking water As divided into drinking water exposure levels.
Variables from Fig. 3c plotted on log scale axes to show contrasting exposure-response relationships of participants exposed to different concentrations of As in drinking water. Spearman’s correlation coefficients (ρ) are displayed for the different drinking water As ranges.
Figure 7
Figure 7. Arsenic speciation standard chromatogram.
Chromatograms obtained for standard calibration solutions at 1, 10 and 50 μg/ L. Calibration of arsenate (AsV), methylarsonate (MA), dimethylarsinate (DMA) and arsenobetaine (AB) was performed with mixed solutions of arsenic (V) oxide hydrate (As2O5·xH2O), monomethylarsonic acid ((CH3AsO(OH)2), dimethylarsinic acid ((CH3)2AsO(OH)) and arsenobetaine ((CH3)3As + CH2COO-) respectively. Calibration of arsenite (AsIII) has been plotted simultaneously and was achieved with separate solutions of arsenic trioxide (As2O3).
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