Arsenic, cadmium, mercury, sodium, and potassium concentrations in common foods and estimated daily intake of the population in Valdivia (Chile) using a total diet study

Accepted Manuscript Arsenic, cadmium, mercury, sodium, and potassium concentrations in common foods and estimated daily intake of the population in Valdivia (Chile) using a total diet study Ociel Muñoz, Pedro Zamorano, Olga Garcia, José Miguel Bastías PII:

S0278-6915(17)30121-7

DOI:

10.1016/j.fct.2017.03.027

Reference:

FCT 8946

To appear in:

Food and Chemical Toxicology

Received Date: 30 November 2016 Revised Date:

14 March 2017

Accepted Date: 15 March 2017

Please cite this article as: Muñoz, O., Zamorano, P., Garcia, O., Bastías, J.M., Arsenic, cadmium, mercury, sodium, and potassium concentrations in common foods and estimated daily intake of the population in Valdivia (Chile) using a total diet study, Food and Chemical Toxicology (2017), doi: 10.1016/j.fct.2017.03.027. This is a PDF file of an unedited manuscript that has been accepted for publication. As a service to our customers we are providing this early version of the manuscript. The manuscript will undergo copyediting, typesetting, and review of the resulting proof before it is published in its final form. Please note that during the production process errors may be discovered which could affect the content, and all legal disclaimers that apply to the journal pertain.

ACCEPTED MANUSCRIPT

Arsenic, Cadmium, Mercury, Sodium, and Potassium Concentrations in Common Foods and Estimated Daily Intake of the Population in Valdivia

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(Chile) Using a Total Diet Study

Ociel Muñoza*, Pedro Zamoranoa, Olga Garciaa, José Miguel Bastíasb

Food Science and Technology Institute (ICYTAL), Faculty of Agricultural Sciences, Universidad

Austral de Chile. Campus Isla Teja s/n. Valdivia, Chile.

Food Engineering Department, Universidad del Bió-Bió. Avenida Andrés Bello 720, Chillán, Chile.

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*Corresponding author: Telephone: +56-63-2221253. E-mail: [email protected]

ACCEPTED MANUSCRIPT Abstract

This study was designed to estimate the dietary intake of total arsenic, inorganic arsenic, cadmium, mercury, sodium, and potassium by the general adult population (aged 18-65) of Valdivia, Chile.

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Calculations were based on a 24-h dietary recall survey. The highest dietary intake of t-As (73.0 µg/day), i-As (20.0 µg/day), Cd (18.0 µg/day), Hg (5.8 µg/day), Na+ (3112.8 mg/day), and K+ (2077.5 mg/day) were for 70-kg adults.

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Estimating carcinogenic risk (CR >4x10-4) due to exposure to i-As indicated that consumers remain at low risk for cancer. The cumulative health risk was evaluated by summing the target hazard quotient

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of cadmium (0.26) mercury (0.27) and inorganic arsenic (0.96); this calculation allows us to express the total target hazard quotient as 1.50 where a value >1 indicates that there is a potential health risk for the population. Total intake of Cd and Hg were therefore within the limits estimated as being safe whereas Na+ and K+ intake for the Valdivia population did not follow the recommended values

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established by the World Health Organization (WHO). The Na+ intake exceeded the daily recommended intake while K+ intake was lower than the daily recommended intake. This indicates a

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health risk for the Valdivia population

Keywords: Inorganic arsenic, Cadmium, Mercury, Sodium, Potassium, Total diet study

ACCEPTED MANUSCRIPT 1. Introduction

Sodium and potassium Knowledge of the eating habits of a population is essential not only to establish the nutritional status

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but also to determine the causes of diseases related to food consumption. A diet with inadequate nutrient intake, such as high salt (NaCl) content, can be harmful to health because it increases the risk of hypertension (Karppanen and Mervaala, 2006) and cardiovascular disease (Campbell et al.,

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2011). An increasing correlation exists between high salt intake and the risk of overweight (Song et al., 2013). The World Health Organization (WHO) recommends reducing Na+ intake to < 2 g/day (5

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g/day salt) for adults (WHO, 2012b). Another important metal for health is potassium (K+); it is a vital electrolyte for a healthy nervous system and a regular heart rate. Potassium concentration is important for cell metabolism and membrane excitability (Bielecka-Dabrowa et al., 2012). Moreover, the WHO suggests a K+ intake of at least 90 mmol/day (3510 mg/day) for adults. An increase in K+

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intake from food and a reduction in Na+ intake is recommended to reduce blood pressure and risk of cardiovascular disease, stroke, and coronary heart disease in adults (WHO, 2012b). Currently, Na+ intake in western countries exceeds recommendations whereas K+ intake is lower than the

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recommended values (Tanase et al., 2011); (Donfrancesco et al., 2013). On the other hand, food can also contain undesired elements that can cause acute intoxications if

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ingested. Among the toxic elements to which one is exposed, heavy metals, such as cadmium (Cd) and mercury (Hg), as well as arsenic (As) metalloid, are all chemical elements widely distributed in nature in both soil and water (Munoz et al., 2005). Once these heavy metals reach the water source, their transport and accumulation by the food chain is inevitable and finally attain humans. Cadmium (Cd)

ACCEPTED MANUSCRIPT Cadmium accumulates in the human body and negatively affects various organs such as the liver, kidneys, lungs, bones, placenta, brain, and the central nervous system (Castro-González and Méndez-Armenta, 2008). Other harmful effects that have been observed include reproductive and developmental toxicity, as well as hepatic, hematological, and immunological effects (Apostoli and

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Catalani, 2011).

The FAO/WHO Joint Expert Committee on Food Additives (JECFA) (WHO, 2010) pointed out that the existing health-based guidance value for Cd was expressed on a weekly basis (provisional tolerable

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weekly intake, PTWI); because Cd has an exceptionally long half-life, a monthly value was considered more appropriate. The Committee therefore withdrew the PTWI of 7 µg/kg body weight

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(bw). To encourage this view, the Committee decided to express the tolerable intake as a monthly value as a provisional tolerable monthly intake (PTMI), which was established as 25 µg/kg bw. Cadmium is classified as “carcinogenic to humans” (group 1) by the International Agency for

Arsenic (As)

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Research on Cancer (IARC, 1993).

Arsenic is widely distributed in natural waters and is often associated with geological sources and

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anthropogenic contributions. The use of arsenical insecticides and fossil fuel combustion can be an important source of As. The toxic effects of As primarily depend on the oxidation state and chemical

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species. Inorganic arsenic (i-As) is considered to be carcinogenic and is mainly related to lung, kidney, and bladder cancer, as well as skin diseases (ATSDR, 2007). In 2010, the FAO/WHO JECFA withdrew the PTWI of 15 µg/kg bw/week that had been defined in 1989 (JECFA, 2011). Based on data related to cancer in humans, the European Food Safety Authority (EFSA), has used BMDL01 As at 0.3-8 µg/kg bw/day (confidence limit < 5% of the daily dose that causes a 1% increase in the occurrence of lung, skin, and bladder cancer, as well as skin lesions compared to the controls,

ACCEPTED MANUSCRIPT derived from adjusting a mathematical model to experimental data) (EFSA, 2009). Taking the most conservative limit, the result is a 70-kg person with a daily intake limit of 21 µg/day of i-As.

Mercury (Hg)

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Once released into the environment, Hg is quickly transformed into organic compounds by aquatic microorganisms, mainly as methylmercury (MeHg), which is more toxic than elemental and inorganic forms of Hg. Inorganic Hg occurs as salts of its divalent and monovalent cationic forms (WHO, 2003).

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Mercury salts primarily affect the gastrointestinal tract and kidneys and can cause severe kidney damage (WHO, 2003). Both inorganic and organic Hg compounds are absorbed through the

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gastrointestinal tract and affect other systems via this route.

However, organic Hg compounds are more easily absorbed via ingestion than inorganic Hg compounds (WHO, 2003). More than 90% of MeHg could be absorbed and accumulated in the body with the risk of damaging the neurological, cardiovascular, and reproductive systems (Mergler et al.,

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2007). Some specific pediatric health effects, particularly subtle neurodevelopmental abnormalities, such as visuospatial errors (Chevrier et al., 2009) and decrements in motor speed and attention have been reported (Cheng et al., 2013).

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The United States Environmental Protection Agency (USEPA) proposed 0.1 µg/kg bw/day as a reference dose (RfD) for MeHg (Rice et al., 2000). The JECFA also established a PTWI of 1.6 µg/kg

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bw/week corresponding to 0.23 µg/kg bw/day for MeHg (JECFA, 2003).

Total Diet Studies

Very few studies have been conducted in Chile about the intake of contaminants through food, except for the study carried out in Santiago (Munoz et al., 2005) or the study of the Chilean school meal program by Bastias et al. (Bastias et al., 2010).

ACCEPTED MANUSCRIPT The Total Diet Study (TDS) has been internationally recognized as the most cost-effective way to estimate dietary exposure to food chemicals or nutrients in various population groups and assess associated health risks. It provides a scientific basis for assessing food safety risks and regulating the food supply (Wong et al., 2013).

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A TDS consists in retail purchasing of commonly consumed foods, processing them for consumption, often combining foods into food composites or aggregates, homogenizing, and analyzing them for toxic chemicals and certain nutrients. Exposure through drinking water and water used for cooking

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are included in the TDS assessment. Total diet studies are designed to measure the mean amount of each chemical ingested by different age/sex groups living in a country. These data are necessary to

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assess whether or not specific chemicals pose a risk to human health (Bastias et al., 2010). The WHO recommends, among other approaches, using TDSs to assess intake. This approach is based on a market basket representing the total consumer diet (Kitts, 2003). The TDSs have been conducted in countries such as Brazil (Avegliano et al., 2011), France (Chekri

(Tanase et al., 2011).

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et al., 2012), Italy (Turrini and Lombardi-Boccia, 2002), China (Zhou et al., 2012), and Canada

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Total diet study data differ from other chemical surveillance programs because they focus on chemical compounds in the diet rather than in individual foods and foods are processed as they are

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consumed at home; thus, the impact of home cooking is considered for the decomposition of less stable chemical compounds and the formation of new compounds, and there is an attempt to determine the concentrations of these chemical substances in foods included in the diet (Bastias et al., 2010).

The objective of this study was to conduct a total diet study (TDS) to determine the intake of nutrients, such as sodium and potassium, as well as the intake of contaminants (cadmium, mercury, total

ACCEPTED MANUSCRIPT arsenic, and inorganic arsenic) in foods commonly consumed by the Valdivia population, Chile, to evaluate the health risk associated with ingesting these metals.

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2. Materials and methods

2. 1 Reagents

Deionized water (18 MΩ/cm BARNSTEAD, Easy Pure LF D7382-33) was used to prepare reagents

2.2 Material cleaning and preparation

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As(V), Cd, Hg (1000 mg/L) were used (Merck).

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and standards. All chemicals were of pro analysis quality or better. A commercial standard solution of

All laboratory materials (plastic, glassware, new and used) were rinsed with running tap water and then immersed in a 1% alkaline wash solution (Extran, Merck). After 24 h, materials were rinsed with

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distilled water and then immersed in a 10% v/v HNO3 (Merck) solution for 3 days (new material) or 1 day (used material). For the final step, materials were rinsed three times with distilled water and

2.3 Total diet study

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immersed in ultra-pure water to eliminate all residues.

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Between April and September 2012 (autumn-spring in the Southern Hemisphere), a 24-hours dietary recall survey was carried out with a representative sample of the adult population (aged 18–65) in Valdivia (n = 382) without taking into account gender or social class. All participants were visited at home and the survey was conducted by trained interviewers. A food frequency questionnaire, combined with photos of portion sizes, was used to assess intake. Participants were asked whether the foods were consumed at home or elsewhere. The questionnaire showed consumption of over 300 food items that were grouped into 17 food categories (Table 1) according to Munoz et al. (2005).

ACCEPTED MANUSCRIPT Food items were purchased in common food stores in Valdivia for three different samplings. Food items were then prepared according to the most typical form of consumption. Inedible parts were removed. Cooking methods were grilling, steaming, baking, and boiling with deionized water. No more ingredients were added during cooking. Canned foods were drained immediately after being

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opened. Fresh foods (vegetables and fruit) were washed with distilled water.

Samples were homogenized in a domestic food processor (Moulinex). Each food item was processed in triplicate with different brands, and each brand was analyzed in duplicate. After homogenization,

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proportional amounts of food items were weighed in accordance with the percentage that they represented in their food category (Table 1). All samples were frozen and stored (-20 °C) until further

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analysis.

2.4 Determination of sodium and potassium (Na+ and K+)

The AOAC standard procedures, were used to determine sodium and potassium by atomic

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absorption spectrophotometer (AOAC, 2000), the Samples were thawed at room temperature. Approximately 2 g of each sample were dried in an oven, model UM500 (Memmert), at 105 ± 2 °C until constant weight. Samples were then mineralized in a muffle furnace, model Type 6000

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(Thermolyne), at 550 °C. The ash was dissolved in 10 mL HCl (50% v/v) and filtered through Whatman No. 1 filter paper into a 50 mL volumetric flask. Samples were diluted with HCl (50% v/v).

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They were analyzed in a flame photometer, model PFP7 (Jenway). The detection limit for Na+ and K+ was 12.0 and 5.5 µg/g wet weight (ww), respectively.

2.5 Determination of cadmium (Cd) The analysis was performed by dry mineralization (AOAC, 2000) and atomic absorption spectrophotometry was used to quantify Cd content (Varian, Spectra A-55). Samples (1 ± 0.001 g)

ACCEPTED MANUSCRIPT were placed in 100 mL beakers and the following reagents were added: 5 mL ultra-pure water, 20 mL concentrated HNO3, and 1 mL 7.4% (w/v) MgO. Treated samples were placed on a heating plate (Cientec Vatriax) and 5 mL H2O2 was added. Samples were then placed in a muffle furnace (Nabertherm, L3/P) at 425 °C for 12 hours to obtain white ash. After mineralization, 1 mL ultra-pure

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water and 1 mL concentrated HCl were added to dissolve the ash, which was subsequently filtered with Whatman No. 1 filter paper, and 10% (v/v) HCl was used to reach a final volume of 25 mL. Samples were placed in 50 mL plastic flasks and stored at room temperature for flame atomic

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absorption spectroscopy (FAAS) analysis (Varian, SPECTRA A-55). Instrumental conditions to

detection limit was 0.002 µg/g ww.

2.6 Determination of total mercury (Hg)

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determine Cd were as follows: mixed air/acetylene (2 L/min) and 228.8 nm wavelength. The Cd

The method described by Bastias et al. (2010) was used. In brief, the samples were thawed,

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homogenized, and 1.00 ± 0.01 g of each sample was placed in a tall-form borosilicate glass beaker. Then, 10 mL of concentrated HNO3 was added and the sample was digested at a moderate temperature (< 90°C) for 30 min. It was cooled, 5 mL 30% (v/v) H2O2 was added, and digestion

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continued until the total volume of the mixture was reduced to 5 mL. Aliquots of HNO3 and H2O2 were added when necessary and digestion continued until the solution was completely clear. The digested

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solution was left to equilibrate for 12 hours to eliminate nitrous vapors. The equilibrated solution was then filtered through filter paper (Whatman N° 1) and diluted with 5% (v/v) HCl to a final volume of 25 mL. Total Hg concentration was measured via cold vapor atomic absorption spectroscopy (CV-AAS) with a Varian Spectra A-55 instrument. The detection limit of Hg was 0.0002 µg/g ww.

ACCEPTED MANUSCRIPT 2.7 Determination of total arsenic (t-As) The analysis was performed by dry mineralization and quantified by atomic absorption spectrophotometry (Varian, Spectra A-55) coupled with a hydride generator (Munoz et al., 2002). Samples (1 ± 0.001 g) were treated with 5 mL of deionized water, 20 mL of concentrated HNO3 in the

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presence of a mineralization agent (1 mL MgO 7.4% m/v), and 5 mL of H2O2 until the mixture evaporated by drying and mineralization at 450 °C with a gradual temperature increase. The white ash was dissolved in 1 mL of deionized water and 1 mL HCl. It was filtered (Watman paper Nº 1) and

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50% v/v HCl were added to reach a final volume of 25 mL. Prior to reading the results, a 5% m/v

detection limit of t-As was 0.002 µg/g ww.

2.8 Determination of inorganic arsenic (i-As)

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ascorbic acid and 5% m/v KI reducing mixture was added. Samples were analyzed in triplicate. The

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Inorganic arsenic was determined by acid digestion and extraction with solvents; it was quantified by atomic absorption spectrophotometry (Varian, Spectra A-55) coupled with a hydride generator (Munoz et al., 1999). To the samples (1 ± 0.001 g), 4.1 mL of deionized water and 18.4 mL of HCl

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concentrate were added.

The mixture was left to set overnight. It was then reduced with HBr (2 mL) and hydrazine sulfate

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(1.5% m/v, 1 mL), i-As was extracted with chloroform (3 × 10 mL). The chloroform was retro-extracted with HCl 1 mol/L (2 × 10 mL). For this, 10 mL concentrated HNO3 and 2.5 mL ashing aid suspension (MgO 7.4% m/v) were added. The retro-extraction phases were then evaporated and treated in the same way as t-As. Samples were analyzed in triplicate. The detection limit of i-As was 0.0008 µg/g ww

ACCEPTED MANUSCRIPT 2.9. Human health risk assessment The strategy described by Saha et al. (Saha et al., 2016) (2016) to determine carcinogenic risk was

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followed to assess human health risk.

2.9.1. Estimated daily intake (EDI)

( ×



)

(1)

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=∑

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Estimated daily intake (EDI) for each analyzed metal (tAs, iAs, Cd, Na, K, and Hg) was calculated as:

where Fi is the consumption of a food group (g/day), Cmi is the metal concentration in a food composite sample (mg/g), W is the body weight of a 70-kg adult, and n is the total number of food

2.9.2. Non-carcinogenic risk

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groups consumed.

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The target hazard quotient (THQ), which is used to express the risk of non-carcinogenic effects, is the ratio between the EDI and the oral reference dose (RfD, mg/kg bw/day) (USEPA, 2000). The oral RfD

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represents an estimate of daily exposure to which the human population can be continually exposed over a lifetime without an appreciable risk of harmful effects. The RfDs are based on 0.0003 and 0.001 (mg/kg bw/day) for i-As and Cd, respectively (Cheng et al., 2013; USEPA, 2000). The RfD for total Hg is 0.0003 mg/kg bw/day (USEPA, 2000). The THQ was calculated based on the following equation (USEPA, 2000):

=

(2)

ACCEPTED MANUSCRIPT If the THQ value is less than 1, the exposed population should not experience any adverse health hazard. On the contrary, the exposed population may experience non-carcinogenic health risks if the THQ is equal to 1, and as the value increases, the probability increases. The method for determining THQ was provided in the USEPA Region III risk-based concentration table (USEPA, 2000). The THQ

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calculations were made based on the facts that the ingestion dose is equal to the absorbed contaminant dose, cooking has no effect on the contaminants (USEPA, 1989), and the average body weight of an adult is 70 kg (Saha and Zaman, 2013). It has been reported that exposure to two or

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more pollutants can result in additive and/or interactive effects. Thus, in the present study, cumulative health risk was evaluated by summing the THQ value of individual metals and expressed as total

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THQ (TTHQ) (also called hazard index, HI) as follows: (3)

When the value of TTHQ is greater, the level of concern is greater. The TTHQ value greater than 1

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generally indicates a potential for adverse human health effects and suggests the need to undertake a higher level of research or possibly remedial action.

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2.9.3. Carcinogenic risk

Para la determina de carcinogenic risk (CR) se siguio la metodologia descrita por Saha & zaman

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(Saha and Zaman, 2013). CR indicates the incremental probability of an individual developing cancer over a lifetime due to exposure to a potential carcinogen. The cancer risk due to an exhibition chronic to i-As was obtained using cancer slope factor (CSF) proposed by the USEPA (2000). The equation used to estimate cancer

risk is as follows: =



(4)

ACCEPTED MANUSCRIPT where CSF is the carcinogenic slope factor of 1.5 and 6.1 (mg/kg/day)-1 for i-As and cd respectively set by USEPA (USEPA, 2000, 2010), and EDI is the estimated daily intake of heavy metals (USEPA, 2000, 2010). The acceptable lifetime CR considered by USEPA (2000) is 10-4 - 10-6 (average risk of

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developing cancer over a human lifetime is 1 in 100000).

3. Results and discussion

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Table 2 shows the mean intake for each food group (g/day) and Na+, K+, Cd, Hg, t-As, and i-As content. The dietary intake was calculated by multiplying the concentration of the mineral or contaminant by the mean intake of that group consumed in the daily diet of an average person (Urieta et al., 1996); (Munoz et al., 2005). Non-alcoholic beverages, bread, and vegetables are the principal groups in the Valdivia diet, which provide over 50% of the total diet intake. These results are

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consistent with those obtained in other TDSs conducted in Italy (66%) (Turrini and Lombardi-Boccia, 2002), Lebanon (66%) (Nasreddine et al., 2010), and Hong Kong (77%) (Wong et al., 2013). Bread

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consumption (244 g/day) was similar to results found in Santiago, Chile (242.7 g/day) and lower than the consumption obtained in Italy (263.5 g/day) (Turrini and Lombardi-Boccia, 2002); this indicates

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that the Chilean population is a major bread consumer. Vegetable consumption (241.3 g/day) was similar in most countries, except for Santiago, Chile (327.3 g/day) (Munoz et al., 2005) and Rio de Janeiro, Brazil (507.6 g/day) (Santos et al., 2004), which exhibited higher vegetable consumption. However, the Valdivia population consumed more non-alcoholic beverages, exceeding the consumption in Santiago (329.8 g/day) by over 60% (Munoz et al., 2005). Non-alcoholic beverage intake in Valdivia was lower than in the UK (1252 g/day) (Rose et al., 2010), Italy (839.1 g/day) (Turrini and Lombardi-Boccia, 2002), and Hong Kong (1625 g/day) (Wong et al., 2013). The

ACCEPTED MANUSCRIPT consumption of meat, fish and seafood, and milk products in Valdivia (78 g, 19 g, and 113 g, respectively) were greater than in the UK (20 g, 14 g, and 82 g, respectively) (Rose et al., 2010) but lower than the consumption of meat, fish and seafood in Cataluña, Spain (126.6 g and 65.4 g,

and depends on cooking customs and food availability.

3.1 Sodium (Na+)

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respectively) (Castells et al., 2008). Food consumption usually differs from one country to another

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The Na concentrations in the analyzed food groups ranged from 0.04 mg/g (potatoes) to 21.72 mg/g (condiments and sauces). In decreasing order, the highest mean levels were found in the spices food

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group (21.72 mg/g) followed by meat products (7.90 mg/g), bread (5.04 mg/g), fats and oils (3.02 mg/g), and sweets (259 mg/g). The remaining food groups contained less than 1.71 mg/g Na+. The condiments and sauces group mainly consists of tomato sauce, soy sauce, soup, and salt; the latter shows a higher Na+ concentration. The food groups in the literature exhibiting the highest Na+

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contents vary depending on the country of origin. In China, (Jiang et al., 2015) report the highest concentration in the vegetable seasoning food item (7.86 mg/g) followed by pork meat from the meat and meat products group (4.22 mg/g). In France, the highest mean levels were found in the salts,

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spices, soup, sauces (8.89 mg/g), and meat and offal (5.20 mg/g) food groups (Chekri et al., 2012). Tanase et al. (Tanase et al., 2011) (2011) report that the ingredients and sauces (15.9 mg/g) and

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soups and fast food (5.15 mg/g) food groups are those that contribute the most Na+ in Canada’s total diet. (Gimou et al., 2014) note that the food groups in Cameroon usually containing the most Na+ were ‘condiments, salt, and flavorings (69.00 mg/g) because of the high raw stock cube and salt composite content (273.00 mg/g).

ACCEPTED MANUSCRIPT The results of the present study and the mentioned literature support the paradigm that most Na+ intake arises from processed foods (bread, bread products, and processed meat among others) more than from unprocessed foods or those of natural origin.

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The condiments and sauces group exhibited the highest Na+ content (21.72 mg/g). However, consumption was low (17.8 g/day) and this group contributed only 12.42% of Na+ EDI (386.62 mg/day).

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On the other hand, meat products (in spite of containing a consumption of 40.4 g/day) were the third highest contributor of Na+ with an EDI of 319.16 mg/day (10.25% of the total); they were also the

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second food group with higher Na+ concentration (7.90 mg/g).

The bread group had the third highest Na+ content (5.04 mg/g), and was at the same time the second highly consumed food group in which the Na-1 EDI reached 1231.3 mg/day (Figure 1). These results are similar to those obtained from the TDSs in Brazil (Avegliano et al., 2011), France (Chekri et al.,

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2012), and Canada (Tanase et al., 2011) where the highest Na contents are found in processed foods instead of fresh and natural products.

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Total Na+ EDI for Valdivia was 3112.8 mg/day, similar to the Na+ intake obtained in New Zealand (2785-2933 mg/day) (Thomson et al., 2008); (MAF, 2009), and it was higher than in Brazil (1928

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mg/day) (Avegliano et al., 2011). The WHO (WHO, 2012b) recommends a Na+ intake of 2000 mg/day. The EDI in Valdivia was over 55% the recommended value. Given that bread consumption in Chile is one the highest worldwide, the Chilean Ministry of Health together with the Chilean Union Federation of Industrial Bakers ratified a voluntary agreement to halve the amount of salt in bread within 4 years. The bakeries implementing this agreement had to gradually decrease the amount of salt from 700 mg/100g Na+ to 400 mg/100g Na+ in 2014 (MINSAL, 2010). The present study shows

ACCEPTED MANUSCRIPT that the mean Na+ content is 504 mg/100g, indicating that the bread group contributes an EDI of 1231 mg/day.

3.2 Potassium (K+)

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The sweets group had the highest K+ concentration (3.05 mg/g) followed by vegetables (2.19 mg/g) and legumes and nuts (1.89 mg/g). The sweets group includes cakes, which are made of wheat flour with a high K+ content. The vegetables group had the highest intake (Figure 2) followed by bread and

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potatoes.

The vegetables group consists of avocado, peas, and green beans, which have a high K+

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concentration. These results are different from those obtained in Brazil where the highest K+ concentrations were in prime grade beef (5.3 mg/g), standard grade beef (4.0 mg/g), and sauces (3.7 mg/g) (Avegliano et al., 2011) and in Canada where herbs and spices (15.9 mg/g) was the composite sample consisting of potato chips (plain and salted) (13.3 mg/g) and yeast (10.4 mg/g) (Tanase et al.,

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2011). The French TDS shows the highest K+ concentrations in cereals and cereal products (4.3 mg/g), ice cream, meat and offal (3.9 mg/g), and sweeteners, honey, and confectionery (3.4 mg/g) (Chekri et al., 2012).

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The EDI for total K+ in Valdivia was 2077.5 mg/day, which is higher than in Brazil (861 mg/day) (Avegliano et al., 2011). The WHO (WHO, 2012a) recommends a K+ intake over 3510 mg/day. The

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EDI in Valdivia was 40% lower than the recommended value. The intake of Na+ (2000 mg/day) and K+ (3510 mg/day) is recommended by the WHO, and the Na+:K+ ratio is approximately 1:1.8, which is considered beneficial for health. The EDI Na+:K+ ratio in the Valdivia population is approximately 1:0.7, which poses a risk of hypertension in this population.

ACCEPTED MANUSCRIPT 3.3 Cadmium (Cd) The food group with the highest Cd content is fish and seafood (Table 2); however, Cd consumption is low and the EDI provided by this group is only 0.57 µg/day (3.2%). Figure 3 reveals that the bread group has the highest EDI (4.88 µg/day) followed by the non-alcoholic beverages (3.78 µg/day) and

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cereals (1.98 µg/day) groups. The Cd EDI obtained from bread is much higher than the Cd intake reported by other TDSs for this food group; for example, 2.46 µg/day in the UK (Rose et al., 2010) and 2.9 µg/day in Lebanon (Nasreddine et al., 2006). However, a study conducted in Cataluña, Spain

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had a Cd intake of 6.06 µg/day for the bread group (Castells et al., 2008), which is lower than the intake reported for this country. For non-alcoholic beverages, the Cd EDI for this food group was

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higher than the value obtained in the study carried out in Lebanon (3 µg/day) (Nasreddine et al., 2006).

The Cd EDI in Valdivia (18.12 µg/day) is similar to the estimates for Santiago, Chile (20 µg/day) (Munoz et al., 2005), Cataluña, Spain (21.57 µg/day) (Castells et al., 2008), Cataluña, Spain (16

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µg/day) (Llobett et al., 2003), Canary Islands (16 µg/day) (Rubio et al., 2006), Korea (14.3 µg/day) (Lee et al., 2006), the UK (9.52-11.56 µg/day) (Rose et al., 2010), Germany (14 µg/day) (Wilhelm et al., 2002), New Zealand (14.04 µg/day) (MAF, 2009), Canada (13.03 µg/day) (Health-Canada, 2007),

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Lebanon (12 µg/day) (Nasreddine et al., 2006), Serbia (11.51 µg/day) (Škrbić et al., 2013), and Belgium (9.52 µg/day) (Vromman et al., 2010); however, the Valdivia value is much lower than the

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estimate obtained in Hulurao, China (31 µg/day) (Zheng et al., 2007). Chilean legislation (Food Sanitary Regulations, RSA) only establish limits for Cd content in edible salt and bottled mineral water (RSA, 2013); this is quite different from the European Union that establishes maximum Cd content for meat, fish, seafood, cereals, and vegetables (CEE, 2001) In June 2010, the FAO/WHO JECFA changed the PTWI for Cd (7 µg/kg bw/week) established in 1989 because of the exceptionally long mean life of Cd; this weekly value was replaced by a monthly value, PTMI, of 25 µg/kg bw/month for a 68-kg adult. In Europe, the CONTAM Panel (EFSA, 2009a)

ACCEPTED MANUSCRIPT established a tolerable weekly intake (TWI) of 2.5 µg/kg bw (25 µg/day for a 70-kg adult); this does not coincide with the recommendation established by the FAO/WHO because the European recommendation is lower. The Cd EDI obtained in the present study is therefore 31.8% of the PTMI recommended by the FAO/WHO and 72% of the TWI recommended by the EFSA; hence, Cd would

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not pose a risk to human health. On the other hand, the calculated THQ value for Cd was 0.26, which also indicates that this metal does not pose a risk to the health of the Valdivia population.

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3.4 Mercury (Hg)

The groups exhibiting the highest Hg concentrations were fish and seafood (26.6 µg/kg) and cereals

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(9 µg/kg) (Table 2). The Hg concentration in the fish and seafood group did not exceed the maximum limit established by the RSA (0.5-1.5 mg/kg bw) (RSA, 2013). None of the other groups reached the maximum stipulated in Chilean legislation.

Figure 4 illustrates that the non-alcoholic beverages group had the highest Hg EDI (1.13 µg/day)

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followed by bread (0.98 µg/day) and cereals (0.94 µg/day). It is important to mention that the fish and seafood group had the highest Hg content; however, this group is included in the groups with the highest EDIs of this contaminant because fish and seafood consumption is low (18.6 g/day).

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Estimated exposure to Hg in the diet of the Valdivia population (5.7 µg/day) is similar to the estimate for Santiago, Chile (5.0 µg/day) (Munoz et al., 2005). These values were lower than those reported in

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China (8.86 µg/day) (Li et al., 2006), Cataluña, Spain (14.54 µg/day) (Castells et al., 2008), and Canada (22 µg/day ) (Dabeka et al., 2003). However, the Hg EDI in Valdivia was high when compared to other countries such as New Zealand (0.094 µg/day) (MAF, 2009), the Jinhu area in China (0.12µg/day) (Sun et al., 2011), Korea (1.61µg/day) (Lee et al., 2006) and the UK (1.4-3.4 µg/day) (Rose et al., 2010).

ACCEPTED MANUSCRIPT In 2003, the JECFA revised its risk assessment for MeHg in fish and adopted a lower PTWI of 1.6 µg/kg bw/week to replace the previous PTWI of 3.3 µg/kg bw/week of total Hg for the general population (JECFA, 2004). The FAO/WHO recommends a total Hg PTWI of 5 µg Hg/kg bw/week, which is equivalent to 50

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µg/day for a 70-kg adult; this value is almost ten times greater than the Hg intake by the Chilean population under study (5.7 µg/day). Thus, Hg EDI does not pose a risk to the health of the Valdivia population. The THQ calculation, which is used to express the risk of non-carcinogenic effects of

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mercury, using an RfD of 0.0003 mg/kg bw/day (ATSDR, 1999) provides a value of 0.27 that is < 1;

3.5 Total arsenic (t-As)

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this indicates that the exposed population might not experience any adverse health effects

The fish and seafood group had the highest t-As concentration (1.84 µg/g) followed by cereals (0.04

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µg/g) and meat (0.03 µg/g) (Table 2).

The fish and seafood group had the highest As content In most consulted TDSs; this is the case for studies carried out in Santiago, Chile (1.35 µg/g) (Munoz et al., 2005) with variations among countries

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probably because of the type of fish consumed: the UK (3.99 µg/g) (Rose et al., 2010), Cataluña, Spain (5.41 µg/g) (Castells et al., 2008), and Canada (1.66 µg/g) (Dabeka et al., 1993).

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The Food Sanitary Regulations (RSA, 2013) establish a maximum limit for t-As in food products, which was not exceeded in any of the groups analyzed in the present study. However, the value established by the RSA for fish and seafood cannot be directly compared to the fish and seafood group because this legislation establishes a maximum limit of t-As for fish (1 µg/g tAs) and i-As for mollusks, crustaceans, and gastropods (2 µg/g i-As); the group with the highest concentration in both studies consisted of both fish and seafood.

ACCEPTED MANUSCRIPT Figure 5 displays the groups with the highest t-As EDIs, that is, fish and seafood (34.31 µg/day), nonalcoholic beverages (10.66 µg/day), and bread (5.48 µg/day). The fish and seafood group contribute 26% t-As to EDI in the present study. The estimation of t-As EDI in the total diet in Valdivia (73.02 µg/day) is similar to results from studies

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conducted in Santiago, Chile (77 µg/day) (Munoz et al., 2005), Canada (64.26 µg/day) (HealthCanada, 2007), France (54-56 µg/day) (Nougadere et al., 2012), but higher than estimates reported in Korea (38.5 µg/day) (Lee et al., 2006). On the other hand, t-As EDI obtained in New Zealand

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(102.6 µg/day) (MAF, 2009), the UK (115.5-117.6 µg/day) (Rose et al., 2010), the Ron Phibun District, Thailand (68.2-564 µg/day) (Ruangwises and Saipan, 2010), the Dan Chang District,

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Thailand (92.2-561 µg/day) (Ruangwises et al., 2011), Cataluña, Spain (339.05 µg/day) (Castells et al., 2008), India (568 µg/day) (Uchino et al., 2006), and Belgium (285-649 µg/day) (Baeyens et al., 2009) were higher than the values found in the present study.

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3.6 Inorganic arsenic (i-As)

The groups with the highest i-As concentrations were fish and seafood (0.043 µg/g), condiments (0.026 µg/g), and eggs (0.015 µg/g) (Table 2). The fish and seafood group in studies conducted in

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Cataluña, Spain (0.134 µg/g) (Castells et al., 2008) and the UK (0.015 mg/kg) (Rose et al., 2010) obtained the highest i-As concentrations.

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The highest i-As EDIs are shown in Figure 5 for the non-alcoholic beverages (4.027 µg/day), bread (3.18 µg/day), and vegetables (2.17 µg/day) groups. The EDI (19.78 µg/day) obtained in the present study is similar to reported intakes in other studies, such as in the Ron Phibun District, Thailand (15.8-146 µg/day) (Ruangwises and Saipan, 2010), New Zealand (18.3 µg/day) (MAF, 2009), the Dan Chang District, Thailand (20.2-120 µg/day) (Ruangwises et al., 2011), Cataluña, Spain (27.40 µg/day) (Castells et al., 2008), and Cataluña, Spain (35.05 µg/day) (Martí-Cid et al., 2008).

ACCEPTED MANUSCRIPT The FAO/WHO 1989 recommendation for i-As PTWI was 15 µg/kg bw (equivalent to 150 µg/day for a 70-kg person); in accordance with this recommendation, the i-As EDI value was 19.78 µg/day, which is lower than the recommended maximum. The EDI obtained in the present study was lower than the value established by the EFSA (EFSA, 2009) (0.3-8 µg/kg bw/day), which is the equivalent of 21-560

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µg/day intake for a 70-kg person. This reaffirms that the EDI for i-As in the Valdivia population would not represent a danger to the population.

The THQ calculation, which is used to express the risk of non-carcinogenic effects of i-As, using an

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RfD of 0.00030 mg/kg bw/day (USEPA, 2000) provides a value of 0.96 that is slightly < 1; this indicates that the exposed population might not experience any adverse health effects (Saha et al.,

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2016). Likewise, the CR calculation values for i-As obtained in this study were 0.00043, exceeding the cancer risk benchmark (1 in 100 000 inhabitants) by reaching a risk value of 44 in 100 000 inhabitants. Risk is considered low for the population under study.

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4. Conclusions

The estimated sodium and potassium intake of the Valdivia population does not follow the recommended values established by the WHO. Sodium intake exceeds the daily recommended value

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and potassium intake is less than the recommended value. This indicates that the health of the Valdivia population is at risk if no clear policy is established with respect to sodium intake through

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food consumption; the population could exhibit health problems such as hypertension and/or cardiovascular disease. As for the EDIs of cadmium, mercury, total arsenic, and inorganic arsenic of the Valdivia population, these do not exceed the toxicological reference values established by the FAO/WHO or the EFSA, and no health risk exists. However, the cumulative Non-carcinogenic risk was evaluated by summing the target hazard quotient of cadmium (0.26) mercury (0.27) and inorganic arsenic (0.96); this calculation allows us to express the total target hazard quotient as 1.50 where a value > 1 indicates that there is a potential health risk for the population. On the other hand,

ACCEPTED MANUSCRIPT the risk of contracting cancer due to the exposure to inorganic arsenic reaches a value of 0.00043, and a value of 0.00158 for Cadmiun The mean CR value for the food consumption was 0.00201, which was about 20 to 2000 times higher than an acceptable range of 1x10-6 to 1x10-4 (USEPA, 2010).

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It also has been reported that the exposure to two or more contaminants may result in additive and/or interactive effects, which indicates an increased risk of adverse health effects (Ji et al., 2013). Given the lack of Total Diet Studies in Chile, conducting periodic studies by establishing a chemical

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food security vigilance program is recommended. This scrutiny will allow identifying nutrient deficiency or excess and the degree of exposure of the population to chemical contaminants, which

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would help to prevent possible health problems and establish recommendations for the country.

Acknowledgments

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The authors are grateful to the Direction of Research Development of the University Austral of Chile

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(DID research grant n°. DID-2015-11) for financial support.

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ACCEPTED MANUSCRIPT TABLES Table 1. Food groups included in the Valdivia Total Diet Study and the quantity consumed (g/day) Condiments and sauces

Cereals

Fats and oils

Fish and seafood

12.5

Rice

44.3

Mayonnaise

5.9

Hake

4.2

Soup

1.9

Pasta

21.9

Vegetable oil

5.3

Salmon

4.0

Salt

1.8

Cookies

17.9

Butter

2.5

Tuna

2.1

Other spices

1.6

Fried tortilla

10.2

Margarine

1.7

Snook

2.1

Total

17.8

Wheat flour

4.4

Other fats

0.3

Clams

1.6

Wheat bran cookies

2.3

Total

15.7

Mackerel

1.5

Others

3.0

Silverside

0.8

Total

104.0

Mussels

0.5

Sweets

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Tomato sauce

Cakes

30.4

Sweeteners

14.4

Chocolate

7.7

Meat products

Jams and marmalades

6.5

Bologna

8.8

Milk

Jellies

3.7

Sausage

8.0

Whole milk

Other sweet products

4.4

Pâté

6.9

Flavored milk

Total

67.0

13.1

19.1

6.5

Powdered milk

18.4

Tomatoes

70.8

Skim milk

7.4

Lettuce

38.8

3.5

Cultured milk

4.7

Avocado

32.9

0.6

Other

3.8

Peas

32.6

40.4

Total

116.4

Pumpkin

14.8

Onion

10.8

Others

14.0

Total

White wine

5.2

Malt

2.1

Milk products

Chicha

1.0

Yogurt

Others

3.2

Cheese

Total

50.4

Ice cream

9.8

Beans

Desserts

9.6

Chickpeas

Cream

3.1

Other

0.1

Water

331.6 Others

2.6

Total

25.3

Soda pop

103.0 Total

112.8

Boxed juices

82.2

Mineral water

17.0

Fruit

Other drinks

5.8

Apple

Total

539.6 Peach

Turkey

6.2

Lentils

Legumes and nuts

9.5

Carrots

5.4

30.2

Corn

7.9

Red beet

5.0

6.3

Other vegetables

23.8

1.5

Total

241.3

EP

TE D

Green beans

57.5

Bread White bread

173.8

23.3

Homemade bread

44.2

10.5

Whole wheat bread

11.5

Orange

10.4

French bread

9.8

Lemon

9.9

Other breads

5.0

47.8

Banana

9.7

Total

244.3

18.1

Grapes

5.4

8.6

Pear

5.0

Potatoes Potatoes

AC C

Pork

Vegetables

6.0

24.9

Chicken

18.6

Ham

Red wine

Red meat

Total

63.0

Beer

Meat

0.9 0.8

Hotdog Hamburger

Non-alcoholic beverages

Other seafood

Other fish

SC

Eggs

M AN U

Alcoholic beverages

Eggs

1.7

Chestnut

2.5

Other meat

1.3

Pineapple

1.9

Total

77.5

Other fruit

10.9

Total

89.6

129.0

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Table 2. Mean concentrations of Na, K, Cd, Hg, t-As, and i-As in the total diet food groups.

Alcoholic beverages

Mean intake (g/day) 50.4

Bread

244.3

5.04

1.05

0.020

0.004

0.022

0.013

Cereals

104.0

1.04

0.57

0.019

0.009

0.041

0.018

Condiments and sauces

17.8

21.72

1.34

0.010

0.005

0.031

0.026

Eggs

13.1

1.06

0.84

0.016

0.003

0.018

0.015

Fats and oils

15.7

3.02

0.09

Fish and seafood

18.6

1.71

1.70

Fruit

89.6

0.06

0.85

Legumes and nuts

25.3

0.83

1.89

Meat

77.5

1.38

1.83

Meat products

40.4

7.90

Milk

116.4

1.65

Milk products Non-alcoholic beverages Potatoes

112.8

1.67

539.6

0.06

129.0

0.04

Sweets

67.0

Vegetables

241.3

0.001

Total Arsenic (µg/g) 0.017

Inorganic Arsenic (µg/g) 0.009

Potassium (mg/g)

Cadmium (µg/g)

Mercury (µg/g)

0.07

0.32

0.005

M AN U

SC

RI PT

Sodium (mg/g)

0.001

0.018

0.008

0.031

0.026

1.845

0.043

0.002

0.003

0.015

0.006

0.008

0.002

0.013

0.008

0.007

0.001

0.033

0.008

1.62

0.008

0.003

0.013

0.013

1.67

0.009

0.002

0.018

0.012

0.82

0.008

0.001

0.018

0.011

0.18

0.007

0.002

0.020

0.007

1.78

0.010

0.006

0.012

0.012

2.59

3.05

0.002

0.003

0.022

0.010

2.19

0.005

0.001

0.019

0.009

EP

TE D

0.028

AC C

Food Group

1.02

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FIGURES Figure 1. Sodium intake for each food group (mg/day, wet weight). Arithmetic means (bar charts) and standard deviations (error bars) of the three samplings.

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Figure 2. Potassium intake for each food group (mg/day, wet weight). Arithmetic means (bar charts) and standard deviations (error bars) of the three samplings. Figure 3. Cadmium intake for each food group (µg/day, wet weight). Arithmetic means (bar charts) and standard deviations (error bars) of the three samplings.

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Figure 4. Mercury intake from each food group (µg/day, wet weight). Arithmetic means (bar charts) and standard deviations (error bars) of the three samplings.

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Figure 5. Total and inorganic arsenic intake for each food group (µg/day, wet weight). Arithmetic means (bar charts) and standard deviations (error bars) of the three samplings.

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