Sponsored jointly by FAO and WHO


    Food and Agriculture Organization of the United Nations


    pesticide residues in food:
    1981 evaluations

     the monographs

    data and recommendations
    of the joint meeting
    of the
    FAO panel of experts on pesticide residues
    in food and the environment
    and the
    WHO expert group on pesticide residues

    Geneva, 23 November-2 December 1981

    Rome 1982



         The 1968 Meeting reviewed bromide ion, and data relevant to this
    material are also included in the various reviews of brominated
    fumigants, especially bromomethane, carried out in 1965, 1966, 1967,
    1968, 1971 and 1979*. At the 1980 Meeting it was considered that a
    general review of bromide residues in relation to dietary intake
    should be considered in 1981 or at a future meeting. This monograph
    addendum sets out some data on intake as measured in total diet
    studies and some information on 'natural' crop levels.



         Manske and Corneliussen (1974) reported that bromide ion residues
    were present in 81 out of 120 food composites examined in their total
    diet survey carried out in the USA in June and August 1970; the range
    of results reported was from 0.5 to 51 mg/kg. Bromide analysis of the
    total diet samples was subsequently discontinued and has not been
    resumed. Results reported are shown in Table 1; comparable data had
    been obtained in earlier years.

    TABLE 1.  Bromide ion residues in total diet food composite groups,
              1970, USA
    Food group          Residues found (mg/kg)                  Average
    Dairy products      1.5, 2.0, 3.0, 4.0, 5.0, 5.0, 5.5         3.7
    Meat, fish and
     poultry            2.0, 3.5, 4.5, 5.5, 6.5, 7.5, 8.0         5.4
    Grain and cereal    7.0, 9.0, 14, 14, 14, 22, 25, 30         17
    Potatoes            1.0, 1.0, 2.0, 4.0, 13, 16                6.2
    Leafy vegetables    0.5, 1.0, 1.5, 2.5, 2.5, 3.0,
                         4.0, 4.0, 5.1                            7.8
    Legume vegetables   1.5, 1.5, 2.0, 2.0, 4.0, 5.5              2.8
    Root vegetables     0.5, 1.5, 3.5, 4.0, 4.0, 5.0, 6.0         3.5
    Garden fruits       0.5, 3.0, 3.5, 3.5, 4.5, 5.0, 6.0         3.7
    Fruits              0.5, 1.5, 1.5, 5.5, 6.0, 6.5              3.6
    Oils and fats       2.5, 5.5, 12, 12, 12                      8.8
    Sugars, etc.        0.5, 3.5, 5.5, 6.0, 7.5, 9.5, 12, 23      8.4
    Beverages           1.5, 2.0, 2.0, 2.5, 3.0                   2.2


    *    See Annex II for FAO and WHO documentation.

         A report on total bromine residues observed in a total diet
    survey carried out in the United Kingdom in 1978-79 was made available
    to the Meeting (UK 1981). Table 2 shows the results obtained on each
    food group; five complete sets of food composites were examined.
    Levels are broadly similar to those shown in the survey by Manske and
    Corneliussen (1974) in the USA.

    TABLE 2.  Total bromine content of total diet samples, 1978-79, UK

    Food Group             Total bromine residues          Daily intake
                                  (mg/kg)                  of bromine
                           Range            Mean

    Cereals                6 to 11           7.4              1.7
    Meats                  4 to 5            4.4              0.7
    Fish                   3 to 6            4.6              0.1
    Fats                   <5                5              < 0.4
    Fruits and sugars      1 to 5            2.4              0.4
    Root vegetables        2 to 4            2.6              0.5
    Other vegetables       6 to 40          19.2              2.1
    Beverages              <1                1              < 0.1
    Milk                   3 to 10           6                2.4

    Total                                                     8.4

         Data on the bromine ion content of summer and winter duplicate
    24-hour diets of workers were received from the Netherlands (Greve and
    Verschraagen 1977, 1978). Table 3 shows the ranges and means of the
    bromide ion content of the diets and the corresponding daily intakes
    per person.

        TABLE 3.  Bromide ion content of duplicate diets in the Netherlands

                                  Bromide ion content           Daily bromide ion intake
    No. in       Season           (mg/kg)                       per person (mg)
                                  Range          Mean           Range          Mean

    100          Summer, 1976     1.2-11.7       3.6            2.9-15         7.8
    101          Winter, 1978     1.1-8.2        3.2            1.8-17         7.6
         A further report from the Netherlands gave details of a two-year
    total diet (market basket) study based on the diets of 16 to 18-year-
    old boys (de Vcs and van Dokkum 1980). Table 4 shows the detailed
    results on the 12 samples in each of the 12 groups into which the
    diets were divided. Maximum intake per person has been calculated from
    these results to be 13.4 mg, with a mean figure of 9.4 mg. In the
    Netherlands, the maximum permissible daily intake is regarded as being
    10 mg per person.

    TABLE 4.  Bromide ion content of total diet groups

    Food Group                  Range            Mean           Median
                                (mg/kg)          (mg/kg)        (mg/kg)

    Grain products              10-19             13             12
    Potatoes and potato
      products                  0.55-16            3.4            2.4
    Green vegetables            0.9-5.8            2.1            1.7
    Root vegetables             0.36-3.2           2.0            2.1
    Leguminous vegetables       0.70-5.0           1.7            1.4
    Fruits                      0.07-4.9           0.82           0.28
    Meat and meat
      products                  2.1-4.0            3.1            3.1
    Fish                        4.6-8.0            6.6            6.7
    Milk and milk
      products                  1.7-5.5            3.6            3.9
    Oils and fats               5-22              11             10
    Sugar and preserves         0.7-2.2            1.3            1.3
    Beverages and drinking
      water                     0.09-0.30          0.19           0.20

         Inorganic bromine in soils in the United Kingdom do not normally
    exceed 5 mg/kg dry weight, except for coastal soils which can attain
    levels of 100 mg/kg. Levels in rain water and surface waters generally
    do not exceed 1 mg. Information drawn from a review of the literature
    indicates that natural bromine levels in fresh fruit and vegetables
    can generally be expected to be below 10 mg/kg fresh weight and will
    not normally exceed 50 mg/kg fresh weight. Table 5 gives some UK
    'natural' levels of total bromine, which were found from the analysis
    of a limited survey on the elemental composition of field crops,
    undertaken in 1976 (UK 1981).

    TABLE 5.  'Natural' levels of total bromine in crops grown in
              the UK
    Crop1               Range of total bromine levels in five different
                                   cultivars of each crop
                                   (mg/kg fresh weight)
    Wheat                              0.6 - 1.0
    Barley                             1.9 - 3.7
    Cabbage                            0.3 - 2.0
    Potatoes                           0.3 - 1.0
    Broad beans                        0.5 - 1.1
    Peas                               0.5 - 3.0
    1  Grain and vegetable samples were obtained from various
    experimental stations, prepared as for cooking or eating, sliced or
    shredded, air dried and analysed by neutron activation techniques.

         In 1979, 10 samples of wheat flour intended for human consumption
    were analysed for bromide ion content. Levels found ranged from 1.4 to
    9.0 mg/kg, with a mean value of 4.5 mg/kg (UK 1981).

         The use of bromomethane as a soil sterilant in glasshouses can
    give rise to bromide ion residues in subsequent crops. Retail samples
    of tomatoes, cucumbers and lettuces, home produced and imported, have
    therefore been examined for total bromine levels. In tomatoes, levels
    were generally below 5 mg/kg, but exceeded 30 mg/kg in 12 of the
    samples. Of 107 samples of cucumbers, 102 had less than 5 mg/kg of
    total bromine, but two had more than 100 mg/kg. Residue levels in
    lettuce were much more evenly spread, ranging up to 2 000 mg/kg;
    although the majority were below 100 mg/kg, 20 percent of the samples
    examined exceeded this figure (UK 1981).

         A range of 22 samples of bottled, canned and draught beers was
    examined for bromide ion content; results are shown in Table 6. Levels
    are remarkably consistent and generally low, with a maximum of
    2.1 mg/kg (UK 1981).

    TABLE 6.  Bromide ion content of various beers
                                            Bromide ion concentration
    Commodity              No. of 1                (mg/kg)
                                            Range               Mean
    Bottled beers             32            0.37 to 1.5         0.8
    Canned beers              20            0.85 to 2.1         1.4
    Draught beers             36            0.53 to 1.3         0.9
    1  Each sample was analysed four times.

         The use of organobromine fumigants in food storage practice and
    in the treatment of soil used for the production of glasshouse crops
    has resulted in bromine residues in foodstuffs being raised above
    'natural' levels.

         Cereals, vegetables (other than root vegetables) and milk are the
    most important contributors to bromine residues in the average diet.
    Extensive data on bromine residues in milk are not available, apart
    from the data obtained in the analysis of the UK total diet samples
    where the levels found ranged between those found in other dietary
    items. Further work is desirable to study levels of bromine in milk
    and milk products, because the consumption of milk is high and this
    item of the diet can contribute significantly to the overall intake of
    bromine. The high bromine contribution from the cereals group is
    probably a reflection both of the extensive use of bromomethane as a
    cereal fumigant and of the large daily consumption of such foods as
    bread or breakfast cereals.

         The 'other vegetables' group of the total diet includes lettuces,
    which appear to be items most likely to give rise to high dietary
    intakes of bromine. Average consumption of lettuce containing average
    amounts of bromine residues is not likely to lead to a daily intake in
    excess of the present ADI.


         Methods for the determination of bromine in foods, as organic,
    inorganic or total, have been reviewed by Getzendaner (1975). The gas-
    liquid chromatographic procedure developed for bromide ion in grain
    (Heuser and Scudamore 1970), has been adapted for use on lettuce as
    reported by Greve and Grevenstuck (1979), and versions of this method
    are now widely accepted for use on various foodstuffs.



         Some data on dietary intakes of bromide ion in USA (1970), UK
    (1978-79) and the Netherlands (1976-80) have been reviewed, together
    with some additional information regarding 'natural' and post-
    treatment levels in some crops. The average daily intakes of 8.4 mg
    (UK) and 9.4 (Netherlands) compare favourably with the calculated
    allowable daily intake for a 60 kg adult of 60 mg.



    1.   Data on dietary intake of bromide ion from countries other than
         the Netherlands, USA and UK, especially those with different
         dietary patterns.

    2.   Further data on the bromide ion content of milk and dairy


    de Vos, R.H. and van Dokkum, W. Kwantitatief onderzoek naar de
    1980      aanwezigheid van additieven in chemische contaminanten in
              totale dagvoedingen. Rapport nr. R. 6331 (CIVO/TNO).

    Getzendaner, M.E. A review of bromine determination in foods. Journal
    1975      of the Association of Official Analytical Chemists, 58:
              711 - 716.

    Greve, P.A. and Grevenstuck, W.B.F. Gas-liquid chromatographic
    1979      determination of bromide ion in lettuce: interlaboratory
              studies. Journal of the Association of Official Analytical
              Chemists, 62: 1155 - 1159.

    Greve, P.A. and Verschraagen, C. Anorganisch bromide in totale dieten.
    1977      Intern rapport nr. 75/77 Tox-RoB (RIV). (Unpublished)

    1978      Anorganisch bromide in duplicaat 24-unrsvoedingen. Intern.
              rapport nr. 162/78 RA (RIV). (Unpublished)

    Heuser, S.G. and Scudamore, K.A. Selective determination of ionised
    1970      bromide and organic bromides in foodstuffs by gas-liquid
              chromatography. Pesticide Science, 1: 244 - 249.

    Manske, D.E. and Corneliussen, P.E. Pesticide residues in total diet
    1974      samples (VII) Pesticides Monitoring Journal, 8: 110 - 124.

    UK        Information on bromide ion residues from the United Kingdom.
    1981      (Unpublished).

    See Also:
       Toxicological Abbreviations
       Bromide ion (FAO/PL:1968/M/9/1)
       Bromide Ion (FAO/PL:1969/M/17/1)
       Bromide Ion (Pesticide residues in food: 1983 evaluations)
       Bromide ion (Pesticide residues in food: 1988 evaluations Part II Toxicology)