Salicylates in foods
Transcription
Salicylates in foods
..,t1a.tad fro. JOt'2KAl. 0' ra! .wa.C.\X DttTE'T!C ASSOCUrtJR Yol. UNa. a Aqu.tlt l'ljllll5 Copyt'15tc: � '-r1c.aa 1H..uc1c �1.Uo. Pnaud .La. tJ.S ...... Volume 85 August 1985 Number 8 Research 95 0 �==�----------------------------�---------------------------- Salicylates in foods Anne R. Swain, Stephen P. Dutton, and A. Stewart Truswell' Human Nutrition Unit. University of Sydney, New South Wales, Australia To determine salicylate content, 333 food items were anaivzed. Foods were homogenized with 25% sodium hydroxide, allowed to stand overnight, acidified with concentrated hydrochloric acid, and then extracted with warm diethyl ether over 5 hours. The extract was dried a�d taken up in dilute sodium bicarbonate solution tor analysis. Salicylic acid was separated by high perform ance liquid chromatography and quantified by reading at 235 nm. Salicylic acid standards were used throughout to standardize extractions and analyses. This is the most comprehensive set of data on food salicylates yet pU.b lished; extraction appears to have been more complete tor some foods, giving higher values than those previously published. ,'vlost fruits, eS;Jecially berry fruits and dried fruits, contain salicylate. Vegetables show a wide range from 0 to 6 mg salicylate per 100 gm food (for gherkins). Some herbs and spices were found to contain very high amounts per 100 gm, e.g., curry powder, paprika, thyme, garam masala, and rosemary. Among beverages, tea provides substantial amounts of salicylate. Licorice and peppermint candies and some honeys contain sal icylates. Cereals, meat, fish, and dairy products contain none or negligible amounts. The Feingold diet for treatment of hyperactivity in chil dren was devised to exclude foods that contain artificial colorings, artificial flavorings, and natural salicylates. Exclusion of fruits and vegetables was based on German analyses of sal icylate content done at the turn of the century. Information on the exact quantities of salicylate in foods has not been generally available , nor has it been 'The .uthor<; t�ank Mr<;. S. Vindedz,s and Or. F B. Wh,tehead ;or copies of unpublished references '24 and 51) Th�v are .ery grateful to Professor A. Basten, Josephme Rogers, MaXlne Hosk,ng, Dr. Roberc Lobl.y, Dr. Shervl Van Nunen and Professor R. CI.ncy for support and encouragement and 10 Ceo" Hutct'ison ror IHPLC' methodology. The adVice on high performance liqUid chromatography authors also thank Dr. I. R. Brown and M. P. Smyth !Mass Specuometry Un,t, School oi Chemistry, Linlyef>ity or Sydney) ior the CC-.MS salicylate peaks irom the HPLC. co�f"mation of certain whether permitted foods are completely free of salicylate. There have been claims from fruit canners that some of the fruits excluded by Feingord did not contain appreciable salicylate. Emphasis on salicylates in hyperactivity has decreased; there has been more interest lately in artificial colors (1). Meanwhile, interest has been growing in the role of salicylates in some cases of urticaria and of asthma. It has long been known that urticaria may follow the ingestion of acetyl salicylic acid medication, but it is now realized that salicylates in foods also can precipitate acute urticaria or exacerbate chronic urticaria. Salicylate-sensitive urticaria was first nored by Calnan (2,3). Warin (4) in 1960 reported that 22 of 70 patients with chronic urticaria developed exacerbations after adminis tration of aspirin. Moore-Robinson and Warin (5) reported an incidence of 22% of 228 patients, and Champion et al. (6) in 1969 found that 21% of 268 patients with chronic urticaria reacted to aspirin. lames and Warin (7) in 1970 reported further investigations in a series of 100 patients with chronic urticaria. Ninety-six patients had been given test doses of aspirin in a "patient blind" manner; 37 of the 96 patients gave a positive reaction to the test dose. Several authors reported that diets constructed to ex clude salicylate mav induce prolonged remission of urti caria in those patients who have shown a positive re sponse to oral aspirin challenge (8-11). In 1972, Lackey (12) discussed the part played by salicylates in various foods. Seventy-five percent of the patients of Warin and Smith (11) either cleared or considerably improved after being on the appropriate diet for a 2-month period. This improvement was in line with the results obtained by others, including Michaelsson and Juhlin (8) in 1973 and Doeglas (9) in 1975. More recently, Ros et al. (13) reported their results with exclusion diets. Fifty-nine patients who reacted to salicylates, preservatives, and azo dyes were given a diet designed to reduce consumption of those items. This produced remission in 24% and improvement in 57%. Similarly, Juhlin (14) in 1981 reported that most patients improve when given a diet free from the chemi cals to which they reacted. It is well known that aspirin may exacerbate asthma. McDonald et al. (15) reported that 8 of 42 patients with severe asthma and no history of aspirin exacerbations reacted to an aspirin challenge ci 540 mg. Journal of The American Dietetic Association Research Because we could find no comprehensive list of amounts of salicylate in foods, we extended a clinical study of oral challenges (aspirin, tartrazine, preservatives, and brewers yeast) in patients with chronic urticaria (16,17) and started to estimate salicylates in some local fruits and vegetables. Early reports on salicylates in foods used thin-layer chromatography (18-24). More recently, most reports in the literature have used gas chromatography with mass spectrometry (25-49). Details of how the salicylate was extracted before estimation have usually been sparse or even lacking. We used thin-layer chromatography at first a!1d then for more precise quantitation developed a sensitive specific method of high performance liquid chromatography and combined it with an efficient liquid extraction procedure. We have used the following method to measure salicylate in most common foods. Extraction efficiencies were calculated. They varied with the composition of the food. Fruits, vegetables. condi ments, and beverages gave extraction rates of greater them 85%, compared with cereals and protein foods for which the extraction rate was approximately 60%. Validation was carried out by extracting several foods 20 times along with spiked samples. Several foods were selected which, by previous analysis, had been found to contain salicylate in amounts that were relatively low (carrots and pumpkin), medium (orange and pineapple), or high (thyme). The roods had varied physical attributes. For a further discussion of the methodology, see the appendix. Method Samples of foods and beverages weighing approximately 100 gm were homogenized in a commercial blender, along with 100 ml 25% sodium hydroxide and 2 gm calcium chloride. Duplicate samples corresponding to 50 gm food or beverage were weighed out. To one sample of each pair,S mg salicylic acid standard was added. 80th samples were allowed to stand overnight. The two ho mogenates were then acidified with concentrated hydro chloric acid (HCI) (AR grade) and placed in separate liquid extractors. Two hundred milliliters diethyl ether was placed m a round-bottomed flask, along with several glass boiling beads to prevent bumping. The flask was then placed in a heating mantle and connected to the liquid extractors and condensers. Extraction was carried out for 5 hours. The ether extract was next allowed to cool and to evaporate to dryness in the fume cupboard. The sample was then taken up in 20 ml 2% sodium bicarbonate (NaHCO)l and filtered prior to analysis. The high performance chromatographic system con� sisted of a Varian 5060 pumping system with Rheodyne 7125 injection valve, several different detectors, Varian COS III computing integrator, and Houston Omniscribe recorder. The column was a Waters ),I.Bondpak (18 reverse phase column (300mm x 4 .6mm ) fitted with a precolumn packed with Vydac RP P389 packing material. The eluent was monitored with a Varian Vari-Chrom variable wavelength detector with waveiength at 235 nm con nected to the recorder; 20 ),1.1 samples were injected. The isocratic solvent was 20% methanol (Ajax Unicnrom), 80% glass-distilled water with 0.01 mMol orthophosphoric acid and ion paiting reagent of 0.0025 mMoI tetra butylammonium phosphate (TBAP) made to pH 7.0 with 25% sodium hydroxide solution . The sali cylic acid standard was 0.25 gm/L in 2% NaHCO) and was stored at 4OC. The column was operated with an isocratic solvent at ambient temperature and a flow program which resulted in a back pressure of 90 to 150 atmospheres. The flow rate was 1.0 mllminute for 7 minutes, increasing to 2.0 ml! minute over the next 3 minutes. Results from triplicate or multiple extractions were used to calculate the total salicylate per 100 gm food sample. Results and discussion This article presents a list of foods that we have analyzed for salicylate. When present in significant amounts, sali cylate is reported as milligrams per 100 gm edible portion. Items are arranged by food groups in Table 1. The two right-hand columns of the table summarize information currently available in the literature. Fruits We found that most fruits contained considerable amounts'of salicylate. Raisins and prunes had the highest amounts. Most berry fruits are significant sources of salicylate, with a range from 0.76 mg/l00 gm for mulber ries to 4.4 mgl100 gm for raspberries. Apples showed considerable variation of salicylate content between vari eties. Dried fruits have relatively high salicylate coments compared with their fresh counterparts because of the removal of water during the drying process. Heat process ing for canning does not seem to affect appreCiably the salicylate content of fruit. We had the impression that those fruits low in salicylate often have a less piq'Jant flavor, e.g., mangos, pawpaws, and pears, compared with pineapples, oranges, and the berry fruits. Vegetables Within the vegetable group, salicylate content varied widely among the raw foods. It ranged from negiigible in bamboo shoots, dried beans, green cabbage, celery, lentils, lettuce, dried peas, and swedes to a high of 6.1 mg/l00 gm in gherkins. Fresh tomatoes contain only small amounts of salicy late, 0.13 mg/100 gm. However, many commonly used tomato products are considerable sources of salicylate: canned tomatoes, 0.53 mg; tomato paste, 1.44 mg; tomato sauce, 2.38 mg; and tomato soup, 0.54 mg. The increase in available salicylate in th"! processed tomato products compared with the fresh can be attributed to the use of a fully ripe raw material, to cooking, and to concentration, but it is probably due mainly to the addition of flavoring herbs and spices. Condiments Some of the herbs and spices contain much more salicy late than has previously been reported for any food. We found that curry powder contains 218 mg salicylate per 100 gm. Others almost as high were paprika, thyme, dill powder, garam masala, oregano, and turmeric. Although amounts of these condiments used in food are 951 Table 1. Salicylates in 333 foods'" type food 952 fnlit apple apricot Ardmona John West Soc om in John West Australian rockmelon sweet lohn West Morello Sour cranberry S. &. w. cu rrants black currant red currant (from Queensland) custard apple dates figs guava gra pes CaI ·D ate S. & W. Kadota Calamata string Gold Reel Red Malaila Sul tan a S. & w. light seedless Berfi Dark Sanitarium Light currants I.P.e. raisins A.D.F.A. sultana grapefruit Berri kiwi fruit lemon loganberry leq ua! lychee mandarin mango mulberry nectarine orange John West Berri passion fruit pawpaw peach pear persimmon pineapple salicyla.te reported in literature references mglfOOgmt Golden Delicious Red Delicious Granny Smith lonathan Ardmona Mountain Maid Letona avocado banana blackberry blueberry boysenberry canteloupe cherry state Letona letona Packham (with skin! Packham (Aa sk in l William (With skin) Letona Bartlett Go l de n C irc le fresh fresh fresh fresh canned juice fresh canned nectar fresh fresh canned canned canned fresh fresh canned canned canned sauce frozen frozen fresh fresh dried fresh canned dried canned fresh f resh canned juice juice dried dried dried fresh jUice fresh fresh canned fresh canned fresh fresh fresh fres h fresh lUlce fresh fresh fresh canned nectar fresh fresh fres h canned fresh fresh canned aOBj 0.19 0.59 0.38 0.55* 0.19i 2.58 1.42* 0.14* Q.6Gi m 1.86 2.76 2.04 1..50* 0.85 2.78 0.30 1.64 1.44 3.06 5.06 SO yes yes 53 50,51 yes 51 yes yes 50 25, 3 3 yes 23.27.51 yes 23 yes 28.29 yes 25,50 Q.21 3.73 4.50* 51 0.18 0.94 } 0.25 0.64 2.02 1 .88 0.16 25 o.ea 0.18 5.80 &.62* 7.80 0.&8* 0.42 0.32 0.18; 4.40 0.26 0.36 0.56* 0.11 0.76 0.49 2.39* 0.18: 0.14* 0.08* 0.58: 0.68* 0.10: 0.27* 0; 0.3a 0* 0.18* 2.10; 1.36 yes yes 25,53 51 y es 18,50 yes yes SO 18 yes 51 yes yes yes yes SO 1 8,50,52 Sl,52 26,30 y es yes yes 50.51 31,32.50 51 y es 50,51,52 ·Most trade names are those of products of various Australian companies. Some varieties of foods also ir e Australian. tEdible portion. ;Multipie extractions. #Ashoor (24) found no detectable salicylate in grapefruit, lemon. orange. strawberry, and langelc. "For coffee. milligrams salicylate per 100 ml made from 2 gm powder in 100 ml waler. IiFor t ea . milligrams salicylate ;.>er 100 ml infusion made from two standard tea bags (4 gm dry leaves). Table 1. Salicylates in 333 foods· (cont) type food plum Golden Circle Blood (red) Kelsey (green) Wilson (red) S_ f> C. dark red letona prunes pomegranate raspberries rhubarb strawberry tamar i llo tangelo wa termelon youngberry vegetable Triangle Spears Sunshine blackeye Borlotti broad. "vicia faba" brown green French l ima mung soya soya grits bean ;;prouts beet root Golden Circle broccoli brussels sorouts c ab bage c arrot cauliflower celery chicory dwves choko cucumoer eggplant endive horser ad i si'! leek lentil l ettu c e marrow m ush r oom okra olive onion parsnip peas juice 0.16* 0.21 0.095 0.11 1.16 6.87 0_07 fresh fresh fresh canned can ned fresh fresh frozen fresh fresh fresh fresh fresh canned 5.14 3.88 0.13 1.36* 0_10 0_72 0.48* 3.06 fresh fresh alfalfa aspara gus bamboo shoots beans salicylate stare green red (Chayate) 1'10 pee l) Aristocrat gherkin (WIth peell {no peel) Eskal brown red (Cucurbita pepol Champ l gn on Zanae black Krait green Krait chick-pea green 0.70 0.14* 0.32* 0 0 0.08 canned canned dried dried fresh dried fresh dr i ed dried dried dried fresh fresh canned fresh fresh iresh fresh fresh fresh fresh fresh iresh ir!!sh fresh canned fresh fresh iresh canned fresh dried dried fresh fresh fresh c anned can ned canned canned fresh fresh dried fresh reported in literature references yes 51 yes 50 yes 50,51 yes 25,33,50 yes SO yes 25,33.50.53 yes SO no yes 24# 20,50 yes 50 yes yes 20,50,51 51 yes 39 yes 21.50 yes yes yes yes SO 19 21.51 no no 22 22 yes yes y�s 20 20 20 o.n 0.002 0.11* 0 0 0 0 0.06 0_18* 0.32* 0.65; 0.07 0; 0.08* 0.23* 0.16* 0; 102 0.03 0.01* 0]8; &.14; 088:1: 0.30::: 1.9 o 18 SO no 22 yes 19 no 22 yes no 41 yes 20,50,51 0.08 0 0 0::: 0.17 024 1.26 0.59 0.34* 1.29:;: 0.16* 0.45 0 0.04* "Most t rade names are those of products of various Australian companies_ . Some varieties of foods also are Australian. tEdible portion. ;Multiple extractions. #Ashoor (24) found no detectable salicylate in grapefruit. lemon. orange. strawberry. and (angelo. III'For coffee. milligrams salicylate per 100 ml made from 2 gm powder in 100 ml water UFO( tea, milligrams salicylate per 100 m! II1fusion made from t\vO standard tea bags (4 gm dry leaves). . 22 953 Table 1. Salicylates in 333 foods· 954 type food peppers pimientos potato pumpkin radish shallots spinach squash swede sweet corn sweet potato tomato (com.) green split pea yellow split pea green chili red chili yellow-green chili sweet, green (Capsicum) Arson sweet red white (with peel) white (no peel) red, small baby Mountain Maid niblets Mountain Maid creamed white yellow letona Goulbum Valley Heinz letona Campbell leggo Tom Pi pe r Heinz Kiaora P.M.U. Fountain Heinz tumip watercress zucch;ni IXL. P.M.U. Rosel la state dried dried fresh fresh fresh fresh canned fresh fresh fresh fresh fresh fresh frozen fresh salicylate reported In literature references yes 20.SO yes 34.50 yes yes 20,51 21 yes 22,51 0 0.02 0.64* 1.20; 0.62* 1.20* 0.15 0.12* 0* 0. 1 2* 1.24* 0.03 0.58 0.16* fresh fresh 0.63 0 0.13* yes SO canned 0.26* yes SO canned fresh fresh fresh 0.39* 0.50* 0.48* 0.13* yes SO,51 yes yes 0.53:1: yes 50 20,35,36,37 50,51 51 } } yes 50 yes 50,51 l yes 49,SO,51 ,52 no 20 canned juice juice juice paste paste paste soup soup soup sauce sauce sauce sauce sa uc e fresh fresh fresh O.lot 0.12:1: 0.18* 0.57* 1.44* 0.43* 0.54* 0.54* 0.32; OW 2.48:1: 1.06* 0.98* 2.15* 0.16* 0.84* 1.00 condiments allspice aniseed bay leaf bas i l "BonoxH canella cardamom caraway cayenne celery c h il i cinnamon cloves coriander cum;n curry pow der powder leaves powder powder powder powder powder powder flakes po wder powder whole leaves powder powder dry dry dry dry liquid dry dry dry dry dry dry dry dry dry fresh dry dry 5.2 22.8 2.52 3.4 0.28 42.6 7.7 2.82 17.6 10.1 1.38 1.30 15.2* 5.74 0.20 45.0 218 SS yes yes "Most trade names are those oi products of various Australian compan ie s . Some varieties of foods also are Australian. tEdible portion. *Multiple extractions. liIAshoor (24) found no detectable salicylate in grapefruit. lemon. orange, strawoory, and tangelo. "For coffee, milligrams salicylate pe r 100 ml made from 2 gm powder in 100 ml water. IIFor tea, milligrams salicylate per 100 ml infusion made from !WO standard tea bags!4 gm dry leaves� 56,57,58 54 Table 1. Salicylates in 333 foods· (cont.) type food d ill fennel fenugreek fi ve sp i c e garam masala garlic ginget m ac e "Marmite" mint mixed herbs mustard nutmeg oregano paprika parsley pep pe r pimiento rosemary saffron sage soy sauce Tabasco Pepper t andor i tarragon turmeric thyme vanilla vinegar Worcestershire sauce "Vegemite powder powder powder powder powder bulbs root state fresh dry dry dry dry dry fresh fresh d ry powder Sanitarium common garden leaves powder dry dry powder dry powder hot powder sweet powder leaves black powder white powder powder powder powder leaves paste fresh d ry dry 0.10:1: dry dry dry dry liquid liquid liquid liquid paste no 22 yes 22 yes 21,22 26 2.4:1: 56 20 3 6.2* powder references 4.5 32.2 0.71* 9.4* 55.6 dry dry dry dry dry dry sauce reported in literature 30.8 66.8 5.7 0.06* liquid Krait 6.9 94.4 0.8 12.2 dfy fresh Mcllhenny powder powder leaves essertce malt white salicylate 1.1* 4.9 68 0 21.7 0 0.45 38,40 0 34.8 76.4 183 1.44 0 1.33 64.3 0.81* drinks ".A.ktavite" cereal coiieefr Bambu Dandelion "Eceo" "�atu(e's Cupoa" "Reform" Coca-Cola coffeel! herbal teal! Andronicus Instant Bushells Instant Bushells Turkish Style Gibsons Instant Hams Mocha Kenya Harris Instant I Harris Instant I1 International Roast ,"1axwell House Instant Moccona Instant Moccona DecaffeInated Nescafe Instant Nescafe Decaffein ared Robert Timms Instant c amom i lle fruit peppermint rose hip powder powder powder powder powder powder liquid powder powder powder powder beans powder oowder ;:lO\"der powder granules powder granules powder powder 0 0.15 0.08 0 2.26 0,38 0,25 0 021 o 19 0.12 0.45 ° 0,10 0,96 yes 0.84 0,64 ° 0.59 " v bag bag bag 0,16 006 0,36 110 bag 0.40 "Most trade names are those of products of various ,,",ustralian companies.. Some var ieties of foods also are Australian, tEdible portion. ;Multiple extractions. #.A.shoor (24) found no detectable salicylate in grapefruit. lemon. oran� strawberry. and tangelo. "For coffee, milligrams salicylate per 100 ml ma.de from 2 gm powder in 100 m! water, I,Fo r tea , milligrams salicylate oer 100 rnl iniusion made from !'Wo stand.vd tea bags 14 gm dry leaves� 45 955 Table 1. Salicylates in 333 foods· (cont.) 956 food HMilo" ·Ovaltine" rose hip reaU teaU type Oel rosa Asco BH/y Burmese Green Bushells Golden Days Decaffeinated Harris Indian Green Peony Jasmine Old Chinese Tetley Twining s: Earl Grey English Breakfast DarjeeHng Irish Breakfast lapsang Souchong Lemon Scented Orange Pekoe Prince of Wales cereals arrowroot barley buckwheat maize millet oats r ice rye wheat powder unpearled grains mea l gr ains hulled grains meal brown grains white grains rolled grains pecan nuts pine nuts pistachiO nuts poppyseed sesame seed sunflower seed walnuts water chestnut golden syrup maple syrup powder powder syrup ba g le aves le aves bag 0.01 0 1.17 6.4 2.48 2.97 4 .78 bag bag leaves leaves leaves bag 0.37 4.0 2.97 T .9 1.9 bag bag leaves bag bag bag l eaves bag 3.0 3.0 4.24 3.89 2.40 7.34 2.75 dry dry d ry 0 0 0 0.43 0 0 0 0; 0; dry dry dry dry dry dry dry 2.97 0 5ocomin fresh fresh fr esh dry fresh fresh fresh paste fresh fresh fresh dry dry dry fresh canned 3.0 0.46 0.07 0.26 0.14 0.52 1.12 0.23 0.12 0.51 0.55 0 0.23 0.12 0.)0 2.92 powder powder Allowrie Aristocrat Capillano Mudgee "No Frills" C.S.R. Camp dry dry l iqu i d liqUid l i qLJ i d liquid liquid liquid liquid dessicated unshelled Sanltarium butter reported in literature 5.57 0 wgars carob cocoa honey salicylate dry nuts and seeds almonds Brazil nuts cashew nuts coconut hazelnuts Macadamia nuts peanuts state 0; 0; 2.5 3.7 10.14 3.9 11.24 0.10; 0 "Most trade names are those of proo\,;cts of various Austra!ian companies. Some varieties of foods also are Australian. tEdible portion. �Multlple extractions. #Ashoor (24) found no detectable >alicylate in grapefrUit, lemon. orange, strawberry, and tangelo. fiFor coffee, milligrams salicylate per 100 ml made from 2 gm powder in 100 ml water. IIFor tea, milligrams salicylate per 100 ml infusion made from two standard tea bags (4 gm dry leavesl. references 46,47,48 Table 1. Salicylates in 333 foods" (conC./ type food sugar molasses confectionery caramel licorice pep perm i nts dairy cheese milk yogurt kidney lamb liver oyster pork pra",n sa l mon scallop tripe tuna salicylate white g ranulated C.5.R. dry liquid 0 Pascall Cream Barratts Giant Aliens SI.ong Mint Aliens "Koolmint" Lifesavers "'Minties" Aliens "Steamrollers" dry dry dry dry dry dry dry dry 0.12 9.78 7.96 Blue Vein Camembert Cheddar cottage Mozarella Tasty Cheddar fresh full cream full cream fresh fresh f resh meat, fish and eggs beef c hi c ken egg scate w hite yolk LUr'lc!1time Pink Seakist fresh fresh fresh liquid fresh fresh fresh fresh fresh fresh fresh fresh fresh fresh fresh canned fresh fresh canned reported in literature references no 43 yes 42 0.22 0.77 7.58 0.86 1.78 2.92 0.05 0.01 0 0 0.Q2 0 0; 0 0; 0; 0 0 0 0; 0.05 0 0 0.04 0 0.02 0 0 alcoholic drinks beer cider liqueurs port sherry spirits Reschs Dinner Ale Toohevs Draught Toc" s Sheaf Stout Bulmer's Dry Bulmer's Sweet Lilydale Dry Mercury Dry Ben ed icti ne CO l nt re a u Drambui Tia ,,",Iaria McWilliams Royal Reserve Stonyiell Mellow Lmdemans Royal Reserve Sweet Mildara Supreme Dry Penfolds Royal Reserve Sweet brandy-Hennessy g m- Gil bey s rum-Bur'ldaberg fum-Captain Morgar'l ' 0.35 } 0.23 0.32 0.17 0.19 0.1:0.16 9.04 0.66 1.68 0.83 1.4 4.2 0.56 0.46 0.49 O. + 0 076 } 1.28 ·Most trade names are those of products of various Australian compani�s. Some varieties of foods also are Australian. tEdible portion. *Multiple extractions. #Ashoor (24) found no detectable salicylate in grapefruit, lemon, orange, 5lrawberry, and tangelo. �For coffee, milligrams salicylate per 100 ml made from 2 gm powder in 100 ml water. IIFor tea, milligrams salicylate per JOO ml infusion made from two st3ndard tea bags (4 gm dry leavesl 957 958 Volume 85 August 1985 Research Number 8 Table 1. Salicylates in 333 foods- Icont.) food wines type state vodka-Smirnoff whiskey-Johnnie Walker Buton Dry Vermouth Kaiser Stuhl Rose Lindemans Riesling McWilHams Dry White Wine McWilliams Cabernet Sauvignon McWil1iams Private Bin Claret McWilliams Reserve Claret Penfolds Traminer Riesling Bin 202 Seaview Rhine Riesling Stonyfell Ma Chere Yalumba Champagne salicylate o o 0.46 0.37 0.81 0.10 reported in literature references no 43 yes 43,44 0.86 0.90 0.35 0.81 0.89 0.69 1.02 "Most trade names are those oi products of various Australian companies. Some varieties of foods also are Australian. tEdible portion. ;Multiple extractions. #Ashoor (24) found no detectable salicylate in grapefruit. lemon. orange. strawberry. and tangelo. "For coffee. milligrams salicylate per 100 ml made irom 2 gm powder in 100 ml water. IIFor tea. milligrams salicylate per 100 ml infusion made from two standard tea bags (4 gm dry leavesl small, they can make a significant contribution to dietary salicylate. Drinks The drinks in Table 1 are divided into two subgroups. alcoholic and nonalcoholic. Within the nonalcoholic beverages. salicylate varies widely from negl igible in milk. cocoa, and decaffeinated coffee to a high of 7.3 mg salicylate per 100 ml in one of the teas. Teas are thus an important source of salicylate in the usual diet. We analyzed 18 difierent brands and varieties. All contained more than 1.9 mg'l00 ml except decaffein ated tea, which contained only 0.37 mg. Salicylate is soluble in methylene chloride. a solvent commonly used for extraction of caffeine. Table 1 includes data for nine coffees and five coffee substitutes. All but one contain less than 0.96 mg salicy late per 100 ml. The higher value of 2.26 mg for one cereal coffee may reflect the raw materials, such as chicory, used in its manufacture. Of the alcoholic beverages, wines appear to contain about the same amount as grape juice (range 0.35 to 1.0 mgilOO ml). Cider contains a low level similar to apple juice. We found that beer contains appreciable amounts. which was not previously reported in the literature. T here was a big range of salicylate in the liqueurs that we tested, with Benedictine highest. presumably from one of the secret ingredients. Sweets little research has been done by others on the presence of salicylate in popular sweets and confectionery. However, porsch et a!. (55) and others have identified salicylate in anise and mint. We therefore analyzed a representative number of licorices and peppermints. which have been listed in Table 1. Values for cocoa and carob-negligible amounts-are also included. The peppermints contained variable amounts. It would appear that high salicylate contents in mint candies come mostly from additional flavorings like methyl salicylate. Legumes, nuts, and seeds legumes are generally safe for salicy!ate-sensitive people. AU dry legumes that were analyzed had less than 0.08 mg/l00 gm in the dry state. Soybean5 are low in salicylate; Similarly the fermented product, soy sauce , contained negligible amounts. Table 1 contains information on 10 nuts. Almonds, water chestnuts, and peanuts (in skin) were moderately high (3.0, 2.9, and 1.1 mg salicylate per 100 gm, respec tively). Other nuts contained small to moderate amounts (0.07 to 0.5 mgi100 gm), Coconut contains a small amount. Sesame seeds, poppy seeds. and sunflower seeds (included here with the nuts) contain negligible amounts of salicylate. Cereals Salicylate levels in nine whole.grain cereals are negligi ble. with the exception of a yello.... :naize meal which contributed 0.43 mgilOO gm. Meat, poultry, fish, eggs, and dairy products Beef, lamb, pork, and chicken all have negligible salicy late content. liver was found to contain 0.05 mgilOO gm. Only two fish have been analyzed so far. and both contained no salicylate. Oysters had none; prawns and scallops contained 0.04 and 0.02 mgil00 gm, respec tively, having more salicylate than most meats or fish but sti 11 very small amounts. Dairy products, including cheese, do not contain ap preciable amounts of salicylates. Journal of The American Dietetic Research Association 959 C:!61 Winter, M , Conclusion The values for salicylate in foods that we have obtained work out to a range from about 10 mg to 200 mglday salicylate in Western diets. This is of the same order of magnitude as the challenge dose of salicylate used in clinical testing (60), usually a 300-mg aspirin tablet. The usual adult pharmacological dose of aspirin is 600 mg (two tablets) at a time, often several times a day, Previous figures for salicylates in most foods are so much smaller than this that it is difficult to see how the food could have similar effects to salicylate medication in sensitive individ· uals. tl7l (28) and 1<1011, R.: Ober das arOmd Chim Acta 55:101. 1972, Gierschner. K . . 8aumann, G.: Arom atic substances in irult Reit:hstolfe dnd Acta Chem Scand 21:945, 1967. tUI L Aroma 01 cranbernes. 23:109, 1 %9. viu$idaea. ACta Chem Scand, Mu",,1', j(,E.: The Do, I.E., !)a:unkhe, and Olson, OX, 01 comparison of volatiles "nific;ial ripening. Ill. Juice of vacc oni um flavour 01 purple passionfruit Food Tl?Chnol Aust 1973 (31) passlonsirucht. Hel" A!'Omen Koerpt!rilegemlttel 18(1):3. 1968. Anjou, K., and Ven Syclow, E,: Aroma at cranberries, I. Vaccini um vithidaea. t291 Anjou. K .. and Von $ydow. DO) de< gelben j peach fru.t l.E.: IsolatIOn, identification and ,1$ rela ted Food Sci 34.&18,1969. Kemp. T.R., Knavei, D.E., and Stoltz. l.P.: 25:446, 10 ha"'E'st maturity and Characterization of some volill.le components of muskmelon fruit. Phytochemistry 10:478,1971, (3) McGlumphy, I.H.: Fruit flavcrs. Food Technol 5.351. 1951. (34) Bunery, R. G" Sieiert, R,M .. and Ling, L.C.: Characterization 01 some volalil!!, polato components. Agric Food Chem 18:538, 1970. (35) lahnson. A.E., Nursten, H.E., and Williams, A.A.: Vegetablevolatill/S, Survey of components identified, Chem Indust July 1971, p. 1212. References III NanonalA.dvisorv Comminee on Hy perki nesis and Food ,"-dditlves: Final Report of the Nul"lion Fo undation , 1980 (21 Calnan, CO Wa shington, DC, Release of h,Slamlne In unl ca r ' a N ut" tion Foundation, plgmentosa. Lancet 1''19&, 1957 (31 Calnan, C.D . . Urtlcaflal r eacti ons Br ,"led I 2'649. 1964, (41 Wa"n, R, P. ThO? efleet oi asplfln I n chronIC un.Clna. Br I Dermaloi 72' 351), 1%0 15i Moore·Roblnson M . . and Warm, R.P Etlee! 01 salinlat", on IJltlcana . Br Med) 4 262, 1967 (6) Champion R.H . . Roberts. 5 0. a. . Carpenter. R.G., ana Roger.I,H .. UrtiCaria and an!!.oedema . A re"e"" oi 554 p ati en". Br I Derm atol 61 588, 1969 \7) :a. 191 110) 111) i 1 21 ! 13) \ 14.. la mes, ) .. dnd WMin, R.P.: Chron.c ,"llC3na. The eifl?Ct 01 aspirin. Br I Derma!ol 82204 1970. Mlcr.aelsson, G .. and I"hlin, l.· L:rt.car:a mduced bv prese",ati ves dnd dye additives in food and drugs. Br I Oermatol 88:515. 19�3, Ooeglas, H.M.: Reactions to asp,,;n and rood addltl\es In patIents wllh chronic urtIcaria, including Ihe phYSICal "ri.canas Br I DermalOI 98: 135, 1975 Doegiol5, H.M, D,etarv trealmE.'�1 oi pa tIents with chronic urticaria and Intolerance to aspifl" and lood add!!!"es. Dermatologlca 154: 308, 1977 Warm R.P, and Sm.th, R.I. . Challenge tesI bane" If' ch ron.c "nlC."., Br I Oermato l �4.401 1 ��6. lockey. S. D. React.ons 10 hIdden agems 'n roods. oeverages an d drugs"'nn Allergy 29'-461 l'Fl Ros, A, ", .. Juhiln. L., and ''''.chdeiss on. G. .... !oilow up sway oi Pd!lO!'lts wi th rec...:rent urtlcana .arl(l h\i�r;en;li;� Ity to aspIrin. ben zoate') and dzodvt'S. Br I Oe'l'1'1arol 95.19 19�6 Junhn. L Recurrent u�iLlrla' Cw,iCJl 1r,\'e�tq�,a{IOn Of 330 ;)dtlent5 Sr I De'matol 10-iL 369 1981 : 1" \lcOenald. I.IL 'vlath leson 0 � ana 5te\ enson. 0 0 ""sp",n .ntOierance ,t"\ dstnrr.d Detect i on bY oraj Cl1dlien,se J -\i!erg\ 30 198 1972 n6, C.bson � it and Clan(\. R.L. �n '.us'ral.an e,clUSlon diet. Mea I Ausr 1 290. 19"8, 11;: C.bson, .... R. and C a�C\. R L. \\andge"'�nl 0; chroniC ,d,ep.t",c urt,ea"a b, Ine ,aent.riCatIOn and e,cl""on or d,et." ',;etors CI,n ... :lerg_ 10699 1980 1181 510"r. H. . and Herrmann. � t r 9, 120, Cl fl 1221 1nl 1241 125i Lber da' \orkammen '0" \erb.ndun"en der nvdro:(vzimr;,aUrel1 r-\-dro).,\-·oe'il,}�,:!dure:'"' '..trod n\drO:(\Cumdrtne- In cll� ru;rruchten l iur Lebensm Lnters For,ch 159305 1r5 ScnMlot!e'f"L H , ana Herrrnann J\ :,.., ber :lIe pne'1QiSdL!fe" d€': gern\Jse�. ! H... dro,\\llrnto;auren IJ'10 "'''dro\v�f'1l:�.auren def Kohl.H1ern und andere-r uuc"",'en·blat!er Z lebensm L otees �or;ch i 59.139 1975 Schmlot:e.n. H and Herrm.!nn K. �O<;' "'� pnen01s';uren des gemuses 11 H,droxyz,mtsauren u"d hvaro"benzoesavren d er i'uC111 und samengem"searten Z Lebensm Lnter> Fo!",;, 159· 213 19 �5 Stc;'r. H and H errmann . K Ur.er d.e phenolsallre" cl", ge m u;es . III H�dro"\llmtsduren 'Jod h .. drox\-benzoesaw(!?n des ·�VU(Zeigernui�S. l Lebernm Unte rs Forsch 159119.1975 Schmid tlein H., and Herrmann, I( uber dl" phenols.i ...."n des gemu;.:; IV Hvdro'lC\llmr�.jure!'l una hyd rox \ Ot:n zoesauren welfarer gemu5:earten und del kanon",n Z LeoeMm L'nters ForKh 159:255. 1975. Stchr, H \\osel. H and Her rman n , K.· The ;:1henolics or IrUlts VII The phenol/cs of (hem !!s and p lums and the chdnge! in Ciltl?CntnS and hydro,· vc.nn.lmlC ac.d der"atl\es dUflng the d e v e lopmen t 0; rru.ts. l �eben,m Unte" Forsch 159 ,11! 85. 1975 Ashoof, 5., and Chu, F.S. . Anal'>ls 0; sak,I'e 4c.d ana methrl sail" :ate 'n !fllits and a lmonds Food Reseafch I"Sliture L'n"erSI!V 0; WiSCOnSin, Mad,son Unpubl ished tVpeSCflpt. ,""umen, H.E.. and Wdilams, ."'.A Fr\ll/ dlomas ... sU""ey or components .dentd,,�d. Chem Indust M.lrch 190i, p �86 (36) Pyne. A.W, and 30:192, Wick, E.L: Volatile componentS of tomatoes. 1965. ()7) Buttery, R.e., Se,fen, R.M., Gaudagni, O,G., and ) �ood Sei ling, Le.: Characteriza 19: 524, tion ot additional volatile components 01 tomato. JAg,,,:. Food Cnem 1971 (3 SI Hay mon, L. W., and Aurand, L.W. : Characterizanon ohola!!le conS!; tuenls of Tab.lsco peppers. J A81ic Food Chem 19: 1131, 1971. (39) AraL S, Suzuki. H . . 1401 FUI.mak., M" and Sdkurai. y,: Fla'vour comoonents In ;Q)·bean. Ill. Volatde 'any ac.ds and volanle amines. ·... 81IC 8iol08 Chem ITokvo) 30:363, 1906. Buttery, R,e., Sel;ert. It M" Gdudagnl. D.G .. and Ling. L.C.: Characrenza lion oi some vol ati le consr.tuenrsoi bell peppers. I Agnc Food Chem I i: 1322, 1969 1411 Fedeh, E.. and laclnl G.: :,'4ildn. 521�1161. 1970. Odorous componel'ts ot oiive oil. Ch ,m Indust ,421 LleblC;", H.M . . Koenl8, W. ... . . and Ba,er. L ...nalvSlS 01 lne flavour 01 rum by gas·liquid Chromatography an d mass spectrometrv. I Chromalogr Sci 8 :527 , 19...0 :431 Kahn, I.H.· Compound s .denliiied In whIskeY. wine. beer : ... tabul.ttlon. ) Assac Off Ana l Chem 52.1166.196'1. ,.1.11 Chn ,ten sen, E,,',,,, and CdPUll. .... · The quantitative anaiyslsof ilavanoidcl and re La ted compounds In wine bv gas·liqu.d chromatography. Enolo gy \"tlculture 19&8 p 238. J.. 5ipma. G" ,(ettenes. D.K . . and PVp;'e" I" ,"ew vo l ati l e cGn'ponenls of roasted coifee. ) ASnc Food Ch em 1&: ICOO. 1961l. .4E" 5allo, R. . and Kuwabaf<l. U .. Volallle IIa-cur of black lea, Agflc Biolog Chem 145\ Storte!sma, ) 1 :389, 1967 T.: The aroma 0; various leas, In CharalamOOU5. G .. and Inglen. eds F' a\or 0; Foods and Be,erages: Chem.slry and Technology. New ITokyo. 14�1 Yaman. sh .. G E.. York' "'eademlC Press. 1978. The CnemlSI',. oi [IH and tea manuiacluflng. .>,d;, Food Res 11 201 1962. 149! Dae "en s P and Larvelle L. Column chromalograpillc cleanu p and gas "qu.d determin ation oi nvdro" benZOIC esters 'n food. J ...SSOC Oti Anal (hem 561515. 1973 '.501 Rabemon CL. and i<<"mode, W I.. 5alicyl" acio ,r; ir",sh ana canned fruit ""'!Ietalo'.,s,) Sc: Food -'lgrrc J2 aa3. 1981. ;511 \\' Sal."lic acid ."d methvl sal.cyiate ;n canned Oe!monle Foods, \ 9�&. L:nou bli shed tvpesmot \\hll;r",lo F S . . and Woodh,lI, I. S. SalicyliC led in nu,t and \e1!et,aOI�S. Report 01 Researcn 19�7·1978. Svdnt'y, ."'ust. (SiRO DIy ,"on of ,48) Slahl. WH. Research If! Fun" T. E and Bellane a , :'-i . . eds F�aroli s H a ndbook oi FlavOt Ingredients. CI.�,eiand. Cle vel and Chem.cal Rubber Co., 1971, pp In and -106 T Studies of Ihe components of essenna l 0.1 of 1541 De' a ma , T, and 1383. 19i1. clove Yak u gak u ,531 Sell a nc•. , 155) Porscn. F.. Fatnow, H . . and W:nkler. H. . The co nS(ltuents of Slar anISeed oil. Dragoco Rep 12,123. 19b5. Qu a li tat.v e analysis of the �sen tla( 011 of cassia (clOnamomum Agr,,; food Ch em !O' 7 �7. 1972 '5�\ Dodge, F 0 : of od 0; cassiallndust Eng.neer Chem 10'1005, 19 1 8 ,561 Onishl, I., and Yamamoto, K.: Es senllal 0.15 of tobacco leaves. Chem Abstr 50 1 5 025 , 1956. 159) HO�N'!Z, W.: Food additIves: DirI?CI. In Horwill. w., ed,: Offic ial Methods of Analvsls. Washmgton, DC: "' s soc . atl on oi OffiCial AnalvllCal ChemI Sts. 1975, 15&1 He,de R casSia blumeJ. pp. 304·365. (60) Van 'unen, S . ... " $WJlr'I, A,R. Krdis. S., Basten, >\ . . Cdtenbv, P.A., and Lablav. R.H,: D ieta ry modification In chr on iC ,diopdthiC ultlca"a andlor ang.oedema. Proce<!dings of XI InlernatlOnal Congress oi Ailergology CI.nlcal Imm unology, London. 198!. and 960 Research Appendix: Discussion of methodology We started with shaking homogenized food in ether in a 2 L separating funnel evaporating to dryness and then taking up in a small volume of ether for TLC on silica gel. Quantification was unreliable. We tried gas chromatography of trimethylsilyl deriv atives, but the method proved unsatisfactory in our hands. High performance' liquid chromatography (HPLC) was next tried, and we found a modified AOAC (59) extraction procedure to be straightforward and reproducible and to give good recoveries of added standards. The modification we now use is stronger sodium hydroxide (NaOH) (25% overnight instead of 10% NaOH for over 2 hours). This is done with the aIm of completing hydrolysis and convert ing all salicylate compounds to free salicylate. Our acidification step is also different. HCI is used to bring the pH to 2.0. Because there was marked emulsion formation in the separat ing funnel with some food homogenates and because recoveries of added standard were only around 50%, we changed the extraction procedure and used ether in glass extractors over 5 hours. This gives good recoveries of added standard salicylic acid and benzoic acid. Specificity of the salicylate peak was checked by two meth ods. First. several phenolic compounds chemically similar to salicylic acid and which might occur in foods were run on the column. All 20 compounds had retention ti mes different from the retention time of salicyclic acid (Table 2). Thymol was tested as well. but no peak was seen with our usual so lvent system. W h en the so lvent was 50% methanol: 50% water. thymol had a retention time of 24 minutes and salicylic acid of 2 minutes. Second, the salicylate peaks tram 11 foods were collected and analyzed by gas chromatographv and mass spectrometry in the Mass Spectrometry Unit of Sydney Unlversity's School of Chem istry. The foods were two vegetables (maize and radish), two fruits (red currants and datesl. three herbs or spices (curry. cumin. and rosemary), two sugary foods ( honey and l i cort ce !. one sample of wine. and one sam pl e of tea. Samples of sodium salicylate (AR: were run on the HPLC to determine retention times. to optimlze conditions for collecti ng the salicylate pe ak . Peaks from foods with retention times identical to the sa li cyl a te ;tandard were collected. aCIdified \'Vlth 1 m! 3 M hydrochloric acid. extracted wi th diethyl ether tAR 10 ml. 3 tlmes l and w ashed with di sti l l ed water no ml. 3 times). The ether solution was drawn off. dried over anhydrous magnesium sulphate. and filtered through cotton wool into a 1 ml "Reac t1Vlal" (Regis). The volume was evaporated to 10 f-LI with dry n it r o g e n under g entl e heat. Bis (trimeth�"silyl) t r i fluoroacetamlde I BSTFAI i Regi s ) 100 jJ.1 was added 10 a dry environment and refluxed gently for 1 hour, The solution was August 1985 Volume 85 Number 8 Table 2. High perfonnance liquid chromatography· compound retention time (minutes) p-amino benzene para amino benzoic acid phthalic acid salicylamide salicin 40H ben zoic acid vaninic acid sulphosalicylic acid anthranilic acid gentisic acid aspirin benzoic acid catechol theophylline quercetin van i llin acetanilide phenol salicylic acid coumarin methyl salicylate 2.46 3.20 3.31 3.32 3.43 3.46 3.51 4.68 6.01 6.75 7.10 8.20 8.23 8.34 11.30 11.72 14.41 14.81 16.81 18.88 58.43 'Solvent: 20'" methanol. 80% glass distilled water. 0.01 mmol H,PO" 0.0025 mmol TBAP pH 7.0 reduced to 10 JoLI under dry nitrogen and injected into the gas chromatograph. The column of the gas chromatograph. a Pye 104, was glass .2 m x 6 mm. packed with QV , 7 (3%) on Chromosorb W 1l00il20 mesh). Helium flow through the column was 30 mll min. The gas chromatograph was interfaced (via an AEI glassjet separator) to an AEI M5·30 mass spectrometer operating at 4 KV with an ionization voltage of 70 ev. The chromatographic trace was produced by the t ota l ion current monitor of the masS spectrometer run at 20 ev except when scanning !l0 second! decad e ), when the ionizingvollage returns to 70 ev. All the peaks from our own HPlC were found to contain a significant amount ot salicylate. Our results are considerably higher than those reported in the literature, e .g . . about 10 times higher for pineapple juice but more than 100 times higher for pineapples. We believe this can be exp I ained pa rtly by the eni c len t extraction proced ure we have developed but p ro bably mostl y by the conversion of bound salicylate to free salicylic acid so that we are measuring total salicylate in the foods.