Supplemental Table 1.Fruit and vegetable items in the food frequency questionnaire and pesticide data program, and corresponding scores for 1st, 2nd and 3rd measure, and PRBS.

Definition of measure contamination / 1st / 2nd / 3rd / PRBS
Items in FFQ / Items in PDP / score / score / score
peas or lima beans (FFC) / sweet pea, fz / 0 / 0 / 0 / 0
dried plums or prunes / dried plum / 0 / 0 / 0 / 0
onions / onions / 0 / 0 / 0 / 0
beans or lentils / beans / 0 / 0 / 0 / 0
avocado / avocado / 0 / 0 / 0 / 0
corn (FFC) / corn, fz / 0 / 0 / 0 / 0
cabbage or cole slaw / cabbage / 0 / 0 / 0 / 0
Orange juice, regular or calcium fortified / orange juice / 0 / 0 / 0 / 0
tomato sauce / tomato paste / 0 / 0 / 0 / 0
apple juice or cider / apple juice / 0 / 0 / 1 / 1
cauliflower / cauliflower / 1 / 0 / 0 / 1
grapefruit / grapefruit / 1 / 0 / 0 / 1
cantaloupe / cantaloupe / 0 / 1 / 1 / 2
tofu / soybeans / 2 / 0 / 0 / 2
bananas / bananas / 1 / 1 / 1 / 3
eggplant, summer squash, zucchini / eggplant, summer squash (0.5: 0.5)a / 0 / 2 / 1 / 3
yam or sweet potatoes / sweet potatoes / 1 / 2 / 0 / 3
oranges / oranges / 2 / 0 / 1 / 3
broccoli / broccoli / 1 / 1 / 1 / 3
carrots / carrots / 1 / 0 / 2 / 3
head lettuce, leaf lettuce / lettuce / 1 / 0 / 2 / 3
celery / celery / 1 / 0 / 2 / 3
tomatoes / tomatoes / 1 / 2 / 1 / 4
apple sauce / apple sauce / 2 / 0 / 2 / 4
blueberry (FFC) / blueberry, Fs, Fz (0.5:0.5)a / 2 / 0 / 2 / 4
kale, mustard, chard greens / kale / 1 / 2 / 1 / 4
winter squash / winter squash / 1 / 2 / 1 / 4
fresh apple or pear / apple, pear (0.7:0.3)a / 2 / 1 / 2 / 5
string beans / green beans / 1 / 2 / 2 / 5
grape or raisin / grape, raisin (0.6: 0.4)a / 2 / 1 / 2 / 5
potatoes / potatoes / 2 / 2 / 1 / 5
spinach, cooked / spinach, frozen / 1 / 2 / 2 / 5
peach or plum / peach, plum (0.7: 0.3)a / 2 / 2 / 2 / 6
strawberries (FFC) / strawberries, fresh / 2 / 2 / 2 / 6
spinach, raw / spinach, fresh / 2 / 2 / 2 / 6
green/yellow/red peppers / sweet peppers / 2 / 2 / 2 / 6

Abbreviations:FFC, fresh, frozen, or canned; Fs, fresh; Fz, frozen; PDP, pesticide data program; PRBS, pesticide residue burden score.

a Ratio weighted for pesticide residue for each produce according to the ratio of consumption of each producefrom the USDA report

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Supplemental table 2. Selective urinary pesticide metabolites and their corresponding parent compounds measured in the Environment and Reproductive Health Study.

Metabolites Abbreviation / Metabolite / Parent compound(s) / Chemical class / Intra-class correlations (95%CI )
TCPY / 3,5,6-trichloro-2-pyridinol / chlorpyrifos, chlorpyrifos-methyl / Organophosphate / 0.03 (0.00, 0.97)
PNP / para-Nitrophenol / parathion; methyl parathion / Organophosphate / 0.26 (0.12, 0.49)
IMPY / 2-isopropyl-4-methyl-6-hydroxypyrimidine / diazinon / Organophosphate / 0.26 (0.10, 0.53)
3-PBA / 3-phenoxybenzoic acid / cyhalothrin, cypermethrin, deltamethrin, fenpropathrin, permethrin, tralomethrin / Pyrethroid / 0.37 (0.21, 0.56)
4-F-3-PBA / 4-fluoro-3-phenoxybenzoic acid / cyfluthrin / Pyrethroid / NA1
trans-DCCA / trans-3-(2,2-Dichlorovinyl)-2,2-dimethylcyclopropane carboxylic acid / permethrin; cypermethrin; cyfluthrin / Pyrethroid / NA1
2,4-D / 2,4-dichlorophenoxyacetic acid / 2,4-Denoxyacetic acid (and its esters) / chlorophenoxy herbicide / 0.21 (0.08, 0.47)

Abbreviations: CI, confidence interval; NA, not available.

1Due to low detection frequency, we did not calculate intra-class correlations for 4-F-3PBA and trans-DCCA.

Supplemental table 3. Molar sum and individual concentrations of SG-adjusted urinary concentrations of pesticide biomarkers according to quartile of high pesticide residue fruit and vegetable intake, restricting the analysis where urine sample provided within 6 months to FFQ completion (84 men, 144 urine samples).

Quartile of high pesticide fruit and vegetable intake / Q1 / Q2 / Q3 / Q4 / P, trend
Range of intake (serving/day) / 0.2, 0.8 / 0.8, 1.2 / 1.2, 1.8 / 1.9, 4.3
N / 19 / 22 / 21 / 22
Number of urine samples / 31 / 38 / 37 / 38
Adjusted1 mean(95% CI) for summed2 values of urinary pesticide biomarkers
molar sum of the urinary pesticide metabolites(μmol/L) / 17 (14, 22) / 19 (15, 25) / 23 (17, 31) / 28 (21, 38)* / 0.02
sum of ranks of the urinary pesticide metabolites / 192 (170, 218) / 204 (178, 234) / 235 (204, 270) / 270 (234, 312)* / 0.0002
Adjusted1 mean (95%CI) for individual urinary pesticide biomarkers (μg/L)
TCPY concentrations / 1.00 (0.60, 1.68) / 0.72 (0.44, 1.17) / 1.02 (0.61, 1.71) / 1.49 (0.82, 2.70) / 0.09
IMPY concentrations / 0.16 (0.11, 0.23) / 0.20 (0.14, 0.30) / 0.24 (0.16, 0.35) / 0.25 (0.17, 0.38)* / 0.11
PNP concentrations / 0.56 (0.42, 0.75) / 0.51 (0.38, 0.69) / 0.73 (0.51, 1.05) / 0.85 (0.60, 1.19)* / 0.04
3-PBA concentrations / 0.52 (0.27, 0.98) / 0.63 (0.33, 1.18) / 0.76 (0.42, 1.38) / 0.92 (0.54, 1.57) / 0.15
2,4-D concentrations / 0.31 (0.24, 0.41) / 0.37 (0.24, 0.56) / 0.43 (0.32, 0.57) / 0.51 (0.36, 0.70)* / 0.01

Abbreviations: IMPY, 2-isopropyl-4-methyl-6-hydroxy-pyrimidine; PNP, para-nitrophenol; PRBS, pesticide residue burden score;SG-adjusted, specific gravity adjusted;TCPY, 3,5,6-trichloro-2-pyridinol;2,4-D, 2,4-dichlorophenoxyacetic acid; 3-PBA,3-phenoxybenzoic acid.

1Adjusting for age, race, BMI, total physical activity, smoking status, education, organic fruit and vegetable consumption, years and season of urine sample collections, and residential pesticide use history.

2 Including TCPY, IMPY, PNP, 3-PBA, and 2,4-D

*P-value <0.05 compared to men in the lowest quartile of intake.

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