Appendix 3. 1-Hydroxypyrene.

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Jonge-neelen et al. 1985 (15) Jonge-neelen et al. 1988 Cross--sectional & longitudi-nal Longitu-dinal 3 workers from creostate impreg-nating plant (a, b, c): a = process operator, b = wood handler, c = chief operator control: 16 non-ex-posed men (7: non smoker; 9: smoker) 1 smoker operator from wood preserving Creostate impregnating plant (smokers and non-smokers) Operator wood preserving plant (hot creostate) (smokers) 1-OHPY 1-OHPY HPLC HPLC (Range) Course of 11 days: A) Approx. (1–17) B) Approx. (5.5–39) C) Approx. (1–11) Estimated from the graph Range Operator: 20–90 Estimated from the graph Smoking habit Coefficient of variation (CV) was 2.6% Data shown on the graph

Appendix 3. 1-Hydroxypyrene

Table A3.1. 1-HP Occupational

Study Study

design

Sample

size Exposure Biomarker

Intraindividual variabilitya (µmol 1-OHPY/mol creatinine; *µg 1-OHPY/g creatinine) Confounders Other source of variation Repeat- ability-(va-riability intra-labora-tory) Reprodu-cibility Notes Labo-ratory technique Interindividual variabilitya (µmol 1-OHPY/mol creatinine; *µg 1-OHPY/g creatinine) Correlation between dose/expo-sure vs. 1-OHPY con-centration

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146 Appen dix 3. 1-Hydr oxypyr en e Jonge-neelen et al. 1988 (16) Jonge-neelen et al. 1988 (16) Cross--sectional & longitudi-nal Cross--sectional & longitudinal 31 road paving workers (10 different paving sites: a, b, c, d, e, f, g, h, i, k) 4 smoker gate keepers 3 non smoker gate Asphalt pavers Diesel exhaust gas-gate keeper (smokers and non smokers) 1-OHPY 1-OHPY HPLC HPLC Mean A (n = 3): pre-work: 2.3, post-work: 3.1; B (6): pre-work: 1.5, post-work: 1.6 C (2): pre-work: 1.5, post-work: 2.8; D (4): pre-work: 1.1, post-work: 0.9 E (2): pre-work: 3.1, post-work: 3.2; F (3): pre-work: 1.4, post-work: 2.2 G (3): pre-work: 1.5, post-work: 3.1; H (3): pre-work: 0.5, post-work: 0.6 I (3): pre-work: 2.1, post-work: 2.8 K (2): pre-work: 0.8, post-work: 1.2 Mean±SD smokers (n = 4): pre-work: 0.42±0.19, post-work: Smoking habit Table A3.1. 1-HP Occupational — cont.

Study Study

design

Sample

Intraindividual variabilitya (µmol 1-OHPY/mol creatinine; *µg 1-OHPY/g creatinine) Confounders Other source of variation Repeat- ability-(va-riability intra-labora-tory) Reprodu-cibility Notes Labo-ratory technique Interindividual variabilitya (µmol 1-OHPY/mol creatinine; *µg 1-OHPY/g creatinine) Correlation between dose/expo-sure vs. 1-OHPY con-centration

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1-HP Occu p a ti o na l Jonge-neelen et al. 1988 (16) Jonge-neelen et al. 1990 (11) Cross--sectional & longitudi-nal Cross--sectional & longitudi-nal keepers at harbour track termi-nal 2 operators from the ink factory (A, B) 56 battery workers into 5 job cate-gories and 44 controls Ink factory (smoker and non smoker) Coke oven-bat-tery (non-smok-ers, smokers) (5 job cate-gories) The total PAH in breathing zone air ranged up to 186 µg/m3 1-OHPY 1-OHPY 1-OHPY HPLC HPLC HPLC 0.67±0.24 non smokers (3): pre-work: 0.26±0.08, post-work: 0.47±0.21 Mean A (smoker): pre-work: 0.63, post-work: 0.67 B (non smoker): pre-work: 0.16, post-work: 0.47 Smoker workers GM (range): 1. day: pre-shift (n = 25): 0.98(0.26–3.5), end of shift (25): 3.0 (0.46–11.2) 2. day: pre-shift (30): 1.31(nd–4.1), end of shift (30): 2.75 (0.41–10.1) 3. day: pre-shift (26): 1.36 (0.23–4.7), end of shift (25): 3.37 (0.58–7.3) control (28): 0.51 (0.04–1.24); Non smoker wor-kers GM (range):

Smoking habit

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148 Appen dix 3. 1-Hydr oxypyr en e Jonge-neelen et al. 1990 (11) — cont. Van Schoot-en et al. 1995 (6) Cross--sectional & longitudinal 20 workers from bake oven, 16 workers from anode factory, 13 workers from pot-relining Alluminium plant (smokers) personal PAH geometric mean-µg/m3 (range) a) bake oven (22): 8.7 (3.0–107) 1-OHPY HPLC 1. day: pre-shift (n = 19): 0.77 (0.24–1.7), end of shift (19): 1.78 (0.7–3.9) 2. day: pre-shift (22): 1.23 (0.24–3.3), end of shift (23): 1.75 (0.36–6.9) 3. day: pre-shift (22): 1.28 (0.56–2.5), end of shift (22): 1.92 (0.39–11.2) control (14): 0.17 (0.01–0.93) Smoking habit, occupa-tional history, alcohol consumption, medication, use of protec-tive equip-ment CV was 11.6% Strong cor-relation between 1-OHPY and aver-age PAH cc. of the 5 job cat.: P = 0.0002 smoker vs. non smoker a.m. values (n = 51) P = 0.005 relation-ship between num-ber of cigarettes smoked during the last week and 1-OHPY concentra-Table A3.1. 1-HP Occupational — cont.

Study Study

design

Sample

Intraindividual variabilitya (µmol 1-OHPY/mol creatinine; *µg 1-OHPY/g creatinine) Confounders Other source of variation Repeat- ability-(va-riability intra-labora-tory) Reprodu-cibility Notes Labo-ratory technique 1-OHPY range: 0.17–26.9 mean±SD Smoker: I. High exposure: (number) 1st day pre-shift vs. 5th day post-shift a) bake oven: (n = 6): 1.00±0.72; Interindividual variabilitya (µmol 1-OHPY/mol creatinine; *µg 1-OHPY/g creatinine) Correlation between dose/expo-sure vs. 1-OHPY con-centration

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1-HP Occu p a ti o na l department, 24 workers from elec-trolysis department and 32 controls (foundry department of the same aluminum plant) b) anode f. (40): 23 (1.1–854) c) pot-relining (41): 150 (0.9–1709) d) electrolysis (23): 1.0 (0.3–4.6) e) foundry (16): 0.4 (0.1–3.8) rs = 0.90; P = 0.02 tion in pre-shift, as well as in urine post-shift level (6): 8.43±4.08 b) anode factory: (2): 1.34±0.52; (2):4.84±3.64 c) pot-reliing: (6):0.81±0.48; (6): 6.72±4.25 II. Low exposure: d) electrolysis:(13): 0.58±0.31; (13):0.88±0.42 e) foundry: (16): 0.47±0.37; (17): 0.62±0.31 Non smoker: I. High exposure: (number) 1st day pre-shift vs. 5.day post-shift a) bake oven: (10): 0.58±0.31; (9): 3.65±2.11 b) anode factory:(4): 0.41±0.18; (5):3.25±1.89 c.) pot-relining: (4):0.28±0.17; (2): 6.20±8.44 II. Low exposure: d) electrolysis:(13): 0.30±0.18; (9): 0.48±0.27 e) foundry: (14): 0.35±0.32; (15): 0.47±0.20

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150 Appen dix 3. 1-Hydr oxypyr en e Bentsen et al. 1998 (14) Merlo et al. 1998 (17) Cross--sectional & longitudi-nal Cross--sectional & longitudi-nal 13 male workers: mixing: 3; truck driving: 3; mould filling: 6; miscella-neous: 1 94 traffic police officers in Genoa, Italy and 52 control Electrode paste plant PAH (par-ticulate) (medi-an- µg/m3_): with Gelman sampler: 3.7 (2.0–10.6) with IOM sampler: 14.0 (3.8–40.2) Urban air traffic police office (smokers and non-smokers) BP: geometric mean ng/m3 police officers: 3.67 control: 0.05 1-OHPY 1-OHPY HPLC HPLC Age, smoking habits, use of respiratory protective equipment Smoking habit, age, gender, diet Not signifi-cant correlation between 1-OHPY and total PAH: Gelman: r = -0.41 (Pearson), P = 0.24 IOM: r = -0.08 (Pearson), P = 0.83 Respiratory protec-tive mask reduced the mean post-shift concentration by 20%, and the next day pre-shift 1-OHPY by 60%

Female police vs. males police and females control: P < 0.05. No association between 1-OHPY and diet Table A3.1. 1-HP Occupational — cont.

Study Study

design

Sample

Intraindividual variabilitya (µmol 1-OHPY/mol creatinine; *µg 1-OHPY/g creatinine) Confounders Other source of variation Repeat- ability-(va-riability intra-labora-tory) Reprodu-cibility Notes Labo-ratory technique

Median (range) all work-categories: pre-shift (n = 10): (6.50–28.70); post-shift (10): 20.6 (8.30–34.90) Mean±SD Current smoking habits I.: non-smoker: control (n = 32): 0.067±0.05, police(57): 0.102±0.111; II.: ≤15 cigarettes/day: con-trol (7): 0.13±0.107, police (20): Interindividual variabilitya (µmol 1-OHPY/mol creatinine; *µg 1-OHPY/g creatinine) Correlation between dose/expo-sure vs. 1-OHPY con-centration

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1-HP Occu p a ti o na l 0.194±0.191; III.: > 15 cigarettes/day: con-trol (4): 0.265±0.148, police (12): 0.213±0.186 Environmental tobacco smoke I.: no passive smok-ing: control (22): 0.063±0.569, police (8): 0.101±0.116; II.: ≤ 4 h/day: control (8): 0.068±0.032, police (26): 0.100±0.095; III.: > 4 h/day: control (2): 0.095±0.021, police (23): 0.103±0.125 Gender Females: control (16): 0.106±0.11 police (9): 0.293±0.307 Males: control (27): 0.082±0.057 police (80): 0.124±0.116 Seasonality I.: June–July: control (10): 0.096±0.130,

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152 Appen dix 3. 1-Hydr oxypyr en e Merlo et al. 1998 (17) — cont. Pan et al. 1998 (12) Cross--sectional 99 coke oven work-ers and 24 controls

Coke oven (per-sonal — geomet-ric mean (SD) µg/m3_): Total PAHs: Top: 264.9 (3.2), push side: 139.3 (2.5), coke side: 82.4 (1.6); Bottom: 134.0 1-OHPY HPLC Smoking habits, alco-hol consump-tion, indoor air pollution, habit of eat-ing roasted foods, use of personal protectors Good cor-relation between personal pyrene levels and 1-OHPY: smokers: r = 0.73; P < 0.01;

1-OHPY did not significantly differ between daily PAH exposure at home (current coal heating, coal cooking or linking of roasted foods) Table A3.1. 1-HP Occupational — cont.

Study Study

design

Sample

Intraindividual variabilitya (µmol 1-OHPY/mol creatinine; *µg 1-OHPY/g creatinine) Confounders Other source of variation Repeat- ability-(va-riability intra-labora-tory) Reprodu-cibility Notes Labo-ratory technique police (21): 0.110±0.092; II.: October– –November: control (11): 0.084±0.056, police (25): 0.099±0.073; III.: January–March: control (14): 0.109±0.102, police (28): 0.238±0.262 IV.: April–May: control (8): 0.088±0.067, police (15): 0.152±0.133 Working sites geo-metric mean±SD: Top (n = 25): 12.0±1.9 Middle-push side (10): 9.1±2.0, coke side (15): 5.7±1.6 Bottom (25): 4.0±2.0 Control (24): 0.6±1.9 Interindividual variabilitya (µmol 1-OHPY/mol creatinine; *µg 1-OHPY/g creatinine) Correlation between dose/expo-sure vs. 1-OHPY con-centration

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1-HP Occu p a ti o na l Wu et al. 1998 (19) Cross--sectional & longitudi-nal 5 topside oven workers, 6 sideoven workers, 2 controls (3.2); Control: 10.2 (1.8); Pyrene: Top: 4.27 (6.75), push side: 1.6 (5.75), coke side: 0.46 (3.62); Bottom: 0.86 (8.02); Control: 0.02 (1.79) Coke oven — topside and side oven ambient ben-zene-soluble fraction (BSF) concentration mean ±SD (µg/m3_): topside oven: 626±951 sideoven: 60±53 controls: 20±17 1-OHPY HPLC Mean±SD topside oven (n = 5): 1. day pre-shift: 41±9*; 3. day post-shift: 334±63* sideoven (6): 1. day pre-shift: 10±3*; 3. day post-shift: 57±26* Smoking status, age, regular use of respirators Repeated analysis of three samples: CV 9% non-smo-kers: r = 0.76; P < 0.01 1-OHPY (post-shift on the 3.day afternoon mi-nus pre-shift on the 1. day mor-ning) corre-lated with BSF: rs = 0.80; P = 0.001 1-OHPY (pre-shift on the 4. day morn-ing minus pre-shift on the 1. day morning) correlated with BSF: rs = 0.86; P =0.0002

Regular use of res-pirators did not sig-nificantly predict pre-shift 1-OHPY concentration

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154 Appen dix 3. 1-Hydr oxypyr en e Schoket et al. 1999 (13) Schoket et al. 1999 (13) Schoket et al. 1999 (13) Cross--sectional Cross--sectional Cross--sectional 70 workers from hungar-ian primary aluminum plants (plant I, plant II) And 73 oc-cupacionally unexposed control 48 garage mechanics from 3 hungarian garages and 60 urban control 61 workers from hungar-ian rubber vulcanizing Aluminum plant Diesel exhaust gas-garage (smokers, non-smokers) Vulcanizing rub-ber plant (smokers, non-smokers) 1-OHPY 1-OHPY 1-OHPY HPLC HPLC HPLC Smoking habit Smoking habit P = 0.001 garage workers vs. urban control P = 0.02 workers: smoking/ /non-smoking Table A3.1. 1-HP Occupational — cont.

Study Study

design

Sample

Intraindividual variabilitya (µmol 1-OHPY/mol creatinine; *µg 1-OHPY/g creatinine) Confounders Other source of variation Repeat- ability-(va-riability intra-labora-tory) Reprodu-cibility Notes Labo-ratory technique Mean±SD Plant I. (n = 24): 4.11±3.6; Plant II. (45): 22.2±14.2; Control (73): 0.32±0.48 (mean±SD) Mean±SD Smokers: workers (n = 24): 0.38±0.21; controls (33): 0.22±0.27; Non-smokers: workers (24): 0.22±0.27; controls (27): 0.18±0.45 Mean±SD Smokers: workers (n = 45): 0.24±0.17; Interindividual variabilitya (µmol 1-OHPY/mol creatinine; *µg 1-OHPY/g creatinine) Correlation between dose/expo-sure vs. 1-OHPY con-centration

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1-HP Occu p a ti o na l Perico et al. 2001 (18) Lee et al. 2003 (8) Cross--sectional & longitudinal Cross-sec-tional plant and control 21 non smoking city police (8 men and 13 women) subgroups: I: 13 traffic police in high-density traffic (hdt) II: 8 police in a low-densi-ty traffic (ldt) 70 painters using gener-al paints and 27 on-site con-trols using non paints Urban air non-smokers working as city policemen mean (SD) in ng/m3 ∑8 PAHs: HDT winter (36): 53.6±31.8, summer (35): 22.2±14.9; LDT winter (25): 24.4±11.4, summer (23): 4.1±1.6 General painting on shipyard 1-OHPY 1-OHPYG HPLC IAC-SFS Mean ±SD HDT winter (n = 36): 249.6±171.0*, summer (35): 237.6±419.6*; LDT winter (25): 130.0±77.5*, summer (23): 242.1±327.5* Not to eat barbecued meat or fish Smoking habits, alco-hol consump-tion, use of personal pro-tective equip-ment Recovery was between 85% and 96%, with a precision inferior to 10% Recovery was 82% and the CV was 9% Correlation between 1-OHPY and ∑PAHs: HDT (71): rs = 0.43 P = 0.0002, LDT (48): rs = 0.01 P = 0.96, winter (61): rs = 0.37, P = 0.003, summer (58): rs = 0.22, P = 0.10 HDT vs. LDT winter: P = 0.0004 winter vs. summer HDT: P = 0.004 P < 0.001 general paint users vs. on-site control P = = 0.014 general vs. coal tar paint users smokers (n = 122) vs. non-smokers (53): P = 0.001 controls (42): 0.37±0.59; Non-smokers: workers (12): 0.13±0.20; controls (31): 0.27±0.29 Mean ±SD(range) workers (n = 62): 1.38±1.57 (0.19–9.64) on-site control (23): 0.62±0.62 (0.09–2.16)

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156 Appen dix 3. 1-Hydr oxypyr en e Lee et al. 2003 (8) Marczin-sky et al. 2005 (20) Cross-sec-tional Longitu-dinal 111 painters using coal tar paints and 27 on-site controls using non paints 17 male workers (10 smok-ers, 7 non-smokers)

Coal tar painting on shipyard Arithmetic mean ±SD (range) Total PAH (µg/m3_): 4.82±5.41 (0.08–22.49) Fireproof materi-al producing plant median (range) before vs. 3 months after alteration ∑16 PAHs (µg/m3_{): 29.62} (6.55–149.22) vs. 120.11 (60.75–372.21) B(a]P (µg/m3_): 0.165 (< 0.07–0.54) vs. < 0.07 (< 0.0716.43) Pyrene (µg/m3_): 1.11 vs. 1.23 1-OHPYG 1-OHPY IAC-SFS HPLC Median before (n = 17): 6.73* 3 months after (17): 6.67* Smoking habits, alcohol consumption, use of personal protective equipment Smoking status, use of protective glove and take a shower after work Recovery was 82% and the CV was 9% No cor-relation between 1) ∑16 PAHs and 1-OHPY [(33) before and after alter-ation]: rs = 0.141, P =0.4348 2) Pyrene and 1-OHPY (30): rs = 0.296, P = 0.1121 Post-shift P < 0.001coal tar paint users vs. on-site control P = = 0.014 general vs. coal tar paint users smokers (n = 122) vs. non-smokers (53): P=0.001 Table A3.1. 1-HP Occupational — cont.

Study Study

design

Sample

Intraindividual variabilitya (µmol 1-OHPY/mol creatinine; *µg 1-OHPY/g creatinine) Confounders Other source of variation Repeat- ability-(va-riability intra-labora-tory) Reprodu-cibility Notes Labo-ratory technique Mean ±SD (range) workers (n = 92): 2.24±2.31 (0.14–13.34) on-site control (23): 0.62±0.62 (0.09–2.16) Interindividual variabilitya (µmol 1-OHPY/mol creatinine; *µg 1-OHPY/g creatinine) Correlation between dose/expo-sure vs. 1-OHPY con-centration

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1-HP Occu p a ti o na l Ruchi-rawat et al. 2005 (25) Cross--sectional 11 monks and nuns (control) 11 clothes vendors 14 grilled-meat vendors Ambient air total pahs (ng/m3_): monks and nuns: 5.34±0.65 clothes vendors: 16.07±1.64 grilled-meat vendors: 34.27±7.02 1-OHPY HPLC P < 0.01 pm 1-OHPY: clothes vendor group vs. control P < 0.05 clothes vendors: am vs. pm P < 0.05 a.m. and p.m.: control vs. grilled-meat vendors Median (range) 1-OHPY morning: clothes vendors (n = 11): 0.04 (0.00–0.18) grilled meat ven-dors(14): 0.10 (0.01–0.54) control (11): 0.02 (0.01–0.13) 1-OHPY afternoon: clothes vvendprs (11): 0.11 (0.04–0.24) grilled meat vendors (14): 0.10 (0.03–0.43) control (11): 0.03 (0.01–0.12)

a_{Data as reported by the authors largely overlap between the intra-individual and inter-individual variability categories.}

1-OHPY — 1-hydroxypyrene; HPLC — high-performance liquid chromatography; PAH — polycyclic aromatic hydrocarbon; BSF — benzene-soluble fraction; HDT — high-density traffic; LDT — low-density traffic; 1-OHPYG — 1-hydroxypyrene glucuronide; CV — coefficient of variation; B[a]P — benzo[a]pyrene; n.d. — no data observed; GM — geometric mean.

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158 Appen dix 3. 1-Hydr oxypyr en e Jonge-neelen et al. 1985 (15) Santella et al. 1994 (22) Case--control & longitudi-nal Case---control & longitudi-nal 2 female non-smoking eczema patient (a, b) treated with coal tar oinment control: 16 non-treated men (7: non smoker 9: smoker) 57 psoriasis patients trat-ed with coal tar ointment and 53 untreated volunteers Coal tar ointment (40 g ointment containing 10% coal-tar.) Coal tar ointment 1-OHPY 1-OHPY HPLC HPLC Data shown on the graph Age, gender, cigarette/day Coefficient of variation (CV) was 2.6% 40 g oint-ment containing 10% coal-tar vs. excretion of 1-OHPY increased ~ 200 times case/ /control PAH metabolite vs. 1-OHPY: patients (n = 51): r = 0.389 (Pearson); P = 0.005 control (45): r = 0.300 (Pearson); P = 0.045 P < 0.0001 patient-volunteer differences there was no significant association between the number of days treated and either the level of 1-OHPY or urinary PAH metabolites. Table A3.2. 1-HP Medicinal

Study Study

design

Sample

Intraindividual variabilitya (µmol 1-OHPY/mol creatinine; *µg 1-OHPY/g creatinine) Confounders Other source of variation Repeatability -(variability intra-labora-tory) Reprodu-cibility Notes Labo-ratory technique Data shown on the graph Mean±SD(range) Treated patients (n = 53): 546±928 (10–5160) untreated volunteers (45): 0.14±0.17 (0.02–0.98) Interindividual variabilitya (µmol 1-OHPY/mol creatinine; *µg 1-ohpy/g creatinine) Correlation between dose/expo-sure vs. 1-OHPY con-centration

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1-HP Me dicin al Godschalk 1998 (5) Case, longi-tudinal 3 male and 7 female atopic eczema patients treated with coal tar oint-ment

Coal tar ointment (3%)

1-OHPY HPLC Median (range) Before treatment (n = 10): 0.39 (0.12–1.57); 1 day of treatment (n = 8): 96.5 (21.5–493.2); 1 week of treat-ment (n = 10): 139.7 (26–510.5); 1 week after treatment (n = 10): 1.25 (0.51–6.6) Day-to-day variation: 14% and intra-assay variation: 6%

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160 Appen dix 3. 1-Hydr oxypyr en e Van Rooij et al. 1994 (24) Ovrebo et al. 1995 (30) Case--control Cross--sectional & longitudinal 76 dutch smoker and non smoker male volun-teers (aged 21–64) 66 workers from coke oven plants in Silesia (plant b, plant d, plant e) 66 people from indus-trialized environment in Silesia (Gliwice, Bytom, Święto-chłowice) Environmental smoking habit Occupational (coke oven plants) and environmental (industrialised and non industrialised environment) seasonal variations personal pah (geomatric mean-µg/m3_): I. Environmental (Gliwice): winter (12): 0.40; 1-OHPY 1-OHPY HPLC HPLC Smoking, age, diet, alcohol consumption Smoking habit Coefficient of variation (CV) was 13% Correlation between number of cigarette smoked and 1-OHPY: rs = 0.67; P = 0.0001 (n = 76)

am./pm. 1-OHPY higher in the evening than in the morning (P = 0.02) The consumption of alcohol had no significant effect on 1-OHPY excretion (P = 0.41) I: P = 0.02 (winter–summer) II: P = 0.62 (winter–summer) III: P = 0.15 (winter–summer) winter (I–II–III): P < 0.005; summer (I–II–III): P < 0.005 Non smoker–smo-ker: I: winter P < 0.0005, summer Table A3.3. 1-HP Environmental

Study Study

design

Sample

Intraindividual variabilitya (µmol 1-OHPY/mol creatinine; *µg 1-OHPY/g creatinine) Confounders Other source of variation Repeatability -(variability intra-labora-tory) Reprodu-cibility Notes Labo-ratory technique Mean (range) smoker (n = 37): 0.25 (0.10–0.79) non-smoker (39): 0.12 (0.04–0.29) Seasonal variation (geometric mean): I: Environmental (Gliwice, Bytom, Świętochłowice): winter (n = 60): 0.63, summer (32): 0.39 II: Occupational: winter (60): 3.81, summer (40): 3.19 III: Environmental (B.P.): winter (31): 0.17, summer (45): 0.22 Interindividual variabilitya (µmol 1-OHPY/mol creatinine; *µg 1-OHPY/g creatinine) Correlation between dose/expo-sure vs. 1-OHPY con-centration

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1-HP En vir o nmen tal Levin 1995 Rewiew (23) Cross--sectional 66 people from nonin-dustrialized environment (Biała Podlaska) smokers and non smokers Median background 1-OHPY in smokers and non summer (10): 0.06 II. Occupational: winter (54): 2.08; summer (33): 1.38 Environmental smoking habit 1-OHPY HPLC Smoking habit P = 0.0023 II: winter P = 0.57, summer P = 0.12 III: winter P = 0.01, summer P < 0.0001 Non smokers

(geo-metric mean): I: Environmental, Silesia: winter (29): 0.38, summer (12): 0.19 II: Occupational, Silesia: winter (21): 3.25, summer (15): 2.19 III: Environmental, B.P.: winter (19): 0.13, summer (18): 0.14 Smokers (geometric mean): I: Environmental, Silesia: winter (31): 1.01, summer (20): 0.59 II: Occupational, Silesia: winter (39): 4.15, summer (25): 3.99 III: Environmental, B.P.: winter (12): 0.25, summer (27): 0.30 Median non smoker: Denmark (n = 27): < 0.07 Sweden (48): 0.03

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162 Appen dix 3. 1-Hydr oxypyr en e Levin 1995 Rewiew (23) — cont. smoker individuals from various countries

Table A3.3. 1-HP Environmental — cont.

Study Study

design

Sample

Intraindividual variabilitya (µmol 1-OHPY/mol creatinine; *µg 1-OHPY/g creatinine) Confounders Other source of variation Repeatability -(variability intra-labora-tory) Reprodu-cibility Notes Labo-ratory technique Germany (90): 0.04 Canada (95): 0.07 Italy (19): 0.08 Turkey (15): 0.24 arithmetic mean Netherlands (52): 0.26 Netherlands (14): 0.17 USA (10): 0.27 China (74): 0.68 aritmetic mean Smoker: Denmark (76): < 0.07 Sweden (10): 0.09 Germany (49): 0.12 Canada (45): 0.13 Italy (22): 0.13 Turkey (14): 0.33 arithmetic mean Netherlands (38): 0.28 Netherlands (28): 0.51 USA (11): 0.76 China (84): 0.76 aritmetic mean Interindividual variabilitya (µmol 1-OHPY/mol creatinine; *µg 1-OHPY/g creatinine) Correlation between dose/expo-sure vs. 1-OHPY con-centration

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1-HP En vir o nmen tal Van Wijnen et al. 1996 (31) Siwinska et al. 1998 (9) Cross--sectional & longitudinal Case-case & longitu-dinal 644 Dutch children from 5 areas (1–6 years) 30 children (12 girls and 18 boys — age: 8 years) in the Upper Silesia industrial region Environmental Environmental 1-OHPY 1-OHPY HPLC HPLC Data shown on the graph Sex, age Gender, ETS, day of exami-nation The preci-sion of the analysis of 1-OHPY was 13.1% (intraday variation n = 56 duplicate analyses) and 19.6% (interday variation, n = 53 duplicate analyses) Inacurracy as reco-very rate was 88% at a con-centration of 40 µg/l (10) and 88.9% at 6 µg/l. Between day impre-cision a CV was 13.3% at a con-centration of 6 µg/l Between laboratory-variation was 12.4% (10 samples) I. Gender: no significant differenceII. Age: no significant difference (when corrected for creatinine concentration) P = 0.0001 (sex) P = 0.0103 (ETS) P = 0.0007 (day of examina-tion): when calculated for volume of urine P = 0.0005 (day of examina-tion): when corrected for creatinine I.: Gender (n = 644) geometric mean: boys: 0.19, girls:0.22 II.: Age (n = 644) geometric mean: 1 year: 0.19, 2 years: 0.22, 3 years: 0.25, 4 years: 0.2, 5 years: 0.2, 6 years: 0.18 Median boys: 0.65 girls: 0.52

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164 Appen dix 3. 1-Hydr oxypyr en e Siwinska — cont. Pastorelli et al. 1999 (34) Cross--sectional & longitudi-nal 18 smokers and 47 non-smokers office employees (non-smo-kers) Environmental smoking habit Non smokers: 24 h personal monitoring (ng/m3_): summer (37): 1.67±1.64; winter (35): 4.18±2.37 overall: 2.97±2.39 Smokers: 24 h personal moni-toring (ng/m3_): summer (18): 1.69±2.43; winter (15): 5.48±2.1 overall: 3.4±2.96

1-OHPY HPLC Age, gender,

smoking habit (11) and 5.5% at 3 µg/l (10) Positive correlation between 1-OHPY and num-ber of ciga-rettes smo-ked/day: summer: rs = 0.6, P < 0.001; winter: rs = 0.5, P < 0.001 P < 0.013 (winter non--smoker/summer non-smoker) P < 0.001 (overall smoker/non--smoker) P < 0.001 (summer smoker/non--smoker) P < 0.001 (winter smoker/ /non-smoker) Table A3.3. 1-HP Environmental — cont.

Study Study

design

Sample

Intraindividual variabilitya (µmol 1-OHPY/mol creatinine; *µg 1-OHPY/g creatinine) Confounders Other source of variation Repeatability -(variability intra-labora-tory) Reprodu-cibility Notes Labo-ratory technique Mean±SD Non smokers (ng/ml urine): summer (n = 37): 0.21±0.28; winter (35): 0.26±0.19 overall: 0.24±0.24 mean±SD Smokers (ng/ml urine): summer (18): 0.51±0.27; winter (15): 0.58±0.38 overall: 0.54±0.31 Interindividual variabilitya (µmol 1-OHPY/mol creatinine; *µg 1-OHPY/g creatinine) Correlation between dose/expo-sure vs. 1-OHPY con-centration

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1-HP En vir o nmen tal Siwinska et al. 1999 (28) Cross--sectional 136 children from Bytom (out-dated industry) 128 children from Dąbrowa Górnicza (modern infrastru-cture) 148 children from Pilica (rural area) (age: 7–8 years) Environmental BaP cc. in air (12-month period): median (5–95%) (ng/m3₎ Bytom (78): 64.5 (54.7–88.9) Dąbrowa Górnicza (72): 50.5 (23.3–97.6) Pilica (65): 42.0 (25.3–49.7) 1-OHPY HPLC Heating or cooking facilities ETS geographical areas Day-to-day imprecision a CV was 13.3% at a concen-tration of 6 µg/l (11) and 5.5% at 3 µg/l (10). Inacurracy as recovery rate was 88% at a con-centration of 40 µg/l (10) and 88.9% at 6 µg/l P = 0.047 Region Mean±standard error I.: Indoor coal-burning stove: all children (n = 194):0.43 (0.38–0.51), Pilica children (94): 0.46 (0.37–0.57) II.: other heating or cooking facilities all children (218): 0.30 (0.27–0.33) Pilica children (54): 0.20 (0.07–0.41) Pilica: highest num-ber of children living with indoor coal heating/cooking (64%); median (5–95% confidencia interval of median)

III.: exposed to ETS: all children (286): 0.36 (0.33–0.40) Bytom children (108): 0.49 (0.44–0.60)

IV.: not exposed to ETS: all children (126): 0.32 (0.21–0.40) Bytom children (28): 0.38 (0.29–0.56)

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166 Appen dix 3. 1-Hydr oxypyr en e Siwinska et al. 1999 (28) — cont. Kyrto-poulos et al. 2001 (33) Cross--sectional & longitudi-nal 219 people from Athens and 134 people from Halkida Environmental PAH (ng/m3_): mean (range) Athens: summer (101): 5.03 (1.29–13.90), winter (104): 10.87 (1.23–50.24) Halkida: summer (66): 1.80 (0.27–8.60), winter (72): 7.26 (0.81–29.30) 1-OHPY HPLC Winter (186): 0.054±0.066 (0.002–0.624) summer (167): 0.050±0.068 (0.001–0.563) [mean±SD (range)] Current and recent places of residence; eating and drinking habit; ETS; sunlight; current or past expo-sure to geno-toxic agents; family health history a.m./p.m. /bed time The exact numbers of individ-ual variations were obtained from the authors in personal communication Table A3.3. 1-HP Environmental — cont.

Study Study

design

Sample

Intraindividual variabilitya (µmol 1-OHPY/mol creatinine; *µg 1-OHPY/g creatinine) Confounders Other source of variation Repeatability -(variability intra-labora-tory) Reprodu-cibility Notes Labo-ratory technique In Bytom up to 82% of the children exam-ined were exposed to ETS; median (5-95%confidencia interval of median) Region: Bytom: 0.589±0.070, Dąbrowa Górnicza: 0.352±0.069, Pilica: 0.513±0.056 Mean±SD (range) Athens (n = 219): 0.057±0.078 (0.001–0.624) Halkida (134): 0.043±0.044 (0.002–0.265); male (102): 0.038±0.035 (0.002–0.199); female (251): 0.058±0.076 (0.001–0.624) Interindividual variabilitya (µmol 1-OHPY/mol creatinine; *µg 1-OHPY/g creatinine) Correlation between dose/expo-sure vs. 1-OHPY con-centration

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1-HP En vir o nmen tal Hansen et al. 2005 (26) Joseph et al. 2005 (35) Cross--sectional & longitudi-nal Cross-sec-tional 103 children from Copenhagen and 101 children from rural residences of Denmark (age: 3–13 years) 151 people from Tobac-co Reduction Intervention Program Environmental Environmental smoking habit 1-OHPY 1-OHPY HPLC HPLC Rural: mean (range) I. Boys, Monday (51): 0.17 (0.01–1.66); Tuesday–Friday (50): 0.09 (0.01–0.59) II. Girls, Monday (46): 0.1 (0.01–0.54); Tuesday-Friday (50): 0.08 (0.01–0.27); Urban: mean(range) I. Boys, Monday (n = 55): 0.13 (0.01–0.53) Tuesday–Friday (n = 57): 0.1 (0.01–0.41) II. Girls, Monday (n = 45): 0.12 (0.1–0.63); Tuesday–Friday (n = 45): 0.13 (0.01–0.43) Time spent indoor/out-door time exposed: ETS, cooking habit Age, gender, cigarette/day r = 0.16; P = 0.12 hours spent outside and 1-OHPY (rural) r = 0.34; P < 0.001 positive correlation hours spent outside and 1-OHPY (urban) Correlation between cigarettes per day and P = 0.03 (urban vs. rural) No statiscically significant difference for cooking habits, ETS and trans-portation Rural (total) mean

(range) Monday (n = 97): 0.14 (0.01–1.66); Tuesday–Friday (n = 100): 0.09(0.01–0.59)

Urban (total) mean (range) Monday (n = 100): 0.12 (0.01–0.63) Tuesday–Friday (n = 102): 0.11(0.01–0.43) pmol/mg creatinine; mean(SD) Adult healthy smokers: Cohort I: 15–45

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168 Appen dix 3. 1-Hydr oxypyr en e Joseph et al. 2005 (35) — cont. Kang et al. 2005 (27) Cross-sec-tional (TRIP) — cohort I. 152 people from Reduc-tion of smok-ing in Car-diac Patients (ROSCAP) — cohort II. 86 people from Adult Cross-sec-tional Study (ACSS) — cohort III. 11 people from Low Level smok-ing Study (LLSS) — cohort IV 150 children (age: 12–13 years) and their moth-ers (150) Environmental Pollution Stan-dard Index of PM data shown on the graph

1-OHPYG IAC-SFS Geographical

region 1-OHPY: r = 0.126, P < 0.05 rs = 0.83, P = 0.04 statistically significant association Half-life of 1-OHPY: < 1 day Table A3.3. 1-HP Environmental — cont.

Study Study

design

Sample

Intraindividual variabilitya (µmol 1-OHPY/mol creatinine; *µg 1-OHPY/g creatinine) Confounders Other source of variation Repeatability -(variability intra-labora-tory) Reprodu-cibility Notes Labo-ratory technique cig./day: 1.6 (1.1) Cohort III: < 15 cig./day: 1.6 (1.1)

Adults with heart disease Cohort II: > 15 cig./day: 2.2 (4.7) Cohort IV.: < 15 cig./day: 1.0 (0.6) Data shown on the graph Interindividual variabilitya (µmol 1-OHPY/mol creatinine; *µg 1-OHPY/g creatinine) Correlation between dose/expo-sure vs. 1-OHPY con-centration

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1-HP En vir o nmen tal Ruchi-rawat et al. 2005 (25) Huang et al. 2006 (32) Cross--sectional & longitudi-nal Case-case from six geographi-cal regions in Korea 20 children from Chonburi (control) 22 children from Bangkok (boys; age: 10-12 years) 310 children (age: 6–11 years) 693 adolescents (age: 11–19 years) 1309 adults Environmental PAH (ng/m3_): Chonburi: 0.71 (0.25–3.67) Bangkok: 6.89 (3.7–10.57) median (range) Environmental 1-OHPY 1-OHPY HPLC HPLC Gender, ethnic groups, age, diet, smoking status between Pollution Standard Index of PM and 1-OHPYG (n = 6 locations) P ≤ 0.001 Chonburi vs. Bangkok (1-OHPY) No significant differences between gender or ethnic groups (if corrected the data for creati-nine levels) P = 0.007 (child-Median (range) 1-OHPY morning: Chonburi: 0.12 (0.03–0.26) Bangkok: 0.16 (0.08–0.37) 1-OHPY afternoon: Chonburi: 0.08 (0.04–0.27) Bangkok: 0.2 (0.05–0.68) 1-OHPY following morning: Chonburi: 0.14 (0.03–0.43) Bangkok: 0.3 (0.07–0.99) Geometric mean (95% confidence limits) children: 94.1 (76.9–115)*; adolescents: 71.5 (60.4–84.5)*; adults: 72.3 (61.6–84.8)*

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170 Appen dix 3. 1-Hydr oxypyr en e Huang et al. — cont. Myelzin-ska et al. 2006 (29) Mucha et al. 2006 (36) Cross-sec-tional Cross-sec-tional (age: 20 years and ol-der) from US 74 children: 47 boys and 27 girls from upper Silesia — Katowice and Sosnowiec (age: 5–14 years) 42 children from Kyiv and 48 children Environmental Environmental PAH in ambient air (ng/m3_{) mean} (range) 1-OHPY 1-OHPY HPLC HPLC Age, ETS, coal stove, parents' edu-cation Gender, ETS ren-adolescents) P = 0.001 (child-ren-adults) P < 0.050 coal stove no vs. yes P < 0.050 parents' education low vs. median No significant difference between 1-OHPY levels according to gender Table A3.3. 1-HP Environmental — cont.

Study Study

design

Sample

Intraindividual variabilitya (µmol 1-OHPY/mol creatinine; *µg 1-OHPY/g creatinine) Confounders Other source of variation Repeatability -(variability intra-labora-tory) Reprodu-cibility Notes Labo-ratory technique Mean(SD) boys (n = 47): 0.51 (0.29); girls (27): 0.58 (0.35) age: < 9 (52): 0.57 (0.34); ≥ 9 (20): 0.48(0.20); ETS: non (26): 0.51 (0.4); yes (40): 0.56 (0.25); Coal stove: no (46): 0.43 (0.21); yes (24): 0.74 (0.36) Parents' education: low (36): 0.63 (0.35); median (29): 0.43 (0.2) Mean±SD (range) I. City: Kyiv (n = 41):0.34±0.2 (0.11–0.81), Interindividual variabilitya (µmol 1-OHPY/mol creatinine; *µg 1-OHPY/g creatinine) Correlation between dose/expo-sure vs. 1-OHPY con-centration

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1-HP En vir o nmen tal from Mariupol (age: 3 years) BaP: 11.8 (6.9–18.8); Pyrene: 7.6 (0.02–20.6)

(but the girls had higher mean 1-OHPY concentra-tion than boys)

I.: P < 0.01 (Kyiv-Mariupol) II.: not significant difference (gender) III.: p = 0.004 (ETS exposed children) Mariupol (32): 0.69±0.5 (0.12–2.18)

II. Gender and city: Kyiv boys: 0.31±0.21, girls: 0.37±0.19; Mariupol boys: 0.62±0.45, girls: 0.74±0.53 III. City and ETS (smokers present in the home): Kyiv: yes (14): 0.37±0.16, no (26): 0.33±0.21; Mariupol: yes (15): 0.83±0.59, no (17): 0.56±0.37

PAH — polycyclic aromatic hydrocarbon; 1-OHPY — 1-Hydroxypyrene; 1-OHPYG — 1-Hydroxypyrene glucuronide; HPLC — high-performance liquid chromatography; IAC-SFS — immunoaffinity chromatography-synchronous fluorescence spec-troscopy; n.d. — no data observed; CV — coefficient of variation.

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172 Appen dix 3. 1-Hydr oxypyr en e Van Maanen et al. 1994 (37) Longi-tudinal 1st_study: 21 healty non-smokers 2nd_study: 6 non-smo-kers Hamburgers on 5 consecu-tive days mean daily intake: 1st_study: 1.5 Ķg BP/kg hamburger, 4.5 µg PY/kg hamburger 2nd_study: 0.038 µg BP/kg hamburger 0.9 µg PY/kg hamburger 1-OHPY HPLC nmol/24 h; mean±SD 1st_study: 1. day-before con-sumption:1.9±1.3; 2. day-start of con-sumption: 2.5±1.0; 3. day: 2.4±1.2; 4. day: 5.2±2.3; 5. day: 2.5±1.2 2nd_study: 1. day-before con-sumption: 2.5±1.3; 2. day-start of con-sumption:1.8±1.0; 3. day: 1.8±1.0; 4. day: 2.4±1.6; 5. day: 1.7±0.7; 6. day-end of con-sumption: 1.0±0.6; 7. day-after consumption: 1.6±0.6 P = 0.002 1. study control day vs. 3. day of con-sumption P = 0.022; 3. day of consump-tion 1. study vs. 2. study no signifi-cant rise during the consump-tion period of 2. study Table A3.4. 1-HP Dietary

Study Study

design

Sample

Intraindividual variabilitya (µmol 1-OHPY/mol creatinine; *µg 1-OHPY/g creatinine) Confounders Other source of variation Repeatability -(variability intra-labora-tory) Reprodu-cibility Notes Labo-ratory technique Notea Interindividual variabilitya (µmol 1-OHPY/mol creatinine; *µg 1-OHPY/g creatinine) Dose response

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1-HP Die ta ry Kang et al. 1995 (7) Longi-tudinal 10 healthy non-smoking males Charbroiled beef on 5 con-secutive days mean daily intake: 25.2±3.8 ng BP/kg beef

1-OHPYG IAC-SFS pmol/ml urine; mean±SEM (range) before feeding period (n = 20): 0.23±0.11 after 1.day of feeding (10): 6.5±1.5 (2–16.6) 72 h after feeding period (10): 0.55±0.18 Coefficient of variation of the assay was 8–10% during the period of sample analysis P < 0.0002 1-OHPYG levels 1st_day of expo-sure vs. baseline (increase of 10 to 80 fold, pmol/ml urine) Notea

BP — benzo(a] pyrene; PY — pyrene; PAH — polycyclic aromatic hydrocarbon; 1-OHPY — 1-hydroxypyrene; 1-OHPYG — 1-hydroxypyrene glucuronide; HPLC — high-performance liquid chromatography; IAC-SFS — immunoaffinity chromatography-synchronous fluorescence spectroscopy.