A follow up of the decrease of non exchangeable organically bound tritium levels in the surroundings of a nuclear research center

In the past decades limited amounts of tritium were handled on the CEA site of Bruyères le Châtel with authorised atmospheric releases. A small fraction of the tritium released entered into environmental samples under three forms: (i) as part of free water (TFWT - Tissue Free Water Tritium), or associated with organic matter in two ways; either (ii) bound to the oxygen and nitrogen atoms of the material as exchangeable organically bound tritium (E-OBT), or (iii) bound to carbon atoms as non exchangeable organically bound tritium (NE-OBT). The first two components provide only a picture of atmospheric tritium concentrations at the sampling time as they are in equilibrium with atmospheric moisture and soil humidity. Unlike these exchangeable forms, however, NE-OBT is tightly bound to the organic matter and provides an integrated record of atmospheric tritium during the growing phase of the vegetation. We mapped NE-OBT in tree leaf samples in an area of about 25 × 30 km² around the centre of the CEA site and compared the results with those obtained during a previous sampling exercise in 1989. At this time, the activity levels were almost ten times higher than those observed presently in a similar area almost 20 years later which is consistent with the decrease of atmospheric releases issued from the centre. As the activity levels are now close to environmental background specific attention was also paid to the analytical procedure to ensure reliable low level NE-OBT detection.     

Study of the comparative dynamics of the incorporation of tissue free-water tritium (TFWT) in bulrushes (Typha latifolia) and carp (Cyprinus carpio) in the Almaraz nuclear power plant cooling reservoir

The Almaraz nuclear power plant (Spain) uses the water of Arrocampo reservoir for cooling, and consequently raises the radioactive levels of the aquatic ecosystem of this reservoir. From July 2002 to June 2005, monthly samples of surface water, bulrushes (Typha latifolia) and carp (Cyprinus carpio) were collected from this reservoir. They were analyzed to determine the temporal evolution of the levels of ³H in surface water and of its transfer from the surface water to free-water in the tissues (TFWT) of the aforementioned two organisms. The tritium levels in the surface water oscillate with a biannual period, with their values in the study period ranging between 53 and 433 Bq/L. The incorporation of tritium to bulrushes and carp was fairly similar, the respective mean concentration factors being 0.74 and 0.8 (unitless, as Bq/L tissue water per Bq/L reservoir water). The temporal evolution of the levels fairly closely followed that observed for the surface water tritium, although detailed analysis showed the dominant periodicity for the bulrushes to be annual. This difference reflects the influence on the incorporation of tritium to bulrushes of diverse environmental and metabolic factors, especially evapotranspiration and the seasonal growth of this plant.     

Air infiltration measurements in a home using a convenient perfluorocarbon tracer technique

Using miniature perfluorocarbon tracer (PFT) sources and miniature passive samplers, both about the size of a cigarette, tests conducted in the laboratory and in a typical home successfully demonstrated the utility of the PFT kit as a means for implementing wide-scale infiltration measurements in homes. The PFT diffusion plug source, an elastomer containing a dissolved perfluorocarbon compound, was shown to emit vapors at the rate of about 0.1 to 5 nL/min, providing steady-state concentrations in a home of about 1 to 10 pL/L, i.e., parts per trillion by volume, when one source is deployed for each 300–500 ft² (28–46 m²) of living space. The emission rate from the diffusion source was predictable, but its dependence on both temperature and time suggested the development of alternative approaches. One such alternative, a liquid PFT permeation source, had emission rates which could be tailored over the range 10–20 nL/min, were independent of age for as long as the liquid remained ( 5 yr), and had significantly lower temperature dependence. A number of passive adsorption tube samplers performed reproducibly and identically (to within ±2%–3%) in laboratory tests. Together with a programmable tracer sampler, the miniature diffusion sources and samplers were deployed in a typical home; six PFT sources were uniformly deployed, three on each level of a two-story house. Multiple location sampling, as well as sampling in rooms with and without a miniature source, demonstrated that even in a house without forced-air circulation, a well-mixed modeling approach is justified. Analyses of the tracer samplers were performed back in the laboratory with an automatic electron-capture gas-chromatography system. The effects of the inside/outside temperature differential, as well as that of an open fireplace compared with a wood-burning stove, on the measured air infiltration rates were clearly demonstrated. Comparisons of the PFT tracer method with that of the SF₆ tracer decay approach showed the results of the two methods to be identical within experimental precision. With this miniature source and sampling tracer kit, infiltration rates in the range 0.2–5 air changes per hour can be measured over time-averaged periods of as little as 1 day up to several years.     

Rain scavenging of tritiated water vapour: a numerical Eulerian stationary model

The tradition in tritium washout modeling is to unite the washout model with a Gaussian plume model describing dispersion of tritium vapour in the atmosphere. In the present study, an alternative approach is proposed. A numerical Eulerian model that describes washout independently of dispersion is developed.The sensitivity analysis to model parameters has shown that the washout process is influenced most significantly by rainfall parameters and air temperature: different raindrop size distributions cause differences of up to about 70% in the washout outputs; a change of 15 °C in the air temperature causes an effect of about 50%.Results are presented showing calculated values of washout outputs (tritium concentration in rain, tritium downward flux, washout coefficient) for different tritium vapour profiles, rainfall rates and air temperatures. The general conclusion is that the washout process is too complex to be described comprehensively by the simple washout coefficient concept. We suggest the approach proposed here for directly calculating the tritium downward flux and concentration in the rainwater is preferable.     

Monitoring and assessment of radionuclide discharges from Temelín Nuclear Power Plant into the Vltava River (Czech Republic)

The paper summarizes impacts of the Temelín Nuclear Power Plant (NPP) on the Vltava and Labe River basins. The study is based on the results of long-term monitoring carried out before the plant operation (1989–2000), and subsequently during the plant operation (2001–2005). In the first period, the main objective was to determine background radionuclide levels remaining in the environment after global fallout and due to the Chernobyl accident. A decrease in the concentrations of ⁹⁰Sr, ¹³⁴Cs and ¹³⁷Cs, which was observed before the plant operation, continued also during the subsequent period. Apart from tritium, the results of the observation did not indicate any impacts of the plant on the concentrations of activation and fission products in the hydrosphere. The annual average tritium concentrations in the Vltava River were in agreement with predicted values. The maximum annual average tritium concentration (13.5 Bq L⁻¹) was observed in 2004 downstream from the wastewater discharge in the Vltava River at Solenice. Estimated radiation doses for adults due to intakes of river water as drinking water contaminated by tritium are below 0.1 μSv y⁻¹.     

Biotic, temporal and spatial variability of tritium concentrations in transpirate samples collected in the vicinity of a near-surface low-level nuclear waste disposal site and nearby research reactor

The results of a 21 month sampling program measuring tritium in tree transpirate with respect to local sources are reported. The aim was to assess the potential of tree transpirate to indicate the presence of sub-surface seepage plumes.Transpirate gathered from trees near low-level nuclear waste disposal trenches contained activity concentrations of ³H that were significantly higher (up to ∼700 Bq L⁻¹) than local background levels (0-10 Bq L⁻¹). The effects of the waste source declined rapidly with distance to be at background levels within 10s of metres. A research reactor 1.6 km south of the site contributed significant (p < 0.01) local fallout ³H but its influence did not reach as far as the disposal trenches.The elevated ³H levels in transpirate were, however, substantially lower than groundwater concentrations measured across the site (ranging from 0 to 91% with a median of 2%). Temporal patterns of tree transpirate ³H, together with local meteorological observations, indicate that soil water within the active root zones comprised a mixture of seepage and rainfall infiltration. The degree of mixing was variable given that the soil water activity concentrations were heterogeneous at a scale equivalent to the effective rooting volume of the trees. In addition, water taken up by roots was not well mixed within the trees. Based on correlation modelling, net rainfall less evaporation (a surrogate for infiltration) over a period of from 2 to 3 weeks prior to sampling seems to be the optimum predictor of transpirate ³H variability for any sampled tree at this site.The results demonstrate successful use of ³H in transpirate from trees to indicate the presence and general extent of sub-surface contamination at a low-level nuclear waste site.     

He mass spectrometry for very low-level measurement of organic tritium in environmental samples

The design, setup and performance of a mass spectrometric system for the analysis of low to very low-level tritium in environmental samples are described. The tritium concentration is measured indirectly by the ³He ingrowth from radioactive decay after complete initial degassing of the sample. The analytical system is fully computer-controlled and consists in a commercial helium isotope mass spectrometer coupled with a high vacuum inlet system. A detection limit of 0.15 Bq/kg is routinely obtainable for sample sizes of 20 g of water equivalent and an accumulation time of three months. Larger samples (and/or longer accumulation time) can be used to obtain lower detection limits. In addition to the benefit of a lower detection limit, another advantage of this non-destructive method lies in the simplicity of the analytical procedure which strongly limits the risk of contamination. An inter-comparison was successfully performed with the conventional beta counting technique on lyophilized grass samples, in a range of tritium concentrations of environmental interest. It shows that the ³He mass spectrometry method yields results that are fully consistent with the conventional liquid scintillation technique over a wide range of tritium concentrations.     

Experimental investigation and modelling of tritium washout by precipitation in the area of the nuclear power plant of Paks, Hungary

Tritium occurs in nature in trace amounts, but its concentration is changing due to natural and artificial sources. Studies focusing on natural tritium have to take into account the effect of artificial sources. Also, the impact of tritium is an important issue in environmental protection, e.g. in connection with the emissions from nuclear power plants. The present work focuses on the rain washout of tritium emitted from the Paks nuclear power plant in Hungary. Rainwater collectors were placed around the plant and after a period of precipitation, rainwater was collected and analysed for tritium content. Samples were analysed using low-level liquid scintillation counting, with some also subject to the more accurate ³He ingrowth method. The results clearly show the trace of the tritium plume emitted from the plant; however, values are only about one order of magnitude higher than environmental background levels. A washout model was devised to estimate the distribution of tritium around the plant. The model gives slightly higher concentrations than those measured in the field, but in general the agreement is satisfactory. The modelled values demonstrate that the effect of the plant on rainwater tritium levels is negligible over a distance of some kilometres.     

Tritium concentrations in the atmospheric environment at Rokkasho, Japan before the final testing of the spent nuclear fuel reprocessing plant

This study aimed at obtaining background tritium concentrations in precipitation and air at Rokkasho where the first commercial spent nuclear fuel reprocessing plant in Japan has been under construction. Tritium concentration in monthly precipitation during fiscal years 2001-2005 had a seasonal variation pattern which was high in spring and low in summer. The tritium concentration was higher than that observed at Chiba City as a whole. The seasonal peak concentration at Rokkasho was generally higher than that at Chiba City, while the baseline concentrations of both were similar. The reason for the difference may be the effect of air mass from the Asian continent which is considered to have high tritium concentration. Atmospheric tritium was operationally separated into HTO, HT and hydrocarbon (CH₃T) fractions, and the samples collected every 3 d-14 d during fiscal year 2005 were analyzed for these fractions. The HTO concentration as radioactivity in water correlated well with that in the precipitation samples. The HT concentration was the highest among the chemical forms analyzed, followed by the HTO and CH₃T concentrations. The HT and CH₃T concentrations did not have clear seasonal variation patterns. The HT concentration followed the decline previously reported by Mason and Östlund with an apparent half-life of 4.8 y. The apparent and environmental half-lives of CH₃T were estimated as 9.2 y and 36.5 y, respectively, by combining the present data with literature data. The Intergovernmental Panel on Climate Change used the atmospheric lifetime of 12 y for CH₄ to estimate global warming in its 2007 report. The longer environmental half-life of CH₃T suggested its supply from other sources than past nuclear weapon testing in the atmosphere.     

Environmental tritium (³H) and hydrochemical investigations to evaluate groundwater in Varahi and Markandeya river basins, Karnataka, India

The present study aimed at assessing the activity of natural radionuclides (³H) and hydrochemical parameters (viz., pH, EC, F⁻, NO₃⁻, Cl⁻, Ca²⁺, Mg²⁺) in the groundwater used for domestic and irrigation purposes in the Varahi and Markandeya river basins to understand the levels of hydrochemical parameters in terms of the relative age(s) of the groundwater contained within the study area. The recorded environmental ³H content in Varahi and Markandeya river basins varied from 1.95 ± 0.25 T.U. to 11.35 ± 0.44 T.U. and 1.49 ± 0.75 T.U. to 9.17 ± 1.13 T.U. respectively. Majority of the samples in Varahi (93.34%) and Markandeya (93.75%) river basins being pre-modern water with modern recharge, significantly influenced by precipitation and river inflowing/sea water intrusion. The EC-Tritium and Tritium-Fluoride plots confirmed the existence of higher total dissolved solids (SEC > 500 μS/cm) and high fluoride (MAC > 1.5 mg/L) in groundwater of Markandeya river basin, attributed to relatively longer residence time of groundwater interacting with rock formations and vice versa in case of Varahi river basin. The tritium-EC and tritium-chloride plots indicated shallow and deep circulating groundwater types in Markandeya river basin and only shallow circulating groundwater type in Varahi river basin. Increasing Mg relative to Ca with decreasing tritium indicated the influence of incongruent dissolution of a dolomite phase. The samples with high nitrate (MAC > 45 mg/L) are waters that are actually mixtures of fresh water (containing very high nitrate, possibly from agricultural fertilizers) and older ‘unpolluted’ waters (containing low nitrate levels), strongly influenced by surface source.     

Tritium profiles in snowpacks

The release of tritiated water (HTO) to the atmosphere during the winter can contribute significantly to snow contamination and to water-soil-plant contamination after the spring thaw. The dose significance of such a release depends on the persistence of tritiated water in the snowpack, which is primarily controlled by the HTO diffusion process in snow and the rate of re-emission into the atmosphere from the snowpack surface. Monitoring data collected after an acute winter release at Chalk River Laboratories and data obtained in winter over a chronically contaminated area were analyzed to estimate the diffusion coefficient of HTO in the snowpack. Under conditions of cold and dry snow, the diffusion coefficient lay in the range 1-2 × 10⁻¹⁰ m² s⁻¹, an order of magnitude lower than diffusion in water but an order of magnitude higher than self-diffusion in ice. These results confirm the theoretical predictions (Bales, 1991). Values up to six times higher were found for warmer periods and just before spring melt, when other processes contribute to profile evolution. The low diffusion rate of tritium in cold, dry snow means that tritium remains in the snowpack throughout the winter, to be released during spring thaw to potentially contaminate surface water, soil and crops.     

Re-emission of heavy water vapour from soil to the atmosphere

The re-emission process of tritiated water (HTO) deposited on a soil surface is an important process to assess tritium doses to the general public around nuclear fusion facilities in future. A field experiment using heavy water (HDO) as a substitute for HTO was carried out in the summertime to investigate the re-emission process of HTO from soil to the atmosphere. In the experiment, the time variations of depth profiles of HDO concentrations in soil exposed to HDO vapour and soil mixed with HDO were measured during the re-emission process on the field. The HDO concentrations in soil water in top soil layers of both the exposed and mixed soil rapidly decreased with time during the re-emission. However, the decrease of exposed soil was much greater than that of mixed soil. The re-emission process was analysed using a model including the evaporation of HDO from soil, the exchange between soil HDO and air H2O, and the diffusion of HDO in soil. It was found that the model is applicable to calculating the time variations of detailed depth profiles of HDO concentration in soil water in surface soil layers, using an estimated exchange velocity.     

Development and application of a diffusional sampler for NO2

Within a span of less than 10 years a new type of quantitative air sampling device has been developed; it derives the power for the collection of the contaminant on the sorbent from the random motion of the gas molecules themselves rather than from an external source. This type of passive device is adaptable to either area or personal sampling. The advantages, including low cost, lack of maintenance, minimal space requirements, and lack of explosion or fire hazard, are of great importance in either type of sampling. Their very light weight is particularly advantageous in personal sampling. It should be borne in mind that these are samplers and usually not complete analytical systems. In most of the devices reported the final analysis is carried out in the laboratory as it is for active samplers. To be effective it is necessary that the sorbent be efficient and have sufficient capacity for collection of the contaminant, and that the samplers have sufficient shelf life before and after sampling to permit distribution to the field and return to the laboratory for final analysis.     

Modelling tritium flux from water to atmosphere: application to the Loire River

Tritium (³H or T) is one of the major radionuclides released by nuclear power plants (NPP) into rivers. However, tritiated water (HTO) flux from water to air is seldom considered when assessing health effects of such releases. The aim of this paper is to present the result of a research program, called LORA, conducted on the Loire River (France). To improve our understanding of HTO flux from surface water to air, three field campaigns were organised during the NPP’s radioactive releases to measure simultaneously the activity concentrations in air on the riverbank, using an innovative system, and in river water. The measurements showed that during radioactive releases, water vapour was enriched in ³H. These results were used to calibrate exchange velocities. The average of these estimated exchange velocities was more than one order of magnitude higher than those calculated in the literature from indoor experiments. The variability of these values was also larger, showing that outdoor studies cover a wide range of conditions influencing HTO flux. No correlation was observed between exchanges velocities and meteorological conditions. However, there was a significant difference between day and night with a higher value observed during the day. Two approaches used to calculate HTO evaporation from water (i.e. the approach based on water evaporation and the approach considering that HTO follows its own concentration gradient) were included in a hydrodynamic model, which was used to evaluate HTO air activity along the Loire River. In conclusion, only the approach considering that HTO follows its own gradient led to a good agreement between measurements and predictions. A one-year simulation was done to estimate the contribution of this process to the dose. Its contribution can be considered as negligible in this case compared to the other pathways such as ingestion of water or foodstuffs.     

Tritium in surface waters of the Yenisei River basin

This paper reports an investigation of the tritium content in the surface waters of the Yenisei River basin near the Mining and Chemical Combine (MCC). In 2001 the maximum tritium concentration in the Yenisei River did not exceed 4 +/- 1 Bq l(-1), which is consistent with the data of 1998-99. However, it has been found that there are surface waters containing enhanced tritium as compared with the background values for the Yenisei River. For instance, in the Ploskii Stream and the Shumikha River the maximum tritium concentrations amount to 168 and 81 Bq l(-1), respectively. The source of tritium in these surface waters is the last operating reactor at the MCC, which still uses the Yenisei water as coolant. In water and sediment samples of the Bolshaya Tel River (a tributary of the Yenisei River) the tritium content turned out to be at least 10 times higher than the background values for the Yenisei River. The measurements conducted at the RPA RADON (Moscow) revealed not only tritium but also the artificial radionuclide (14)C in the Bolshaya Tel samples. The data obtained suggest that the Bolshaya Tel River receives the major part of tritium from sediments rather than from the water catchment area. This allows the conclusion that there is water exchange between the surface waters and the radioactively contaminated underground horizons of the "Severny" testing site.     

Measured and modelled tritium concentrations in freshwater Barnes mussels (Elliptio complanata) exposed to an abrupt increase in ambient tritium levels

To improve understanding of environmental tritium behaviour, the International Atomic Energy Agency (IAEA) included a Tritium and C-14 Working Group (WG) in its EMRAS (Environmental Modelling for Radiation Safety) program. One scenario considered by the WG involved the prediction of time-dependent tritium concentrations in freshwater mussels that were subjected to an abrupt increase in ambient tritium levels. The experimental data used in the scenario were obtained from a study in which freshwater Barnes mussels (Elliptio complanata) were transplanted from an area with background tritium concentrations to a small Canadian Shield lake that contains elevated tritium. The mussels were then sampled over 88 days, and concentrations of free-water tritium (HTO) and organically-bound tritium (OBT) were measured in the soft tissues to follow the build-up of tritium in the mussels over time.The HTO concentration in the mussels reached steady state with the concentration in lake water within one or two hours. Most models predicted a longer time (up to a few days) to equilibrium. All models under-predicted the OBT concentration in the mussels one hour after transplantation, but over-predicted the rate of OBT formation over the next 24 h. Subsequent dynamics were not well modelled, although all participants predicted OBT concentrations that were within a factor of three of the observation at the end of the study period. The concentration at the final time point was over-predicted by all but one of the models. The relatively low observed concentration at this time was likely due to the loss of OBT by mussels during reproduction.     

Effect of cigarette smoking on residential NO2 levels

Two studies evaluating the levels and sources of nitrogen dioxide in approximately 90 employee homes in the Richmond area with continuous sampling during the weeks of August 5, 1980, and February 9, 1981, were performed using samplers in the living room, bedroom, kitchen, and outdoors. Additional data were collected concerning appliance usage, heating/cooling plant, ventilation and cigarette smoking. Results were analyzed using BMDP routines. The largest contributor to NO₂ concentration was found to be gas-fired kitchen appliances. The mean kitchen level for homes with gas appliances during the winter study was 188 μg/m³. Excluding participants with gas kitchens, incremental influence due to cigarette smoking was detected. The 7-day, 3-room average level of NO₂ in the homes of nonsmokers and smokers without gas-fired appliances was 12 and 15 μg/m³, respectively, in the summer. The corresponding winter values were 19 and 22 μg/m³. Furthermore, the individual levels of NO₂ in the homes of smokers were generally below both the adjacent outdoor level and the National Ambient Air Quality Standard limit for annual exposure.     

Inorganic iodine incorporation into soil organic matter: evidence from iodine K-edge X-ray absorption near-edge structure

The transformation of inorganic iodine (I⁻ and IO₃⁻) incubated in soils with varying amounts of organic matter (Andosols from the surface layer of an upland field and forest, as well as Acrisols from surface and subsurface layers of an upland field) was investigated by using the iodine K-edge X-ray absorption near-edge structure (XANES). After 60 d of reaction, both I⁻ and IO₃⁻ were transformed into organoiodine in surface soils containing sufficient amounts of organic matter, whereas IO₃⁻ remained unchanged in the subsurface soil of Acrisols with low organic matter contents. Transformation of IO₃⁻ into organoiodine was not retarded when the microbial activity in soil was reduced by γ-ray irradiation, suggesting that microbial activity was not essential for the transformation of inorganic iodine into organoiodine. Soil organic matter has the ability to transform inorganic iodine into organoiodine.     

Reconstruction of atmospheric concentrations and deposition of uranium and decay products released from the former uranium mill at Uravan, Colorado

Radionuclide concentrations in air from uranium milling emissions were estimated for the town of Uravan, Colorado, USA and the surrounding area for a 49-yr period of mill operations beginning in 1936 and ending in 1984. Milling processes with the potential to emit radionuclides to the air included crushing and grinding of ores; conveyance of ore; ore roasting, drying, and packaging of the product (U(3)O(8)); and fugitive dust releases from ore piles, tailings' piles, and roads. The town of Uravan is located in a narrow canyon formed by the San Miguel River in western Colorado. Atmospheric transport modeling required a complex terrain model. Because historical meteorological data necessary for a complex terrain model were lacking, meteorological instruments were installed, and relevant data were collected for 1 yr. Monthly average dispersion and deposition factors were calculated using the complex terrain model, CALPUFF. Radionuclide concentrations in air and deposition on ground were calculated by multiplying the estimated source-specific release rate by the dispersion or deposition factor. Time-dependent resuspension was also included in the model. Predicted concentrations in air and soil were compared to measurements from continuous air samplers from 1979 to 1986 and to soil profile sampling performed in 2006. The geometric mean predicted-to-observed ratio for annual average air concentrations was 1.25 with a geometric standard deviation of 1.8. Predicted-to-observed ratios for uranium concentrations in undisturbed soil ranged from 0.67 to 1.22. Average air concentrations from 1936 to 1984 in housing blocks ranged from about 2.5 to 6 mBq m(-3) for (238)U and 1.5 to 3.5 mBq m(-3) for (230)Th, (226)Ra, and (210)Pb.     

Contribution of tobacco smoke to environmental benzene exposure in Germany

The concentrations of environmental tobacco smoke (ETS) constituents including benzene were measured in the living rooms of 10 nonsmoking households and 20 households with at least one smoker situated in the city and suburbs of Munich. In the city, the median benzene levels during the evening, when all household members were at home, were 8.1 and 10.4 μg/m³ in nonsmoking and smoking homes, respectively. The corresponding levels of 3.5 and 4.6 μg/m³ were considerably lower in the suburbs. Median time-integrated 1-week benzene concentrations in the city were 10.6 μg/m³ in nonsmoking homes and 13.1 μg/m³ in smoking homes. In the suburbs, the corresponding values were 3.2 and 5.6 μg/m³. While the benzene concentrations in nonsmoking homes located in the city were significantly higher (p < 0.05) than in suburban nonsmoking households, no difference was found between smoking and nonsmoking households located either in the city or in the suburbs. Individual exposures to benzene and to specific markers for tobacco smoke of all household members (82 nonsmokers and 32 smokers) were determined by questionnaire, personal monitoring, and biomonitoring. Within the city, the benzene exposure determined by personal samplers was 11.8 μg/m³ for nonsmokers living in nonsmoking homes and 13.3 μg/m³ for nonsmokers in smoking homes. The corresponding values for nonsmokers living in the suburbs were 5.9 and 6.9 μg/m³, respectively. Neither difference was statistically significant. Nonsmokers living in nonsmoking households in the city had significantly higher exposure to benzene compared to their counterparts living in the suburbs (personal samplers: 11.8 vs 5.9 μg/m³, p < 0.001; benzene in exhalate: 2.4 vs. 1.1 μg/m³, p < 0.05; trans,trans-muconic acid excretion in urine: 92 vs. 54 μg/g creatinine, p < 0.05). Nonsmokers from all households with smokers were significantly more exposed to benzene than nonsmokers living in the nonsmoking households (personal samplers: 13.2 vs. 7.0 μg/m³, p < 0.05; benzene in exhalate: 2.6 vs. 1.8 μg/m³, p < 0.01; trans,trans-muconic acid excretion in urine: 73 vs. 62 μg/g creatinine), but the contribution of ETS to the total benzene exposure was relatively low compared to that from other sources. Analysis of variance showed that at most 15% of the benzene exposure of nonsmokers living in smoking homes was attributable to ETS. For nonsmokers living in nonsmoking households benzene exposure from ETS was insignificant.