Transformations,Lifetimes, and Sources of NO2, HONO,and HNO3 in Indoor Environments

Recent research has demonstrated that nitrogen oxides are transformed to nitrogen acids in indoor environments, and that significant concentrations of nitrous acid are present in indoor air. The purpose of the study reported in this paper has been to investigate the sources, chemical transformations and lifetimes of nitrogen oxides and nitrogen acids under the conditions existing in buildings. An unoccupied single family residence was instrumented for monitoring of NO, NO₂, NO_y, MONO, HNO₃, CO, temperature, relative humidity, and air exchange rate. For some experiments, NO₂ and HONO were injected into the house to determine their removal rates and lifetimes. Other experiments investigated the emissions and transformations of nitrogen species from unvented natural gas appliances. We determined that HONO is formed by both direct emissions from combustion processes and reaction of NO₂ with surfaces present indoors. Equilibrium considerations influence the relative contributions of these two sources to the indoor burden of HONO. We determined that the lifetimes of trace nitrogen species varied in the order NO ~ HONO > NO₂ >HNO₃. The lifetimes with respect to reactive processes are on the order of hours for NO and HONO, about an hour for NO₂, and 30 minutes or less for HNO3. The rapid removal of NO₂ and long lifetime of HONO suggest that HONO may represent a significant fraction of the oxidized nitrogen burden in indoor air.     

Indoor pollutant levels from the use of unvented natural gas fireplaces in Boulder, Colorado

High CO and NO2 concentrations have been documented in homes with unvented combustion appliances, such as natural gas fireplaces. In addition, polycyclic aromatic hydrocarbons (PAH) are emitted from incomplete natural gas combustion. The acute health risks of CO and NO2 exposure have been well established for the general population and for certain high-risk groups, including infants, the elderly, and people with heart disease or asthma. Health effects from PAH exposure are less well known, but may include increased risk of cancer. We monitored CO emissions during the operation of unvented natural gas fireplaces in two residences in Boulder, CO, at various times between 1997 and 2000. During 1999, we expanded our tests to include measurements of NO2 and PAH. Results show significant pollutant accumulation indoors when the fireplaces were used for extended periods of time. In one case, CO concentrations greater than 100 ppm accumulated in under 2 hr of operation; a person at rest exposed for 10 hr to this environment would get a mild case of CO poisoning with an estimated 10% carboxyhemoglobin level. Appreciable NO2 concentrations were also detected, with a 4-hr time average reaching 0.36 ppm. Similar time-average total PAH concentrations reached 35 ng/m3. The results of this study provide preliminary insights to potential indoor air quality problems in homes operating unvented natural gas fireplaces in Boulder.     

Formation of indoor nitrous acid (HONO) by light-induced NO<Subscript>2</Subscript> heterogeneous reactions with white wall paint

Gaseous nitrogen dioxide (NO₂) represents an oxidant that is present in relatively high concentrations in various indoor settings. Remarkably increased NO₂ levels up to 1.5 ppm are associated with homes using gas stoves. The heterogeneous reactions of NO₂ with adsorbed water on surfaces lead to the generation of nitrous acid (HONO). Here, we present a HONO source induced by heterogeneous reactions of NO₂ with selected indoor paint surfaces in the presence of light (300 nm?<?λ?<?400 nm). We demonstrate that the formation of HONO is much more pronounced at elevated relative humidity. In the presence of light (5.5 W m^?2), an increase of HONO production rate of up to 8.6?·?10⁹ molecules cm^?2 s^?1 was observed at [NO₂]?=?60 ppb and 50 % relative humidity (RH). At higher light intensity of 10.6 (W m^?2), the HONO production rate increased to 2.1?·?10¹⁰ molecules cm^?2 s^?1. A high NO₂ to HONO conversion yield of up to 84 % was observed. This result strongly suggests that a light-driven process of indoor HONO production is operational. This work highlights the potential of paint surfaces to generate HONO within indoor environments by light-induced NO₂ heterogeneous reactions.     

Harmful effects of atmospheric nitrous acid on the physiological status of Scots pine trees

An open top chamber experiment was carried out in the summer of 2003 to examine the effect of nitrous acid (HONO) gas on the physiological status of Scots pine saplings (Pinus sylvestris). Four-year-old pine trees were exposed to two different levels of HONO gas (at ca. 2.5 ppb and 5.0 ppb) and a control (filtered air) from early evening to early morning (18:00-6:00), in duplicate open top chambers. Significant decreases in the ratios of chlorophylls a to b, an increase in the carbon to nitrogen (C/N) ratio, and a reduction of maximum yield of PS II (F(v)/F(m)) in pine needles were also observed after the 2 months' fumigation. Cation contents of pine needles were also decreased by the fumigation with HONO gas. The results could be explained by the harmful effects of OH radicals, generated from photolysis of HONO gas, and/or aqueous phase HONO (NO(2)(-)/HONO), on the photosynthetic capacity of pine needles.     

The Effects of Infiltration and Insulation on the Source Strengths and Indoor Air Pollution from Combustion Space Heating Appliances

Many energy conservation strategies for residences involve reducing house air exchange rates. Reducing the air exchange rate of a house can cause an increase in pollutant levels if there is an indoor pollution source and if the indoor pollutant source strength remains constant. However, if the indoor pollutant source strength can also be reduced, then it is possible to maintain or even improve indoor air quality. Increasing the insulation level of a house is a means of achieving energy conservation goals and, in addition, can reduce the need for space heating and thereby reduce the pollutant source strengths of combustion space heaters such as unvented kerosene space heaters, unvented gas space heaters, and wood stoves. In this paper, the indoor air quality trade-off between reduced infiltration and increased insulation in residences is investigated for combustion space heaters. Two similar residences were used for the experiment. One residence was used as a control and the other residence had infiltration and insulation levels modified. An unvented propane space heater was used as the source in this study. A model was developed to describe the dependence of both indoor air pollution levels and the appliance source strengths on house air exchange rates and house insulation levels. Model parameters were estimated by applying regression techniques to the data. Results show that indoor air pollution levels in houses with indoor combustion space heating pollution sources can be held constant (or lowered) by reducing the thermal conductance by an amount proportional to (or greater than) the reduction of the air exchange rate.     

Simultaneous measurements of formaldehyde and nitrous acid in dews and gas phase in the atmosphere of Santiago,Chile

The amounts of formaldehyde and nitrous acid (HONO) in gas phase and dews of Santiago de Chile were simultaneously measured. Formaldehyde concentrations values in the liquid phase (dews) correlate fairly well with those in the gaseous phase and are even higher than those expected from gas–dew equilibrium. On the other hand, nitrite concentrations in dews were considerably smaller (ca. 15 times) than those expected from the gas-phase concentrations. This under-saturation is attributed to diffusion limitations due to the relatively large HONO solubility. In agreement with this, under-saturation increases with the rate of dew formation and the pH of the collected waters, factors that should increase the rate of gas to liquid HONO transfer required to reach equilibrium.     

Indoor nitrogen dioxide exposure and children's pulmonary function

Elevated concentrations of nitrogen dioxide (NO2) are produced in the home by the use of unvented gas appliances. In studies on potential health effects of indoor exposure to NO2, exposure has mostly been estimated from the presence or absence of sources like gas cookers in the home. This leads to misclassification of exposure, as NO2 concentrations in the home depend also on source use, ventilation habits, time budgets, etc. The availability of cheap, passive monitoring devices has made it possible to measure indoor concentrations of NO2 directly in health effects studies, albeit with averaging times of one to several days. So far, it has not been evaluated whether this increases the sensitivity of a study to detect health effects of NO2. In this paper, a comparison is made between NO2 sources and weekly average indoor NO2 measurements, as predictors of pulmonary function in a study among children aged 6-12 years. The relationship between exposure and lung functions was found to be generally non-significant in this study. The results further suggested that in this study, measuring indoor NO2 concentrations with passive monitors offered no advantage over the simple use of source presence as exposure variable.     

Heterogeneous conversion of nitric acid to nitrous acid on the surface of primary organic aerosol in an urban atmosphere

Nitrous acid (HONO), nitric acid (HNO₃), and organic aerosol were measured simultaneously atop an 18-story tower in Houston, TX during August and September of 2006. HONO and HNO₃ were measured using a mist chamber/ion chromatographic technique, and aerosol size and chemical composition were determined using an Aerodyne quadrupole aerosol mass spectrometer. Observations indicate the potential for a new HONO formation pathway: heterogeneous conversion of HNO₃ on the surface of primary organic aerosol (POA). Significant HONO production was observed, with an average of 0.97 ppbv event^?1 and a maximum increase of 2.2 ppb in 4 h. Nine identified events showed clear HNO₃ depletion and well-correlated increases in both HONO concentration and POA-dominated aerosol surface area (SA). Linear regression analysis results in correlation coefficients (r²) of 0.82 for HONO/SA and 0.92 for HONO/HNO₃. After correction for established HONO formation pathways, molar increases in excess HONO (HONO_excess) and decreases in HNO₃ were nearly balanced, with an average HONO_excess/HNO₃ value of 0.97. Deviations from this mole balance indicate that the residual HNO₃ formed aerosol-phase nitrate. Aerosol mass spectral analysis suggests that the composition of POA could influence HONO production. Several previously identified aerosol-phase PAH compounds were enriched during events, suggesting their potential importance for heterogeneous HONO formation.     

Real-time indoor and outdoor measurements of black carbon in an occupied house: an examination of sources

Black carbon (BC) was measured every 5 min for two years (May 1998-May 2000) inside and immediately outside a northern Virginia house (suburban Washington, DC) occupied by two nonsmokers. Two aethalometers, which measure BC by optical transmission through a quartz fiber tape, were employed indoors and outdoors. Meteorological parameters were obtained on an hourly basis from nearby Dulles airport. Indoor activities were recorded to identify indoor sources such as combustion activities, which occurred 9% of the time during the first year and 4% of the time during the second year. At times without indoor sources, indoor/outdoor BC ratios averaged 0.53 in the first year and 0.35 in the second year. The main outdoor source of BC was the general regional background, contributing 83-84% of the total during each of the two years. Morning rush hour traffic contributed 8-9% of the total BC. An evening peak in the fall and winter, thought to include contributions from wood burning, was responsible for approximately 8% of the annual average BC concentration. The main indoor sources of BC were cooking and candle burning, contributing 16 and 31%, respectively, of the annual average indoor concentrations in the two years. Relative humidity (RH) affected the outdoor aethalometer in both years. An artifact associated with the tape advance was noted for the aethalometer, but a correction factor was developed that reduced the associated error by a factor of 2.     

Measurements of personal exposure to nitrogen dioxide in four Mexican cities in 1996

Nitrogen dioxide is a ubiquitous pollutant in urban areas. Indoor NO2 concentrations are influenced by penetration of outdoor concentrations and by indoor sources. The objectives of this study were to evaluate personal exposure to NO2, taking into account human time-activity patterns in four Mexican cities. Passive filter badges were used for indoor, outdoor, and personal NO2 measurements over 48 hr and indoor workplace measurements over 16 hr. Volunteers completed a questionnaire on exposure factors and a time-activity diary during the sample period. An unpaired t test, an analysis of variance (ANOVA), and a linear regression were performed to compare differences among cities and mean personal NO2 concentrations involving housing characteristics, as well as to determine which variables predicted the personal NO2 concentration. Sampling periods were in April, May, and June 1996 in Mexico City, Guadalajara, Cuernavaca, and Monterrey. All 122 volunteers in the study were working adults, with a mean age of 34 (SD +/- 7.38); 64% were female, and the majority worked in public offices and universities. The highest NO2 concentrations were found in Mexico City (36 ppb for outdoor, 57 ppb for indoor, and 39 ppb for personal concentration) and the lowest in Monterrey (19 ppb for outdoor, 24 ppb for indoor, and 24 ppb for personal concentration). Significant differences in NO2 concentrations were found among the cities in different microenvironments. During the sampling period, volunteers spent 85% of their time indoors. The highest personal NO2 concentration was found when volunteers kept their windows closed (p = 0.03). In the regression model adjusted by city and gender, the best predictors of personal NO2 concentration were outdoor levels and time spent outdoors (R2 = 0.68). These findings suggest that outdoor NO2 concentrations were an important influence on the personal exposure to NO2, due to the specific characteristics and personal behavior of the people in these Mexican cities.     

Fast nitrogen oxide photochemistry in Summit,Greenland snow

During the 1999 summer field season at Summit, Greenland, we conducted several series of experiments to follow up on our 1998 discovery that NO_x is released from the sunlit snowpack. The 1999 experiments included measurements of HONO in addition to NO and NO₂, and were designed to confirm, for Greenland snow, that the processes producing reactive nitrogen oxides in the snow are largely photochemical. Long duration experiments (up to 48 h) in a flow-through chamber and in the natural snowpack revealed sun-synchronous diurnal variations of all three reactive nitrogen oxides. In a second set of experiments we alternately shaded or exposed snow (again in the natural snowpack and in the chamber) to ambient sunlight for short periods to reduce any temperature changes during variations in light intensity. All three N oxides increased (decreased) very rapidly when sunlit (shaded). In all experiments NO₂ was approximately 3-fold more abundant than NO and HONO (which were at similar levels). Higher concentrations of NO₃⁻ in the snow resulted in higher mixing ratios of HONO, NO and NO₂ in the snow pore air, consistent with our hypothesis that photolysis of NO₃⁻ is the source of the reactive N oxides.     

Effect of chimneys on indoor air concentrations of PM10 and benzo[a]pyrene in Xuan Wei,China

This paper reports the effect of chimneys in reducing indoor air pollution in a lung cancer epidemic area of rural China. Household indoor air pollution concentrations were measured during unvented burning (chimneys blocked) and vented burning (chimneys open) of bituminous coal in Xuan Wei, China. Concentrations of particulate matter with an aerodynamic diameter of 10 μm or less (PM₁₀) and of benzo[a]pyrene (BaP) were measured in 43 homes during normal activities. The use of chimneys led to significant decreases in indoor air concentrations of particulate matter with an aerodynamic diameter of 10 μm or less (PM₁₀) by 66% and of benzo[a]pyrene (BaP) by 84%. The average BaP content of PM₁₀ also decreased by 55% with the installation of a chimney. The reduction of indoor pollution levels by the installation of a chimney supports the epidemiology findings on the health benefits of stove improvement. However, even in the presence of a chimney, the indoor air concentrations for both PM₁₀ and BaP still exceeded the indoor air quality standards of China. Movement up the energy ladder to cleaner liquid or gaseous fuels is probably the only sustainable indoor air pollution control measure.     

Dissociation of sulfur hexafluoride tracer gas in the presence of an indoor combustion source

As an odorless, nontoxic, and inert compound, sulfur hexafluoride (SF6) is one of the most widely used tracer gases in indoor air quality studies in both controlled and uncontrolled environments. This compound may be subject to reactions with water vapor under elevated temperature to form acidic inorganic compounds such as HF and H2SO4. Thus, in the presence of unvented combustion sources such as kerosene heaters, natural gas heaters, gas log fireplaces, candles, and lamps, the SF6 dissociation may interfere with measurements of the emissions from these sources. Tests were conducted in a research house with a vent-free natural gas heater to investigate these potential interferences. It was observed that the heater operation caused about a 5% reduction of SF6 concentration, which can be an error source for the ventilation rate measurement and consequently the estimated pollutant emission rates. Further analysis indicates that this error can be much greater than the observed 5% under certain test conditions because it is a function of the ventilation flow rate. Reducing the tracer gas concentration has no effect on this error. A simple theoretical model is proposed to estimate the magnitude of this error. The second type of interference comes from the primary and secondary products of the SF6 dissociation, mainly H2SO4, SO2, HF, and fine particulate matter (PM). In the presence of approximately 5 ppm SF6, the total airborne concentrations of these species increased by a factor of 4-10. The tests were performed at relatively high SF6 concentrations, which is necessary to determine the interferences quantitatively. The second type of interference can be significantly reduced if the SF6 concentration is kept at a low ppb level.     

Gaseous nitrous acid (HONO) and nitrogen oxides (NOx) emission from gasoline and diesel vehicles under real-world driving test cycles

Reactive nitrogen species emission from the exhausts of gasoline and diesel vehicles, including nitrogen oxides (NO_x) and nitrous acid (HONO), contributes as a significant source of photochemical oxidant precursors in the ambient air. Multiple laboratory and on-road exhaust measurements have been performed to estimate the NO_x emission factors from various vehicles and their contribution to atmospheric pollution. Meanwhile, HONO emission from vehicle exhaust has been under-measured despite the fact that HONO can contribute up to 60% of the total hydroxyl budget during daytime and its formation pathway is not fully understood. A profound traffic-induced HONO to NO_x ratio of 0.8%, established by Kurtenbach et al. since 2001, has been widely applied in various simulation studies and possibly linked to under-estimation of HONO mixing ratios and OH radical budget in the morning. The HONO/NO_x ratios from direct traffic emission have become debatable when it lacks measurements for direct HONO emission from vehicles upon the fast-changing emission reduction technology. Several recent studies have reported updated values for this ratio. This study has reported the measurement of HONO and NO_x emission as well as the estimation of exhaust-induced HONO/NO_x ratios from gasoline and diesel vehicles using different chassis dynamometer tests under various real-world driving cycles. For the tested gasoline vehicle, which was equipped with three-way catalyst after-treatment device, HONO/NO_x ratios ranged from 0 to 0.95 % with very low average HONO concentrations. For the tested diesel vehicle equipped with diesel particulate active reduction device, HONO/NO_x ratios varied from 0.16 to 1.00 %. The HONO/NO_x ratios in diesel exhaust were inversely proportional to the average speeds of the tested vehicles.

Implications: Photolysis of HONO is a dominant source of morning OH radicals. Conventional traffic-induced HONO/NO_x ratio of 0.8% has possibly linked to underestimation of the total HONO budget and consequently underestimation of OH radical budget. The recently reported HONO/NO_x ratio of ~1.6% was used to stimulate HONO emission, which resulted in increased HONO concentrations during morning peak hours and its impact of 14% OH increment in the morning. However, the results were still lower than the measured concentrations. More studies should be conducted to establish an updated traffic-induced HONO/NO_x ratio.     

Measurements of atmospheric nitrous acid and nitric acid

A highly sensitive technique for the measurement of atmospheric HONO and HNO₃ is reported. The technique is based on aqueous scrubbing using two coil samplers, followed by conversion of HNO₃ to nitrite, derivatization of nitrite to a highly light-absorbing azo dye with sulfanilamide (SA) and N-(1-naphthyl) ethylenediamine (NED), and high performance liquid chromatography (HPLC) analysis. HNO₃ concentration was obtained by the difference of the two channels. Two scrubbing solutions were used for sampling the two species: a 1-mM phosphate buffer solution (pH 7) for the measurement of HONO and a 180 mM NH₄Cl/NH₃ buffer solution (pH 8.5) for the measurement of HONO+HNO₃. The scrubbing solution flow rate was 0.24 ml min⁻¹ and the gas sampling flow rate was 2 l min⁻¹. HNO₃ in the NH₄Cl/NH₃ buffer solution was quantitatively reduced to nitrite along an on-line 0.8-cm Cd reductor column. Nitrite in both channels was derivatized with 2 mM SA and 0.2 mM NED in 25 mM HCl. Quantitative derivatization was achieved within 5 min at 55°C. The azo dye derivative was then separated from the SA/NED reagent by reversed-phase HPLC and detected with a UV-vis detector at 540 nm. With an on-line SEP-PAK C-18 cartridge for the reagent purification, the method detection limit is estimated to be better than 1 pptv for HONO and about 20 pptv for HNO₃. The sample integration time was about 2 min and the sampling frequency is every 10 min. Data collected in downtown Albany and Whiteface Mountain, NY, are shown as examples of applications of this technique in both urban and remote clean environments.     

A real-time monitoring and assessment method for calculation of total amounts of indoor air pollutants emitted in subway stations

Subway systems are considered as main public transportation facility in developed countries. Time spent by people in indoors, such as underground spaces, subway stations, and indoor buildings, has gradually increased in the recent past. Especially, operators or old persons who stay in indoor environments more than 15 hr per day usually influenced a greater extent by indoor air pollutants. Hence, regulations on indoor air pollutants are needed to ensure good health of people. Therefore, in this study, a new cumulative calculation method for the estimation of total amounts of indoor air pollutants emitted inside the subway station is proposed by taking cumulative amounts of indoor air pollutants based on integration concept. Minimum concentration of individual air pollutants which naturally exist in indoor space is referred as base concentration of air pollutants and can be found from the data collected. After subtracting the value of base concentration from data point of each data set of indoor air pollutant, the primary quantity of emitted air pollutant is calculated. After integration is carried out with these values, adding the base concentration to the integration quantity gives the total amount of indoor air pollutant emitted. Moreover the values of new index for cumulative indoor air quality obtained for 1 day are calculated using the values of cumulative air quality index (CAI). Cumulative comprehensive indoor air quality index (CCIAI) is also proposed to compare the values of cumulative concentrations of indoor air pollutants. From the results, it is clear that the cumulative assessment approach of indoor air quality (IAQ) is useful for monitoring the values of total amounts of indoor air pollutants emitted, in case of exposure to indoor air pollutants for a long time. Also, the values of CCIAI are influenced more by the values of concentration of NO2, which is released due to the use of air conditioners and combustion of the fuel. The results obtained in this study confirm that the proposed method can be applied to monitor total amounts of indoor air pollutants emitted, inside apartments and hospitals as well. Implications: Nowadays, subway systems are considered as main public transportation facility in developed countries. Time spent by people in indoors, such as underground spaces, subway stations, and indoor buildings, has gradually increased in the recent past. Especially, operators or old persons who stay in the indoor environments more than 15 hr per day usually influenced a greater extent by indoor air pollutants. Hence, regulations on indoor air pollutants are needed to ensure good health of people. Therefore, this paper presents a new methodology for monitoring and assessing total amounts of indoor air pollutants emitted inside underground spaces and subway stations. A new methodology for the calculation of cumulative amounts of indoor air pollutants based on integration concept is proposed. The results suggest that the cumulative assessment approach of IAQ is useful for monitoring the values of total amounts of indoor air pollutants, if indoor air pollutants accumulated for a long time, especially NO2 pollutants. The results obtained here confirm that the proposed method can be applied to monitor total amounts of indoor air pollutants emitted, inside apartments and hospitals as well.     

Revisiting nitrous acid (HONO) emission from on-road vehicles: A tunnel study with a mixed fleet

Nitrous acid (HONO) is an important precursor of OH radicals in the atmosphere. In urban areas, emissions from vehicles are the main source of air pollutants, including reactive nitrogen. Previously reported emission ratios of HONO (HONO/NO_x) from vehicles were measured in the late 1990s and need to be updated due to the significant changes in emission control technologies. We measured the emission ratio of a fleet of vehicles (38% diesel on average) from March 11 to 21, 2015, in a road tunnel in Hong Kong. The emission ratio of 1.24% (±0.35%) obtained is greater than the commonly adopted 0.8% or 0.3%. The elevated emission ratio is found to be related to the presence of vehicles equipped with diesel particle filters (DPFs). Positive correlation between HONO and black carbon (BC) shows that HONO and BC were emitted together, while the lack of correlation or even anticorrelation between HONO/NO_x and BC indicates that the BC-mediated conversion of NO₂ to HONO in the dark was insignificant in the immediate vicinity of the emission sources.

Implications: Vehicular emission is a key source for HONO in the urban atmosphere. However, the most commonly used emission ratio HONO/NO_x in modeling studies was measured more than 15 years ago. Our tunnel study suggests that a mixed fleet nowadays has a higher emission ratio, possibly because of the diesel particle filter (DPF) retrofit program and the growing share of Euro IV or more advanced diesel vehicles. Our study also provides new insight into the role of black carbon in HONO formation from vehicles.     

Potential effects of particulate matter from combustion during services on human health and on works of art in medieval churches in Cyprus

Indoor and outdoor particulate matter (PM_0.3-10) number concentrations were established in two medieval churches in Cyprus. In both churches incense was burnt occasionally during Mass. The highest indoor PM_0.5-1 concentrations compared with outdoors (10.7 times higher) were observed in the church that burning of candles indoors was allowed. Peak indoor black carbon concentration was 6.8 μg m⁻³ in the instances that incense was burning and 13.4 μg m⁻³ in the instances that the candles were burning (outdoor levels ranged between 0.6 and 1.3 μg m⁻³). From the water soluble inorganic components determined in PM₁₀, calcium prevailed in all samples indoors or outdoors, whilst high potassium concentration indoors were a clear marker of combustion. Indoor sources of PM were clearly identified and their emission strengths were estimated via modeling of the results. Indoor estimated PM_0.3-10 mass concentrations exceeded air quality standards for human health protection and for the preservation of works of art.     

Sources and concentrations of indoor nitrogen dioxide in Barcelona, Spain

Sources and concentrations of indoor nitrogen dioxide (NO2) were examined in Barcelona, Spain, during 1996-1999. A total of 340 dwellings of infants participating in a hospital-based cohort study were selected from different areas of the city. Passive filter badges were used for indoor NO2 measurement over 7-30 days. Dwelling inhabitants completed a questionnaire on housing characteristics and smoking habits. Data on outdoor NO2 concentrations were available for the entire period of the study in the areas of the city where indoor concentrations were determined. Bivariate analysis was performed to investigate relationships between indoor NO2 concentrations on one hand and outdoor NO2 concentrations, housing, and occupant characteristics on the other. Stepwise multiple linear regression was performed with variables that were found to have a significant bivariate relationship. Indoor NO2 mean values ranged between 23.57 ppb in 1996 and 27.02 ppb in 1999, with the highest yearly value of 27.82 ppb in 1997. In the same time period, mean outdoor NO2 concentration ranged between 25.26 and 25.78 ppb with a peak of 30.5 ppb in 1998. Multiple regression analysis showed that principal sources of indoor NO2 concentrations were the use of a gas cooker, the absence of an extractor fan when cooking, and cigarette smoking. The absence of central heating was also associated with higher NO2 concentrations. Finally, each ppb increase in outdoor NO2 was associated with a 1% increase in indoor concentrations.