Hugo Destaillats

Lawrence Berkeley National Laboratory, Berkeley, California, United States

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Publications (61)137.57 Total impact

  • [Show abstract] [Hide abstract]
    ABSTRACT: Thirdhand smoke (THS) is the complex mixture of cigarette smoke chemicals that linger in the environment after cigarettes are smoked. Research has shown that the majority of semi-volatile organic compounds released during smoking stick to indoor surfaces before they can be removed by ventilation. This “tar” can react with ambient air to create new chemicals, some of which are volatile and re-enter the air. To identify the volatile organic compounds (VOCs) released from THS-contaminated surfaces, we exposed paper, 100% cotton cloth and 100% polyester cloth to secondhand cigarette smoke. The materials were exposed in a stainless steel exposure chamber, for 163 hours over 110 days. After the exposure, half the samples were stored in amber glass vials at -20 C. The others were placed on a shelf in the laboratory and allowed to react and desorb or “air out” under ambient conditions for 42 days. Control samples were not exposed to smoke and were treated in parallel. The VOCs emitted by the samples were then identified and quantified using real-time proton-transfer reaction mass spectrometer (PTR-MS). Our results show that the samples emitted a broad spectrum of VOCs, including acetonitrile, furan, toluene, formaldehyde, acetaldehyde and acrolein. The samples that had desorbed for 42 days at room temperature still emitted VOCs at levels well above the control samples that had not been exposed to smoke. We conclude that THS may be a significant source of VOC exposures indoors and that VOC emissions from THS persist for months after the last cigarette.
    142nd APHA Annual Meeting and Exposition 2014; 11/2014
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    ABSTRACT: Tobacco smoke residues lingering in the indoor environment, also referred to as thirdhand smoke (THS), can be a source of long-term exposure to harmful pollutants. THS composition is affected by chemical transformations and by air/surface partitioning over timescales of minutes to months. This study identified and quantified airborne THS pollutants available for respiratory exposure, identified potential environmental tracers, and estimated health impacts to non-smokers. In a ventilated 18-m3 laboratory chamber, six cigarettes were machine-smoked, and levels of particulate matter (PM2.5) and 58 volatile organic compounds (VOCs) were monitored during an aging period of 18 hours. Results were compared with field measurements carried out in a smoker's home 8 hours after the last cigarette was smoked. Initial chamber levels of individual VOCs in freshly emitted secondhand smoke (SHS) were in the range 1 - 300 μg m-3. The commonly used SHS tracers 3-ethenyl pyridine (3-EP) and nicotine were no longer present in the gas phase after 2 hours, likely due mostly to sorption to surfaces. By contrast, other VOCs persisted in the gas phase for at least 18 hours, particularly furans, carbonyls and nitriles. The concentration ratio of acetonitrile to 3-EP increased substantially with aging. This ratio may provide a useful metric to differentiate freshly emitted (SHS) from aged smoke (THS). Among the 29 VOCs detected in the smoker's home at moderate to high concentrations, 18 compounds were also detected in simultaneously sampled outdoor air, but acetonitrile, 2-methyl furan and 2,5-dimethyl furan appeared to be specific to cigarette smoke. Acrolein, methacrolein and acrylonitrile exceeded concentrations considered harmful by the State of California. An initial exposure and impact assessment was carried out for a subset of pollutants by computing disability-adjusted life years (DALYs) lost, using available toxicological and epidemiological information. Exposure to PM2.5 contributed to more than 90% of the predicted harm. Acrolein, furan, acrylonitrile and 1,3-butadiene were considered to be the most harmful VOCs. Depending on which criteria are used to establish the separation between SHS and THS, 5% to 60% of the predicted health damage could be attributed to THS exposure. Benefits and limitations of this approach are discussed.
    Environmental science & technology. 10/2014;
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    ABSTRACT: To investigate the impacts of an energy efficiency retrofit, indoor air quality and resident health was evaluated at a low-income senior housing apartment complex in Phoenix, Arizona before and after a green energy building renovation. Indoor and outdoor air quality sampling was carried out simultaneously with a questionnaire to characterize personal habits and general health of residents. Measured indoor formaldehyde levels before the building retrofit routinely exceeded reference exposure limits, but in the long term follow-up sampling, indoor formaldehyde decreased for the entire study population by a statistically significant margin. Indoor PM levels were dominated by fine particles and showed a statistically significant decrease in the long term follow-up sampling within certain resident subpopulations (i.e. residents who report smoking and residents who had lived longer at the apartment complex). This article is protected by copyright. All rights reserved.
    Indoor Air 06/2014; · 3.30 Impact Factor
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    ABSTRACT: Highly reflective roofs can decrease the energy required for building air conditioning, help mitigate the urban heat island effect, and slow global warming. However, these benefits are diminished by soiling and weathering processes that reduce the solar reflectance of most roofing materials. Soiling results from the deposition of atmospheric particulate matter and the growth of microorganisms, each of which absorb sunlight. Weathering of materials occurs with exposure to water, sunlight, and high temperatures. This study developed an accelerated aging method that incorporates features of soiling and weathering. The method sprays a calibrated aqueous soiling mixture of dust minerals, black carbon, humic acid, and salts onto preconditioned coupons of roofing materials, then subjects the soiled coupons to cycles of ultraviolet radiation, heat and water in a commercial weatherometer. Three soiling mixtures were optimized to reproduce the site-specific solar spectral reflectance features of roofing products exposed for 3 years in a hot and humid climate (Miami, Florida); a hot and dry climate (Phoenix, Arizona); and a polluted atmosphere in a temperate climate (Cleveland, Ohio). A fourth mixture was designed to reproduce the three-site average values of solar reflectance and thermal emittance attained after 3 years of natural exposure, which the Cool Roof Rating Council (CRRC) uses to rate roofing products sold in the US. This accelerated aging method was applied to 25 products–single ply membranes, factory and field applied coatings, tiles, modified bitumen cap sheets, and asphalt shingles–and reproduced in 3 days the CRRC's 3-year aged values of solar reflectance. This accelerated aging method can be used to speed the evaluation and rating of new cool roofing materials.
    Solar Energy Materials and Solar Cells 01/2014; 122:271–281. · 5.03 Impact Factor
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    ABSTRACT: Cigarette smoking remains a significant health threat for smokers and nonsmokers alike. Secondhand smoke (SHS) is intrinsically more toxic than directly inhaled smoke. Recently, a new threat has been discovered - Thirdhand smoke (THS) - the accumulation of SHS on surfaces that ages with time, becoming progressively more toxic. THS is a potential health threat to children, spouses of smokers and workers in environments where smoking is or has been allowed. The goal of this study is to investigate the effects of THS on liver, lung, skin healing, and behavior, using an animal model exposed to THS under conditions that mimic exposure of humans. THS-exposed mice show alterations in multiple organ systems and excrete levels of NNAL (a tobacco-specific carcinogen biomarker) similar to those found in children exposed to SHS (and consequently to THS). In liver, THS leads to increased lipid levels and non-alcoholic fatty liver disease, a precursor to cirrhosis and cancer and a potential contributor to cardiovascular disease. In lung, THS stimulates excess collagen production and high levels of inflammatory cytokines, suggesting propensity for fibrosis with implications for inflammation-induced diseases such as chronic obstructive pulmonary disease and asthma. In wounded skin, healing in THS-exposed mice has many characteristics of the poor healing of surgical incisions observed in human smokers. Lastly, behavioral tests show that THS-exposed mice become hyperactive. The latter data, combined with emerging associated behavioral problems in children exposed to SHS/THS, suggest that, with prolonged exposure, they may be at significant risk for developing more severe neurological disorders. These results provide a basis for studies on the toxic effects of THS in humans and inform potential regulatory policies to prevent involuntary exposure to THS.
    PLoS ONE 01/2014; 9(1):e86391. · 3.53 Impact Factor
  • Mohamad Sleiman, Hugo Destaillats, Lara A Gundel
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    ABSTRACT: Reactive oxygen species (ROS) and free radicals play important roles in the chemical transformation and adverse health effects of environmental aerosols. This work presents a simple and sensitive method for sampling and analysis of ROS using a packed column coated with a profluorescent nitroxide scavenger, proxyl fluorescamine (PF). Quantification was performed by extraction and analysis using HPLC with fluorescence detection. For comparison, the conventional method of collecting aerosols into dichlorofluorescin (DCFH) aqueous solution was used as a reference. The method was successfully applied to the determination of ROS in a model secondary organic aerosol (SOA) system generated by ozonolysis of nicotine, as well as in secondhand tobacco smoke (SHS). ROS concentrations between 50-565nmolm(-3) were detected in fresh SOA and SHS samples. After SHS aging for 22h, 13-18% of the initial ROS mass remained, suggesting the presence of persistent ROS. The new method offers better stability and reproducibility along with sensitivity comparable to that of DCFH (method detection limit of 3.2 and 1.4nmolm(-3) of equivalent H2O2 for PF and DCFH respectively). The PF probe was stable during storage at room temperature and not reactive with ozone or NOx, whereas DCFH in the particle-collecting liquid system was strongly influenced by ozone and NOx interferences. This case study provides a good basis for employing solid-phase supported PF for field measurement of specific ROS in other combustion systems (i.e. biomass burning, candles, and diesel exhaust) and environmental aerosols.
    Talanta 11/2013; 116:1033-9. · 3.50 Impact Factor
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    ABSTRACT: Formaldehyde emissions from fiberglass and polyester filters used in building heating, ventilation and air conditioning (HVAC) systems were measured in bench-scale tests using 10 and 17 cm2 coupons over 24 to 720 h periods. Experiments were performed at room temperature and four different relative humidity settings (20, 50, 65 and 80 % RH). Two different air flow velocities across the filters were explored: 0.013 and 0.5 m/s. Fiberglass filters emitted between 20 and 1000 times more formaldehyde than polyester filters under similar RH and airflow conditions. Emissions increased markedly with increasing humidity, up to 10 mg/h-m2 at 80% RH. Formaldehyde emissions from fiberglass filters coated with tackifiers (impaction oils) were lower than those from uncoated fiberglass media, suggesting that hydrolysis of other polymeric constituents of the filter matrix such as adhesives or binders was likely the main formaldehyde source. These laboratory results were further validated by performing a small field study in an unoccupied office. At 80% RH, indoor formaldehyde concentrations increased by 48-64 %, from 9-12 µg/m3 to 12-20 µg/m3, when synthetic filters were replaced with fiberglass filtration media in the HVAC units. Better understanding of reaction mechanisms and assessing their overall contributions to indoor formaldehyde levels will allow for an efficient control of this pollution source.
    Environmental Science & Technology 04/2013; · 5.48 Impact Factor
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    ABSTRACT: Exposure to thirdhand smoke (THS) is a newly described health risk. Evidence supports its widespread presence in indoor environments. However, its genotoxic potential, a critical aspect in risk assessment, is virtually untested. An important characteristic of THS is its ability to undergo chemical transformations during aging periods, as demonstrated in a recent study showing that sorbed nicotine reacts with the indoor pollutant nitrous acid (HONO) to form tobacco-specific nitrosamines (TSNAs) such as 4-(methylnitrosamino)-4-(3-pyridyl)butanal (NNA) and 4-(methylnitrosamino)-1-(3-pyridyl)-1-butanone (NNK). The goal of this study was to assess the genotoxicity of THS in human cell lines using two in vitro assays. THS was generated in laboratory systems that simulated short (acute)- and long (chronic)-term exposures. Analysis by liquid chromatography-tandem mass spectrometry quantified TSNAs and common tobacco alkaloids in extracts of THS that had sorbed onto cellulose substrates. Exposure of human HepG2 cells to either acute or chronic THS for 24h resulted in significant increases in DNA strand breaks in the alkaline Comet assay. Cell cultures exposed to NNA alone showed significantly higher levels of DNA damage in the same assay. NNA is absent in freshly emitted secondhand smoke, but it is the main TSNA formed in THS when nicotine reacts with HONO long after smoking takes place. The long amplicon-quantitative PCR assay quantified significantly higher levels of oxidative DNA damage in hypoxanthine phosphoribosyltransferase 1 (HPRT) and polymerase β (POLB) genes of cultured human cells exposed to chronic THS for 24h compared with untreated cells, suggesting that THS exposure is related to increased oxidative stress and could be an important contributing factor in THS-mediated toxicity. The findings of this study demonstrate for the first time that exposure to THS is genotoxic in human cell lines.
    Mutagenesis 03/2013; · 3.50 Impact Factor
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    ABSTRACT: doi: 10.1021/jz302119g
    Journal of Physical Chemistry Letters 01/2013; · 6.59 Impact Factor
  • REHVA Journal. 01/2012; 48(3):27-19.
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    ABSTRACT: a b s t r a c t This study explores the potential environmental and energy benefits of using activated carbon fiber (ACF) filters for air cleaning in HVAC systems. The parallel aims for the air cleaning system were to enable reduced indoor exposures to volatile organic compounds (VOCs) and to simultaneously allow reduced rates and energy consumption for outdoor air ventilation. We evaluated the use of ACF media to adsorb VOCs from indoor air during repeated simulated 12-h to 24-h periods of occupancy. In a cyclic regen-eration process, VOCs were desorbed from the ACF media and vented outdoors to enable the next cycle of air cleaning. The VOC removal efficiency of the ACF media was measured using a 9.5-cm 2 ACF specimen exposed to a mixture of VOCs that included toluene, benzene, o-xylene, 1-butanol, limonene, undecane and formaldehyde at 29 C and 30% relative humidity. The concentrations of these model pollutants upstream of the ACF media were in the range 20e30 ppb, to simulate realistic conditions. Velocities through the ACF media were typical of those in normal particle filter systems (w0.5 m s À1). Initial tests were conducted to develop a modified multi-component Freundlich isotherm and estimate the maximum adsorption capacity of the media, which was determined to be 90 mg VOC per gram of ACF. Three different ACF regeneration methods were explored using relatively cleaner outdoor air under ambient conditions, with this air humidified, and with the filter heated. It was found that heating the ACF media to w150 C by circulation of a DC current through the fibers for a short period (15 min) yielded the best VOC removal results, allowing for subsequent consistent removal efficiencies of 70e80% for most VOCs. Regeneration with unheated outdoor air was also effective and used less energy (subsequent removal efficiency was 50e60% for most VOCs). ACF did not perform as well in eliminating formalde-hyde, for which a maximum removal of 25e30% was achieved with heated regeneration. A mass balance model indicated that the combination of ACF air cleaning and a 50% reduction in ventilation will decrease indoor concentrations of VOCs by 60%e80% and reduce formaldehyde concentrations by 12%e40%. Energy modeling indicated the potential to reduce the energy required for heating and cooling of ventilation air by 35% to almost 50%.
    Building and Environment. 01/2012; 47.
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    ABSTRACT: We investigated the adsorption capacity and photocatalytic removal efficiency of formaldehyde using a hectorite-TiO(2) composite in a bench flow reactor. The same experimental conditions were applied to pure TiO(2) (Degussa P25) as a reference. The catalysts were irradiated with either a UVA lamp (365 nm) or with one of two UVC lamps of 254 nm and 254+185 nm, respectively. Formaldehyde was introduced upstream at concentrations of 100-500 ppb, with relative humidity (RH) in the range 0-66% and residence times between 50 and 500 ms. Under dry air and without illumination, saturation of catalyst surfaces was achieved after ≈ 200 min for P25 and ≈ 1000 min for hectorite-TiO(2). The formaldehyde uptake capacity by hectorite-TiO(2) was 4.1 times higher than that of P25, almost twice the BET surface area ratio. In the presence of humidity, the difference in uptake efficiency between both materials disappeared, and saturation was achieved faster (after ≈ 200 min at 10% RH and ≈ 60 min at 65% RH). Under irradiation with each of the three UV sources, removal efficiencies were proportional to the Ti content and increased with contact time. The removal efficiency decreased at high RH. A more complete elimination of formaldehyde was observed with the 254+185 nm UV source.
    Journal of hazardous materials 12/2011; 211-212:233-9. · 4.14 Impact Factor
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    ABSTRACT: There is broad consensus regarding the health impact of tobacco use and secondhand smoke exposure, yet considerable ambiguity exists about the nature and consequences of thirdhand smoke (THS). We introduce definitions of THS and THS exposure and review recent findings about constituents, indoor sorption-desorption dynamics, and transformations of THS; distribution and persistence of THS in residential settings; implications for pathways of exposure; potential clinical significance and health effects; and behavioral and policy issues that affect and are affected by THS. Physical and chemical transformations of tobacco smoke pollutants take place over time scales ranging from seconds to months and include the creation of secondary pollutants that in some cases are more toxic (e.g., tobacco-specific nitrosamines). THS persists in real-world residential settings in the air, dust, and surfaces and is associated with elevated levels of nicotine on hands and cotinine in urine of nonsmokers residing in homes previously occupied by smokers. Much still needs to be learned about the chemistry, exposure, toxicology, health risks, and policy implications of THS. The existing evidence on THS provides strong support for pursuing a programmatic research agenda to close gaps in our current understanding of the chemistry, exposure, toxicology, and health effects of THS, as well as its behavioral, economic, and sociocultural considerations and consequences. Such a research agenda is necessary to illuminate the role of THS in existing and future tobacco control efforts to decrease smoking initiation and smoking levels, to increase cessation attempts and sustained cessation, and to reduce the cumulative effects of tobacco use on morbidity and mortality.
    Environmental Health Perspectives 05/2011; 119(9):1218-26. · 7.26 Impact Factor
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    ABSTRACT: Exposure to tobacco pollutants that linger indoors after smoking has taken place (thirdhand smoke, THS) can occur over extended periods and is modulated by chemical processes involving atmospheric reactive species. This study investigates the role of ozone and indoor surfaces in chemical transformations of tobacco smoke residues. Gas and particle constituents of secondhand smoke (SHS) as well as sorbed SHS on chamber internal walls and model materials (cotton, paper, and gypsum wallboard) were characterized during aging. After smoldering 10 cigarettes in a 24-m3 room size chamber, gas-phase nicotine was rapidly removed by sorption to chamber surfaces, and subsequently re-emitted during ventilation with clean air to a level of ∼10% that during the smoking phase. During chamber ventilation in the presence of ozone (180ppb), ozone decayed at a rate of 5.6h−1 and coincided with a factor of 5 less nicotine sorbed to wallboard. In the presence of ozone, no gas phase nicotine was detected as a result of re-emission, and higher concentrations of nicotine oxidation products were observed than when ventilation was performed with ozone-free air. Analysis of the model surfaces showed that heterogeneous nicotine-ozone reaction was faster on paper than cotton, and both were faster than on wallboard. However, wallboard played a dominant role in ozone-initiated reaction in the chamber due to its large total geometric surface area and sink potential compared to the other substrates. This study is the first to show in a room-sized environmental chamber that the heterogeneous ozone chemistry of sorbed nicotine generates THS constituents of concern, as observed previously in bench-top studies. In addition to the main oxidation products (cotinine, myosmine and N-methyl formamide), nicotine-1-oxide was detected for the first time.
    Atmospheric Environment 01/2011; 45(28):4959-4965. · 3.11 Impact Factor
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    ABSTRACT: The use of highly reflective “cool” roofing materials can decrease demand for air conditioning, mitigate the urban heat island effect, and potentially slow global warming. However, initially high roof solar reflectance can be degraded by natural soiling and weathering processes. We evaluated solar reflectance losses after three years of natural exposure reported in two separate databases: the Rated Products Directory of the US Cool Roof Rating Council (CRRC) and information reported by manufacturers to the US Environmental Protection Agency (EPA)'s ENERGY STAR® rating program. Many product ratings were culled because they were duplicative (within a database) or not measured. A second, site-resolved version of the CRRC dataset was created by transcribing from paper records the site-specific measurements of aged solar reflectance in Florida, Arizona and Ohio.Products with high initial solar reflectance tended to lose reflectance, while those with very low initial solar reflectance tended to become more reflective as they aged. Within the site-resolved CRRC database, absolute solar reflectance losses for samples of medium-to-high initial solar reflectance were 2–3 times greater in Florida (hot and humid) than in Arizona (hot and dry); losses in Ohio (temperate but polluted) were intermediate. Disaggregating results by product type—factory-applied coating, field-applied coating, metal, modified bitumen, shingle, single-ply membrane and tile—revealed that absolute solar reflectance losses were largest for field-applied coating, modified bitumen and single-ply membrane products, and smallest for factory-applied coating and metal products.The 2008 Title 24 provisional aged solar reflectance formula overpredicts the measured aged solar reflectance of 0–30% of each product type in the culled public CRRC database. The rate of overprediction was greatest for field-applied coating and single-ply membrane products and least for factory-applied coating, shingle, and metal products. New product-specific formulas of the form ρa′=0.20+β(ρi−0.20) can be used to estimate provisional aged solar reflectance ρa′ from initial solar reflectance ρi pending measurement of aged solar reflectance. The appropriate value of soiling resistance β varies by product type and is selected to attain some desired overprediction rate for the formula. The correlations for shingle products presented in this paper should not be used to predict aged solar reflectance or estimate provisional aged solar reflectance because the data set is too small and too limited in range of initial solar reflectance.Graphical abstractHighlights► Solar reflectance of a “cool” roof can be degraded by natural soiling and weathering. ► Absolute reflectance losses are 2–3 times greater in Florida (hot and humid) than in Arizona (hot and dry). ► Losses are largest for field-applied coating, modified bitumen and single-ply membrane products. ► Losses are smallest for factory-applied coating and metal products. ► New product-specific formulas estimate aged solar reflectance from initial solar reflectance.
    Solar Energy Materials and Solar Cells 01/2011; 95(12):3385-3399. · 5.03 Impact Factor
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    ABSTRACT: The photocatalytic activity of commercial kaolinite (KGa-1b) was evaluated for the degradation of methylene blue (MB) in aqueous suspension and of toluene in the gas phase. An enhanced photolysis of MB in the presence of kaolinite was detected, albeit at a slower rate than in the presence of the same mass of commercial TiO2 P25. Toluene removal under realistic ambient concentrations was catalyzed by both KGa-1b and P25; however, on a TiO2 content normalized basis, the clay mineral showed a higher photocatalytic rate. In the latter case, toluene degradation was found to be coupled to the presence of kaolinite surfaces, and not proportional to TiO2 content.
    Catalysis Communications - CATAL COMMUN. 01/2011; 12(8):698-702.
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    ABSTRACT: Prior research suggests that chemical processes taking place on the surface of particle filters employed in buildings may lead to the formation of harmful secondary byproducts. We investigated ozone reactions with fiberglass, polyester, cotton/polyester and polyolefin filter media, as well as hydrolysis of filter media additives. Studies were carried out on unused media, and on filters that were installed for 3 months in buildings at two different locations in the San Francisco Bay Area. Specimens from each filter media were exposed to ∼150 ppbv ozone in a flow tube under a constant flow of dry or humidified air (50% RH). Ozone breakthrough was recorded for each sample over periods of ∼1000 min; the ozone uptake rate was calculated for an initial transient period and for steady-state conditions. While ozone uptake was observed in all cases, we did not observe significant differences in the uptake rate and capacity for the various types of filter media tested. Most experiments were performed at an airflow rate of 1.3 L min−1 (face velocity = 0.013 m s−1), and a few tests were also run at higher rates (8–10 L min−1). Formaldehyde and acetaldehyde, two oxidation byproducts, were quantified downstream of each sample. Those aldehydes (m/z 31 and 45) and other volatile byproducts (m/z 57, 59, 61 and 101) were also detected in real-time using Proton-Transfer Reaction-Mass Spectrometry (PTR-MS). Low-ppbv byproduct emissions were consistently higher under humidified air than under dry conditions, and were higher when the filters were loaded with particles, as compared with unused filters. No significant differences were observed when ozone reacted over various types of filter media. Fiberglass filters heavily coated with impaction oil (tackifier) showed higher formaldehyde emissions than other samples. Those emissions were particularly high in the case of used filters, and were observed even in the absence of ozone, suggesting that hydrolysis of additives, rather than ozonolysis, is the main formaldehyde source in those filters. Emission rates of formaldehyde and acetaldehyde were not found to be large enough to substantially increase indoor concentrations in typical building scenarios. Nevertheless, ozone reactions on HVAC filters cannot be ignored as a source of low levels of indoor irritants.
    Atmospheric Environment 01/2011; 45(21):3561-3568. · 3.11 Impact Factor
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    ABSTRACT: Nicotine dynamics in an indoor environment can be greatly affected by building parameters (e.g. relative humidity (RH), air exchange rate (AER), and presence of ozone), as well as surface parameters (e.g. surface area (SA) and polarity). To better understand the indoor fate of nicotine, these parameter effects on its sorption, desorption, and oxidation rates were investigated on model indoor surfaces that included fabrics, wallboard paper, and wood materials. Nicotine sorption under dry conditions was enhanced by higher SA and higher polarity of the substrate. Interestingly, nicotine sorption to cotton and nylon was facilitated by increased RH, while sorption to polyester was hindered by it. Desorption was affected by RH, AER, and surface type. Heterogeneous nicotine-ozone reaction was investigated by Fourier transform infrared spectrometry with attenuated total reflection (FTIR-ATR), and revealed a pseudo first-order surface reaction rate of 0.035 +/- 0.015 min(-1) (at [O(3)] = 6 +/- 0.3 x 10(15) molecules cm(-3)) that was partially inhibited at high RH. Extrapolation to a lower ozone level ([O(3)] = 42 ppb) showed oxidation on the order of 10(-5) min(-1) corresponding to a half-life of 1 week. In addition, similar surface products were identified in dry and high RH using gas chromatography-mass spectrometry (GC-MS). However, FTIR analysis revealed different product spectra for these conditions, suggesting additional unidentified products and association with surface water. Knowing the indoor fate of condensed and gas phase nicotine and its oxidation products will provide a better understanding of nicotine's impact on personal exposures as well as overall indoor air quality.
    Physical Chemistry Chemical Physics 09/2010; 12(35):10356-64. · 4.20 Impact Factor
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    ABSTRACT: The effect of key experimental parameters on the removal of toluene under 254 + 185 nm irradiation was investigated using a benchtop photocatalytic flow reactor. Toluenewas introduced at low concentrations between 10 and 500 ppbv, typical of indoorenvironments, and reacted on TiO2-coated Raschig rings. Two different TiO2-coated rings were prepared: in one case, by dip-coating using a P25 aqueous suspension and, on the other, using an organic/inorganic sol-gel method that produced thin films of mesoporous anatase. Flow rates in the photoreactor varied between 4 L min-1 and 125 mL min-1, leading to residence times in the range 100 ms< tau< 2 s. For these conditions, toluene removal efficiencies were between 30 and 90percent, indicating that the system did not achieve total conversion in any case. For each air flow rate, the conversion oftoluene was significantly higher when the reactor length was 10 cm, as compared with 5 cm; however, only marginal increases in conversions were achieved in the two reactor lengths at equal residence time and different concentration of toluene, suggesting that that the reactor is effectively behaving as an ideal reactor and that the reaction is first-order in the concentration of toluene. Experiments were carried out between 0 and 66percent relative humidity (RH), the fastest reaction rate being observed at moderately low humidity conditions (10percent RH), with respect to both dry air and higher humidity levels. Formaldehyde was formed as a partial oxidation byproduct at low and at high residence times (240 and 960 ms), although higher formaldehyde molar yields (up to 20percent) were observed at low tau (240 ms) and moderate humidity conditions (10 and 33percent), suggesting that both tau and RH can be optimized toreduce the formation of harmful intermediates. Toluene removal efficiency increased with the TiO2 thickness (i.e., mass) until a maximum value of 500 nm, beyond which the removal efficiency decreased. This should be attributed to limitations on the rates of toluene decomposition imposed by radiation transport through the film and/or internal diffusion resistances, which can take place within the porous photocatalytic films.
    Applied Catalysis B: Environmental. 04/2010; 95(s 3–4).
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    ABSTRACT: This study shows that residual nicotine from tobacco smoke sorbed to indoor surfaces reacts with ambient nitrous acid (HONO) to form carcinogenic tobacco-specific nitrosamines (TSNAs). Substantial levels of TSNAs were measured on surfaces inside a smoker's vehicle. Laboratory experiments using cellulose as a model indoor material yielded a > 10-fold increase of surface-bound TSNAs when sorbed secondhand smoke was exposed to 60 ppbv HONO for 3 hours. In both cases we identified 1-(N-methyl-N-nitrosamino)-1-(3-pyridinyl)-4-butanal, a TSNA absent in freshly emitted tobacco smoke, as the major product. The potent carcinogens 4-(methylnitrosamino)-1-(3-pyridinyl)-1-butanone and N-nitroso nornicotine were also detected. Time-course measurements revealed fast TSNA formation, with up to 0.4% conversion of nicotine. Given the rapid sorption and persistence of high levels of nicotine on indoor surfaces-including clothing and human skin-this recently identified process represents an unappreciated health hazard through dermal exposure, dust inhalation, and ingestion. These findings raise concerns about exposures to the tobacco smoke residue that has been recently dubbed "thirdhand smoke." Our work highlights the importance of reactions at indoor interfaces, particularly those involving amines and NO(x)/HONO cycling, with potential health impacts.
    Proceedings of the National Academy of Sciences 02/2010; 107(15):6576-81. · 9.81 Impact Factor

Publication Stats

758 Citations
137.57 Total Impact Points


  • 2006–2014
    • Lawrence Berkeley National Laboratory
      • • Life Sciences Division
      • • Indoor Environment Group
      Berkeley, California, United States
  • 2008–2012
    • Arizona State University
      Phoenix, Arizona, United States
    • University of California, Berkeley
      • Department of Civil and Environmental Engineering
      Berkeley, California, United States
  • 2009–2011
    • Universidad Nacional Autónoma de México
      • School of Chemistry
      Mexico City, The Federal District, Mexico
  • 2007
    • Technical University of Denmark
      • International Centre for Indoor Environment and Energy
      Copenhagen, Capital Region, Denmark
  • 2002
    • University of California, Davis
      • Department of Environmental Toxicology
      Davis, CA, United States