Assessing exposures to household air pollution in public health research and program evaluation.

Exposure to smoke from the use of solid fuels and inefficient stoves for cooking and heating is responsible for approximately 4 million premature deaths yearly. As increasing investments are made to tackle this important public health issue, there is a need for identifying and providing guidance on best practices for exposure and stove performance monitoring, particularly for public health research and evaluation studies. This paper, which builds upon the discussion at an expert consultation on exposure assessment convened by the Global Alliance for Clean Cookstoves, the Centers for Disease Control and Prevention, and PATH in late 2012, aims to provide general guidance on what to monitor, who and where to monitor, and how to monitor household air pollution exposures. In addition, we summarize information about commercially available monitoring equipment and the technical properties of these monitors most important for household air pollution exposure assessment. The target audience includes epidemiologists conducting health studies and program evaluators aiming to quantify changes in exposures to estimate the potential health benefits of cookstoves intervention projects.

Particulate mass and polycyclic aromatic hydrocarbons exposure from secondhand smoke in the back seat of a vehicle.

CONTEXT: Exposure to secondhand smoke (SHS) has been reduced in the USA by banning smoking in public places. These restrictions have not had the same effect on children's exposure to SHS as adults suggesting that children are exposed to SHS in locations not covered by bans, such as private homes and cars. OBJECTIVES: Assess exposure to SHS in the backseat of a stationary vehicle where a child would sit, quantify exposures to fine particulates (PM2.5), polycyclic aromatic hydrocarbons (PAH), carbon monoxide (CO) and nicotine. Estimate the impact on a child's mean daily exposure to PM2.5. METHODS: SHS exposures in stationary vehicles with two different window configurations were monitored. A volunteer smoked three cigarettes in a one-hour period for twenty-two experiments. PM2.5, CO, nicotine and PAH where measured in the backseat of the vehicle. 16 PAH compounds were measured for in gas and particle phases as well as real-time particle phase concentrations. RESULTS: The mean PAH concentration, 1325.1 ng/m(3), was larger than concentrations measured in bars and restaurants were smoking is banned in many countries. We estimate that a child spending only ten minutes in the car with a smoker at the mean PM2.5 concentration measured in the first window configuration--1697 mg/m(3)--will cause a 30% increase to the daily mean PM2.5 personal average of a child. CONCLUSIONS: Estimates made using the measured data and previously reported PM2.5 daily mean concentrations for children in California showing that even short exposure periods are capable of creating large exposure to smoke.

A low-cost particle counter as a realtime fine-particle mass monitor.

Exposure to particles with aerodynamic diameters less than 2.5 µm is estimated to cause significant morbidity and mortality worldwide leading many countries to develop ambient air pollution standards and guidelines. At local scales, community and environmental justice groups are also concerned about PM 2.5 concentrations that may be elevated above regional concentrations typically measured by centrally located monitors and standards as well. In an attempt to develop a low cost, easy to use monitor we evaluated a low-cost optical particle counter, the Dylos™, as a fine particulate mass sensor. Modified into a system called the Berkeley Aerosol Information Recording System (BAIRS), we compared performance against standard commercial instruments in chambers using polystyrene latex spheres, ammonium sulphate, and woodsmoke and in an urban ambient setting. Overall we find that the limit of detection of the BAIRS is less than 1 µg m (-3) and the resolution is better than 1 µg m(-3) for PM 2.5. The BAIRS sizes small (<0.5 µm) particles, and is able to accurately estimate the mass concentration of particles of varying composition including organic, inorganic, and ambient particles. It is able to measure concentrations up to 10.0 mg m (-3). In an ambient roof-top test of the BAIRS and a more expensive commercially available light scattering particle monitor the BAIRS response tracked well with the commercial monitor and daily means were within 80% of each other. We conclude that with appropriate modification the system could be developed into an accurate low cost realtime particle mass monitor for use in a wide range of applications.

SOA formation from partitioning and heterogeneous reactions: model study in the presence of inorganic species.

A predictive model for secondary organic aerosol (SOA) formation by both partitioning and heterogeneous reactions was developed for SOA created from ozonolysis of alpha-pinene in the presence of preexisting inorganic seed aerosols. SOA was created in a 2 m3 polytetrafluoroethylene film indoor chamber under darkness. Extensive sets of SOA experiments were conducted varying humidity, inorganic seed compositions comprising of ammonium sulfate and sulfuric acid, and amounts of inorganic seed mass. SOA mass was decoupled into partitioning (OM(P)) and heterogeneous aerosol production (OM(H)). The reaction rate constant for OM(H) production was subdivided into three categories (fast, medium, and slow) to consider different reactivity of organic products for the particle phase heterogeneous reactions. The influence of particle acidity on reaction rates was treated in a previous semiempirical model. Model OM(H) was developed with medium and strong acidic seed aerosols, and then extrapolated to OM(H) in weak acidic conditions, which are more relevant to atmospheric aerosols. To demonstrate the effects of preexisting glyoxal derivatives (e.g., glyoxal hydrate and dimer) on OM(H), SOA was created with a seed mixture comprising of aqueous glyoxal and inorganic species. Our results show that heterogeneous SOA formation was also influenced by preexisting reactive glyoxal derivatives.

Semiempirical model for organic aerosol growth by acid-catalyzed heterogeneous reactions of organic carbonyls.

Aerosol growth by heterogeneous reactions of diverse carbonyls in the presence and absence of acidified seed aerosols was studied in a 4 m long flow reactor (2.5 cm i.d.) and a 2-m3 indoor Teflon film chamber under darkness. The acid catalytic effects on heterogeneous aerosol production were observed for diverse carbonyls in various ranges of humidities and compositions of seed inorganic aerosols. Particle population data measured by a scanning mobility particle sizer were used to calculate organic aerosol growth. To accountforthe aerosol growth contributed by heterogeneous reactions, the increase in organic aerosol mass was normalized bythe organic mass predicted by partitioning or the square of predicted organic mass. The carbonyl heterogeneous reactions were accelerated in the presence of acid catalysts (H2SO4), leading to higher aerosol yields than in their absence. The experimental data from aerosol yields in the flow reactorwere semiempirically fitted to the model parameters to predict the organic aerosol growth. The model parameters consist of environmental characteristics and molecular structure information of organic carbonyls. Basicity constants of carbonyls were used to describe the proton affinity of carbonyls for the acid catalysts. Particle environmental factors, such as humidity, temperature, and inorganic seed composition, were expressed by excess acidity and the parameters obtained from an inorganic thermodynamic model. A stepwise regression analysis of the aerosol growth model for the experimental data revealed that either the chemical structure information of carbonyls or characteristic environmental parameters are statistically significant in the prediction of organic aerosol growth. It was concluded thatthis model approach is applicable to predict secondary organic aerosol formation by heterogeneous reaction.

Atmospheric organic aerosol production by heterogeneous acid-catalyzed reactions.

Exploratory evidence from our laboratories shows that acidic surfaces on atmospheric aerosols lead to very real and potentially multifold increases in secondary organic aerosol (SOA) mass and build-up of stabilized nonvolatile organic matter as particles age. One possible explanation for these heterogeneous processes are the acid-catalyzed (e.g., H2SO4 and HNO3) reactions of atmospheric multifunctional organic species (e.g., multifunctional carbonyl compounds) that are accommodated onto the particle phase from the gas phase. Volatile organic hydrocarbons (VOCs) from biogenic sources (e.g., terpenoids) and anthropogenic sources (aromatics) are significant precursors for multifunctional organic species. The sulfur content of fossil fuels, which is released into the atmosphere as SO2, results in the formation of secondary inorganic acidic aerosols or indigenous acidic soot particles (e.g., diesel soot). The predominance of SOAs contributing to PM2.5 (particulate matter, that is, 2.5 microm or smaller than 2.5 microm), and the prevalence of sulfur in fossil fuels suggests that interactions between these sources could be considerable. This study outlines a systematic approach for exploring the fundamental chemistry of these particle-phase heterogeneous reactions. If acid-catalyzed heterogeneous reactions of SOA products are included in next-generation models, the predicted SOA formation will be much greater and have a much larger impact on climate-forcing effects than we now predict. The combined study of both organic and inorganic acids will also enable greater understanding of the adverse health effects in biological pulmonary organs exposed to particles.