Household Air Pollution Interventions to Improve Health in Low- and Middle-Income Countries: An Official American Thoracic Society Research Statement.

Background: An estimated 3 billion people, largely in low- and middle-income countries, rely on unclean fuels for cooking, heating, and lighting to meet household energy needs. The resulting exposure to household air pollution (HAP) is a leading cause of pneumonia, chronic lung disease, and other adverse health effects. In the last decade, randomized controlled trials of clean cooking interventions to reduce HAP have been conducted. We aim to provide guidance on how to interpret the findings of these trials and how they should inform policy makers and practitioners.Methods: We assembled a multidisciplinary working group of international researchers, public health practitioners, and policymakers with expertise in household air pollution from within academia, the American Thoracic Society, funders, nongovernmental organizations, and global organizations, including the World Bank and the World Health Organization. We performed a literature search, convened four sessions via web conference, and developed consensus conclusions and recommendations via the Delphi method.Results: The committee reached consensus on 14 conclusions and recommendations. Although some trials using cleaner-burning biomass stoves or cleaner-cooking fuels have reduced HAP exposure, the committee was divided (with 55% saying no and 45% saying yes) on whether the studied interventions improved measured health outcomes.Conclusions: HAP is associated with adverse health effects in observational studies. However, it remains unclear which household energy interventions reduce exposure, improve health, can be scaled, and are sustainable. Researchers should engage with policy makers and practitioners working to scale cleaner energy solutions to understand and address their information needs.

Assessing the Effects of Stove Use Patterns and Kitchen Chimneys on Indoor Air Quality during a Multiyear Cookstove Randomized Control Trial in Rural India.

We conducted indoor air quality (IAQ) measurements during a multiyear cookstove randomized control trial in two rural areas in northern and southern India. A total of 1205 days of kitchen PM2.5 were measured in control and intervention households during six ∼3 month long measurement periods across two study locations. Stoves used included traditional solid fuel (TSF), improved biomass, and liquefied petroleum gas (LPG) models. Intent-to-treat analysis indicates that the intervention reduced average 24 h PM2.5 and black carbon in only one of the two follow-up measurement periods in both areas, suggesting mixed effectiveness. Average PM2.5 levels were ∼50% lower in households with LPG (for exclusive LPG use: >75% lower) than in those without LPG. PM2.5 was 66% lower in households making exclusive use of an improved chimney stove versus a traditional chimney stove and TSF-exclusive kitchens with a built-in chimney had ∼60% lower PM2.5 than those without a chimney, indicating that kitchen ventilation can be as important as the stove technology in improving IAQ. Diurnal trends in real-time PM2.5 indicate that kitchen chimneys were especially effective at reducing peak concentrations, which leads to decreases in daily PM2.5 in these households. Our data demonstrate a clear hierarchy of IAQ improvement in real world, "stove-stacking" households, driven by different stove technologies and kitchen characteristics.

Pellet-Fed Gasifier Stoves Approach Gas-Stove Like Performance during in-Home Use in Rwanda.

Nearly all households in Rwanda burn solid fuels for cooking. A private firm in Rwanda is distributing forced-draft pellet-fed semigasifier cookstoves and fuel pellets. We measured in-use emissions of pollutants including fine particulate matter (PM2.5), organic and elemental carbon (OC, EC), black carbon (BC), and carbon monoxide (CO) in 91 uncontrolled cooking tests (UCTs) of both pellet and baseline (wood; charcoal) stoves. We observed >90% reductions in most pollutant emission factors/rates from pellet stoves compared to baseline stoves. Pellet stoves performed far better than gasifier stoves burning unprocessed wood, and consistent with ISO tiers 4 and 5 for PM2.5 and CO, respectively. Pellet stoves were generally clean, but performance varied; emissions from the dirtiest pellet tests matched those from the cleanest traditional stove tests. Our real-time data suggest that events occurring during ignition and the end of testing (e.g., refueling, char burnout) drive high emissions during pellet tests. We use our data to estimate potential health and climate cobenefits from stove adoption. This analysis suggests that pellet stoves have the potential to provide health benefits far above previously tested biomass stoves and approaching modern fuel stoves (e.g., LPG). Net climate impacts of pellet stoves range from similar to LPG to negligible, depending on biomass source and upstream emissions.

Seasonally Varying Secondary Organic Aerosol Formation From In-Situ Oxidation of Near-Highway Air.

The extent to which motor vehicles contribute to ambient secondary organic aerosol (SOA) remains uncertain. Here, we present in situ measurements of SOA formation at a near-highway site with substantial tree-cover 10 m from Interstate 40 near Durham, North Carolina. In July 2015 (summer) and February 2016 (winter), we exposed ambient air to a range of oxidant (O3 and OH) concentrations in an oxidation flow reactor (OFR), resulting in hours to weeks of equivalent atmospheric aging. We observed substantial seasonal variation in SOA formation upon OFR aging; diurnally varying OA enhancements of ∼3-8 µg m-3 were observed in summer and significantly lower enhancements (∼0.5-1 µg m-3) in winter. Measurements in both seasons showed consistent changes in bulk OA properties (chemical composition; volatility) with OFR aging. Mild increases in traffic-related SOA precursors during summer partly explains the seasonal variation. However, biogenic emissions, with sharp temperature dependence, appear to dominate summer OFR-SOA. Our analysis indicates that SOA observed in the OFR is similar (within a factor of 2) to that predicted to form from traffic and biogenic precursors using literature yields, especially in winter. This study highlights the utility of the OFR for studying the prevalence of SOA precursors in complex real-world settings.

In-Use Emissions and Estimated Impacts of Traditional, Natural- and Forced-Draft Cookstoves in Rural Malawi.

Emissions from traditional cooking practices in low- and middle-income countries have detrimental health and climate effects; cleaner-burning cookstoves may provide "co-benefits". Here we assess this potential via in-home measurements of fuel-use and emissions and real-time optical properties of pollutants from traditional and alternative cookstoves in rural Malawi. Alternative cookstove models were distributed by existing initiatives and include a low-cost ceramic model, two forced-draft cookstoves (FDCS; Philips HD4012LS and ACE-1), and three institutional cookstoves. Among household cookstoves, emission factors (EF; g (kg wood)-1) were lowest for the Philips, with statistically significant reductions relative to baseline of 45% and 47% for fine particulate matter (PM2.5) and carbon monoxide (CO), respectively. The Philips was the only cookstove tested that showed significant reductions in elemental carbon (EC) emission rate. Estimated health and climate cobenefits of alternative cookstoves were smaller than predicted from laboratory tests due to the effects of real-world conditions including fuel variability and nonideal operation. For example, estimated daily PM intake and field-measurement-based global warming commitment (GWC) for the Philips FDCS were a factor of 8.6 and 2.8 times higher, respectively, than those based on lab measurements. In-field measurements provide an assessment of alternative cookstoves under real-world conditions and as such likely provide more realistic estimates of their potential health and climate benefits than laboratory tests.

Primary and Photochemically Aged Aerosol Emissions from Biomass Cookstoves: Chemical and Physical Characterization.

Secondary organic aerosol (SOA) formation during photo-oxidation of primary emissions from cookstoves used in developing countries may make important contributions to their climate and air quality impacts. We present results from laboratory experiments with a field portable oxidation flow reactor (F-OFR) to study the evolution of emissions over hours to weeks of equivalent atmospheric aging. Lab tests, using dry red oak, measured fresh and aged emissions from a 3 stone fire (TSF), a "rocket" natural draft stove (NDS), and a forced draft gasifier stove (FDGS), in order of increasing modified combustion efficiency (MCE) and decreasing particulate matter emission factors (EF). SOA production was observed for all stoves/tests; organic aerosol (OA) enhancement factor ranged from 1.2 to 3.1, decreasing with increased MCE. In primary emissions, OA mass spectral fragments associated with oxygenated species (primary biomass burning markers) increased (decreased) with MCE; fresh OA from FDGS combustion was especially oxygenated. OA oxygenation increased with further oxidation for all stove emissions, even where minimal enhancement was observed. More efficient stoves emit particles with greater net direct specific warming than TSFs, with the difference increasing with aging. Our results show that the properties and evolution of cookstove emissions are a strong function of combustion efficiency and atmospheric aging.

Exploring Divergent Volatility Properties from Yield and Thermodenuder Measurements of Secondary Organic Aerosol from α-Pinene Ozonolysis.

There are large uncertainties in the parameters dictating the gas-particle partitioning of secondary organic aerosols (SOA), although this process has major influences on their atmospheric lifecycle. Here, we extract parameters that describe the partitioning of SOA from α-pinene ozonolysis using measurements from a dual-thermodenuder (TD) system that constrains both the equilibrium and the kinetic properties that dictate SOA phase partitioning. Parallel TDs that vary in temperature and residence time were used with an evaporation-kinetics model to extract parameter values. An evaporation coefficient of an order of 0.1 best describes the observed evaporation, suggesting equilibration time scales of atmospheric SOA on the order of minutes to hours. A total of 20-40% of SOA mass consists of low-volatility material (saturation concentration of <0.3 µg m(-3)) in the TD-derived SOA volatility distribution. While distinct from existing parametrizations from aerosol growth experiments, derived values are consistent with recent observations of slow room-temperature evaporation of SOA and contributions from extremely low volatility organic compounds formed during α-pinene ozonolysis. The volatility parameters thus determined suggest that SOA yields and enthalpies of evaporation are substantially higher, and products less volatile, than is currently assumed in atmospheric models. These results will help improve the representation of SOA in air-quality and climate models.

Health and Climate-Relevant Pollutant Concentrations from a Carbon-Finance Approved Cookstove Intervention in Rural India.

Efforts to introduce more efficient stoves increasingly leverage carbon-finance to scale up dissemination of interventions. We conducted a randomized intervention study to evaluate a Clean Development Mechanism approved stove replacement impact on fuelwood usage, and climate and health-relevant air pollutants. We randomly assigned 187 households to either receive the intervention or to continue using traditional stoves. Measurements of fine particulate matter (PM2.5) and absorbance were conducted in cooking areas, village center and at upwind background site. There were minor and overlapping seasonal differences (post- minus preintervention change) between control and intervention groups for median (95% CI) fuel use (-0.60 (-1.02, -0.22) vs -0.52 (-1.07, 0.00) kg day(-1)), and 24 h absorbance (35 (18, 60) vs 36 (22, 50) × 10(-6) m(-1)); for 24 h PM2.5, there was a higher (139 (61,229) vs 73(-6, 156) µg m(-3))) increase in control compared to intervention homes between the two seasons. Forty percent of the intervention homes continued using traditional stoves. For intervention homes, absorbance-to-mass ratios suggest a higher proportion of black carbon in PM2.5 emitted from intervention compared with traditional stoves. Absent of field-based evaluation, stove interventions may be pursued that fail to realize expected carbon reductions or anticipated health and climate cobenefits.

Development, Demonstration, and Evaluation of Routine Monitoring of Aerosol Carbon, Oxygen, and Sulfur Content.

Traditional online measurements of the chemical composition of particulate matter have relied on expensive and complex research-grade instrumentation based on mass spectrometry and/or chromatography. However, routine monitoring requires lower-cost alternatives that can be operated autonomously, and such tools are lacking. Routine monitoring of particulate matter, especially organic aerosol, relies instead on offline techniques such as filter collection that require significant operator effort. To address this gap, we present here a new online instrument, the "ChemSpot", that provides information on organic aerosol mass loading, volatility, and degree of oxygenation, along with sulfur content. The instrument grows particles with water condensation, impacts them onto a passivated surface with low heat capacity, and uses stepped thermal desorption of analytes to a combination of flame ionization detector (FID) and flame photometric detector (FPD) and then to a CO2 detector downstream of the FID/FPD setup. By relying on detectors designed for gas chromatography, calibration is achieved almost entirely through the introduction of gases without the need for regular introduction of particle-phase calibrants. Particle collection efficiency of greater than 95% was achieved consistently, and the collection cell was shown to rapidly and precisely heat to ∼800 °C at a rate as fast as 10 °C per second. Measurements of total organic carbon, volatility distribution of organic aerosol, total sulfur, and oxygen-to-carbon ratio (O:C) collected during a continuous multi-week period are presented here to demonstrate the autonomous operation of "ChemSpot". Colocated measurements with a mass spectrometer, an aerosol chemical speciation monitor (ACSM), show good correlation and relatively low bias between the instruments (mean absolute percentage error of 21% and 27% for organic carbon and equivalent sulfate measurements, respectively).

Development of Volatility Distributions for Organic Matter in Biomass Burning Emissions.

The volatility distribution of organic emissions from biomass burning and other combustion sources can determine their atmospheric evolution due to partitioning/aging. The gap between measurements and models predicting secondary organic aerosol has been partially attributed to the absence of semi- and intermediate volatility organic compounds (S/I-VOC) in models and measurements. However, S/I-VOCs emitted from these sources and typically quantified using the volatility basis framework (VBS) are not well understood. For example, the amount and composition of S/I-VOCs and their variability across different biomass burning sources such as residential woodstoves, open field burns, and laboratory simulated open burning are uncertain. To address this, a novel filter-in-tube sorbent tube sampling method collected S/I-VOC samples from biomass burning experiments for a range of fuels and combustion conditions. Filter-in-tube samples were analyzed using thermal desorption-gas chromatography-mass spectrometry (TD/GC/MS) for compounds across a wide range of volatilities (saturation concentrations; -2 ≤ logC* ≤ 6). The S/I-VOC measurements were used to calculate volatility distributions for each emissions source. The distributions were broadly consistent across the sources with IVOCs accounting for 75% - 90% of the total captured organic matter, while SVOCs and LVOCs were responsible for 6% - 13% and 1% - 12%, respectively. The distributions and predicted partitioning were generally consistent with literature. Particulate matter emission factors spanned two orders of magnitude across the sources. This work highlights the potential of inferring gas-particle partitioning behavior of biomass burning emissions using filter-in-tube sorbent samples analyzed offline. This simplifies both sampling and analysis of S/I-VOCs for studies focused on capturing the full range of organics emitted.

Toxicity of fresh and aged anthropogenic smoke particles emitted from different burning conditions.

There is substantial evidence that photochemical reactions in the atmosphere cause physico-chemical transformation of combustion smoke, but how this processing modifies potential health effects in exposed populations is not well understood. Here we utilized a new approach to simulate photochemical aging of anthropogenic smoke emissions (a mixture of plastic, plywood, and cardboard smoke) from two different burning conditions (smoldering vs. flaming) and investigated their adverse outcomes associated with mutagenic activity and the relative potencies of different polycyclic aromatic hydrocarbons (PAHs). Aging resulted in increased oxygenated volatile organic compound (VOC) emissions but largely degraded particle-bound PAH components in the smoke. Chemical transformation during aging was more dramatic for flaming versus smoldering smoke. Due to the PAH degradation, mutagenicity of the aged smoke from flaming combustion was much lower (up to 4 times) than that of the fresh smoke on per-particle mass basis. However, on the basis of particle emitted per fuel mass burned, the aged and fresh smoke particles exhibited similar mutagenic activities, which were up to 3 times higher for smoldering versus flaming smoke emissions. Similarly, the PAH toxicity equivalent (PAH-TEQ) of the aged smoldering smoke was 3 times higher than that of the aged flaming smoke particles, suggesting that some PAHs (e.g., indeno[c,d]pyrene and benzo[b]fluoranthene) in the smoldering smoke were more photochemically stable during aging. These findings increase understanding of the evolution of smoke emitted at different burning conditions and the role of photochemical transformations on mutagenicity and PAH-induced toxicity.

Climate and health relevant emissions from in-use Indian three-wheelers fueled by natural gas and gasoline.

Auto-rickshaws in India use different fuels and engine technologies, with varying emissions and implications for air quality and climate change. Chassis dynamometer emission testing was conducted on 30 in-use auto-rickshaws to quantify the impact of switching from gasoline to compressed natural gas (CNG) in spark-ignition engines. Thirteen test vehicles had two-stroke CNG engines (CNG-2S) and 17 had four-stroke CNG engines (CNG-4S), of which 11 were dual-fuel and operable on a back-up gasoline (petrol) system (PET-4S). Fuel-based emission factors were determined for gaseous pollutants (CO(2), CH(4), NO(X), THC, and CO) and fine particulate matter (PM(2.5)). Intervehicle variability was high, and for most pollutants there was no significant difference (95% confidence level) between "old" (1998-2001) and "new" (2007-2009) age-groups within a given fuel-technology class. Mean fuel-based PM(2.5) emission factor (mean (95% confidence interval)) for CNG-2S (14.2 g kg(-1) (6.2-26.7)) was almost 30 times higher than for CNG-4S (0.5 g kg(-1) (0.3-0.9)) and 12 times higher than for PET-4S (1.2 g kg(-1) (0.8-1.7)). Global warming commitment associated with emissions from CNG-2S was more than twice that from CNG-4S or PET-4S, due mostly to CH(4) emissions. Comprehensive measurements and data should drive policy interventions rather than assumptions about the impacts of clean fuels.

In-use emissions from biomass and LPG stoves measured during a large, multi-year cookstove intervention study in rural India.

We conducted an emission measurement campaign as a part of a multiyear cookstove intervention trial in two rural locations in northern and southern India. 253 uncontrolled cooking tests measured emissions in control and intervention households during three ~3-month-long measurement periods in each location. We measured pollutants including fine particulate matter (PM2.5), organic and elemental carbon (OC, EC), black carbon (BC) and carbon monoxide (CO) from stoves ranging from traditional solid fuel (TSF) to improved biomass stoves (rocket, gasifier) to liquefied petroleum gas (LPG) models. TSF stoves showed substantial variability in pollutant emission factors (EFs; g kg-1 wood) and optical properties across measurement periods. Multilinear regression modeling found that measurement period, fuel properties, relative humidity, and cooking duration are significant predictors of TSF EFs. A rocket stove showed moderate reductions relative to TSF. LPG stoves had the lowest pollutant EFs, with mean PM2.5 and CO EFs (g MJdelivered-1) >90% lower than biomass stoves. However, in-home EFs of LPG were substantially higher than lab EFs, likely influenced by non-ideal combustion performance, emissions from food and possible influence from other combustion sources. In-home emission measurements may depict the actual exposure benefits associated with dissemination of LPG stoves in real world interventions.

Updating the conceptual model for fine particle mass emissions from combustion systems.

Atmospheric transformations determine the contribution of emissions from combustion systems to fine particulate matter (PM) mass. For example, combustion systems emit vapors that condense onto existing particles or form new particles as the emissions are cooled and diluted. Upon entering the atmosphere, emissions are exposed to atmospheric oxidants and sunlight, which causes them to evolve chemically and physically, generating secondary PM. This review discusses these transformations, focusing on organic PM. Organic PM emissions are semi-volatile at atmospheric conditions and thus their partitioning varies continuously with changing temperature and concentration. Because organics contribute a large portion of the PM mass emitted by most combustion sources, these emissions cannot be represented using a traditional, static emission factor. Instead, knowledge of the volatility distribution of emissions is required to explicitly account for changes in gas-particle partitioning. This requires updating how PM emissions from combustion systems are measured and simulated from combustion systems. Secondary PM production often greatly exceeds the direct or primary PM emissions; therefore, secondary PM must be included in any assessment of the contribution of combustion systems to ambient PM concentrations. Low-volatility organic vapors emitted by combustion systems appear to be very important secondary PM precursors that are poorly accounted for in inventories and models. The review concludes by discussing the implications that the dynamic nature of these PM emissions have on source testing for emission inventory development and regulatory purposes. This discussion highlights important linkages between primary and secondary PM, which could lead to simplified certification test procedures while capturing the emission components that contribute most to atmospheric PM mass.

Determinants of Cookstoves and Fuel Choice Among Rural Households in India.

Roughly 2.8 billion people depend on solid fuels for cooking needs, resulting in a tremendous burden of disease from exposure to household air pollution. Despite decades of effort to promote cleaner cooking technologies, displacement of polluting technologies has progressed slowly. This paper describes results of a randomized controlled trial in which eight communities in two regions of rural India were presented with a range of cooking choices including improved solid fuel stoves and clean cooking options like liquefied petroleum gas (LPG) and induction stoves. Using survey data and logistic and multinomial regression, we identify factors associated with two outcomes: (1) pre-intervention ownership of non-solid fuel technologies and (2) household preferences for clean fuels from the range of cooking options offered. The analysis allows us to examine the influence of education, wealth, gender empowerment, stove pricing, and stove exchanges, among other variables. The majority of participants across all communities selected the cleanest options, LPG and induction, irrespective of price, but there is some variation in preferences. Wealth and higher caste stand out as significant predictors of pre-intervention ownership and non-solid fuel cooking options as well as preference for cleaner technologies offered through the intervention. The experimental treatments also influence preferences in some communities. When given the opportunity to exchange, communities in one region are more likely to choose solid fuel stoves (P < 0.05). Giving free stoves had mixed results; households in one region are more likely to select clean options (P < 0.05), but households in the other region prefer solid fuels (P < 0.10).

Clean cooking and the SDGs: Integrated analytical approaches to guide energy interventions for health and environment goals.

Development and implementation of clean cooking technology for households in low and middle income countries (LMICs) offer enormous promise to advance at least five Sustainable Development Goals (SDGs): 3. Good health and well-being; 5. Gender equality; 7. Affordable and clean energy; 13. Climate action; 15. Life on land. Programs are being implemented around the world to introduce alternative cooking technologies, and we are well on the way to achieving the goal set by the Global Alliance for Clean Cookstoves to reach 100 million homes with cleaner and more efficient cooking methods by 2020. Despite evidence that household air pollution (HAP) from solid fuel combustion is responsible for 3-4 million early deaths per year, many cookstove programs are motivated and/or financed by climate change mitigation schemes and deploy alternative stoves that use solid fuels such as wood and charcoal. However, recent studies have demonstrated that improved biomass-burning stoves typically only incrementally improve air quality and yield modest or minimal health benefits. Likewise, their contributions to climate change mitigation and other SDGs may be limited. Evidence indicates that cleaner fuels, such as liquefied petroleum gas (LPG), ethanol and biogas, offer greater potential benefits not only to health, but also greater progress towards climate goals and other relevant SDGs. We present a modeled estimate of these potential gains for a diverse group of 40 LMICs. Our model suggests that cookstove programs using LPG stoves and fuel will yield greater reductions in both Disability Adjusted Life Years and Global Warming Commitment in these countries than those using improved biomass stoves. Cost and infrastructure requirements for clean fuels such as LPG are widely recognized constraints. In view of these constraints we present an analytical method to simultaneously consider health and climate needs at the national level for the same 40 countries in the context of estimated LPG expansion potentials. Comparative analyses integrating priorities across SDGs at the national and regional levels may guide more practical and effective household energy development choices going forward.

Emission factors of health- and climate-relevant pollutants measured in home during a carbon-finance-approved cookstove intervention in rural India.

We present results of an emission characterization effort, completed as part of a larger intervention trial, of a carbon-finance-approved program replacing traditional cookstoves with "rocket"-style natural draft stoves. The 100 emission tests were conducted across 31 households in control and intervention groups, with repeated tests in most households during preintervention and postintervention periods. While mean fine particulate matter (PM2.5) emission factor for intervention stoves was significantly lower than for traditional stoves in baseline measurements, they were only marginally lower than traditional stoves during follow-up. Intervention stove PM2.5 emissions had a larger contribution from light-absorbing (elemental) carbon than traditional stoves. Repeated measurements in control households provide evidence for strong seasonality, likely due to differences in fuel moisture/types, in traditional stove emissions, with important implications for study design. Seasonality observed in control household emission factors (baseline > follow-up) was in the opposite direction as that observed in indoor PM2.5 concentrations (baseline < follow-up), highlighting that seasonally varying conditions (e.g., ventilation rates) may modify the link between emissions and exposures. Emission factor differences in paired (pre/post) tests from the same households were similar to differences in the medians of entire groups, suggesting variability is dominated by test-to-test variation. Emission reductions from intervention stoves were significantly smaller than laboratory performance would suggest or that are required to strongly reduce exposures. Field emissions assessment like that presented here should be prioritized early in technology assessment and development to provide rigorous estimates of the benefits reasonably expected from interventions with the potential for substantial benefits to human health and the environment.

Constraining the volatility distribution and gas-particle partitioning of combustion aerosols using isothermal dilution and thermodenuder measurements.

The gas-particle partitioning of primary organic aerosol (POA) emissions from a diesel engine and the combustion of hard- and soft-woods in a stove was investigated by isothermally diluting them in a smog chamber or by passing them through a thermodenuder and measuring the extent of evaporation. The experiments were conducted at atmospherically relevant conditions: low concentrations and small temperature perturbations. The partitioning of the POA emissions from both sources varied continuously with changing concentration and temperature. Although the POA emissions are semivolatile, they do not completely evaporate at typical atmospheric conditions. The overall partitioning characteristics of diesel and wood smoke POA are similar, with wood smoke being somewhat less volatile than the diesel exhaust. The gas-particle partitioning of aerosols formed from flash-vaporized engine lubricating oil was also studied; diesel POA is somewhat more volatile than the oil aerosol. The experimental data from the dilution- and thermodenuder-based techniques were fit using absorptive partitioning theory to derive a volatility distribution of the POA emissions from each source. These distributions are suitable for use in chemical transport models that simulate POA concentrations.

Rethinking organic aerosols: semivolatile emissions and photochemical aging.

Most primary organic-particulate emissions are semivolatile; thus, they partially evaporate with atmospheric dilution, creating substantial amounts of low-volatility gas-phase material. Laboratory experiments show that photo-oxidation of diesel emissions rapidly generates organic aerosol, greatly exceeding the contribution from known secondary organic-aerosol precursors. We attribute this unexplained secondary organic-aerosol production to the oxidation of low-volatility gas-phase species. Accounting for partitioning and photochemical processing of primary emissions creates a more regionally distributed aerosol and brings model predictions into better agreement with observations. Controlling organic particulate-matter concentrations will require substantial changes in the approaches that are currently used to measure and regulate emissions.