Exposure Assessment For Air-To-Skin Uptake of Semivolatile Organic Compounds (SVOCs) Indoors.

Semivolatile organic compounds (SVOCs) are ubiquitous in the indoor environment and a priority for exposure assessment because of the environmental health concerns that they pose. Direct air-to-skin dermal uptake has been shown to be comparable to the inhalation intake for compounds with certain chemical properties. In this study, we aim to further understand the transport of these types of chemicals through the skin, specifically through the stratum corneum (SC). Our assessment is based on collecting three sequential forehead skin wipes, each hypothesized to remove pollutants from successively deeper skin layers, and using these wipe analyses to determine the skin concentration profiles. The removal of SVOCs with repeated wipes reveals the concentration profiles with depth and provides a way to characterize penetration efficiency and potential transfer to blood circulation. We used a diffusion model applied to surface skin to simulate concentration profiles of SVOCs and compared them with the measured values. We found that two phthalates, dimethyl and diethyl phthalates, penetrate deeper into skin with similar exposure compared to other phthalates and targeted SVOCs, an observation supported by the model results as well. We also report the presence of statistically significant declining patterns with skin depth for most SVOCs, indicating that their diffusion through the SC is relevant and eventually can reach the blood vessels in the vascularized dermis. Finally, using a nontarget approach, we identified skin oxidation products, linked to respiratory irritation symptoms, formed from the reaction between ozone and squalene.

Global Effect Factors for Exposure to Fine Particulate Matter.

We evaluate fine particulate matter (PM2.5) exposure-response models to propose a consistent set of global effect factors for product and policy assessments across spatial scales and across urban and rural environments. Relationships among exposure concentrations and PM2.5-attributable health effects largely depend on location, population density, and mortality rates. Existing effect factors build mostly on an essentially linear exposure-response function with coefficients from the American Cancer Society study. In contrast, the Global Burden of Disease analysis offers a nonlinear integrated exposure-response (IER) model with coefficients derived from numerous epidemiological studies covering a wide range of exposure concentrations. We explore the IER, additionally provide a simplified regression as a function of PM2.5 level, mortality rates, and severity, and compare results with effect factors derived from the recently published global exposure mortality model (GEMM). Uncertainty in effect factors is dominated by the exposure-response shape, background mortality, and geographic variability. Our central IER-based effect factor estimates for different regions do not differ substantially from previous estimates. However, IER estimates exhibit significant variability between locations as well as between urban and rural environments, driven primarily by variability in PM2.5 concentrations and mortality rates. Using the IER as the basis for effect factors presents a consistent picture of global PM2.5-related effects for use in product and policy assessment frameworks.

Modeling the Emergence of Antibiotic Resistance in the Environment: an Analytical Solution for the Minimum Selection Concentration.

Environmental antibiotic risk management requires an understanding of how subinhibitory antibiotic concentrations contribute to the spread of resistance. We develop a simple model of competition between sensitive and resistant bacterial strains to predict the minimum selection concentration (MSC), the lowest level of antibiotic at which resistant bacteria are selected. We present an analytical solution for the MSC based on the routinely measured MIC, the selection coefficient (sc) that expresses fitness differences between strains, the intrinsic net growth rate, and the shape of the bacterial growth dose-response curve with antibiotic or metal exposure (the Hill coefficient [κ]). We calibrated the model by optimizing the Hill coefficient to fit previously reported experimental growth rate difference data. The model fit varied among nine compound-taxon combinations examined but predicted the experimentally observed MSC/MIC ratio well (R2 ≥ 0.95). The shape of the antibiotic response curve varied among compounds (0.7 ≤ κ ≤ 10.5), with the steepest curve being found for the aminoglycosides streptomycin and kanamycin. The model was sensitive to this antibiotic response curve shape and to the sc, indicating the importance of fitness differences between strains for determining the MSC. The MSC can be >1 order of magnitude lower than the MIC, typically by the factor scκ This study provides an initial quantitative depiction and a framework for a research agenda to examine the growing evidence of selection for resistant bacterial communities at low environmental antibiotic concentrations.

Characterizing Aggregated Exposure to Primary Particulate Matter: Recommended Intake Fractions for Indoor and Outdoor Sources.

Exposure to fine particulate matter (PM2.5) from indoor and outdoor sources is a leading environmental contributor to global disease burden. In response, we established under the auspices of the UNEP/SETAC Life Cycle Initiative a coupled indoor-outdoor emission-to-exposure framework to provide a set of consistent primary PM2.5 aggregated exposure factors. We followed a matrix-based mass balance approach for quantifying exposure from indoor and ground-level urban and rural outdoor sources using an effective indoor-outdoor population intake fraction and a system of archetypes to represent different levels of spatial detail. Emission-to-exposure archetypes range from global indoor and outdoor averages, via archetypal urban and indoor settings, to 3646 real-world cities in 16 parametrized subcontinental regions. Population intake fractions from urban and rural outdoor sources are lowest in Northern regions and Oceania and highest in Southeast Asia with population-weighted means across 3646 cities and 16 subcontinental regions of, respectively, 39 ppm (95% confidence interval: 4.3-160 ppm) and 2 ppm (95% confidence interval: 0.2-6.3 ppm). Intake fractions from residential and occupational indoor sources range from 470 ppm to 62 000 ppm, mainly as a function of air exchange rate and occupancy. Indoor exposure typically contributes 80-90% to overall exposure from outdoor sources. Our framework facilitates improvements in air pollution reduction strategies and life cycle impact assessments.

A multivariate analysis of CalEnviroScreen: comparing environmental and socioeconomic stressors versus chronic disease.

BACKGROUND: The health-risk assessment paradigm is shifting from single stressor evaluation towards cumulative assessments of multiple stressors. Recent efforts to develop broad-scale public health hazard datasets provide an opportunity to develop and evaluate multiple exposure hazards in combination. METHODS: We performed a multivariate study of the spatial relationship between 12 indicators of environmental hazard, 5 indicators of socioeconomic hardship, and 3 health outcomes. Indicators were obtained from CalEnviroScreen (version 3.0), a publicly available environmental justice screening tool developed by the State of California Environmental Protection Agency. The indicators were compared to the total rate of hospitalization for 14 ICD-9 disease categories (a measure of disease burden) at the zip code tabulation area population level. We performed principal component analysis to visualize and reduce the CalEnviroScreen data and spatial autoregression to evaluate associations with disease burden. RESULTS: CalEnviroScreen was strongly associated with the first principal component (PC) from a principal component analysis (PCA) of all 20 variables (Spearman ρ = 0.95). In a PCA of the 12 environmental variables, two PC axes explained 43% of variance, with the first axis indicating industrial activity and air pollution, and the second associated with ground-level ozone, drinking water contamination and PM2.5. Mass of pesticides used in agriculture was poorly or negatively correlated with all other environmental indicators, and with the CalEnviroScreen calculation method, suggesting a limited ability of the method to capture agricultural exposures. In a PCA of the 5 socioeconomic variables, the first PC explained 66% of variance, representing overall socioeconomic hardship. In simultaneous autoregressive models, the first environmental and socioeconomic PCs were both significantly associated with the disease burden measure, but more model variation was explained by the socioeconomic PCs. CONCLUSIONS: This study supports the use of CalEnviroScreen for its intended purpose of screening California regions for areas with high environmental exposure and population vulnerability. Study results further suggest a hypothesis that, compared to environmental pollutant exposure, socioeconomic status has greater impact on overall burden of disease.

Indoor Air Pollutant Exposure for Life Cycle Assessment: Regional Health Impact Factors for Households.

Human exposure to indoor pollutant concentrations is receiving increasing interest in Life Cycle Assessment (LCA). We address this issue by incorporating an indoor compartment into the USEtox model, as well as by providing recommended parameter values for households in four different regions of the world differing geographically, economically, and socially. With these parameter values, intake fractions and comparative toxicity potentials for indoor emissions of dwellings for different air tightness levels were calculated. The resulting intake fractions for indoor exposure vary by 2 orders of magnitude, due to the variability of ventilation rate, building occupation, and volume. To compare health impacts as a result of indoor exposure with those from outdoor exposure, the indoor exposure characterization factors determined with the modified USEtox model were applied in a case study on cooking in non-OECD countries. This study demonstrates the appropriateness and significance of integrating indoor environments into LCA, which ensures a more holistic account of all exposure environments and allows for a better accountability of health impacts. The model, intake fractions, and characterization factors are made available for use in standard LCA studies via www.usetox.org and in standard LCA software.

Risk-Based High-Throughput Chemical Screening and Prioritization using Exposure Models and in Vitro Bioactivity Assays.

We present a risk-based high-throughput screening (HTS) method to identify chemicals for potential health concerns or for which additional information is needed. The method is applied to 180 organic chemicals as a case study. We first obtain information on how the chemical is used and identify relevant use scenarios (e.g., dermal application, indoor emissions). For each chemical and use scenario, exposure models are then used to calculate a chemical intake fraction, or a product intake fraction, accounting for chemical properties and the exposed population. We then combine these intake fractions with use scenario-specific estimates of chemical quantity to calculate daily intake rates (iR; mg/kg/day). These intake rates are compared to oral equivalent doses (OED; mg/kg/day), calculated from a suite of ToxCast in vitro bioactivity assays using in vitro-to-in vivo extrapolation and reverse dosimetry. Bioactivity quotients (BQs) are calculated as iR/OED to obtain estimates of potential impact associated with each relevant use scenario. Of the 180 chemicals considered, 38 had maximum iRs exceeding minimum OEDs (i.e., BQs > 1). For most of these compounds, exposures are associated with direct intake, food/oral contact, or dermal exposure. The method provides high-throughput estimates of exposure and important input for decision makers to identify chemicals of concern for further evaluation with additional information or more refined models.

Building a Human Health Risk Assessment Ontology (RsO): A Proposed Framework.

Over the last decade the health and environmental research communities have made significant progress in collecting and improving access to genomic, toxicology, exposure, health, and disease data useful to health risk assessment. One of the barriers to applying these growing volumes of information in fields such as risk assessment is the lack of informatics tools to organize, curate, and evaluate thousands of journal publications and hundreds of databases to provide new insights on relationships among exposure, hazard, and disease burden. Many fields are developing ontologies as a way of organizing and analyzing large amounts of complex information from multiple scientific disciplines. Ontologies include a vocabulary of terms and concepts with defined logical relationships to each other. Building from the recently published exposure ontology and other relevant health and environmental ontologies, this article proposes an ontology for health risk assessment (RsO) that provides a structural framework for organizing risk assessment information and methods. The RsO is anchored by eight major concepts that were either identified by exploratory curations of the risk literature or the exposure-ontology working group as key for describing the risk assessment domain. These concepts are: (1) stressor, (2) receptor, (3) outcome, (4) exposure event, (5) dose-response approach, (6) dose-response metric, (7) uncertainty, and (8) measure of risk. We illustrate the utility of these concepts for the RsO with example curations of published risk assessments for ionizing radiation, arsenic in drinking water, and persistent pollutants in salmon.

Phthalate exposure and risk assessment in California child care facilities.

Approximately 13 million U.S. children less than 6 years old spend some time in early childhood education (ECE) facilities where they may be exposed to potentially harmful chemicals during critical periods of development. We measured five phthalate esters in indoor dust (n = 39) and indoor and outdoor air (n = 40 and 14, respectively) at ECE facilities in Northern California. Dust and airborne concentrations were used to perform a probabilistic health risk assessment to compare estimated exposures with risk levels established for chemicals causing reproductive toxicity and cancer under California's Proposition 65. Di(2-ethylhexyl) phthalate (DEHP) and butyl benzyl phthalate (BBzP) were the dominant phthalates present in floor dust (medians = 172.2 and 46.8 µg/g, respectively), and dibutyl phthalate (DBP), diethyl phthalate (DEP), and diisobutyl phthalate (DIBP) were the dominant phthalates in indoor air (medians = 0.52, 0.21, and 0.10 µg/m(3), respectively). The risk assessment results indicate that 82-89% of children in California ECE had DBP exposure estimates exceeding reproductive health benchmarks. Further, 8-11% of children less than 2 years old had DEHP exposure estimates exceeding cancer benchmarks. This is the largest study to measure phthalate exposure in U.S. ECE facilities and findings indicate wide phthalate contamination and potential risk to developing children.

Role of lignin in reducing life-cycle carbon emissions, water use, and cost for United States cellulosic biofuels.

Cellulosic ethanol can achieve estimated greenhouse gas (GHG) emission reductions greater than 80% relative to gasoline, largely as a result of the combustion of lignin for process heat and electricity in biorefineries. Most studies assume lignin is combusted onsite, but exporting lignin to be cofired at coal power plants has the potential to substantially reduce biorefinery capital costs. We assess the life-cycle GHG emissions, water use, and capital costs associated with four representative biorefinery test cases. Each case is evaluated in the context of a U.S. national scenario in which corn stover, wheat straw, and Miscanthus are converted to 1.4 EJ (60 billion liters) of ethanol annually. Life-cycle GHG emissions range from 4.7 to 61 g CO2e/MJ of ethanol (compared with ∼ 95 g CO2e/MJ of gasoline), depending on biorefinery configurations and marginal electricity sources. Exporting lignin can achieve GHG emission reductions comparable to onsite combustion in some cases, reduce life-cycle water consumption by up to 40%, and reduce combined heat and power-related capital costs by up to 63%. However, nearly 50% of current U.S. coal-fired power generating capacity is expected to be retired by 2050, which will limit the capacity for lignin cofiring and may double transportation distances between biorefineries and coal power plants.

Energy and human health.

Energy use is central to human society and provides many health benefits. But each source of energy entails some health risks. This article reviews the health impacts of each major source of energy, focusing on those with major implications for the burden of disease globally. The biggest health impacts accrue to the harvesting and burning of solid fuels, coal and biomass, mainly in the form of occupational health risks and household and general ambient air pollution. Lack of access to clean fuels and electricity in the world's poor households is a particularly serious risk for health. Although energy efficiency brings many benefits, it also entails some health risks, as do renewable energy systems, if not managed carefully. We do not review health impacts of climate change itself, which are due mostly to climate-altering pollutants from energy systems, but do discuss the potential for achieving near-term health cobenefits by reducing certain climate-related emissions.

Indoor residence times of semivolatile organic compounds: model estimation and field evaluation.

Indoor residence times of semivolatile organic compounds (SVOCs) are a major and mostly unavailable input for residential exposure assessment. We calculated residence times for a suite of SVOCs using a fugacity model applied to residential environments. Residence times depend on both the mass distribution of the compound between the "mobile phase" (air and dust particles settled on the carpet) and the "non-mobile phase" (carpet fibers and pad) and the removal rates resulting from air exchange and cleaning. We estimated dust removal rates from cleaning processes using an indoor-particle mass-balance model. Chemical properties determine both the mass distribution and relative importance of the two removal pathways, resulting in different residence times among compounds. We conducted a field study after chlorpyrifos was phased out for indoor use in the United States in 2001 to determine the decreases in chlorpyrifos air concentrations over a one-year period. A measured average decrease of 18% in chlorpyrifos air concentrations indicates the residence time of chlorpyrifos is expected to be 6.9 years and compares well with model predictions. The estimates from this study provide the opportunity to make more reliable estimates of SVOCs exposure in the indoor residential environment.

Achieving deep cuts in the carbon intensity of U.S. automobile transportation by 2050: complementary roles for electricity and biofuels.

Passenger cars in the United States (U.S.) rely primarily on petroleum-derived fuels and contribute the majority of U.S. transportation-related greenhouse gas (GHG) emissions. Electricity and biofuels are two promising alternatives for reducing both the carbon intensity of automotive transportation and U.S. reliance on imported oil. However, as standalone solutions, the biofuels option is limited by land availability and the electricity option is limited by market adoption rates and technical challenges. This paper explores potential GHG emissions reductions attainable in the United States through 2050 with a county-level scenario analysis that combines ambitious plug-in hybrid electric vehicle (PHEV) adoption rates with scale-up of cellulosic ethanol production. With PHEVs achieving a 58% share of the passenger car fleet by 2050, phasing out most corn ethanol and limiting cellulosic ethanol feedstocks to sustainably produced crop residues and dedicated crops, we project that the United States could supply the liquid fuels needed for the automobile fleet with an average blend of 80% ethanol (by volume) and 20% gasoline. If electricity for PHEV charging could be supplied by a combination of renewables and natural-gas combined-cycle power plants, the carbon intensity of automotive transport would be 79 g CO2e per vehicle-kilometer traveled, a 71% reduction relative to 2013.

Intake fraction for the indoor environment: a tool for prioritizing indoor chemical sources.

Reliable exposure-based chemical characterization tools are needed to evaluate and prioritize in a rapid and efficient manner the more than tens of thousands of chemicals in current use. This study applies intake fraction (iF), the integrated incremental intake of a chemical per unit of emission, for a suite of indoor released compounds. A fugacity-based indoor mass-balance model was used to simulate the fate and transport of chemicals for three release scenarios: direct emissions to room air and surface applications to carpet and vinyl. Exposure through inhalation, dermal uptake, and nondietary ingestion was estimated. To compute iF, cumulative intake was summed from all exposure pathways for 20 years based on a scenario with two adults and a 1-year-old child who ages through the simulation. Overall iFs vary by application modes: air release (3.1 × 10(-3) to 6.3 × 10(-3)), carpet application (3.8 × 10(-5) to 6.2 × 10(-3)), and vinyl application (9.0 × 10(-5) to 1.8 × 10(-2)). These iF values serve as initial estimates that offer important insights on variations among chemicals and the potential relative contribution of each pathway over a suite of compounds. The approach from this study is intended for exposure-based prioritization of chemicals released inside homes.

Fuel miles and the blend wall: costs and emissions from ethanol distribution in the United States.

From 1991 to 2009, U.S. production of ethanol increased 10-fold, largely due to government programs motivated by climate change, energy security, and economic development goals. As low-level ethanol-gasoline blends have not consistently outperformed ethanol-free gasoline in vehicle performance or tailpipe emissions, national-level economic and environmental goals could be accomplished more efficiently by concentrating consumption of gasoline containing 10% ethanol (i.e., E10) near producers to minimize freight activity. As the domestic transportation of ethanol increased 10-fold in metric ton-kilometers (t-km) from 2000 to 2009, the portion of t-km potentially justified by the E10 blend wall increased from less than 40% to 80%. However, we estimate 10 billion t-km took place annually from 2004 to 2009 for reasons other than the blend wall. This "unnecessary" transportation resulted in more than $240 million in freight costs, 90 million L of diesel consumption, 300,000 metric tons of CO(2)-e emissions, and 440 g of human intake of PM(2.5). By 2009, the marginal savings from enabling Iowa to surpass E10 would have exceeded 2.5 g CO(2)-e/MJ and $0.12/gallon of ethanol, as the next-closest customer was 1600 km away. The use of a national network model enables estimation of marginal transportation impacts from subnational policies, and benefits from policies encouraging concentrated consumption of renewable fuels.

Providing the missing link: the exposure science ontology ExO.

Environmental health information resources lack exposure data required to translate molecular insights, elucidate environmental contributions to diseases, and assess human health and ecological risks. We report development of an Exposure Ontology, ExO, designed to address this information gap by facilitating centralization and integration of exposure data. Major concepts were defined and the ontology drafted and evaluated by a working group of exposure scientists and other ontology and database experts. The resulting major concepts forming the basis for the ontology are "exposure stressor", "exposure receptor", "exposure event", and "exposure outcome". Although design of the first version of ExO focused on human exposure to chemicals, we anticipate expansion by the scientific community to address exposures of human and ecological receptors to the full suite of environmental stressors. Like other widely used ontologies, ExO is intended to link exposure science and diverse environmental health disciplines including toxicology, epidemiology, disease surveillance, and epigenetics.

Water footprint of U.S. transportation fuels.

In the modern global economy, water and energy are fundamentally connected. Water already plays a major role in electricity generation and, with biofuels and electricity poised to gain a significant share of the transportation fuel market, water will become significantly more important for transportation energy as well. This research provides insight into the potential changes in water use resulting from increased biofuel or electricity production for transportation energy, as well as the greenhouse gas and freshwater implications. It is shown that when characterizing the water impact of transportation energy, incorporating indirect water use and defensible allocation techniques have a major impact on the final results, with anywhere between an 82% increase and a 250% decrease in the water footprint if evaporative losses from hydroelectric power are excluded. The greenhouse gas impact results indicate that placing cellulosic biorefineries in areas where water must be supplied using alternative means, such as desalination, wastewater recycling, or importation can increase the fuel's total greenhouse gas footprint by up to 47%. The results also show that the production of ethanol and petroleum fuels burden already overpumped aquifers, whereas electricity production is far less dependent on groundwater.

Intake fraction for particulate matter: recommendations for life cycle impact assessment.

Particulate matter (PM) is a significant contributor to death and disease globally. This paper summarizes the work of an international expert group on the integration of human exposure to PM into life cycle impact assessment (LCIA), within the UNEP/SETAC Life Cycle Initiative. We review literature-derived intake fraction values (the fraction of emissions that are inhaled), based on emission release height and "archetypal" environment (indoor versus outdoor; urban, rural, or remote locations). Recommended intake fraction values are provided for primary PM(10-2.5) (coarse particles), primary PM(2.5) (fine particles), and secondary PM(2.5) from SO(2), NO(x), and NH(3). Intake fraction values vary by orders of magnitude among conditions considered. For outdoor primary PM(2.5), representative intake fraction values (units: milligrams inhaled per kilogram emitted) for urban, rural, and remote areas, respectively, are 44, 3.8, and 0.1 for ground-level emissions, versus 26, 2.6, and 0.1 for an emission-weighted stack height. For outdoor secondary PM, source location and source characteristics typically have only a minor influence on the magnitude of the intake fraction (exception: intake fraction values can be an order of magnitude lower for remote-location emission than for other locations). Outdoor secondary PM(2.5) intake fractions averaged over respective locations and stack heights are 0.89 (from SO(2)), 0.18 (NO(x)), and 1.7 (NH(3)). Estimated average intake fractions are greater for primary PM(10-2.5) than for primary PM(2.5) (21 versus 15), owing in part to differences in average emission height (lower, and therefore closer to people, for PM(10-2.5) than PM(2.5)). For indoor emissions, typical intake fraction values are ∼1000-7000. This paper aims to provide as complete and consistent an archetype framework as possible, given current understanding of each pollutant. Values presented here facilitate incorporating regional impacts into LCIA for human health damage from PM.