[Show abstract][Hide abstract] ABSTRACT: Cellulosic ethanol can achieve estimated greenhouse gas (GHG)
emissions reductions greater than 80% relative to gasoline, largely due to
the combustion of lignin for process heat and electricity in biorefineries.
Most studies assume lignin is combusted onsite, but exporting lignin to be
co-fired 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 US 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 to approximately 95 g CO2e/MJ of
gasoline), depending on biorefinery configurations and marginal electricity
sources. Exporting lignin can achieve GHG emissions 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 US coal-fired power generating capacity is
expected to be retired by 2050, which will limit the capacity for lignin
co-firing and may double transportation distances between biorefineries and
coal power plants.
[Show abstract][Hide abstract] ABSTRACT: Information about the distribution of chemical-production mass with respect to use and release is a major and unavailable input for calculating population-scale exposure estimates. Based on exposure models and biomonitoring data, this study evaluates the distribution of total production volumes (and environmental releases if applicable) for a suite of organic compounds. We used Bayesian approaches that take the total intake from our exposure models as the prior intake distribution and the intake inferred from measured biomarker concentrations in the NHANES survey as the basis for updating. By carrying out a generalized sensitivity analysis, we separated the input parameters for which the modeled range of the total intake is within a factor of 2 of the intake inferred from biomonitoring data and those that result in a range greater than a factor of 2 of the intake. This analysis allows us to find the most sensitive (or important) parameters and the likelihood of emission rates for various source emission categories. Pie charts of contribution from each exposure pathway indicate that chemical properties are a primary determinant of the relative contribution of each exposure pathway within a given class of compounds. For compounds with relatively high octanol-water partition coefficients (Kow) such as di-2-ethylhexyl phthalate (DEHP), pyrene, 2,2',4,4'-tetrabromodiphenyl ether (PBDE-47), and 2,2',4,4',5,5'-hexabromodiphenyl ether (PBDE-153), more than 80% of exposure derives from outdoor food ingestion and/or indoor dust ingestion. In contrast, for diethyl phthalate (DEP), di-iso-butyl phthalate (DiBP), di-n-butyl phthalate (DnBP), butylbenzyl phthalate (BBP), and naphthalene, all relatively volatile compounds, either inhalation (indoor and outdoor) or dermal uptake from direct consumer use is the dominant exposure pathway. The approach of this study provides insights on confronting data gaps to improve population-scale exposure estimates used for high-throughput chemical prioritization.
[Show abstract][Hide abstract] ABSTRACT: 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-ethyl hexyl) 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) (medians = 0.52, 0.21, and 0.10 μg/m3, respectively) were the dominant phthalates in indoor air. 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.v.
[Show abstract][Hide abstract] ABSTRACT: Infants and young children spend as much as 50h per week in child care and preschool. Although approximately 13 million children, or 65% of all U.S. children, spend some time each day in early childhood education (ECE) facilities, little information is available about environmental exposures in these environments. We measured flame retardants in air and dust collected from 40 California ECE facilities between May 2010 and May 2011. Low levels of six polybrominated diphenyl ether (PBDE) congeners and four non-PBDE flame retardants were present in air, including two constituents of Firemaster 550 and two tris phosphate compounds [tris (2-chloroethyl) phosphate (TCEP) and tris (1,3-dichloroisopropyl) phosphate (TDCIPP)]. Tris phosphate, Firemaster 550 and PBDE compounds were detected in 100% of the dust samples. BDE47, BDE99, and BDE209 comprised the majority of the PBDE mass measured in dust. The median concentrations of TCEP (319ngg(-1)) and TDCIPP (2265ngg(-1)) were similar to or higher than any PBDE congener. Levels of TCEP and TDCIPP in dust were significantly higher in facilities with napping equipment made out of foam (Mann-Whitney p-values<0.05). Child BDE99 dose estimates exceeded the RfD in one facility for children<3years old. In 51% of facilities, TDCIPP dose estimates for children<6years old exceeded age-specific "No Significant Risk Levels (NSRLs)" based on California Proposition 65 guidelines for carcinogens. Given the overriding interest in providing safe and healthy environments for young children, additional research is needed to identify strategies to reduce indoor sources of flame retardant chemicals.
[Show abstract][Hide abstract] ABSTRACT: Information about the distribution of chemical-production mass with respect to use and release is a major and unavailable input for calculating population-scale exposure estimates. Based on exposure models and biomonitoring data, this study evaluates the distribution of total production volumes (and environmental releases if applicable) for a suite of organic compounds. We used Bayesian approaches that take the total intake from our exposure models as the prior intake distribution and the intake inferred from measured biomarker concentrations in the NHANES survey as the basis for updating. By carrying out a generalized sensitivity analysis, we separated the input parameters for which the modeled range of the total intake is within a factor of 2 of the intake inferred from biomonitoring data and those that result in a range greater than a factor of 2 of the intake. This analysis allows us to find the most sensitive (or important) parameters and the likelihood of emission rates for various source emission categories. Pie charts of contribution from each exposure pathway indicate that chemical properties are a primary determinant of the relative contribution of each exposure pathway within a given class of compounds. For compounds with relatively high octanol–water partition coefficients (Kow) such as di-2-ethylhexyl phthalate (DEHP), pyrene, 2,2′,4,4′-tetrabromodiphenyl ether (PBDE-47), and 2,2′,4,4′,5,5′-hexabromodiphenyl ether (PBDE-153), more than 80% of exposure derives from outdoor food ingestion and/or indoor dust ingestion. In contrast, for diethyl phthalate (DEP), di-iso-butyl phthalate (DiBP), di-n-butyl phthalate (DnBP), butylbenzyl phthalate (BBP), and naphthalene, all relatively volatile compounds, either inhalation (indoor and outdoor) or dermal uptake from direct consumer use is the dominant exposure pathway. The approach of this study provides insights on confronting data gaps to improve population-scale exposure estimates used for high-throughput chemical prioritization.
[Show abstract][Hide abstract] ABSTRACT: The aim of this article is to help confront uncertainty in life cycle assessments (LCAs) used for decision support. LCAs offer a quantitative approach to assess environmental effects of products, technologies, and services and are conducted by an LCA practitioner or analyst (AN) to support the decision maker (DM) in making the best possible choice for the environment. At present, some DMs do not trust the LCA to be a reliable decision-support tool—often because DMs consider the uncertainty of an LCA to be too large. The standard evaluation of uncertainty in LCAs is an ex-post approach that can be described as a variance simulation based on individual data points used in an LCA. This article develops and proposes a taxonomy for LCAs based on extensive research in the LCA, management, and economic literature. This taxonomy can be used ex ante to support planning and communication between an AN and DM regarding which type of LCA study to employ for the decision context at hand. This taxonomy enables the derivation of an LCA classification matrix to clearly identify and communicate the type of a given LCA. By relating the LCA classification matrix to statistical principles, we can also rank the different types of LCA on an expected inherent uncertainty scale that can be used to confront and address potential uncertainty. However, this article does not attempt to offer a quantitative approach for assessing uncertainty in LCAs used for decision support.
Journal of Industrial Ecology 01/2014; · 2.28 Impact Factor
[Show abstract][Hide abstract] ABSTRACT: The work addresses current knowledge gaps regarding causes for correlations between environmental and biomarker measurements and explores the underappreciated role of variability in disaggregating exposure attributes that contribute to biomarker levels. Our simulation-based study considers variability in environmental and food measurements, the relative contribution of various exposure sources (indoors and food), and the biological half-life of a compound, on the resulting correlations between biomarker and environmental measurements. For two hypothetical compounds whose half-lives are on the order of days for one and years for the other, we generate synthetic daily environmental concentrations and food exposures with different day-to-day and population variability as well as different amounts of home- and food-based exposure. Assuming that the total intake results only from home-based exposure and food ingestion, we estimate time-dependent biomarker concentrations using a one-compartment pharmacokinetic model. Box plots of modeled R2 values indicate that although the R2 correlation between wipe and biological (e.g., serum) measurements is within the same range for the two compounds, the relative contribution of the home exposure to the total exposure could differ by up to 20%, thus providing the relative indication of their contribution to body burden. The novel method introduced in this paper provides insights for evaluating scenarios or experiments where sample, exposure, and compound variability must be weighed in order to interpret associations between exposure data.
PLoS ONE 01/2014; 9(3):e93678. · 3.73 Impact Factor
[Show abstract][Hide abstract] ABSTRACT: Consumer products and building materials emit a number of semivolatile organic compounds (SVOCs) in the indoor environment. Because indoor SVOCs accumulate in dust, we explore the use of dust to determine source strength and report here on analysis of dust samples collected in 30 U.S. homes for six phthalates, four personal care product ingredients, and five flame retardants. We then use a fugacity-based indoor mass-balance model to estimate the whole house emission rates of SVOCs that would account for the measured dust concentrations. Di-2-ethylhexyl phthalate (DEHP) and di-iso-nonyl phthalate (DiNP) were the most abundant compounds in these dust samples. On the other hand, the estimated emission rate of diethyl phthalate (DEP) is the largest among phthalates, although its dust concentration is over two orders of magnitude smaller than DEHP and DiNP. The magnitude of the estimated emission rate that corresponds to the measured dust concentration is found to be inversely correlated with the vapor pressure of the compound, indicating that dust concentrations alone cannot be used to determine which compounds have the greatest emission rates. The combined dust-assay modeling approach shows promise for estimating indoor emission rates for SVOCs. This article is protected by copyright. All rights reserved.
[Show abstract][Hide abstract] ABSTRACT: 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.
[Show abstract][Hide abstract] ABSTRACT: 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. Expected final online publication date for the Annual Review of Public Health Volume 34 is March 17, 2013. Please see http://www.annualreviews.org/catalog/pubdates.aspx for revised estimates.
Annual Review of Public Health 01/2013; · 3.27 Impact Factor
[Show abstract][Hide abstract] ABSTRACT: Exposure to environmental chemicals results from multiple sources, environmental media, and exposure routes. Ideally, modeled exposures should be compared to biomonitoring data. This study compares the magnitude and variation of modeled polycyclic aromatic hydrocarbons (PAHs) exposures resulting from emissions to outdoor and indoor air and estimated exposure inferred from biomarker levels. Outdoor emissions result in both inhalation and food-based exposures. We modeled PAH intake doses using U.S. EPA's 2002 National Air Toxics Assessment (NATA) county-level emissions data for outdoor inhalation, the CalTOX model for food ingestion (based on NATA emissions), and indoor air concentrations from field studies for indoor inhalation. We then compared the modeled intake with the measured urine levels of hydroxy-PAH metabolites from the 2001-2002 National Health and Nutrition Examination Survey (NHANES) survey as quantifiable human intake of PAH parent-compounds. Lognormal probability plots of modeled intakes and estimated intakes inferred from biomarkers suggest that a primary route of exposure to naphthalene, fluorene, and phenanthrene for the U.S. population is likely inhalation from indoor sources. For benzo(a)pyrene, the predominant exposure route is likely from food ingestion resulting from multi-pathway transport and bioaccumulation due to outdoor emissions. Multiple routes of exposure are important for pyrene. We also considered the sensitivity of the predicted exposure to the proportion of the total naphthalene production volume emitted to the indoor environment. The comparison of PAH biomarkers with exposure variability estimated from models and sample data for various exposure pathways supports that both indoor and outdoor models are needed to capture the sources and routes of exposure to environmental contaminants. (C) 2012 Elsevier Ltd. All rights reserved.
[Show abstract][Hide abstract] ABSTRACT: 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 between compounds. We conducted a field study after chlorpyrifos was phased out for indoor use in the U.S. 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.
[Show abstract][Hide abstract] ABSTRACT: Vehicular air pollutant emissions are characterized by a high degree of spatial variability that is correlated with the distribution of people. The consequences of the spatial association between emissions and exposed populations have not been fully captured in lifecycle and other impact assessments. The intake fraction (iF) quantifies aggregate air-pollutant exposures attributable to sources. Utilizing source–receptor (S–R) relationships derived from the US Environmental Protection Agency's AERMOD steady-state plume model, we quantify the intake fraction of conserved pollutants emitted from on-road mobile sources and report here the first characterization across approximately 65,000 census tracts of the conterminous United States. Considering exposures out to 50 km from the source, the population-weighted mean iF is 8.6 parts per million (ppm). The population-weighted median generally increases with geographic scale, from 3.6 ppm for census tracts to 4.2 ppm for counties, and 5.1 ppm for states, while the population-weighted interquartile range (IQR) progressively narrows as geographic scale increases: 0.85–8.8 ppm for census tracts, 1.5–8.5 ppm for counties, and 3.2–7.5 ppm for states. Across the four US Census regions, the population weighted median iF varies from 2.2 ppm (South) to 7.5 ppm (West), and the census-tract IQR spans an order of magnitude in each region (2.1–17 ppm in the West; 0.55–6.9 ppm in the Midwest; 0.45–5.5 ppm in the South; and 1.8–18 ppm in the Northeast). The population-weighted mean intake fraction for populous urban counties is about two orders of magnitude greater than for sparsely populated rural counties. On a population-weighted average basis and considering the 50 km analysis range, 75% of the intake occurs in the same county as emissions.