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ABSTRACTThe potential effects of 21st century climate change on ozone (O3) concentrations in the United States are investigated using global climate simulations to drive higher-resolution regional meteorological and chemical transport models. Community Earth System Model (CESM) and Coupled Model version 3 (CM3) simulations of the Representative Concentration Pathway 8.5 scenario are dynamically downscaled using the Weather Research and Forecasting model, and the resulting meteorological fields are used to drive the Community Multiscale Air Quality model. Air quality is modeled for five 11-year periods using both a 2011 air pollutant emission inventory and a future projection accounting for full implementation of promulgated regulatory controls. Across the U.S., CESM projects daily maximum temperatures during summer to increase 1–4°C by 2050 and 2–7°C by 2095, while CM3 projects warming of 2–7°C by 2050 and 4–11°C by 2095. The meteorological changes have geographically varying impacts on O3concentrations. Using the 2011 emissions dataset, O3increases 1–5 ppb in the central Great Plains and Midwest by 2050 and more than 10 ppb by 2095, but it remains unchanged or even decreases in the Gulf Coast, Maine, and parts of the Southwest. Using the projected emissions, modeled increases are attenuated while decreases are amplified, indicating that planned air pollution control measures ameliorate the ozone climate penalty. The relationships between changes in maximum temperature and changes in O3concentrations are examined spatially and quantified to explore the potential for developing an efficient approach for estimating air quality impacts of other future climate scenarios.Implications: The effects of climate change on ozone air quality in the United States are investigated using two global climate model simulations of a high warming scenario for five decadal periods in the 21st century. Warming summer temperatures simulated under both models lead to higher ozone concentrations in some regions, with the magnitude of the change increasing with temperature over the century. The magnitude and spatial extent of the increases are attenuated under a future emissions projection that accounts for regulatory controls. Regional linear regression relationships are developed as a first step toward development of a reduced form model for efficient estimation of the health impacts attributable to changes in air quality resulting from a climate change scenario.

Extreme heat exposure can lead to premature death. Climate change is expected to increase the frequency, intensity, and duration of extreme heat events, resulting in many additional heat-related deaths globally, as well as changing the nature of extreme cold events. At the same time, vulnerability to extreme heat has decreased over time, probably due to a combination of physiological, behavioural, infrastructural, and technological adaptations. We aimed to account for these changes in vulnerability and avoid overstated projections for temperature-related mortality. We used the historical observed decrease in vulnerability to improve future mortality estimates.

Increasing atmospheric concentrations of carbon dioxide (CO2) affect global nutrition via effects on agricultural productivity and nutrient content of food crops. We combined these effects with economic projections to estimate net changes in nutrient availability between 2010 and 2050.

The changing risk of extreme precipitation is difficult to project. Events are rare by definition, and return periods of heavy precipitation events are often calculated assuming a stationary climate. Furthermore, ensembles of climate model projections are not large enough to fully categorize the tails of the distribution. To address this, we cluster the contiguous United States into self‐similar hydroclimates to estimate changes in the expected frequency of extremely rare events under scenarios of global mean temperature change. We find that, although there is some regional variation, record events are projected in general to become more intense, with 500‐year events intensifying by 10–50% under 2 °C of warming and by 40–100% under 4 °C of warming. This analysis could provide information to inform regional prioritization of resources to improve the resilience of U.S. infrastructure. Spatial clustering can be used to create stable projections of extreme precipitation eventsAnalysis over the United States suggests 1,000‐year events will be up to 5 times more frequent under 2 degree C warmingDifferences in projections between regions are evident, with the U.S. East Coast and mountain regions showing large intensification

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Reduced complexity climate models are useful tools with practical policy applications, yet evaluation of their performance and application is nascent. We call for stakeholder-driven development and assessment to address user needs, including provision of open-source code and guidance to inform model selection and application.

A preliminary analysis has been conducted of the performance of a Chemical Looping system with Oxygen Uncoupling (CLOU) with copper oxide as the oxygen carrier and coal approximated by carbon as the fuel. The advantages of oxygen uncoupling are demonstrated by providing the energy balances, the circulation rate of oxygen carrier, the oxygen carrier mass loadings, the carbon burnout and oxygen partial pressure in the fuel reactor. Experimental data on the cycling of cuprous oxide to cupric oxide and kinetics for the oxidation and decomposition reactions of the oxides were obtained for use in the analysis. For this preliminary study unsupported oxides were utilized. The decomposition temperatures were rapid at the high temperature of 950°C selected for the fuel reactor. The oxidation kinetics peaked at about 800°C with the decrease in rate at higher temperatures, a decrease which is attributed in the literature to the temperature dependence of the diffusional resistance of the CuO layer surrounding the Cu2O; the diffusion occurs through grain boundaries in the CuO layers and the rate of diffusion decreases as a consequence of growth of CuO grains with increasing temperature. The analysis shows the advantages of CLOU in providing rapid combustion of the carbon with carbon burnout times lower than the decomposition times of the oxygen carrier. For the full potential of CLOU to be established additional data are needed on the kinetics of supported oxides at the high temperatures (>850°C) at which oxygen is released by the CuO in the fuel reactor.

Black carbon aerosol plays a unique and important role in Earth's climate system. Black carbon is a type of carbonaceous material with a unique combination of physical properties. This assessment provides an evaluation of black‐carbon climate forcing that is comprehensive in its inclusion of all known and relevant processes and that is quantitative in providing best estimates and uncertainties of the main forcing terms: direct solar absorption; influence on liquid, mixed phase, and ice clouds; and deposition on snow and ice. These effects are calculated with climate models, but when possible, they are evaluated with both microphysical measurements and field observations. Predominant sources are combustion related, namely, fossil fuels for transportation, solid fuels for industrial and residential uses, and open burning of biomass. Total global emissions of black carbon using bottom‐up inventory methods are 7500 Gg yr−1in the year 2000 with an uncertainty range of 2000 to 29000. However, global atmospheric absorption attributable to black carbon is too low in many models and should be increased by a factor of almost 3. After this scaling, the best estimate for the industrial‐era (1750 to 2005) direct radiative forcing of atmospheric black carbon is +0.71 W m−2with 90% uncertainty bounds of (+0.08, +1.27) W m−2. Total direct forcing by all black carbon sources, without subtracting the preindustrial background, is estimated as +0.88 (+0.17, +1.48) W m−2. Direct radiative forcing alone does not capture important rapid adjustment mechanisms. A framework is described and used for quantifying climate forcings, including rapid adjustments. The best estimate of industrial‐era climate forcing of black carbon through all forcing mechanisms, including clouds and cryosphere forcing, is +1.1 W m−2with 90% uncertainty bounds of +0.17 to +2.1 W m−2. Thus, there is a very high probability that black carbon emissions, independent of co‐emitted species, have a positive forcing and warm the climate. We estimate that black carbon, with a total climate forcing of +1.1 W m−2, is the second most important human emission in terms of its climate forcing in the present‐day atmosphere; only carbon dioxide is estimated to have a greater forcing. Sources that emit black carbon also emit other short‐lived species that may either cool or warm climate. Climate forcings from co‐emitted species are estimated and used in the framework described herein. When the principal effects of short‐lived co‐emissions, including cooling agents such as sulfur dioxide, are included in net forcing, energy‐related sources (fossil fuel and biofuel) have an industrial‐era climate forcing of +0.22 (−0.50 to +1.08) W m−2during the first year after emission. For a few of these sources, such as diesel engines and possibly residential biofuels, warming is strong enough that eliminating all short‐lived emissions from these sources would reduce net climate forcing (i.e., produce cooling). When open burning emissions, which emit high levels of organic matter, are included in the total, the best estimate of net industrial‐era climate forcing by all short‐lived species from black‐carbon‐rich sources becomes slightly negative (−0.06 W m−2with 90% uncertainty bounds of −1.45 to +1.29 W m−2). The uncertainties in net climate forcing from black‐carbon‐rich sources are substantial, largely due to lack of knowledge about cloud interactions with both black carbon and co‐emitted organic carbon. In prioritizing potential black‐carbon mitigation actions, non‐science factors, such as technical feasibility, costs, policy design, and implementation feasibility play important roles. The major sources of black carbon are presently in different stages with regard to the feasibility for near‐term mitigation. This assessment, by evaluating the large number and complexity of the associated physical and radiative processes in black‐carbon climate forcing, sets a baseline from which to improve future climate forcing estimates.

Climate change studies are often interdisciplinary by nature, incorporating many domains of science, economics, and political theory. Integrated assessment (IA) aims to bring diverse scientific, economics and social science expertise together to provide analysis and advice that comprehensively addresses all or at least many aspects of the climate change issue. IA methods have been applied to many areas of climate change providing insights into areas such as optimal timing of emission reductions, weighting of different greenhouse gases, or impacts of biofuel policies. Additionally, IAs have identified key uncertainties that should be priorities of future research, such as the need to understand oceanic heat uptake in order to better constrain climate sensitivity and predict future timing of temperature change. These assessments have also served to establish ongoing communication within the community of researchers, and between researchers and policy makers. In complex scientific issues it is often difficult for policy makers and the public to sort out conflicting scientific views, and an authoritative assessment process can provide consensus views on the issue, accepting that in some cases the “consensus” may be that some aspects of the issue remain unresolved. This review explores the history and applications of these IAs, and identifies avenues for future emphasis. We briefly review the whole field of IAs of climate change, but focus on the role of formal computational frameworks in IA models. WIREs Clim Change2011 2 27–44 DOI: 10.1002/wcc.93

First steps toward a broad climate agreement, such as the Kyoto Protocol, have focused on less than global geographic coverage. We consider instead a policy that is less comprehensive in term of greenhouse gases (GHGs), including only the non-CO2 GHGs, but is geographically comprehensive. Abating non-CO2 GHGs may be seen as less of a threat to economic development and therefore it may be possible to involve developing countries in such a policy even though they have resisted limits on CO2 emissions. The policy we consider involves a GHG price of about $15 per ton carbon-equivalent (tce) levied only on the non-CO2 GHGs and held at that level through the century. We estimate that such a policy would reduce the global mean surface temperature in 2100 by about 0.55° C; if only methane is covered that alone would achieve a reduction of 0.3° to 0.4° C. We estimate the Kyoto Protocol in its current form would achieve a 0.25° C reduction in 2100 if Parties to it maintained it as is through the century. Furthermore, we estimate the costs of the non-CO2 policies to be a small fraction of the Kyoto policy. Whether as a next step to expand the Kyoto Protocol, or as a separate initiative running parallel to it, the world could well make substantial progress on limiting climate change by pursuing an agreement to abate the low cost non-CO2 GHGs. The results suggest that it would be useful to proceed on global abatement of non-CO2 GHGs so that lack of progress on negotiations to limit CO2 does not allow these abatement opportunities to slip away.

AbstractParticulate-phase exhaust properties from two different types of ground-based jet aircraft engines—high-thrust and turboshaft—were studied with real-time instruments on a portable pallet and additional time-integrated sampling devices. The real-time instruments successfully characterized rapidly changing particulate mass, light absorption, and polycyclic aromatic hydrocarbon (PAH) content. The integrated measurements included particulate-size distributions, PAH, and carbon concentrations for an entire test run (i.e., “run-integrated” measurements). In all cases, the particle-size distributions showed single modes peaking at 20–40nm diameter. Measurements of exhaust from high-thrust F404 engines showed relatively low-light absorption compared with exhaust from a turboshaft engine. Particulate-phase PAH measurements generally varied in phase with both net particulate mass and with light-absorbing particulate concentrations. Unexplained response behavior sometimes occurred with the real-time PAH analyzer, although on average the real-time and integrated PAH methods agreed within the same order of magnitude found in earlier investigations.

AbstractOver the past several years, numerous studies have linked ambient concentrations of particulate matter (PM) to adverse health effects, and more recent studies have identified PM size and surface area as important factors in determining the health effects of PM. This study contributes to a better understanding of the evolution of particle size distributions in exhaust plumes with unconfined dilution by ambient air. It combines computational fluid dynamics (CFD) with an aerosol dynamics model to examine the effects of different streamlines in an exhaust plume, ambient particle size distributions, and vehicle and wind speed on the particle size distribution in an exhaust plume. CFD was used to calculate the flow field and gas mixing for unconfined dilution of a vehicle exhaust plume, and the calculated dilution ratios were then used as input to the aerosol dynamics simulation. The results of the study show that vehicle speed affected the particle size distribution of an exhaust plume because increasing vehicle speed caused more rapid dilution and inhibited coagulation. Ambient particle size distributions had an effect on the smaller sized particles (∼10 nm range under some conditions) and larger sized particles (>2 μm) of the particle size distribution. The ambient air particle size distribution affects the larger sizes of the exhaust plume because vehicle exhaust typically contains few particles larger than 2 μm. Finally, the location of a streamline in the exhaust plume had little effect on the particle size distribution; the particle size distribution along any streamline at a distance xdiffered by less than 5% from the particle size distributions along any other streamline at distance x.

AbstractIn-service diesel engines are a significant source of particulate matter (PM) emissions, and they have been subjected to increasingly strict emissions standards. Consequently, the wide-scale use of some type of particulate filter is expected. This study evaluated the effect of an Engelhard catalyzed soot filter (CSF) and a Rypos electrically heated soot filter on the emissions from in-service diesel engines in terms of PM mass, black carbon concentration, particle-bound polycyclic aromatic hydrocarbon concentration, and size distribution. Both filters capture PM. The CSF relies on the engine's exhaust to reach the catalyst regeneration temperature and oxidize soot, whereas the electrically heated filter contains a heating element to oxidize soot. The filters were installed on several military diesel engines. Particle concentrations and compositions were measured before and after installation of the filter and again after several months of operation. Generally, the CSF removed at least 90% of total PM, and the removal efficiency improved or remained constant after several months of operation. In contrast, the electrical filters removed 44-69% of PM mass. In addition to evaluating the soot filters, the sampling team also compared the results of several real-time particle measurement instruments to traditional filter measurements of total mass.

AbstractDiluted exhaust from selected military aircraft ground-support equipment (AGE) was analyzed for particulate mass, elemental carbon (EC) and organic carbon (OC), SO42−, and size distributions. The experiments occurred at idle and load conditions and utilized a chassis dynamometer. The selected AGE vehicles operated on gasoline, diesel, and JP-8. These military vehicles exhibited concentrations, size distributions, and emission factors in the same range as those reported for nonmilitary vehicles. The diesel and JP-8 emission rates for PM ranged from 0.092 to 1.1 g/kg fuel. The EC contributed less and the OC contributed more to the particulate mass than reported in recent studies of vehicle emissions. Overall, the particle size distribution varied significantly with engine condition, with the number of accumulation mode particles and the count median diameter (CMD) increasing as engine load increased. The SO42−analyses showed that the distribution of SO42−mass mirrored the distribution of particle mass.

Aromatics growth beyond 2-, 3-ring PAH is analyzed through a radical-molecule reaction mechanism which, in combination with a previously developed PAH model, is able to predict the size distribution of aromatic structures formed in rich premixed flames of ethylene at atmospheric pressure with C/O ratios across the soot threshold limit. Modeling results are in good agreement with experimental data and are used to interpret the ultraviolet absorption and the light scattering measured in flames before soot inception. The model shows that the total number concentration of high molecular mass aromatics and the different moments of the size distribution are functions of both the PAH and H-atom concentrations, two quantities which have different trends as functions of the residence time and the C/O ratio. Regimes of nearly stoichiometric or slightly rich premixed combustion are dominated by reactions between aromatics which lead to the formation of particles with sizes of the order of 3 to 4 nm. At higher C/O ratios the formation of nanoparticles is less efficient. Particles with sizes of the order of 2 nm are predicted in flames at the threshold of soot formation, whereas particles with sizes around 1 to 1.5 nm are predicted in fully sooting conditions.

ABSTRACTFor a recent exploratory study of particulate matter (PM) compositions, origins, and impacts in the El Paso/Juarez (Paso del Norte) airshed, the authors relied on solvent extraction (SX)-gas chromatography/mass spectrometry (GC/MS) procedures to characterize 24-hr quartz fiber (QF) filter samples obtained from nine spatially distributed high-volume (Hi-Vol) PM10samplers as well as on thermal de-sorption (TD)-GC/MS methods to characterize 45 time-resolved (2-hr) filter samples obtained with modified 1-m3/hr PM10samplers. Principal component analysis and related chemometric techniques were used for data reduction and data fusion as well as for multiway data correlation.A high degree of correspondence (R2= 0.821) was found between the rapid TD-GC/MS method (which can be carried out on 2-hr filter slices containing only micro-gram amounts of sample) and conventional SX-GC/MS procedures. The four main source patterns of organic PM components observed in GC/MS profiles of both temporally and spatially resolved receptor samples obtained in the El Paso/Juarez border airshed during the study period are interpreted to represent (1) vehicular emissions plus resuspended urban dust; (2) biomass combustion; (3) native vegetation detritus and resuspended agricultural dust; and (4) waste burning. Moreover, principal component analysis of combined, variance-weighted, temporally resolved TD-GC/MS data and spatially resolved SX-GC/MS data was used to determine approximate source locations for specific PM components identified in time-resolved receptor sample profiles. The same approach can be used to determine approximate circadian concentration profiles of specific PM components identified in spatially resolved receptor sample profiles.