JP

In this thesis, I study polycyclic aromatic hydrocarbons (PAHs) and perfluorocarboxylic acids (PFCAs). PAHs are by-products of burning and therefore have important anthropogenic sources in the combustion of fuels, biomass, etc. PFCAs and their atmospheric precursors are used in making firefighting foams, non-stick coatings, and other surfactant applications.

I quantitatively examine the relative importance of uncertainty in emissions and physicochemical properties (including reaction rate constants) to Northern Hemisphere (NH) and Arctic PAH concentrations. NH average concentrations are more sensitive to uncertainty in the atmospheric lifetime than to emissions rate. The largest uncertainty reductions would come from precise experimental determination of PHE, PYR and BaP rate constants for the reaction with OH.

I calculate long-chain PFCA formation theoretical maximum yields for the degradation of precursor species at a representative sample of atmospheric conditions from a three dimensional chemical transport model, finding that atmospheric conditions farther from pollution sources have both higher capacities to form long chain PFCAs and higher uncertainties in those capacities.

I present results from newly developed simulations of atmospheric PFCA formation and fate using the chemical transport model GEOS-Chem, simulating the degradation of fluorotelomer precursors, as well as deposition and transport of the precursors, intermediates and end-products of the PFCA formation chemistry. I compare the model results to remote deposition measurements and find that it reproduces Arctic deposition of PFOA effectively. Given the most recent precursor emission inventory, the atmospheric indirect source of PFOA and PFNA is 10-45 t/yr globally and 0.2-0.7 t/yr to the Arctic.

The climate response of precipitation to the effects of anthropogenic aerosols is a critical while not yet fully understood aspect in climate science. Results of selected models that participated the Coupled Model Intercomparison Project Phase 5 and the data from the Twentieth Century Reanalysis Project suggest that, throughout the tropics and also in the extratropical Northern Hemisphere, aerosols have largely dominated the distribution of precipitation changes in reference to the preindustrial era in the second half of the last century. Aerosol-induced cooling has offset some of the warming caused by the greenhouse gases from the tropics to the Arctic and thus formed the gradients of surface temperature anomaly that enable the revealed precipitation change patterns to occur. Improved representation of aerosol-cloud interaction has been demonstrated as the key factor for models to reproduce consistent distributions of past precipitation change with the reanalysis data.

© 2015 the author

In response to the Renewable Fuel Standard, the U.S. transportation sector now consumes a substantial amount (13.3 billion gallons in 2010) of ethanol. A key motivation for these mandates is to expand the consumption of biofuels in road transportation to both reduce foreign oil dependency and to reduce greenhouse gas (GHG) emissions from the consumption of fossil fuels in transportation. In this paper, we present the impacts of several biofuels expansion scenarios for the U.S. in which scaled increases in the U.S. corn ethanol mandates are modeled to explore the scalability of GHG impacts. The impacts show both expected and surprising results. As expected, the area of land used to grow biofuel crops increases with the size of the policy in the U.S., and some land-use changes occur abroad due to trade in agricultural commodities. Because the land-use changes happen largely in the U.S., there is an increase in U.S. land-use emissions when natural lands are converted to agricultural use in the policy scenarios. Further, the emissions impacts in the U.S. and the rest of the world in these scenarios, including land-use emissions, scale in direct proportion to the size of the U.S. corn ethanol mandates. On the other hand, the land-use emissions that occur in the rest of the world are disproportionately larger per hectare of change due to conversions of more carbon-rich forests to cultivate crops and feed livestock.

This study quantifies the impact of typhoons on rice production in the Philippines. To this end, satellite-derived reflectance data are used to detect the location of rice fields at 500-m resolution. Utilizing typhoon-track data within a wind field model and satellite-derived precipitation measures, fragility curves are then employed to proxy the damage of storms on rice production within each rice field. The results from a panel spatial regression model show that typhoons substantially reduced local provincial production in the quarter of the strike, having caused losses of up to 12.5 million tons since 2001. Using extreme value theory to predict future losses, the results suggest that a typhoon like the recent Haiyan, which is estimated to have caused losses of around 260 000 tons, has a return period of 13 years. This methodology can provide a relatively timely tool for rice damage assessments after tropical cyclones in the region.

© American Meteorological Society 2016

We report ground-based atmospheric measurements and emission estimates for the halons H-1211 (CBrClF2), H-1301 (CBrF3), and H-2402 (CBrF2CBrF2) from the AGAGE (Advanced Global Atmospheric Gases Experiment) and the National Oceanic and Atmospheric Administration global networks. We also include results from archived air samples in canisters and from polar firn in both hemispheres, thereby deriving an atmospheric record of nearly nine decades (1930s to present). All three halons were absent from the atmosphere until ∼1970, when their atmospheric burdens started to increase rapidly. In recent years H-1211 and H-2402 mole fractions have been declining, but H-1301 has continued to grow. High-frequency observations show continuing emissions of H-1211 and H-1301 near most AGAGE sites. For H-2402 the only emissions detected were derived from the region surrounding the Sea of Japan/East Sea. Based on our observations, we derive global emissions using two different inversion approaches. Emissions for H-1211 declined from a peak of 11 kt yr−1 (late 1990s) to 3.9 kt yr−1 at the end of our record (mean of 2013–2015), for H-1301 from 5.4 kt yr−1 (late 1980s) to 1.6 kt yr−1, and for H-2402 from 1.8 kt yr−1 (late 1980s) to 0.38 kt yr−1. Yearly summed halon emissions have decreased substantially; nevertheless, since 2000 they have accounted for ∼30% of the emissions of all major anthropogenic ozone depletion substances, when weighted by ozone depletion potentials.

This paper provides an overview of the base-year assumptions and baseline projections for the set of models participating in the LAMP and CLIMACAP projects. We present the range in baseline projections for Latin America, and identify key differences between model projections including how these projections compare to historic trends. We find relatively large differences across models in base year assumptions related to population, GDP, energy and CO2 emissions due to the use of different data sources, but also conclude that this does not influence the range of projections. We find that population and GDP projections across models span a broad range, comparable to the range represented by the set of Shared Socioeconomic Pathways (SSPs). Kaya-factor decomposition indicates that the set of baseline scenarios mirrors trends experienced over the past decades. Emissions in Latin America are projected to rise as a result of GDP and population growth and a minor shift in the energy mix toward fossil fuels. Most scenarios assume a somewhat higher GDP growth than historically observed and continued decline of population growth. Minor changes in energy intensity or energy mix are projected over the next few decades.

© 2016 Elsevier

The collective behavior of wind farms in seven Independent System Operator (ISO) areas has been studied. The generation duration curves for each ISO show that there is no aggregated power for some fraction of time. Aggregation of wind turbines mitigates intermittency to some extent, but in each ISO there is considerable fraction of time when there is less than 5% capacity. The hourly wind power time series show benefit of aggregation but the high and low wind events are lumped in time, thus indicating that intermittency is synchronized in each region. The timeseries show that there are instances when there is no wind power in most ISOs because of large-scale high pressure systems. An analytical consideration of the collective behavior of aggregated wind turbines shows that the benefit of aggregation saturates beyond a certain number of generating units asymptotically. Also, the benefit of aggregation falls rapidly with temporal correlation between the generating units.

Climate change impacts on water resources in the United States are likely to be far-reaching and substantial because the water is integral to climate, and the water sector spans many parts of the economy. This paper estimates impacts and damages from five water resource-related models addressing runoff, drought risk, economics of water supply/demand, water stress, and flooding damages. The models differ in the water system assessed, spatial scale, and unit of assessment, but together provide a quantitative and descriptive richness in characterizing water sector effects that no single model can capture. The results, driven by a consistent set of greenhouse gas (GHG) emission and climate scenarios, examine uncertainty from emissions, climate sensitivity, and climate model selection. While calculating the net impact of climate change on the water sector as a whole may be impractical, broad conclusions can be drawn regarding patterns of change and benefits of GHG mitigation. Four key findings emerge: 1) GHG mitigation substantially reduces hydro-climatic impacts on the water sector; 2) GHG mitigation provides substantial national economic benefits in water resources related sectors; 3) the models show a strong signal of wetting for the Eastern US and a strong signal of drying in the Southwest; and 4) unmanaged hydrologic systems impacts show strong correlation with the change in magnitude and direction of precipitation and temperature from climate models, but managed water resource systems and regional economic systems show lower correlation with changes in climate variables due to non-linearities created by water infrastructure and the socio-economic changes in non-climate driven water demand.

Mercury pollution poses risks for both human and ecosystem health. As a consequence, controlling mercury pollution has become a policy goal on both global and national scales. We developed an assessment method linking global-scale atmospheric chemical transport modeling to regional-scale economic modeling to consistently evaluate the potential benefits to the United States of global (UN Minamata Convention on Mercury) and domestic [Mercury and Air Toxics Standards (MATS)] policies, framed as economic gains from avoiding mercury-related adverse health endpoints. This method attempts to trace the policies-to-impacts path while taking into account uncertainties and knowledge gaps with policy-appropriate bounding assumptions. We project that cumulative lifetime benefits from the Minamata Convention for individuals affected by 2050 are $339 billion (2005 USD), with a range from $1.4 billion to $575 billion in our sensitivity scenarios. Cumulative economy-wide benefits to the United States, realized by 2050, are $104 billion, with a range from $6 million to $171 billion. Projected Minamata benefits are more than twice those projected from the domestic policy. This relative benefit is robust to several uncertainties and variabilities, with the ratio of benefits (Minamata/MATS) ranging from ≈1.4 to 3. However, we find that for those consuming locally caught freshwater fish from the United States, rather than marine and estuarine fish from the global market, benefits are larger from US than global action, suggesting domestic policies are important for protecting these populations. Per megagram of prevented emissions, our domestic policy scenario results in US benefits about an order of magnitude higher than from our global scenario, further highlighting the importance of domestic action.

© 2015 the authors

Rivers discharge 28 ± 13 Mmol yr−1 of mercury (Hg) to ocean margins, an amount comparable to atmospheric deposition to the global oceans. Most of the Hg discharged by rivers is sequestered by burial of benthic sediment in estuaries or the coastal zone, but some is evaded to the atmosphere and some is exported to the open ocean. We investigate the fate of riverine Hg by developing a new global 3-D simulation for Hg in the Massachusetts Institute of Technology ocean general circulation model. The model includes plankton dynamics and carbon respiration (DARWIN project model) coupled to inorganic Hg chemistry. Results are consistent with observed spatial patterns and magnitudes of surface ocean Hg concentrations. We use observational constraints on seawater Hg concentrations and evasion to infer that most Hg from rivers is sorbed to refractory organic carbon and preferentially buried. Only 6% of Hg discharged by rivers (1.8 Mmol yr−1) is transported to the open ocean on a global basis. This fraction varies from a low of 2.6% in East Asia due to the barrier imposed by the Korean Peninsula and Japanese archipelago, up to 25% in eastern North America facilitated by the Gulf Stream. In the Arctic Ocean, low tributary particle loads and efficient degradation of particulate organic carbon by deltaic microbial communities favor a more labile riverine Hg pool. Evasion of Hg to the Arctic atmosphere is indirectly enhanced by heat transport during spring freshet that accelerates sea ice melt and ice rafting. Discharges of 0.23 Mmol Hg yr−1 from Arctic rivers can explain the observed summer maximum in the Arctic atmosphere, and this magnitude of releases is consistent with recent observations. Our work indicates that rivers are major contributors to Hg loads in the Arctic Ocean.

© 2015 American Chemical Society

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