Effects of 2000–2050 Changes in Climate and Emissions on Global Tropospheric Ozone and the Policy-Relevant Background Surface Ozone in the United States

We use a global chemical transport model (GEOS-Chem) driven by a general circulation model (NASA Goddard Institute for Space Studies GCM) to investigate the effects of 2000–2050 global change in climate and emissions (the Intergovernmental Panel on Climate Change A1B scenario) on the global tropospheric ozone budget and on the policy-relevant background (PRB) ozone in the United States. The PRB ozone, defined as the ozone that would be present in U.S. surface air in the absence of North American anthropogenic emissions, has important implications for setting national air quality standards. We examine separately and then together the effects of changes in climate and anthropogenic emissions of ozone precursors. We find that the 2000–2050 change in global anthropogenic emissions of ozone precursors increases the global tropospheric ozone burden by 17%. The 2000–2050 climate change increases the tropospheric ozone burden by 1.6%, due mostly to lightning in the upper troposphere, and also increases global tropospheric OH by 12%. In the lower troposphere, by contrast, climate change generally decreases the background ozone. The 2000–2050 increase in global anthropogenic emissions of ozone precursors increases PRB ozone by 2–6 ppb in summer; the maximum effect is found in April (3–7 ppb). The summertime PRB ozone decreases by up to 2 ppb with 2000–2050 climate change, except over the Great Plains, where it increases slightly as a result of increasing soil NOx emission. Climate change cancels out the effect of rising global anthropogenic emissions on the summertime PRB ozone in the eastern United States, but there is still a 2–5 ppb increase in the west.Earth and Planetary SciencesEngineering and Applied Science

Radiative Forcing Due to Major Aerosol Emitting Sectors in China and India

Understanding the radiative forcing caused by anthropogenic aerosol sources is essential for making effective emission control decisions to mitigate climate change. We examined the net direct plus indirect radiative forcing caused by carbonaceous aerosol and sulfur emissions in key sectors of China and India using the GISS-E2 chemistry-climate model. Diesel trucks and buses (67 mW/ sq. m) and residential biofuel combustion (52 mW/ sq. m) in India have the largest global mean, annual average forcings due mainly to the direct and indirect effects of BC. Emissions from these two sectors in China have near-zero net global forcings. Coal-fired power plants in both countries exert a negative forcing of about -30 mW/ sq. m from production of sulfate. Aerosol forcings are largest locally, with direct forcings due to residential biofuel combustion of 580 mW/ sq. m over India and 416 mW/ sq. m over China, but they extend as far as North America, Europe, and the Arcti

Legacy Impacts of All-Time Anthropogenic Emissions on the Global Mercury Cycle

Elevated mercury (Hg) in marine and terrestrial ecosystems is a global health concern because of the formation of toxic methylmercury. Humans have emitted Hg to the atmosphere for millennia, and this Hg has deposited and accumulated into ecosystems globally. Here we present a global biogeochemical model with fully coupled atmospheric, terrestrial, and oceanic Hg reservoirs to better understand human influence on Hg cycling and timescales for responses. We drive the model with a historical inventory of anthropogenic emissions from 2000 BC to present. Results show that anthropogenic perturbations introduced to surface reservoirs (atmosphere, ocean, or terrestrial) accumulate and persist in the subsurface ocean for decades to centuries. The simulated present-day atmosphere is enriched by a factor of 2.6 relative to 1840 levels, consistent with sediment archives, and by a factor of 7.5 relative to natural levels (2000 BC). Legacy anthropogenic Hg re-emitted from surface reservoirs accounts for 60% of present-day atmospheric deposition, compared to 27% from primary anthropogenic emissions, and 13% from natural sources. We find that only 17% of the present-day Hg in the surface ocean is natural and that half of its anthropogenic enrichment originates from pre-1950 emissions. Although Asia is presently the dominant contributor to primary anthropogenic emissions, only 17% of the surface ocean reservoir is of Asian anthropogenic origin, as compared to 30% of North American and European origin. The accumulated burden of legacy anthropogenic Hg means that future deposition will increase even if primary anthropogenic emissions are held constant. Aggressive global Hg emission reductions will be necessary just to maintain oceanic Hg concentrations at present levels.Engineering and Applied Science

The effect on photochemical smog of converting the U.S. fleet of gasoline vehicles to modern diesel vehicles

With the increased use of particle traps and nitrogen oxide (NO_x) control devices to reduce air pollution, “modern” diesel vehicles are being encouraged over gasoline vehicles globally as a central method of slowing global warming. Data to date, though, suggest that the NO_2:NO ratio from modern diesel may exceed that of gasoline, and it is difficult to reduce diesel NO_x below gasoline NO_x without increasing particle emissions. Here, it is calculated that, unless the diesel NO_2:NO ratio and total NO_x are reduced to those of gasoline, modern diesel, which should have lower hydrocarbon (HC) and carbon monoxide (CO) emissions than gasoline, may still enhance photochemical smog at the surface and aloft, on average, over the U.S. relative to gasoline. The reason is that vehicle-produced smog in the U.S. depends more on NO_x and the NO_2:NO ratio than on HCs or CO. It is also found that vehicle NO_x controls may be more effective than NO_2:NO ratio controls at reducing ozone

Effects of 2000-2050 Global Change on Ozone Air Quality in the United States

We investigate the effects on U.S. ozone air quality from 2000–2050 global changes in climate and anthropogenic emissions of ozone precursors by using a global chemical transport model (GEOS-Chem) driven by meteorological fields from the NASA Goddard Institute for Space Studies general circulation model (NASA/GISS GCM). We follow the Intergovernmental Panel on Climate Change A1B scenario and separate the effects from changes in climate and anthropogenic emissions through sensitivity simulations. The 2000–2050 changes in anthropogenic emissions reduce the U.S. summer daily maximum 8-hour ozone by 2–15 ppb, but climate change causes a 2–5 ppb positive offset over the Midwest and northeastern United States, partly driven by decreased ventilation from convection and frontal passages. Ozone pollution episodes are far more affected by climate change than mean values, with effects exceeding 10 ppb in the Midwest and northeast. We find that ozone air quality in the southeast is insensitive to climate change, reflecting compensating effects from changes in isoprene emission and air pollution meteorology. We define a “climate change penalty” as the additional emission controls necessary to meet a given ozone air quality target. We find that a 50% reduction in U.S. NOx emissions is needed in the 2050 climate to reach the same target in the Midwest as a 40% reduction in the 2000 climate. Emission controls reduce the magnitude of this climate change penalty and can even turn it into a climate benefit in some regions.Earth and Planetary SciencesEngineering and Applied Science

Comparison of Adjoint and Analytical Bayesian Inversion Methods for Constraining Asian Sources of Carbon Monoxide Using Satellite (MOPITT) Measurements of CO Columns

We apply the adjoint of an atmospheric chemical transport model (GEOS-Chem CTM) to constrain Asian sources of carbon monoxide (CO) with 2° × 2.5° spatial resolution using Measurement of Pollution in the Troposphere (MOPITT) satellite observations of CO columns in February–April 2001. Results are compared to the more common analytical method for solving the same Bayesian inverse problem and applied to the same data set. The analytical method is more exact but because of computational limitations it can only constrain emissions over coarse regions. We find that the correction factors to the a priori CO emission inventory from the adjoint inversion are generally consistent with those of the analytical inversion when averaged over the large regions of the latter. The adjoint solution reveals fine-scale variability (cities, political boundaries) that the analytical inversion cannot resolve, for example, in the Indian subcontinent or between Korea and Japan, and some of that variability is of opposite sign which points to large aggregation errors in the analytical solution. Upward correction factors to Chinese emissions from the prior inventory are largest in central and eastern China, consistent with a recent bottom-up revision of that inventory, although the revised inventory also sees the need for upward corrections in southern China where the adjoint and analytical inversions call for downward correction. Correction factors for biomass burning emissions derived from the adjoint and analytical inversions are consistent with a recent bottom-up inventory on the basis of MODIS satellite fire data.Engineering and Applied Science

Estimates of Power Plant NOx Emissions and Lifetimes from OMI NO2 Satellite Retrievals

Isolated power plants with well characterized emissions serve as an ideal test case of methods to estimate emissions using satellite data. In this study we evaluate the Exponentially-Modified Gaussian (EMG) method and the box model method based on mass balance for estimating known NOx emissions from satellite retrievals made by the Ozone Monitoring Instrument (OMI). We consider 29 power plants in the USA which have large NOx plumes that do not overlap with other sources and which have emissions data from the Continuous Emission Monitoring System (CEMS). This enables us to identify constraints required by the methods, such as which wind data to use and how to calculate background values. We found that the lifetimes estimated by the methods are too short to be representative of the chemical lifetime. Instead, we introduce a separate lifetime parameter to account for the discrepancy between estimates using real data and those that theory would predict. In terms of emissions, the EMG method required averages from multiple years to give accurate results, whereas the box model method gave accurate results for individual ozone seasons

Linking ozone pollution and climate change: The case for controlling methane

Methane (CH4) emission controls are found to be a powerful lever for reducing both global warming and air pollution via decreases in background tropospheric ozone (O3). Reducing anthropogenic CH4 emissions by 50% nearly halves the incidence of U.S. high-O3 events and lowers global radiative forcing by 0.37 W m−2 (0.30 W m−2 from CH4, 0.07 W m−2 from O3) in a 3-D model of tropospheric chemistry. A 2030 simulation based upon IPCC A1 emissions projections shows a longer and more intense U.S. O3 pollution season despite domestic emission reductions, indicating that intercontinental transport and a rising O3 background should be considered when setting air quality goals

Surface Ozone Background in the United States: Canadian and Mexican Pollution Influences

We use a global chemical transport model (GEOS-Chem) with 1° × 1° horizontal resolution to quantify the effects of anthropogenic emissions from Canada, Mexico, and outside North America on daily maximum 8-hour average ozone concentrations in US surface air. Simulations for summer 2001 indicate mean North American and US background concentrations of 26 ± 8 ppb and 30 ± 8 ppb, as obtained by eliminating anthropogenic emissions in North America vs. in the US only. The US background never exceeds 60 ppb in the model. The Canadian and Mexican pollution enhancement averages 3 ± 4 ppb in the US in summer but can be occasionally much higher in downwind regions of the northeast and southwest, peaking at 33 ppb in upstate New York (on a day with 75 ppb total ozone) and 18 ppb in southern California (on a day with 68 ppb total ozone). The model is successful in reproducing the observed variability of ozone in these regions, including the occurrence and magnitude of high-ozone episodes influenced by transboundary pollution. We find that exceedances of the 75 ppb US air quality standard in eastern Michigan, western New York, New Jersey, and southern California are often associated with Canadian and Mexican pollution enhancements in excess of 10 ppb. Sensitivity simulations with 2020 emission projections suggest that Canadian pollution influence in the Northeast US will become comparable in magnitude to that from domestic power plants.Engineering and Applied Science