Denise L. Mauzerall

Origin of ozone and NOx in the tropical troposphere: A photochemical analysis of aircraft observations over the South Atlantic basin

The photochemistry of the troposphere over the South Atlantic basin is examined by modeling of aircraft observations up to 12-km altitude taken during the TRACE A expedition in September–October 1992. A close balance is found in the 0 to 12-km column between photochemical production and loss of O3, with net production at high altitudes compensating for weak net loss at low altitudes. This balance implies that O3 concentrations in the 0–12 km column can be explained solely by in situ photochemistry; influx from the stratosphere is negligible. Simulation of H2O2, CH3OOH, and CH2O concentrations measured aboard the aircraft lends confidence in the computations of O3 production and loss rates, although there appears to be a major gap in current understanding of CH2O chemistry in the marine boundary layer. The primary sources of NOx over the South Atlantic Basin appear to be continental (biomass burning, lightning, soils). There is evidence that NOx throughout the 0 to 12-km column is recycled from its oxidation products rather than directly transported from its primary sources. There is also evidence for rapid conversion of HNO3 to NOx in the upper troposphere by a mechanism not included in current models. A general representation of the O3 budget in the tropical troposphere is proposed that couples the large-scale Walker circulation and in situ photochemistry. Deep convection in the rising branches of the Walker circulation injects NOx from combustion, soils, and lightning to the upper troposphere, leading to O3 production; eventually, the air subsides and net O3 loss takes place in the lower troposphere, closing the O3 cycle. This scheme implies a great sensitivity of the oxidizing power of the atmosphere to NOx emissions in the tropics.

Environmental health in China: progress towards clean air and safe water

Environmental risk factors, especially air and water pollution, are a major source of morbidity and mortality in China. Biomass fuel and coal are burned for cooking and heating in almost all rural and many urban households, resulting in severe indoor air pollution that contributes greatly to the burden of disease. Many communities lack access to safe drinking water and sanitation, and thus the risk of waterborne disease in many regions is high. At the same time, China is rapidly industrialising with associated increases in energy use and industrial waste. Although economic growth from industrialisation has improved health and quality of life indicators, it has also increased the release of chemical toxins into the environment and the rate of environmental disasters, with severe effects on health. Air quality in Chinas cities is among the worst in the world, and industrial water pollution has become a widespread health hazard. Moreover, emissions of climate-warming greenhouse gases from energy use are rapidly increasing. Global climate change will inevitably intensify Chinas environmental health troubles, with potentially catastrophic outcomes from major shifts in temperature and precipitation. Facing the overlap of traditional, modern, and emerging environmental dilemmas, China has committed substantial resources to environmental improvement. The country has the opportunity to address its national environmental health challenges and to assume a central role in the international effort to improve the global environment.

Photochemistry in biomass burning plumes and implications for tropospheric ozone over the tropical South Atlantic

Photochemistry occuring in biomass burning plumes over the tropical south Atlantic is analyzed using data collected during the Transport and Atmospheric Chemistry Near the Equator-Atlantic aircraft expedition conducted during the tropical dry season in September 1992 and a photochemical point model. Enhancement ratios (ΔY/ΔX, where Δ indicates the enhancement of a compound in the plume above the local background mixing ratio, Y are individual hydrocarbons, CO, O3, N2O, HNO3, peroxyacetyl nitrate (PAN), CH2O, acetone, H2O2, CH3OOH, HCOOH, CH3COOH or aerosols and X is CO or CO2) are reported as a function of plume age inferred from the progression of Δnon-methane hydrocarbons/ΔCO enhancement ratios. Emission, formation, and loss of species in plumes can be diagnosed from progression of enhancement ratios from fresh to old plumes. O3 is produced in plumes over at least a 1 week period with mean ΔO3/ΔCO = 0.7 in old plumes. However, enhancement ratios in plumes can be influenced by changing background mixing ratios and by photochemical loss of CO. We estimate a downward correction of ∼20% in enhancement ratios in old plumes relative to ΔCO to correct for CO loss. In a case study of a large persistent biomass burning plume at 4-km we found elevated concentrations of PAN in the fresh plume. The degradation of PAN helped maintain NOx mixing ratios in the plume where, over the course of a week, PAN was converted to HNO3. Ozone production in the plume was limited by the availability of NOx, and because of the short lifetime of O3 at 4-km, net ozone production in the plume was negligible. Within the region, the majority of O3 production takes place in air above median CO concentration, indicating that most O3 production occurs in plumes. Scaling up from the mean observed ΔO3/ΔCO in old plumes, we estimate a minimum regional O3 production of 17×1010molecules O3 cm−2 s−1. This O3 production rate is sufficient to fully explain the observed enhancement in tropospheric O3 over the tropical South Atlantic during the dry season.

Managing nitrogen for sustainable development

Improvements in nitrogen use efficiency in crop production are critical for addressing the triple challenges of food security, environmental degradation and climate change. Such improvements are conditional not only on technological innovation, but also on socio-economic factors that are at present poorly understood. Here we examine historical patterns of agricultural nitrogen-use efficiency and find a broad range of national approaches to agricultural development and related pollution. We analyse examples of nitrogen use and propose targets, by geographic region and crop type, to meet the 2050 global food demand projected by the Food and Agriculture Organization while also meeting the Sustainable Development Goals pertaining to agriculture recently adopted by the United Nations General Assembly. Furthermore, we discuss socio-economic policies and technological innovations that may help achieve them.

Seasonal characteristics of tropospheric ozone production and mixing ratios over East Asia: A global three‐dimensional chemical transport model analysis

We examine seasonal and geographical distributions of tropospheric ozone production and mixing ratios over East Asia with a global three-dimensional chemical transport model called Model of Ozone and Related Tracers, version 1 (MOZART 1). Net ozone production within the East Asian boundary layer exhibits three distinct seasonal cycles depending on region (north of 20°N, 5–20°N and south of 5°N). North of 20°N, net ozone production over East Asia from spring through autumn is found to have a maximum extending from 25°N–40°N and from central eastern China to Japan, resulting from the strong emission and transport of anthropogenic O3 precursors. In winter, maximum O3 production in this region occurs between 20°N and 30°N. This is a region of long-range transport. Over the Indochina peninsula, between 5°N and 20°N, net O3 production is controlled by the seasonal cycle between wet and dry seasons and has a maximum at the end of the dry season due to emissions from biomass burning. South of 5°N, in the true tropics, O3 mixing ratios are relatively constant throughout the year and do not exhibit a seasonal cycle. A spring-summer maximum of net O3 production is found throughout the troposphere in East Asia. We estimate an annual net O3 production in East Asia of 117 Tg/yr. Both model results and analysis of measurements of O3/CO correlations over East Asia and Japan show strong variability as a function of both photochemical activity and seasonal meteorology, and indicate ozone export off the coast of East Asia in spring. An upper estimate of O3 export from East Asia to the Pacific Ocean in the mid-1980s of 3.3 Gmol/d (58 Tg/yr) is obtained.

Air pollutant emissions from Chinese households: A major and underappreciated ambient pollution source

Significance China suffers from severe outdoor air pollution and associated public health impacts. In response, the government has imposed restrictions on major pollution sources such as vehicles and power plants. We show that due to uncontrolled and inefficient combustion of solid fuels in household devices, emission reductions from the residential sector may have greater air quality benefits in the North China Plain, including Beijing than reductions from other sectors. These benefits would be largest in the winter heating season when severe air pollution occurs. Household emissions, mostly from space heating and cooking with solid fuels, are an important and generally unrecognized source of ambient air pollution in China and other developing countries. Alternative fuels and other ways of reducing emissions would have large benefits. As part of the 12th Five-Year Plan, the Chinese government has developed air pollution prevention and control plans for key regions with a focus on the power, transport, and industrial sectors. Here, we investigate the contribution of residential emissions to regional air pollution in highly polluted eastern China during the heating season, and find that dramatic improvements in air quality would also result from reduction in residential emissions. We use the Weather Research and Forecasting model coupled with Chemistry to evaluate potential residential emission controls in Beijing and in the Beijing, Tianjin, and Hebei (BTH) region. In January and February 2010, relative to the base case, eliminating residential emissions in Beijing reduced daily average surface PM2.5 (particulate mater with aerodynamic diameter equal or smaller than 2.5 micrometer) concentrations by 14 ± 7 μg⋅m−3 (22 ± 6% of a baseline concentration of 67 ± 41 μg⋅m−3; mean ± SD). Eliminating residential emissions in the BTH region reduced concentrations by 28 ± 19 μg⋅m−3 (40 ± 9% of 67 ± 41 μg⋅m−3), 44 ± 27 μg⋅m−3 (43 ± 10% of 99 ± 54 μg⋅m−3), and 25 ± 14 μg⋅m−3 (35 ± 8% of 70 ± 35 μg⋅m−3) in Beijing, Tianjin, and Hebei provinces, respectively. Annually, elimination of residential sources in the BTH region reduced emissions of primary PM2.5 by 32%, compared with 5%, 6%, and 58% achieved by eliminating emissions from the transportation, power, and industry sectors, respectively. We also find air quality in Beijing would benefit substantially from reductions in residential emissions from regional controls in Tianjin and Hebei, indicating the value of policies at the regional level.

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 worlds 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.

Origin of tropospheric ozone at remote high northern latitudes in summer

Author(s): Mauzerall, DL; Jacob, DJ; Fan, SM; Bradshaw, JD; Gregory, GL; Sachse, GW; Blake, DR | Abstract: We quantify the tropospheric ozone budget over remote high northern latitudes in summer using chemical and meteorological measurements between 0 and 6-km made during the summer of 1990 Arctic Boundary Layer Expedition (ABLE 3B). We include all components of the ozone budget, both sinks (in situ photochemical loss and deposition); and sources (in situ photochemical production, advection of pollution ozone into the region, production in biomass wildfire plumes, and downwards transport from the upper troposphere/stratosphere). In situ production and loss of ozone are calculated with a photochemical model. The net influx of pollution ozone from North America and Eurasia is estimated from the average enhancement ratio of ΔO3/ΔC2Cl4 observed in pollution plumes and scaled by the net influx of C2Cl4. The contribution of ozone produced in biomass wildfire plumes is estimated from the average enhancement ratio of ΔO3/ΔCO in aged fire plumes. Regional photochemical production and loss in the 0-6 km column are found to be approximately equal; hence, net photochemical production is near zero. However, when ozone production and loss terms are separated, we find that dispersed in situ photochemical production driven by background NO levels (5-10 pptv) is the largest source term in the ozone budget (62%). Influx of stratospheric ozone is of secondary importance (27%), long-range transport of pollution ozone makes a small contribution (9%), and photochemical production of ozone within biomass wildfire plumes is a relatively negligible term (2%) in the budget. Biomass fires and transport of anthropogenic pollution into the region may however have a major effect on the ozone budget through enhancement of background NOx mixing ratios which increase dispersed photochemical production. Using a I-D time-dependent photochemical model between 0 and 6 km, we obtain good agreement between the observed and model-generated vertical ozone profiles. We find that in situ photochemistry within the 0-6 km column accounts for nearly 90% of the ozone mixing ratio within the boundary layer, while above 5 km it accounts for only about 40%. Although photochemical production of ozone within the 0-6 km column is larger than the other source terms combined, the 1-D model results indicate that influx from above is necessary to account for the observed increase in ozone mixing ratios with altitude. Copyright 1996 by the American Geophysical Union.

Assessing the climatic benefits of black carbon mitigation.

To limit mean global warming to 2 °C, a goal supported by more than 100 countries, it will likely be necessary to reduce emissions not only of greenhouse gases but also of air pollutants with high radiative forcing (RF), particularly black carbon (BC). Although several recent research papers have attempted to quantify the effects of BC on climate, not all these analyses have incorporated all the mechanisms that contribute to its RF (including the effects of BC on cloud albedo, cloud coverage, and snow and ice albedo, and the optical consequences of aerosol mixing) and have reported their results in different units and with different ranges of uncertainty. Here we attempt to reconcile their results and present them in uniform units that include the same forcing factors. We use the best estimate of effective RF obtained from these results to analyze the benefits of mitigating BC emissions for achieving a specific equilibrium temperature target. For a 500 ppm CO2e (3.1 W m-2) effective RF target in 2100, which would offer about a 50% chance of limiting equilibrium warming to 2.5 °C above preindustrial temperatures, we estimate that failing to reduce carbonaceous aerosol emissions from contained combustion would require CO2 emission cuts about 8 years (range of 1–15 years) earlier than would be necessary with full mitigation of these emissions.

Direct measurements of methane emissions from abandoned oil and gas wells in Pennsylvania

Significance Recent studies indicate that greenhouse gas emission inventories are likely missing methane emission sources. We conducted the first methane emission measurements from abandoned oil and gas wells and found substantial emissions, particularly from high-emitting abandoned wells. These emissions are not currently considered in any emissions inventory. We scaled methane emissions from our direct measurements of abandoned wells in Pennsylvania and calculate that they represent 4–7% of current total anthropogenic methane emissions in Pennsylvania. Millions of abandoned wells exist across the country and some are likely to be high emitters. Additional measurements of methane emissions from abandoned wells and their inclusion in greenhouse gas inventories will aid in developing and implementing appropriate greenhouse gas emission reduction strategies. Abandoned oil and gas wells provide a potential pathway for subsurface migration and emissions of methane and other fluids to the atmosphere. Little is known about methane fluxes from the millions of abandoned wells that exist in the United States. Here, we report direct measurements of methane fluxes from abandoned oil and gas wells in Pennsylvania, using static flux chambers. A total of 42 and 52 direct measurements were made at wells and at locations near the wells (“controls”) in forested, wetland, grassland, and river areas in July, August, October 2013 and January 2014, respectively. The mean methane flow rates at these well locations were 0.27 kg/d/well, and the mean methane flow rate at the control locations was 4.5 × 10−6 kg/d/location. Three out of the 19 measured wells were high emitters that had methane flow rates that were three orders of magnitude larger than the median flow rate of 1.3 × 10−3 kg/d/well. Assuming the mean flow rate found here is representative of all abandoned wells in Pennsylvania, we scaled the methane emissions to be 4–7% of estimated total anthropogenic methane emissions in Pennsylvania. The presence of ethane, propane, and n-butane, along with the methane isotopic composition, indicate that the emitted methane is predominantly of thermogenic origin. These measurements show that methane emissions from abandoned oil and gas wells can be significant. The research required to quantify these emissions nationally should be undertaken so they can be accurately described and included in greenhouse gas emissions inventories.