Vaishali Naik

Three decades of global methane sources and sinks

Methane is an important greenhouse gas, responsible for about 20% of the warming induced by long-lived greenhouse gases since pre-industrial times. By reacting with hydroxyl radicals, methane reduces the oxidizing capacity of the atmosphere and generates ozone in the troposphere. Although most sources and sinks of methane have been identified, their relative contributions to atmospheric methane levels are highly uncertain. As such, the factors responsible for the observed stabilization of atmospheric methane levels in the early 2000s, and the renewed rise after 2006, remain unclear. Here, we construct decadal budgets for methane sources and sinks between 1980 and 2010, using a combination of atmospheric measurements and results from chemical transport models, ecosystem models, climate chemistry models and inventories of anthropogenic emissions. The resultant budgets suggest that data-driven approaches and ecosystem models overestimate total natural emissions. We build three contrasting emission scenarios-which differ in fossil fuel and microbial emissions-to explain the decadal variability in atmospheric methane levels detected, here and in previous studies, since 1985. Although uncertainties in emission trends do not allow definitive conclusions to be drawn, we show that the observed stabilization of methane levels between 1999 and 2006 can potentially be explained by decreasing-to-stable fossil fuel emissions, combined with stable-to-increasing microbial emissions. We show that a rise in natural wetland emissions and fossil fuel emissions probably accounts for the renewed increase in global methane levels after 2006, although the relative contribution of these two sources remains uncertain.

Characterizing the tropospheric ozone response to methane emission controls and the benefits to climate and air quality

[1]xa0Reducing methane (CH4) emissions is an attractive option for jointly addressing climate and ozone (O3) air quality goals. With multidecadal full-chemistry transient simulations in the MOZART-2 tropospheric chemistry model, we show that tropospheric O3 responds approximately linearly to changes in CH4 emissions over a range of anthropogenic emissions from 0–430 Tg CH4 a−1 (0.11–0.16 Tg tropospheric O3 or ∼11–15 ppt global mean surface O3 decrease per Tg a−1 CH4 reduced). We find that neither the air quality nor climate benefits depend strongly on the location of the CH4 emission reductions, implying that the lowest cost emission controls can be targeted. With a series of future (2005–2030) transient simulations, we demonstrate that cost-effective CH4 controls would offset the positive climate forcing from CH4 and O3 that would otherwise occur (from increases in NOx and CH4 emissions in the baseline scenario) and improve O3 air quality. We estimate that anthropogenic CH4 contributes 0.7 Wm−2 to climate forcing and ∼4 ppb to surface O3 in 2030 under the baseline scenario. Although the response of surface O3 to CH4 is relatively uniform spatially compared to that from other O3 precursors, it is strongest in regions where surface air mixes frequently with the free troposphere and where the local O3 formation regime is NOx-saturated. In the model, CH4 oxidation within the boundary layer (below ∼2.5 km) contributes more to surface O3 than CH4 oxidation in the free troposphere. In NOx-saturated regions, the surface O3 sensitivity to CH4 can be twice that of the global mean, with >70% of this sensitivity resulting from boundary layer oxidation of CH4. Accurately representing the NOx distribution is thus crucial for quantifying the O3 sensitivity to CH4.

Net radiative forcing due to changes in regional emissions of tropospheric ozone precursors

[1]xa0The global distribution of tropospheric ozone (O3) depends on the emission of precursors, chemistry, and transport. For small perturbations to emissions, the global radiative forcing resulting from changes in O3 can be expressed as a sum of forcings from emission changes in different regions. Tropospheric O3 is considered in present climate policies only through the inclusion of indirect effect of CH4 on radiative forcing through its impact on O3 concentrations. The short-lived O3 precursors (NOx, CO, and NMHCs) are not directly included in the Kyoto Protocol or any similar climate mitigation agreement. In this study, we quantify the global radiative forcing resulting from a marginal reduction (10%) in anthropogenic emissions of NOx alone from nine geographic regions and a combined marginal reduction in NOx, CO, and NMHCs emissions from three regions. We simulate, using the global chemistry transport model MOZART-2, the change in the distribution of global O3 resulting from these emission reductions. In addition to the short-term reduction in O3, these emission reductions also increase CH4 concentrations (by decreasing OH); this increase in CH4 in turn counteracts part of the initial reduction in O3 concentrations. We calculate the global radiative forcing resulting from the regional emission reductions, accounting for changes in both O3 and CH4. Our results show that changes in O3 production and resulting distribution depend strongly on the geographical location of the reduction in precursor emissions. We find that the global O3 distribution and radiative forcing are most sensitive to changes in precursor emissions from tropical regions and least sensitive to changes from midlatitude and high-latitude regions. Changes in CH4 and O3 concentrations resulting from NOx emission reductions alone produce offsetting changes in radiative forcing, leaving a small positive residual forcing (warming) for all regions. In contrast, for combined reductions of anthropogenic emissions of NOx, CO, and NMHCs, changes in O3 and CH4 concentrations result in a net negative radiative forcing (cooling). Thus we conclude that simultaneous reductions of CO, NMHCs, and NOx lead to a net reduction in radiative forcing due to resulting changes in tropospheric O3 and CH4 while reductions in NOx emissions alone do not.

Air Quality and Climate Connections

Multiple linkages connect air quality and climate change. Many air pollutant sources also emit carbon dioxide (CO2), the dominant anthropogenic greenhouse gas (GHG). The two main contributors to non-attainment of U.S. ambient air quality standards, ozone (O3) and particulate matter (PM), interact with radiation, forcing climate change. PM warms by absorbing sunlight (e.g., black carbon) or cools by scattering sunlight (e.g., sulfates) and interacts with clouds; these radiative and microphysical interactions can induce changes in precipitation and regional circulation patterns. Climate change is expected to degrade air quality in many polluted regions by changing air pollution meteorology (ventilation and dilution), precipitation and other removal processes, and by triggering some amplifying responses in atmospheric chemistry and in anthropogenic and natural sources. Together, these processes shape distributions and extreme episodes of O3 and PM. Global modeling indicates that as air pollution programs reduce SO2 to meet health and other air quality goals, near-term warming accelerates due to “unmasking” of warming induced by rising CO2. Air pollutant controls on CH4, a potent GHG and precursor to global O3 levels, and on sources with high black carbon (BC) to organic carbon (OC) ratios could offset near-term warming induced by SO2 emission reductions, while reducing global background O3 and regionally high levels of PM. Lowering peak warming requires decreasing atmospheric CO2, which for some source categories would also reduce co-emitted air pollutants or their precursors. Model projections for alternative climate and air quality scenarios indicate a wide range for U.S. surface O3 and fine PM, although regional projections may be confounded by interannual to decadal natural climate variability. Continued implementation of U.S. NOx emission controls guards against rising pollution levels triggered either by climate change or by global emission growth. Improved accuracy and trends in emission inventories are critical for accountability analyses of historical and projected air pollution and climate mitigation policies. Implications: The expansion of U.S. air pollution policy to protect climate provides an opportunity for joint mitigation, with CH4 a prime target. BC reductions in developing nations would lower the global health burden, and for BC-rich sources (e.g., diesel) may lessen warming. Controls on these emissions could offset near-term warming induced by health-motivated reductions of sulfate (cooling). Wildfires, dust, and other natural PM and O3 sources may increase with climate warming, posing challenges to implementing and attaining air quality standards. Accountability analyses for recent and projected air pollution and climate control strategies should underpin estimated benefits and trade-offs of future policies.

The influence of ozone precursor emissions from four world regions on tropospheric composition and radiative climate forcing

0.4 2.6 to 1.9 1.3 Gg for NOx reductions, 0.1 1.2 to 0.9 0.8 Gg for NMVOC reductions, and 0.09 0.5 to 0.9 0.8 Gg for CO reductions, suggesting additional research is needed. The 100-year global warming potentials (GWP100) are calculated for the global CH4 reduction (20.9 3.7 without stratospheric O3 or water vapor, 24.2 4.2 including those components), and for the regional NOx, NMVOC, and CO reductions (18.7 25.9 to 1.9 8.7 for NOx, 4.8 1.7 to 8.3 1.9 for NMVOC, and 1.5 0.4 to 1.7 0.5 for CO). Variation in GWP100 for NOx, NMVOC, and CO suggests that regionally specific GWPs may be necessary and could support the inclusion

Sensitivity of global biogenic isoprenoid emissions to climate variability and atmospheric CO2

[1]xa0Isoprenoids (isoprene and monoterpenes) are the most dominant class of biogenic volatile organic compounds (BVOCs) and have been shown to significantly affect global tropospheric chemistry and composition, climate, and the global carbon cycle. In this study we assess the sensitivity of biogenic isoprene and monoterpene emissions to combined and isolated fluctuations in observed global climate and atmospheric carbon dioxide (CO2) concentration during the period 1971–1990. We integrate surface emission algorithms within the framework of a dynamic global ecosystem model, the Integrated Biospheric Simulator (IBIS), to simulate biogenic fluxes of isoprenoids as a component of the climate-vegetation dynamics. IBIS predicts global land surface isoprene emissions of 454 Tg C and monoterpenes of 72 Tg C annually and captures the spatial and temporal patterns well. The combined fluctuations in climate and atmospheric CO2 during 1971–1990 caused significant interannual and seasonal variability in global biogenic isoprenoid fluxes that was somewhat related to the El Nino-Southern Oscillation. Furthermore, an increasing trend in the simulated emissions was seen during this period that is attributed partly to the warming trend and partly to CO2 fertilization effect. The isolated effect of increasing CO2 during this period was to steadily increase emissions as a result of increases in foliar biomass. These fluctuations in biogenic emissions could have significant impacts on regional and global atmospheric chemistry and the global carbon budget.

Ozone air quality and radiative forcing consequences of changes in ozone precursor emissions

[1]xa0Changes in emissions of ozone (O3) precursors affect both air quality and climate. We first examine the sensitivity of surface O3 concentrations (O3srf) and net radiative forcing of climate (RFnet) to reductions in emissions of four precursors – nitrogen oxides (NOx), non-methane volatile organic compounds, carbon monoxide, and methane (CH4). We show that long-term CH4-induced changes in O3, known to be important for climate, are also relevant for air quality; for example, NOx reductions increase CH4, causing a long-term O3 increase that partially counteracts the direct O3 decrease. Second, we assess the radiative forcing resulting from actions to improve O3 air quality by calculating the ratio of ΔRFnet to changes in metrics of O3srf. Decreases in CH4 emissions cause the greatest RFnet decrease per unit reduction in O3srf, while NOx reductions increase RFnet. Of the available means to improve O3 air quality, therefore, CH4 abatement best reduces climate forcing.

On the sensitivity of radiative forcing from biomass burning aerosols and ozone to emission location

[1]xa0Biomass burning is a major source of air pollutants, some of which are also climate forcing agents. We investigate the sensitivity of direct radiative forcing due to tropospheric ozone and aerosols (carbonaceous and sulfate) to a marginal reduction in their (or their precursor) emissions from major biomass burning regions. We find that the largest negative global forcing is for 10% emission reductions in tropical regions, including Africa (−4.1 mWm−2 from gas and −4.1 mWm−2 from aerosols), and South America (−3.0 mWm−2 from gas and −2.8 mWm−2 from aerosols). We estimate that a unit reduction in the amount of biomass burned in India produces the largest negative ozone and aerosol forcing. Our analysis indicates that reducing biomass burning emissions causes negative global radiative forcing due to ozone and aerosols; however, regional differences need to be considered when evaluating controls on biomass burning to mitigate global climate change.

Effect of regional precursor emission controls on long-range ozone transport - Part 1: Short-term changes in ozone air quality

Abstract. Observations and models demonstrate that ozone and its precursors can be transported between continents and across oceans. We model the influences of 10% reductions in anthropogenic nitrogen oxide (NO x ) emissions from each of nine world regions on surface ozone air quality in that region and all other regions. In doing so, we quantify the relative importance of long-range transport between all source-receptor pairs, for direct short-term ozone changes. We find that for population-weighted concentrations during the three-month ozone-season, the strongest inter-regional influences are from Europe to the Former Soviet Union, East Asia to Southeast Asia, and Europe to Africa. The largest influences per unit of NO x reduced, however, are seen for source regions in the tropics and Southern Hemisphere, which we attribute mainly to greater sensitivity to changes in NO x in the lower troposphere, and secondarily to increased vertical convection to the free troposphere in tropical regions, allowing pollutants to be transported further. Results show, for example, that NO x reductions in North America are ~20% as effective per unit NO x in reducing ozone in Europe during summer, as NO x reductions from Europe itself. Reducing anthropogenic emissions of non-methane volatile organic compounds (NMVOCs) and carbon monoxide (CO) by 10% in selected regions, can have as large an impact on long-range ozone transport as NO x reductions, depending on the source region. We find that for many source-receptor pairs, the season of greatest long-range influence does not coincide with the season when ozone is highest in the receptor region. Reducing NO x emissions in most source regions causes a larger decrease in export of ozone from the source region than in ozone production outside of the source region.