10.4.3 Simulations of Future Evolution of Methane, Ozone and Oxidants
Simulations using coupled chemistry-climate models indicate that the trend in upper-stratospheric ozone changes sign sometime between 2000 and 2005 due to the gradual reduction in halocarbons. While ozone concentrations in the upper stratosphere decreased at a rate of 400 ppb (–6%) per decade during 1980 to 2000, they are projected to increase at a rate of 100 ppb (1 to 2%) per decade from 2000 to 2020 (Austin and Butchart, 2003). On longer time scales, simulations show significant changes in ozone and CH4 relative to current concentrations. The changes are related to a variety of factors, including increased emissions of chemical precursors, changes in gas-phase and heterogeneous chemistry, altered climate conditions due to global warming and greater transport and mixing across the tropopause. The impacts on CH4 and ozone from increased emissions are a direct effect of anthropogenic activity, while the impacts of different climate conditions and stratosphere-troposphere exchange represent indirect effects of these emissions (Grewe et al., 2001).
The projections for ozone based upon scenarios with high emissions (IS92a; Leggett et al., 1992) and SRES A2 (Nakićenović and Swart, 2000) indicate that concentrations of tropospheric ozone might increase throughout the 21st century, primarily as a result of these emissions. Simulations for the period 2015 through 2050 project increases in ozone of 20 to 25% (Grewe et al., 2001; Hauglustaine and Brasseur, 2001), and simulations through 2100 indicate that ozone below 250 mb may grow by 40 to 60% (Stevenson et al., 2000; Grenfell et al., 2003; Zeng and Pyle, 2003; Hauglustaine et al., 2005; Yoshimura et al., 2006). The primary species contributing to the increase in tropospheric ozone are anthropogenic emissions of NOx, CH4, CO and compounds from fossil fuel combustion. The photochemical reactions that produce smog are accelerated by increases of 2.6 times the present flux of NOx, 2.5 times the present flux of CH4 and 1.8 times the present flux of CO in the A2 scenario. Between 91 and 92% of the higher concentrations in ozone are related to direct effects of these emissions, with the remainder of the increase attributable to secondary effects of climate change (Zeng and Pyle, 2003) combined with biogenic precursor emissions (Hauglustaine et al., 2005). These emissions may also lead to higher concentrations of oxidants including the hydroxyl radical (OH), possibly leading to an 8% reduction in the lifetime of tropospheric CH4 (Grewe et al., 2001).
Since the projected growth in emissions occurs primarily in low latitudes, the ozone increases are largest in the tropics and subtropics (Grenfell et al., 2003). In particular, the concentrations in Southeast Asia, India and Central America increase by 60 to 80% by 2050 under the A2 scenario. However, the effects of tropical emissions are not highly localised, since the ozone spreads throughout the lower atmosphere in plumes emanating from these regions. As a result, the ozone in remote marine regions in the SH may grow by 10 to 20% over present-day levels by 2050. The ozone may also be distributed through vertical transport in tropical convection followed by lateral transport on isentropic surfaces. Ozone concentrations can also be increased by emissions of biogenic hydrocarbons (e.g., Hauglustaine et al., 2005), in particular isoprene emitted by broadleaf forests. Under the A2 scenario, biogenic hydrocarbons are projected to increase by between 27% (Sanderson et al., 2003) and 59% (Hauglustaine et al., 2005) contributing to a 30 to 50% increase in ozone formation over northern continental regions.
Developing countries have begun reducing emissions from mobile sources through stricter standards. New projections of the evolution of ozone precursors that account for these reductions have been developed with the Regional Air Pollution Information and Simulation (RAINS) model (Amann et al., 2004). One set of projections is consistent with source strengths permitted under the Current Legislation (CLE) scenario. A second set of projections is consistent with lower emissions under a Maximum Feasible Reduction (MFR) scenario. The concentrations of ozone and CH4 have been simulated for the MFR, CLE and A2 scenarios for the period 2000 through 2030 using an ensemble of 26 chemical transport models (Dentener et al., 2006; Stevenson et al., 2006). The changes in NOx emissions for these three scenarios are –27%, +12% and +55%, respectively, relative to year 2000. The corresponding changes in ensemble-mean burdens in tropospheric ozone are –5%, +6% and +18% for the MFR, CLE and A2 scenarios, respectively. There are substantial inter-model differences of order ±25% in these results. The ozone decreases throughout the troposphere in the MFR scenario, but the zonal annual mean concentrations increase by up to 6 ppb in the CLE scenario and by typically 6 to 10 ppb in the A2 scenario (Supplementary Material, Figure S10.2).
The radiative forcing by the combination of ozone and CH4 changes by –0.05, 0.18, and 0.30 W m–2 for the MFR, CLE and A2 scenarios, respectively. These projections indicate that the growth in tropospheric ozone between 2000 and 2030 could be reduced or reversed depending on emission controls.
The major issues in the fidelity of these simulations for future tropospheric ozone are the sensitivities to the representation of the stratospheric production, destruction and transport of ozone and the exchange of species between the stratosphere and troposphere. Few of the models include the effects of non-methane hydrocarbons (NMHCs), and the sign of the effects of NMHCs on ozone are not consistent among the models that do (Hauglustaine and Brasseur, 2001; Grenfell et al., 2003).
The effect of more stratosphere-troposphere exchange (STE) in response to climate change is projected to increase the concentrations of ozone in the upper troposphere due to the much greater concentrations of ozone in the lower stratosphere than in the upper troposphere. While the sign of the effect is consistent in recent simulations, the magnitude of the change in STE and its effects on ozone are very model dependent. In a simulation forced by the SRES A1FI scenario, Collins et al. (2003) project that the downward flux of ozone increases by 37% from the 1990s to the 2090s. As a result, the concentration of ozone in the upper troposphere at mid-latitudes increases by 5 to 15%. For the A2 scenarios, projections of the increase in ozone by 2100 due to STE range from 35% (Hauglustaine et al., 2005) to 80% (Sudo et al., 2003; Zeng and Pyle, 2003). The increase in STE is driven by increases in the descending branches of the Brewer-Dobson Circulation at mid-latitudes and is caused by changes in meridional temperature gradients in the upper troposphere and lower stratosphere (Rind et al., 2001). The effects of the enhanced STE are sensitive to the simulation of processes in the stratosphere, including the effects of lower temperatures and the evolution of chlorine, bromine and NOx concentrations. Since the greenhouse effect of ozone is largest in the upper troposphere, the treatment of STE remains a significant source of uncertainty in the calculation of the total greenhouse effect of tropospheric ozone.
The effects of climate change, in particular increased tropospheric temperatures and water vapour, tend to offset some of the increase in ozone driven by emissions. The higher water vapour is projected to offset the increase in ozone by between 10% (Hauglustaine et al., 2005) and 17% (Stevenson et al., 2000). The water vapour both decelerates the chemical production and accelerates the chemical destruction of ozone. The photochemical production depends on the concentrations of NOy (reactive odd nitrogen), and the additional water vapour causes a larger fraction of NOy to be converted to nitric acid, which can be efficiently removed from the atmosphere in precipitation (Grewe et al., 2001). The water vapour also increases the concentrations of OH through reaction with the oxygen radical in the 1D excited state (O(1D)), and the removal of O(1D) from the atmosphere slows the formation of ozone. The increased concentrations of OH and the increased rates of CH4 oxidation with higher temperature further reduce the lifetime of tropospheric CH4 by 12% by 2100 (Stevenson et al., 2000; Johnson et al., 2001). Decreases in CH4 concentrations also tend to reduce tropospheric ozone (Stevenson et al., 2000).
Recent measurements show that CH4 growth rates have declined and were negative for several years in the early 21st century (see Section 2.3.2). The observed rate of increase of 0.8 ppb yr–1 for the period 1999 to 2004 is considerably less than the rate of 6 ppb yr–1 assumed in all the SRES scenarios for the period 1990 to 2000 (Nakićenović and Swart, 2000; TAR Appendix II). Recent studies (Dentener et al., 2005) have considered lower emission scenarios (see above) that take account of new pollution control techniques adopted in major developing countries. In the CLE scenario, emissions of CH4 are comparable to the B2 scenario and increase from 340 Tg yr–1 in 2000 to 450 Tg yr–1 in 2030. The CH4 concentrations increase from 1,750 ppb in 2000 to between 2,090 and 2,200 ppb in 2030 under this scenario. In the MFR scenario, the emissions are sufficiently low that the concentrations in 2030 are unchanged at 1,750 ppb. Under these conditions, the changes in radiative forcing due to CH4 between the 1990s and 2020s are less than 0.01 W m–2.
Current understanding of the magnitude and variation of CH4 sources and sinks is covered in Section 7.4, where it is noted that there are substantial uncertainties although the modelling has progressed. There is some evidence for a coupling between climate and wetland emissions. For example, calculations using atmospheric concentrations and small-scale emission measurements as input differ by 60% (Shindell and Schmidt, 2004). Concurrent changes in natural sources of CH4 are now being estimated to first order using simple models of the biosphere coupled to AOGCMs. Simulations of the response of wetlands to climate change from doubling atmospheric CO2 show that wetland emissions increase by 78% (Shindell and Schmidt, 2004). Most of this effect is caused by growth in the flux of CH4 from existing tropical wetlands. The increase would be equivalent to approximately 20% of current inventories and would contribute an additional 430 ppb to atmospheric concentrations. Global radiative forcing would increase by approximately 4 to 5% from the effects of wetland emissions by 2100 (Gedney et al., 2004).