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Soot Aerosol from Aircraft: Is there Enough to Cause Middle-Latitude Lower Stratospheric Ozone

Soot aerosol from aircraft has been implicated to cause long-term ozone depletion at mid-latitudes in the lower stratosphere at a rate of approx. equals 5%,per decade. During the 1996 SUCCESS field campaign, we sampling aerosols in the exhaust wake of a Boeing 757 aircraft and determined emission indices for sulfuric acid (EIH2SO4=4.8E-2 and 5.7E- 1. g/kgFUEL for 75 and 675 ppm fuel-sulfur, respectively) and soot (EIsoot=7.5E-4 g/kgFUEL). The corresponding fuel-sulfur to H2SO4 conversion efficiency was 25 % and 30%,respctively. Applying the H2SO4 emission index to the 1990 fuel by the world's commercial fleets of 1.3E11 kg, a conversion efficiency of 30% would have led to an annual contribution to the atmospheric sulfur budget by aircraft of 2.E7 kg H2SO4, if the fuels averaged 500 ppmm.The soot emission index given above yielded a 1990 injection of soot aerosol by aircraft of 1.E5 kg. Thus, soot amounts to only one half of one percent of the aerosol generated by aircraft. The fractal nature of soot may increase its actual surface area by about a factor of 10. The findings, however, of (1) stratospheric soot loadings commensurate with aircraft fuel consumption, based on the emission index given above and the assumption of stratospheric residence times of the order of one year; and (2) a trend in stratospheric soot loading of approx.6% per year since 1981, similar to the annual increase of aircraft operations since that time, implicate aircraft as stratospheric polluters. A trend similar to soot of H2SO4 aerosol loading could not be deciphered, neither from in situ measurements nor SAGE II extinction, against the "noise" due to volcanic eruptions, The current single scatter albedo of the stratospheric aerosol is omega = 0.993+/-0.004.

Pueschel, R. F.↗

Soot and Sulfuric Acid from Aircraft: Is There Enough to Cause Detrimental Environmental E-kCTSs?

Aerosol from aircraft can affect the environment in three ways: First, soot aerosol has been implicated to cause Icing-tern ozone depletion at mid-latitudes in the lower stratosphere at a rate of approx. 5% per decade. This effect is in addition and unrelated to the polar ozone holes which are strongly influenced by heterogeneous chemistry on polar stratospheric clouds. Second, the most obvious effect of jet aircraft is the formation of visible contrails in the upper troposphere. The Salt Lake City region experienced an 8% increase in cirrus cloud cover over a 15-year period which covariates with an increase in regional commercial air traffic. If soot particles act as freezing nuclei to cause contrail formation heterogeneously, they would be linked to a secondary effect to cloud modification that very likely is climatologically important. Third, a buildup of soot aerosol could reduce the single scatter albedo of stratospheric aerosol from 0.993+0.004 to 0.98, a critical value that has been postulated to separate stratospheric cooling from warming. Thus arises an important question: Do aircraft emit sufficient amounts of soot to have detrimental effects and warrant emission controls? During the 1996 SUCCESS field campaign, we sampled aerosols in the exhaust wake of a Boeing 757 aircraft and determined emission indices for sulfuric acid (EI(sub H2SO4) = 9.0E-2 and 5.0E-1 g/kg (sub FUEL) for 75 and 675 ppm fuel-sulfur, respectively) and soot aerosol (2.2E-3 less than EI(sub SOOT) = l.lE-2 g/kg (sub FUEL)). The soot particle analysis accounted for their fractal nature, determined electron-microscopically, which enhanced the surface area by a factor of 26 and the volume 11-fold over equivalent-volume spheres. The corresponding fuel-sulfur to H2SO4 conversion efficiency was 10% (for 675 ppmm fuel-S) and 37% (for 75 ppmm fuel-S). Applying the H2SO4 emission index to the 1990 fuel use by the worlds commercial fleets of 1.3E11 kg, a conversion efficiency of 30% of 500 ppmm fuel-S would have led to an annual contribution to the atmospheric sulfur budget by aircraft of 2.E7 kg H2SO4. This is about one part in 1.E4 of anthropogenic sulfate from other sources. The soot emission index given above yielded a 1990 injection of soot aerosol by aircraft of 1.E6 kg. Thus, soot amounts to only five percent of the aerosol generated by aircraft. Its reactivity with ozone would have to be 20 times that of sulfuric acid particles to make it chemically significant. Nevertheless, the findings, of stratospheric soot loadings commensurate with aircraft fuel consumption, based on the emission index given above and the assumption of stratospheric residence times of the order of one year implicate aircraft as stratospheric polluters. A trend similar to soot of H2SO4 aerosol loading could not be deciphered, neither from in situ measurements nor SAGE II satellite extinction, against the "noise" due to volcanic eruptions. Observation of soot particles at 20 km altitude which, if emitted by aircraft were generated at 10-12 km altitude, suggests a displacement of those particles against gravity. Because eddy mixing is virtually absent in the lower stratosphere and isentropic mixing explains lofting to only about 15 km, radiometric forces acting on morphologically and chemically asymmetric soot particles must be considered a possibility. The consequence could be an extended residence time of soot against that of sulfuric acid aerosol that would lower the single scatter albedo with time.

Pueschel, R. F.↗

On Soot Inception in Nonpremixed Flames and the Effects of Flame Structure

A simplified three-step model of soot inception has been employed with high activation energy asymptotics to study soot inception in nonpremixed counterflow systems with emphasis on understanding the effects of hydrodynamics and transport. The resulting scheme yields three zones: (1) a fuel oxidation zone wherein the fuel and oxidizer react to form product as well as a radical R, (e.g., H), (2) a soot/precursor formation zone where the radical R reacts with fuel to form "soot/precursor" S, and (3) a soot/precursor consumption zone where S reacts with the oxidizer to form product. The kinetic scheme, although greatly simplified, allows the coupling between soot inception and flame structure to be assessed. The results yield flame temperature, flame location, and a soot/precursor index S(sub I) as functions of Damkohler number for S formation. The soot/precursor index indicates the amount of S at the boundary of the formation region. The flame temperature indirectly indicates the total amount of S integrated over the formation region because as S is formed less heat release is available. The results show that unlike oxidation reactions, an extinction turning-point behavior does not exist for soot. Instead, the total amount of S slowly decreases with decreasing Damkohler number (increasing strain rate), which is consistent with counterflow flame experiments. When the Lewis number of the radical is decreased from unity, the total S reduces due to reduced residence time for the radical in the soot formation region. Similarly, when the Lewis number of the soot/precursor is increased from unity the amount of S increases for all Damkohler numbers. In addition to studying fuel-air (low stoichiometric mixture fraction) flames, the air-side nitrogen was substituted into the fuel, yielding diluted fuel-oxygen (high stoichiometric mixture fraction) flames with the same flame temperature as the fuel - air flames. The relative flame locations were different however, and, consistent with counterflow flame experiments, this difference was found to dramatically reduce the total amount of S generated because the change in stoichiometric mixture fraction affects residence times, temperatures and concentrations in the soot/precursor formation and consumption zones. Furthermore, while the soot/precursor consumption reaction had a negligible effect on the soot process for fuel-air flames it was very important to diluted fuel - oxygen flames.

Chao, B. H.↗

Electron reflection and secondary emission characteristics of sputter-textured pyrolytic graphite surfaces

Measurements are presented of secondary electron emission and reflected primary electron characteristics of sputter-textured pyrolitic graphite surfaces with microstructures of various sizes and densities, made with an Auger cylindrical mirror analyzer in a high-vacuum chamber at pressures below 1.33 x 10 to the -7th N/sq m (10 to the -9th torr). A dense, tall, thin, spire-like microstructure, obtained at ion energies of 1000 eV and ion current densities of 5 mA/sq cm, is the most effective. The secondary electron emission from such a surface is lower than that of soot, whose secondary emission is among the lowest of any material. At a primary electron energy of 1000 eV, the secondary electron emission yield of smooth CU is about 350% greater than the lowest value obtained for sputter-textured pyrolitic graphite. The reflected primary electron index of smooth Cu is a factor of 80 greater. If the secondary electron emission yield is reduced to 0.3, which is possible with sputter-textured pyrolitic graphite, the traveling wave tube collector efficiency could be improved by as much as 4% over that for smooth copper.

Wintucky, E. G.↗