The characterization of volatile and nonvolatile particle materials present in gas turbine exhaust is critical for accurate estimation of the potential impacts of airport activities on local air quality, atmospheric processes, and climate change. Two field campaigns were performed to collect an extensive set of particle and gaseous emission data for on-wing gas turbine engines. The tests included CFM56, RB211-535E4-B, AE3007, PW4158, and CJ610 engines, providing the opportunity to compare emissions from a wide range of engine technologies. Here we report mass, number, composition, and size data for the nonvolatile (soot) and volatile particles present in engine exhaust. For all engines, soot emissions (EIm-soot) are greater at climbout (85% power) and takeoff (100%) power than idle (4% or 7%) and approach (30%). At the engine exit plane, soot is the only type of particle detected. For exhaust sampled downwind (15–50 m) and diluted by ambient air, total particle number emissions (EIn-total) increases by about one or two orders of magnitude relative to the engine exit plane, and the increase is driven by volatile particles that have freshly nucleated in the cooling exhaust gas both in the free atmosphere and in the extractive sample lines. Fuel sulfur content is the determining factor for nucleation of new particles in the cooling exhaust gases. Compositional analysis indicates that the volatile particles consist of sulfate and organic materials (EIm-sulfate and EIm-organic). We estimate a lower bound S[IV] to S[VI] conversion efficiency of (0.08±0.01)%, independent of engine technology. Measurements of EIm-organic ranged from about 0.1 mg kg−1 to 40 mg kg−1. Lubrication oil was present in particles emitted by all engines and accounted for over 90% of the particulate organic mass under some conditions. The products of incomplete combustion are a likely source of the remaining volatile organic particle material.
We have performed a comprehensive test of the effects of alternative fuels on the trace gas, nonvolatile particulate material (PM), and volatile PM emissions performance of a PW308 aircraft engine. The tests evaluated standard JP-8 jet fuel, a "zero sulfur" and "zero aromatic" synthetic fuel produced from a natural gas feedstock using the Fischer-Tropsch (FT) process, and a 50/50 blend of the FT fuel and JP-8. A Pratt & Whitney PW308 engine was operated under the same thrust and combustion conditions to ensure that the tests captured fuel differences, rather than engine operation differences. Emissions of trace gases, soot particles, and nucleation/growth PM were directly impacted by the sulfur and aromatic content of the fuel. FT fuel combustion greatly reduced SO 2 (>90%), gaseous hydrocarbons (40%), and NO (6-11%) content compared to JP-8 combustion. In general, combustion of the JP-8/FT fuel blend resulted in emissions intermediate to the FT and JP-8 values. FT combustion dramatically reduces soot particle number, mass, and size relative to JP-8, but increases effective soot particle density. In all cases, the drag behavior of the soot particles indicates deviations from spherical shape and effective soot particle densities are consistent with the soot particles being aggregates of primary spherules. As expected, FT combustion plumes support negligible formation of nucleation/growth mode particles (the number of nucleation growth mode particles is <20% the number of soot particles compared to >500% for sulfur containing JP-8). However, particle nucleation/growth for blended fuel combustion is enhanced relative to JP-8, despite the lower sulfur content of the FT/JP-8 fuel blend. A computational model explains the unexpected particle formation result primarily as the effect of much lower soot emissions present in blended fuel combustion exhaust compared to JP-8. Fuel composition, specifically aromatic and sulfur content, affect all aspects of emissions performance and the effect of simultaneously reducing aromatic and sulfur content can lead to surprising behavior.
Abstract. The use of alternative fuels for aviation is likely to increase due to concerns over fuel security, price stability, and the sustainability of fuel sources. Concurrent reductions in particulate emissions from these alternative fuels are expected because of changes in fuel composition including reduced sulfur and aromatic content. The NASA Alternative Aviation Fuel Experiment (AAFEX) was conducted in January–February 2009 to investigate the effects of synthetic fuels on gas-phase and particulate emissions. Standard petroleum JP-8 fuel, pure synthetic fuels produced from natural gas and coal feedstocks using the Fischer–Tropsch (FT) process, and 50% blends of both fuels were tested in the CFM-56 engines on a DC-8 aircraft. To examine plume chemistry and particle evolution with time, samples were drawn from inlet probes positioned 1, 30, and 145 m downstream of the aircraft engines. No significant alteration to engine performance was measured when burning the alternative fuels. However, leaks in the aircraft fuel system were detected when operated with the pure FT fuels as a result of the absence of aromatic compounds in the fuel. Dramatic reductions in soot emissions were measured for both the pure FT fuels (reductions in mass of 86% averaged over all powers) and blended fuels (66%) relative to the JP-8 baseline with the largest reductions at idle conditions. At 7% power, this corresponds to a reduction from 7.6 mg kg−1 for JP-8 to 1.2 mg kg−1 for the natural gas FT fuel. At full power, soot emissions were reduced from 103 to 24 mg kg−1 (JP-8 and natural gas FT, respectively). The alternative fuels also produced smaller soot (e.g., at 85% power, volume mean diameters were reduced from 78 nm for JP-8 to 51 nm for the natural gas FT fuel), which may reduce their ability to act as cloud condensation nuclei (CCN). The reductions in particulate emissions are expected for all alternative fuels with similar reductions in fuel sulfur and aromatic content regardless of the feedstock. As the plume cools downwind of the engine, nucleation-mode aerosols form. For the pure FT fuels, reductions (94% averaged over all powers) in downwind particle number emissions were similar to those measured at the exhaust plane (84%). However, the blended fuels had less of a reduction (reductions of 30–44%) than initially measured (64%). The likely explanation is that the reduced soot emissions in the blended fuel exhaust plume results in promotion of new particle formation microphysics, rather than coating on pre-existing soot particles, which is dominant in the JP-8 exhaust plume. Downwind particle volume emissions were reduced for both the pure (79 and 86% reductions) and blended FT fuels (36 and 46%) due to the large reductions in soot emissions. In addition, the alternative fuels had reduced particulate sulfate production (near zero for FT fuels) due to decreased fuel sulfur content. To study the formation of volatile aerosols (defined as any aerosol formed as the plume ages) in more detail, tests were performed at varying ambient temperatures (−4 to 20 °C). At idle, particle number and volume emissions were reduced linearly with increasing ambient temperature, with best fit slopes corresponding to −8 × 1014 particles (kg fuel)−1 °C−1 for particle number emissions and −10 mm3 (kg fuel)−1 °C−1 for particle volume emissions. The temperature dependency of aerosol formation can have large effects on local air quality surrounding airports in cold regions. Aircraft-produced aerosols in these regions will be much larger than levels expected based solely on measurements made directly at the engine exit plane. The majority (90% at idle) of the volatile aerosol mass formed as nucleation-mode aerosols, with a smaller fraction as a soot coating. Conversion efficiencies of up to 2.8% were measured for the partitioning of gas-phase precursors (unburned hydrocarbons and SO2) to form volatile aerosols. Highest conversion efficiencies were measured at 45% power.
Supercritical water desulfurization (SCWDS) has potential as a technique for removing sulfur from feedstocks such as heavy oil and bitumen. However, a fundamental understanding of SCWDS (such as the underlying chemical mechanisms, relative rates of desulfurization, and the role of SCW and hydrocarbons) is limited. In the present work, we have gained molecular-level insights into this process by measuring the kinetics of decomposition of a variety of organic sulfides in the presence of hydrocarbons and supercritical water in a continuously fed stirred-tank reactor (CSTR). The results are consistent with a free-radical mechanism, with hydrogen abstraction from the sulfide as the rate-determining step. The decomposition rates of the aliphatic and aromatic sulfides varied depending on their molecular structure, with conversions after 31 min at 400 °C ranging from less than 3% (our detection limits) to more than 90%. These differences in the reactivity correlate with the estimated heats of reaction for the critical hydrogen abstraction. The decomposition rates of the sulfides were affected by the presence of hydrocarbon carriers, with the rates being higher in the presence of alkanes than in the presence of toluene, as expected for a free-radical process. Product distributions and rates of radical-induced alkane cracking during this process were likewise affected by the presence of different sulfides. The decomposition of several different sulfides is consistent with 3 / 2 power kinetics, providing further evidence that the reaction proceeds via a radical mechanism. The knowledge developed in the current work provides a fundamental basis for further improvements in SCWDS.
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