Brown and Black Carbon Emitted by a Marine Engine Operated on Heavy Fuel Oil and Distillate Fuels: Optical Properties, Size Distributions, and Emission Factors

Abstract

We characterized the chemical composition and optical properties of particulate matter (PM) emitted by a marine diesel engine operated on heavy fuel oil (HFO), marine gas oil (MGO), and diesel fuel (DF). For all three fuels, ∼80% of submicron PM was organic (and sulfate, for HFO at higher engine loads). Emission factors varied only slightly with engine load. Refractory black carbon (rBC) particles were not thickly coated for any fuel; rBC was therefore externally mixed from organic and sulfate PM. For MGO and DF PM, rBC particles were lognormally distributed in size (mode at drBC≈120 nm). For HFO, much larger rBC particles were present. Combining the rBC mass concentrations with in situ absorption measurements yielded an rBC mass absorption coefficient MACBC,780nm of 7.8 ± 1.8 m2/g at 780 nm for all three fuels. Using positive deviations of the absorption Ångström exponent (AAE) from unity to define brown carbon (brC), we found that brC absorption was negligible for MGO or DF PM (AAE(370,880 nm)≈1.0 ± 0.1) but typically 50% of total 370‐nm absorption for HFO PM. Even at 590 nm, ∼20 of the total absorption was due to brC. Using absorption at 880 nm as a reference for BC absorption and normalizing to organic PM mass, we obtained a MACOM,370nm of 0.4 m2/g at typical operating conditions. Furthermore, we calculated an imaginary refractive index of (0.045 ± 0.025)(λ/370nm)−3 for HFO PM at 370 nm>λ > 660 nm, more than twofold greater than previous recommendations. Climate models should account for this substantial brC absorption in HFO PM.