Measurement report: Characterization of uncertainties in fluxes and fuel sulfur content from ship emissions in the Baltic Sea

• Published in: Atmospheric chemistry and physics 2021-12, Vol.21 (24), p.18175-18194
• Main Authors: Walden, Jari, Pirjola, Liisa, Laurila, Tuomas, Hatakka, Juha, Pettersson, Heidi, Walden, Tuomas, Jalkanen, Jukka-Pekka, Nordlund, Harri, Truuts, Toivo, Meretoja, Miika, Kahma, Kimmo K
• Format: Article
• Language: English
• Subjects: Air-sea flux; Analysis; Boundary layers; Carbon dioxide; Chemical compounds; Computation; Deposition; Eddy covariance; Emissions; Environmental aspects; Fluid dynamics; Fluid flow; Fluxes; Friction; Fuels; Gases; Mathematical models; Measurement; Measuring instruments; Methods; Nanoparticles; Nitrogen; Nitrogen compounds; Oceans; Oxides; Pollutants; Ship routeing; Ships; Sulfur; Sulfur compounds; Sulfur content; Sulphur; Uncertainty; Velocity; Wind speed
• ISSN: 1680-7324; 1680-7316; 1680-7324
• DOI: 10.5194/acp-21-18175-2021

Fluxes of gaseous compounds and nanoparticles were studied using micrometeorological methods at Harmaja in the Baltic Sea. The measurement site was situated beside the ship route to and from the city of Helsinki. The gradient (GR) method was used to measure fluxes of SO2, NO, NO2, O3, CO2, and Ntot (the number concentration of nanoparticles). In addition, the flux of CO2 was also measured using the eddy-covariance (EC) method. Distortion of the flow field caused by obstacles around the measurement mast was studied by applying a computation fluid dynamic (CFD) model. This was used to establish the corresponding heights in the undisturbed stream. The wind speed and the turbulent parameters at each of the established heights were then recalculated for the gradient model. The effect of waves on the boundary layer was taken into consideration, as the Monin–Obukhov theory used to calculate the fluxes is not valid in the presence of swell. Uncertainty budgets for the measurement systems were constructed to judge the reliability of the results. No clear fluxes across the air–sea nor the sea–air interface were observed for SO2, NO, NO2, NOx (= NO + NO2), O3, or CO2 using the GR method. A negative flux was observed for Ntot, with a median value of -0.23×109 m−2 s−1 and an uncertainty range of 31 %–41 %. For CO2, while both positive and negative fluxes were observed, the median value was −0.081 µmol m−2 s−1 with an uncertainty range of 30 %–60 % for the EC methods. Ship emissions were responsible for the deposition of Ntot, while they had a minor effect on CO2 deposition. The fuel sulfur content (FSC) of the marine fuel used in ships passing the site was determined from the observed ratio of the SO2 and CO2 concentrations. A typical value of 0.40±0.06 % was obtained for the FSC, which is in compliance with the contemporary FSC limit value of 1 % in the Baltic Sea area at the time of measurements. The method to estimate the uncertainty in the FSC was found to be accurate enough for use with the latest regulations, 0.1 % (Baltic Sea area) and 0.5 % (global oceans).