Measurement report: Vanadium-containing ship exhaust particles detected in and above the marine boundary layer in the remote atmosphere

Abstract. Each year, commercial ships emit over 1.2 Tg of particulate matter (PM) pollution into the atmosphere. These ships rely on the combustion of heavy fuel oil, which contains high levels of sulfur, large aromatic organic compounds, and metals. Vanadium is one of the metals most commonly associated with heavy fuel oil and is often used as a tracer for PM from ship exhaust. Previous studies have suggested that vanadium-containing PM has impacts on human health and climate due to its toxicological and cloud formation properties, respectively; however, its distribution in the atmosphere is not fully understood, which limits our ability to quantify the environmental implications of PM emitted by ships. Here, we present data obtained from Particle Analysis by Laser Mass Spectrometry (PALMS) instrument on the NASA DC-8 aircraft during the 2016–2018 Atmospheric Tomography Mission (ATom) and show that ~1 % of the accumulation mode particles measured in the marine boundary layer of the central Pacific and Atlantic Ocean contain vanadium. These measurements, which were made without targeting ship plumes, suggest that PM emitted by ships is widespread in the atmosphere. Furthermore, we observed vanadium-containing ship exhaust particles at altitudes up to 13 km, which demonstrates that not all ship exhaust particles are immediately removed via wet deposition processes. In addition, using laboratory calibrations, we determined that most vanadium-containing ship exhaust particles can contain up to a few wt % vanadium. This study furthers our understanding of both the chemical composition and distribution of PM emitted by ships, which will allow us to better constrain the climate, health, and air quality implications of these particle types in the future.