Stable carbon isotope reveals high impact of fishing ship activities on total carbon from PM2.5 in Qingdao, China

Although total carbon (TC) is an important component of fine particulate matter (PM: particulate matter with aerodynamic diameter of <2.5 μm); its sources remain partially unidentified, especially in coastal urban areas. With ongoing development of the global economy and maritime activities, ship-generated TC emissions in port areas cannot be neglected. In this study, from September 11, 2017 to August 31, 2018, we collected 355 p.m. samples in Qingdao, China, to determine the water-soluble ion concentrations, TC concentrations, and stable carbon isotopes (δC). During the open fishing season (OFS; September 11, 2017 to April 30, 2018) and the closed fishing season (CFS; May 1, 2018 to August 31, 2018), the TC concentrations were 9.30 ± 5.38 μg/m and 3.36 ± 2.10 μg/m respectively, and the corresponding δC values were −24.53‰ ± 1.17‰ and −27.03‰ ± 0.91‰, respectively, indicating significant differences (p < 0.05) between the two periods. The differences in TC concentrations and the δC values between the OFS and CFS reflect changes in the source of contamination. Bayesian model was used to quantify the contributions of different TC sources, revealing that ship emissions accounted for approximately 35.3% of the total, which was close to the contribution from the largest source, i.e., motor vehicles (39%). Using the ship emission inventory, Qingdao's ship emissions were further quantified at 455 metric tons, representing 35%–40% of the total TC emissions around Qingdao. Notably, fishing ships contributed approximately 40% of the total ship emissions. These findings underscore the considerable impact of ship emissions, particularly those from fishing ships, on TC concentrations in coastal urban areas.