Modifications on the coastal atmospheric sulfur and cloud condensation nuclei along the Eastern China seas by shipping fuel transition.

Marine fuel combustion from shipping releases SO2 and forms sulfate particles, which may alter low cloud characteristics. A series of strategies were implemented to control the sulfur content of ship fuel oil from 2018 to 2020, offering insights into the effects of the ship fuel oil transition on sulfur-related pollutants and the consequent cloud condensation nuclei (CCN) in the atmosphere. Compared to 2018 in the southeast China waters, shipping SO2 emission decreased by 78 % in 2020, resulting in a 76 % reduction in ship-related total sulfur concentration, and a decrease of 54 % in CCN number concentration under supersaturation 0.2 % (CCN0.2) contributed by shipping. The response of CCN0.2 to ship-related sulfate modification is more pronounced in relatively clean environments than polluted environments, highlighting the uneven changes in coastal CCN along the Eastern China Sea induced by the ship fuel policies. CCN can trigger the formation of cloud droplets, 2020 fuel regulation may have and will reduce the cooling radiative forcing effect with strong spatial heterogeneity. The study provides insights into the variations in coastal atmospheric sulfur-related pollutants and CCN in uneven response to changes in ship fuel oil, prompting the need for further comprehensive assessments of the climate effects resulting from potential shifts in ship fuel use in the future.

On-board measurements of OC/EC ratio, mixing state, and light absorption of ship-emitted particles.

Carbonaceous aerosols play important roles in environmental impacts and climate effects. The characteristics of ship-emitted carbonaceous aerosols keep unclear under the latest global low sulfur fuel oil policy. This study selected four ocean-going vessels burning low sulfur fuel oils for on-board exhaust testing. The emission factors of ship carbonaceous aerosols were obtained under different engine types (main and auxiliary engines), fuel types, and engine loads. Our results showed that fuel and engine types were both important factors affecting carbonaceous aerosol emissions for ship engines. The emission factors of OC and EC from main engines were 1.18 ± 0.62 and 0.06 ± 0.04 g/kg burning heavy fuel oil (HFO), while 0.52 ± 0.35 and 0.04 ± 0.03 g/kg burning marine gas oil (MGO), respectively. The OC/EC ratios of ship-emitted particles were within a large range of 2 to 23. The OC/EC ratios from the main engines were significantly higher than those from the auxiliary engines by a factor of 6.3. The result of chemical mixing states of ship-emitted particles observed by a single particle mass spectrometer (SPAMS) showed that OC and EC were internally mixed and existed as the ECOC-bonded forms in single particles. The measured light absorption of ship-emitted particles with higher OC/EC ratios showed an evident short-wave absorption enhancement based on the aethalometer AE-33. Our results implied that ship-emitted carbonaceous aerosols (especially with high OC/EC ratios) could not be uniformly treated regarding the optical properties to more precisely estimate their potential environmental impacts and climate effects in model systems in the future.

[Pollution Characteristics and Source Analysis of Atmospheric PM2.5-bound Polycyclic Aromatic Hydrocarbons in a Port Area].

In order to explore the pollution characteristics and potential sources of polycyclic aromatic hydrocarbons (PAHs) in the polluted air of a port area, PM2.5 samples (n=59) were collected from Qingdao Port for four seasons from August 2018 to May 2019. The seasonal variation and composition characteristics of PM2.5-bound PAHs were analyzed, the influence of meteorological factors on PAH concentrations was explored using correlation analysis, and the potential sources were analyzed using positive definite matrix factorization and potential source contribution function models. The results showed that the total mean concentration of PAHs was (8.11±12.31) ng·m-3, which was higher in autumn and winter than that in spring and summer. The seasonal molecular compositions of PAHs were similar, dominated by 4-5 ring PAHs (75.43%). Fluoranthene, benzo[e]pyrene, benzo[a]anthracene, phenanthrene, pyrene, and chrysene were the dominant species of PAHs in the study area, which are similar to the major compounds in ship exhaust. Correlation analysis showed that PAH concentrations were significantly negatively correlated with temperature and relative humidity and significantly positively correlated with atmospheric pressure and wind direction and had a poor correlation with wind speed. PMF analysis extracted six contribution factors, and the results indicated that Qingdao Port was mainly influenced by shipping emissions (28.83%), followed by vehicle emissions (20.49%), as well as crude oil volatilization (13.47%). Summer had the greatest impact on shipping emissions. The PSCF results suggested that Beijing-Tianjin-Hebei, Bohai Rim, and northern Shandong were the main source regions for long-range transport.

Source appointment of PM2.5 in Qingdao Port, East of China.

Field measurements were conducted near Qingdao Port to characterize the particulate air pollutants, assess the spatial and seasonal characteristics of the pollutants, and identify the contribution from ship traffic emissions. By utilizing multiple statistical methods and data collected at two sites in Qingdao, we comprehensively explored the PM2.5 seasonal characteristics and source apportionments of different PM2.5 constituents, especially those originating from ship emissions, and identified potential source regions for samples collected in Qingdao. In this study, 118 concurrent daily PM2.5 samples were collected from August 2018 to May 2019 at a port site (QH) and a coastal background site (BG). Vanadium (V) and Nickel (Ni) are the dominant metal elements from crude oil and crude oil combustion emissions. The significant correlations between V and Ni at both sampling sites, indicating that shipping emissions have a significant impact on the port and background area. Additionally, Ni and other metals showed significant correlations at the BG site, implying Ni also emission from the land-based oil at this site. The positive matrix factorization (PMF) model identified six main sources for the PM2.5 samples in Qingdao, and they are coal combustion, industrial emissions/mineral dust, marine vessel emissions, secondary aerosols/biomass burning, sea salt/crustal emissions, and vehicle exhaust, respectively. Marine vessel emissions were the dominant contributor to PM2.5 in Qingdao during the sampling periods (25.05%). The potential source contribution function (PSCF) analysis suggested that the Yellow Sea and Jiaodong Peninsula were the major sources regions for PM2.5 in Qingdao. The Yellow Sea and Bohai Sea were the potential source regions for shipping emissions in Qingdao. Therefore, efforts to control shipping emissions should be strengthened not only at the Qingdao Port but also in surrounding ports.

PM2.5-bound polycyclic aromatic hydrocarbons (PAHs) and their derivatives (nitrated-PAHs and oxygenated-PAHs) in a road tunnel located in Qingdao, China: Characteristics, sources and emission factors.

Daytime and nighttime PM2.5 samples were collected at a road tunnel located in Qingdao, China. The mass concentrations and chemical compositions of polycyclic aromatic hydrocarbons (PAHs), nitrated PAHs (NPAHs) and oxygenated-PAHs (OPAHs) were analysed to determine the variation characteristics and sources. The concentrations in exit were obviously higher than those of entrance in the tunnel. Fluoranthene (FLT) and Pyrene (PYR) were the most abundant PAHs, 2 + 3-nitrofluoranthene (2 + 3N-FLA), 1-nitropyrene (1N-PYR) and 2-nitropyrene (2N-PYR) were the dominant NPAHs, and 9-fluorenone (9-FO) and 9,10-anthraquinone (9,10-ANQ) were the most abundant OPAHs. The high rings (4-6 rings) PAHs accounted for over 90% of the total PM2.5-bound PAH concentrations, most of which were considered as motor vehicle emissions. Based on the diagnostics ratios and PCA results, the most important sources of PAHs and NPAHs were estimated as gasoline and diesel vehicles emissions in the tunnel. In addition, non-exhausts (such as road dust, brake line, asphalt and tires wear) also had some contributions to PAHs and NPAHs. The average emission factors were 60.98, 9.02 and 8.47 µg veh-1 km-1 for total PM2.5-bound PAHs, NPAHs and OPAHs, respectively. The emission factors of high rings (4-6 rings) PAHs were greater than those with low rings (2-3 rings). 1N-PYR had the highest emission factor in all measured NPAHs, while the emission factors for the two highest OPAHs were 9-FO and 9,10-ANQ in this tunnel.

[Characteristics of Atmospheric PM2.5 Pollution and Its Influence on Visibility in Background Areas of Ji'nan].

In order to study the seasonal variations in the chemical composition of atmospheric particulate matter with diameters less than 2.5 µm (PM2.5) and its influence on visibility in background areas, atmospheric PM2.5 samples were collected in spring, summer, autumn, and winter 2016 at Qixingtai in Ji'nan. The pollution characteristics of water-soluble ions components, organic carbon (OC), and elemental carbon (EC) were analyzed, and their regional transmission contributions were studied. The results show that NH4+, SO42-, and NO3- were the main components of water-soluble ions, accounting for 90.24% of the annual total ion concentration. The secondary water soluble inorganic ions were polluted severely. NO3-/SO42- presented obvious seasonal variations of high (low) levels in winter (summer). In each season, SO42- and NH4+ existed mainly in the form of (NH4)2SO4. The value of secondary OC (SOC)/OC ranged from 21.17% to 54.21%, indicating the presence of relatively severe secondary organic pollution in this area. The sulfur oxidation ratio (SOR) value in all seasons was greater than 0.1, indicating that the secondary generation of SO42- occurs in all seasons in this region, and the value of nitrogen oxidation ratio (NOR) in all seasons was higher than the SOR value. The secondary transformation of NO2 in the Qixingtai region was stronger than that of SO2. The range of atmospheric extinction coefficient (Bext) was 172.68-320.61 Mm-1, with an annual mean of 256.48 Mm-1. The atmospheric extinction coefficient showed an obvious seasonal trend of the lowest (highest) in summer (winter). The backward airflow trajectory shows that the Qixingtai was affected mainly by the long-distance transmission from Northwest China and the ocean in spring and summer and by local sources in autumn and winter. A comparison of the characteristics of atmospheric PM2.5 pollution in Ji'nan in 2008 revealed that the influence of motor vehicles on the atmospheric environment has been significantly improved.