Increase in Agricultural-Derived NHx and Decrease in Coal Combustion-Derived NOx Result in Atmospheric Particulate N-NH4+ Surpassing N-NO3- in the South China Sea.

The atmospheric deposition of anthropogenic active nitrogen significantly influences marine primary productivity and contributes to eutrophication. The form of nitrogen deposition has been evolving annually, alongside changes in human activities. A disparity arises between observation results and simulation conclusions due to the limited field observation and research in the ocean. To address this gap, our study undertook three field cruises in the South China Sea in 2021, the largest marginal sea of China. The objective was to investigate the latest atmospheric particulate inorganic nitrogen deposition pattern and changes in nitrogen sources, employing nitrogen-stable isotopes of nitrate (δ15N-NO3-) and ammonia (δ15N-NH4+) linked to a mixing model. The findings reveal that the N-NH4+ deposition generally surpasses N-NO3- deposition, attributed to a decline in the level of NOx emission from coal combustion and an upswing in the level of NHx emission from agricultural sources. The disparity in deposition between N-NH4+ and N-NO3- intensifies from the coast to the offshore, establishing N-NH4+ as the primary contributor to oceanic nitrogen deposition, particularly in ocean background regions. Fertilizer (33 ± 21%) and livestock (20 ± 6%) emerge as the primary sources of N-NH4+. While coal combustion continues to be a significant contributor to marine atmospheric N-NO3-, its proportion has diminished to 22 (Northern Coast)-35% (background area) due to effective NOx emission controls by the countries surrounding the South China Sea, especially the Chinese Government. As coal combustion's contribution dwindles, the significance of vessel and marine biogenic emissions grows. The daytime higher atmospheric N-NO3- concentration and lower δ15N-NO3- compared with nighttime further underscore the substantial role of marine biogenic emissions.

Sources of the Elevating Polycyclic Aromatic Hydrocarbon Pollution in the Western South China Sea and Its Environmental Implications.

The environmental implications of polycyclic aromatic hydrocarbons (PAHs) caused by the vigorous development of offshore oil exploitation and shipping on the marine ecosystem are unclear. In this study, the PAH concentrations were systematically characterized in multiple environmental media (i.e., atmosphere, rainwater, seawater, and deep-sea sediments) in the western South China Sea (WSCS) for the first time to determine whether PAH pollution increased. The average ∑15PAHs (total concentration of 15 US EPA priority controlled PAHs excluding naphthalene) in the water of WSCS has increased and is higher than the majority of the oceans worldwide due to the synergistic influence of offshore oil extraction, shipping, and river input. The systematic model comparison confirms that the Ksoot-air model can more accurately reflect the gas-particle partitioning of PAHs in the atmosphere of the WSCS. We also found that the vertical migration of the elevating PAHs is accelerated by particulate matter, driving the migration of atmospheric PAHs to the ocean through dry and wet deposition, with 16% being contributed by the particle phase. The particulate matter sinking alters the PAH distribution in the water column and generates variation in source apportionment, while the contribution of PAHs loaded on them (>20%) to the total PAH reserves cannot be ignored as before. Hence, the ecological threat of PAHs increases by the oil drilling and shipping industry, and the driving force of particulate matter deserves continuous attention.

Spatiotemporal distribution and potential risks of antibiotics in coastal water of Beibu Gulf, South China Sea: Livestock and poultry emissions play essential effect.

Antibiotics have been the subject of much attention in recent years due to their widespread use and the potential ecological risks and resistance risks. In this study, we conducted an extensive survey of 19 antibiotics in a wide range of waters of the Beibu Gulf during summer and winter (154 samples). The total concentrations of the 19 antibiotics (Σ19ABs, ng/L) were significantly higher in winter (n.d.-364) than in summer (n.d.-70.1) and were mainly concentrated in areas of seagoing rivers (1.50-364). The primary route for antibiotics entering Beibu Gulf was through riverine input. Precisely, florfenicol (FF) (n.d.-278 ng/L) discharged from livestock and poultry farms upstream of Nanliu River, predominantly in swine farming, constitutes the main pollutant in Beibu Gulf throughout the year. The Nanliu River (988 kg/a) accounts for 85% of the gulf's total annual antibiotic emission flux. Source analysis identified livestock and poultry farming, particularly swine farming, as the primary pollution source, contributing 58% in summer. Risk assessment reveals that algae (0.51 ± 0.56) exhibited relatively high sensitivity to antibiotics, presenting a medium-high risk at specific sites in Nanliu River during winter. Additionally, FF discharged from swine farming demonstrates a certain level of antibiotic resistance risk. Therefore, reinforcing control measures for antibiotic discharges from livestock and poultry farming, especially upstream of Nanliu River, can effectively mitigate antibiotic-related risks in the water bodies of Beibu Gulf.

Occurrence, distribution, and sources of organophosphate esters (OPEs) in the air of the Indo-China Peninsula Based on a Passive Air Monitoring Network.

Organophosphate esters (OPEs) are a class of emerging and ubiquitous contaminants that are attracting increasing attention, and their large-scale use as flame retardants and plasticizers has led to their pervasive presence in the environment, although their broader impacts remain unknown. In this study, 11 OPEs were measured in the atmosphere of Southeast Asia and Southwest China during 2016. The ∑11OPEs were higher in this region (78.0-1670 pg/m3, mean 458 pg/m3) than in many remote areas, lower than in developed regions, and comparable to levels in many developing country cities. Generally, the ∑11OPEs were higher in urban (105-1670 pg/m3, mean 538 pg/m3) than in suburban (78.0-1350 pg/m3, mean 388 pg/m3). Seasonal variations of OPEs in the air were more pronounced in Cambodia and Laos, especially for Triphenyl Phosphate (TPHP). Seasonal variations of ∑11OPEs in most regions correspond to changes in temperature and rainfall. Biomass burning may be also a factor in facilitating OPE emissions from biomass materials or soil into the atmosphere of Southeast Asia. The random forest analysis showed that among these, rainfall had the greatest effect on the seasonal variation of atmospheric OPE concentrations, followed by biomass burning and temperature. The inter-regional variation of ∑11OPEs in Southeast Asia was related to population and economic development in each region. Airflow trajectories indicated that the OPEs in this region were mainly from local sources. The health risk assessment revealed that the inhalation exposure risks of OPEs to the residents in the study areas were very low during the sampling period, but may be increasing.

Distribution and adsorption-desorption of organophosphate esters from land to sea in the sediments of the Beibu Gulf, South China Sea: Impact of seagoing river input.

Organophosphate esters (OPEs) have been a class of emerging environmental contaminants. However, studies on their environmental behavior, specifically their adsorption-desorption behavior between sediment and seawater in estuarine and coastal areas, remain limited. To address this gap, our study focused on investigating the levels and behavior of 11 OPEs in sediment samples collected from the Beibu Gulf, South China Sea, encompassing estuaries and coastal regions. The total concentrations of 11 OPEs (Σ11OPEs) in the sediments exhibit a significant decrease in summer, both in seagoing rivers (4.67 ± 2.74 ng/g dw) and the coastal zone (5.11 ± 3.71 ng/g dw), compared to winter levels in seagoing rivers (8.26 ± 4.70 ng/g dw) and the coastal zone (7.71 ± 3.83 ng/g dw). Chlorinated OPEs dominated the sediments, constituting 63 %-76 % of the total. Particularly, port and mariculture areas showed the highest levels of OPEs. Through load estimation analysis, it was revealed that the sedimentary OPEs in Qinzhou Bay (221 ± 128 kg) had the highest load, with input from the Qin River identified as a significant source. Chlorinated OPEs showed a trend of desorption from sediments to the water column with increasing salinity, emphasizing the crucial role of land-based OPEs input through suspended particulate matter in rivers as a pathway to the ocean. The impact of strong flow in estuarine environments was highlighted, as it can scour sediments, generate suspended sediments, and release OPEs into the water bodies. Additionally, the results of the ecological risk assessment indicated that most of the OPEs posed low-risk levels. However, attention is warranted for the contamination levels of some chlorinated OPEs, emphasizing the need for ongoing monitoring and assessment.

Environmental fate and effects of PAHs in tropical mariculture ponds near the northern South China Sea: Rainfall plays a key role.

The behavior and fate of PAHs are affected by multiple meteorological factors, but the main factors driving PAHs in tropical mariculture areas are still not clearly understood. This study continuously monitored PAHs in a few tropical land-based mariculture ponds, discussed their dynamic change trend, migration among the multiple media, and the relevant affected factors. Results indicated that PAHs were widely distributed in these environmental media, and the PAHs' concentration showed an obvious attenuation trend in the mariculture cycle. Wet deposition brought overwhelming majority atmospheric PAHs (92 % ± 5.7 %) to the aqueous system, and >72 % of these PAHs came from oil combustion-related sources and biomass combustion. Compared with the natural sea areas in the same region, mariculture ponds sediment could be changed from a sink at the early stage to a secondary release source of PAHs at the late stage of the rainy season, which intensifies the bioaccumulation of PAHs and the risk of edible carcinogenesis of aquatic products. Our research revealed that rainfall drove the occurrence and environmental behavior of PAHs in the tropical mariculture areas, while land-based mariculture ponds ecosystem affected the regional environmental fate of PAHs and weakened their transmission to the marine environment from land.

Occurrence, distribution, source identification, and risk assessment of organophosphate esters in the coastal waters of Beibu Gulf, South China Sea: Impacts of riverine discharge and fishery.

As emerging pollutants, the environmental geochemistry of organophosphate esters (OPEs) in the coastal zone with multiple functional areas are still less recognized. This study investigated spatiotemporal distribution, sources and risks of 11 widely used OPEs in surface waters from seagoing rivers and multiple coastal functional areas of the Beibu Gulf. The results indicated that significantly higher ∑11OPEs (total concentrations of 11 OPEs, ng/L) occurred in summer (34.2-1227) than in winter (20.6-840), as a result of the high emission caused by climate reasons. In general, higher ∑11OPEs occurred in rivers (41.2-1227) than in the coast (34.2-809) in summer, especially in the urban rivers, while in winter, higher ∑11OPEs occurred in the coast (23.4-840 vs 20.6-319 in rivers) because of obviously higher ∑11OPEs in marine fishery areas (99-840). Source identification revealed that fishery activity, especially fishing vessels, and urban rivers were the main sources of OPEs in the Beibu Gulf. For the individual OPE, only tri-n-butyl phosphate (TNBP) may have ecological risks to aquatic organisms in a few sites, but if considering the additive effects, the OPEs mixtures would pose a high risk to algae and low to medium threats to crustaceans and fish.