The spatial distributions, fluxes, and environmental effects of non-methane hydrocarbons (NMHCs) were investigated in the Yellow Sea (YS) and the East China Sea (ECS) in spring. The average concentrations of ethane, propane, i-/n-butane, ethylene, propylene and isoprene in the seawater were 18.1 ± 6.4, 15.4 ± 4.7, 6.8 ± 2.9, 6.4 ± 3.2, 67.1 ± 26.7, 20.5 ± 8.7 and 17.1 ± 11.1 pmol L⁻¹, respectively. The alkenes in the surface seawater were more abundant than their saturated homologs and NMHCs concentrations (with the exception of isoprene) decreased with carbon number. The spatial variations of isoprene were consistent with the distributions of chlorophyll a (Chl-a) and Chaetoceros, Skeletonema, Nitzschia mainly contributed to the production of isoprene, while the others’ distributions might be related to their photochemical production. Observations in atmospheric NMHCs indicated alkanes in the marine atmosphere decreased from inshore to offshore due to influence of the continental emissions, while alkenes were largely derived from the oceanic source. In addition, no apparent diurnal discrepancy of atmospheric NMHCs (except for isoprene) were found between daytime and night. As the main sink of NMHCs in seawater, the average sea-to-air fluxes of ethane, propane, i-/n-butane, ethylene and propylene were 31.70, 29.75, 18.49, 15.89, 239.6, 67.94 and 52.41 nmol m⁻² d⁻¹, respectively. The average annual emissions of isoprene accounted for 0.1–1.3% of the global ocean emissions, which indicated that the coastal and shelf areas might be significant sources of isoprene. Furthermore, this study represents the first effort to estimate the environmental effects caused by NMHCs over the YS and the ECS and the results demonstrated contributions of alkanes to ozone and secondary organic aerosol (SOA) formation were lower than those of the alkenes and the largest contributor was isoprene.

Mercury (Hg) is among contaminants of public concern due to its prevalent existence, high toxicity, and bioaccumulation through food chains. Elevated Hg has been detected in seafood from the East China Sea (ECS), which is one of the largest marginal seas and an important fishing region in the northwestern Pacific Ocean. However, there is still a lack of knowledge on the distribution of Hg species and their controlling factors in the ECS water column, thus preventing the understanding of Hg cycling and the assessment of Hg risks in the ECS. In this study, two cruises were conducted in October 2014 and June 2015 in order to investigate the distribution of total Hg (THg) and methylmercury (MeHg) and their controlling factors in the ECS. The concentrations of THg and MeHg were determined to be 4.2 ± 2.8 ng/L (THg) and 0.25 ± 0.13 ng/L (MeHg) in water from the ECS. The level of Hg in the ECS occupied the higher rank among the marginal seas, thus indicating significant Hg contamination in this system. Both the THg and MeHg presented complicated spatial distribution patterns in the ECS, with high concentration areas located in both the nearshore and offshore areas. Statistical analyses suggest that temperature (T) and Hg in sediment may be the controlling factors for THg distribution, while dissolved organic matter (DOM), T, and MeHg in the sediment may be the controlling factors for MeHg distribution in the seawater of the ECS. The relative importance of these environmental factors in Hg distribution depends on the water depth. T-salinity (S) diagram analyses showed that water mass mixing may also play an important role in controlling THg and MeHg distribution in the coastal ECS.

The effects of mariculture on mercury (Hg) contamination and speciation in water, sediment and cultured fish in a typical mariculture zone located in Xiangshan bay, Zhejiang province, east China, were studied. Water, sediment and fish samples were collected from mariculture sites (MS) and from corresponding reference sites (RS) 2500 m away from the MS. The THg concentration in overlying water in Xiangshan bay reached as high as 16.6 ± 19.5 ng L−1, indicating that anthropogenic sources in this bay may contribution on Hg contamination in overlying water. Mariculture activities resulted in an increase in THg concentration in water from surface and bottom layers, which may be attributed to the discharge of domestic sewage and the accumulation of unconsumed fish feed and fish excreta in the benthic environment. Methylmercury (MeHg) concentrations in the bottom layer of overlying water and top surface layer of porewater underneath MS were higher than at RS, implying that mariculture activities promote Hg methylation in the interface between sediments and water. In addition, the concentrations of MeHg in sediment and porewater were significantly higher in summer than winter. It was observed that THg and MeHg contents in the muscle of blackhead seabream (Acanthopagrus schlegelii) (fed by the trash fish) were significantly higher (p < 0.001) than those in red snapper (Lutjanus campechanus) or perch (Perca fluviatilis) (fed by pellet fish feed). The THg and MeHg concentrations in the fish meat were closely related to the feeding mode, which indicate that fish feed rather than environmental media is the major pathway for Hg accumulation in fish muscle.

Two oceanographic cruises were carried out in the East China Sea (ECS) during the summer and fall of 2013. The main objectives of this study are to identify the spatial-temporal distributions of gaseous elemental mercury (GEM) in air and dissolved gaseous mercury (DGM) in surface seawater, and then to estimate the Hg0 flux. The GEM concentration was lower in summer (1.61 ± 0.32 ng m−3) than in fall (2.20 ± 0.58 ng m−3). The back-trajectory analysis revealed that the air masses with high GEM levels during fall largely originated from the land, while the air masses with low GEM levels during summer primarily originated from ocean. The spatial distribution patterns of total Hg (THg), fluorescence, and turbidity were consistent with the pattern of DGM with high levels in the nearshore area and low levels in the open sea. Additionally, the levels of percentage of DGM to THg (%DGM) were higher in the open sea than in the nearshore area, which was consistent with the previous studies. The THg concentration in fall was higher (1.47 ± 0.51 ng l−1) than those of other open oceans. The DGM concentration (60.1 ± 17.6 pg l−1) and Hg0 flux (4.6 ± 3.6 ng m−2 h−1) in summer were higher than those in fall (DGM: 49.6 ± 12.5 pg l−1 and Hg0 flux: 3.6 ± 2.8 ng m−2 h−1). The emission flux of Hg0 from the ECS was estimated to be 27.6 tons yr−1, accounting for ∼0.98% of the global Hg oceanic evasion though the ECS only accounts for ∼0.21% of global ocean area, indicating that the ECS plays an important role in the oceanic Hg cycle.

The level of phthalate esters (PAEs) alone is not considered to be a sufficient indicator of PAE pollution due to the quick metabolism of PAEs in the biota. The primary metabolites of PAEs, monoalkyl phthalate esters (MPEs), may also be an important indicator. However, PAE metabolism has scarcely been documented in wild marine organisms. We analysed five PAEs [dimethyl phthalate (DMP), diethyl phthalate (DEP), di-n-butyl phthalate (DBP), di(2-ethylhexyl) phthalate (DEHP), and di-n-octyl phthalate (DNOP)] and their corresponding MPEs [mono-methyl phthalate (MMP), mono-ethyl phthalate (MEP), mono-n-butyl phthalate (MBP), mono-2-ethylhexyl phthalate (MEHP), and mono-n-octyl phthalate (MNOP)] in 95 wild aquatic marine samples (including fish, prawns and molluscs) collected from the Yangtze River Delta area of the East China Sea. The species-dependent distribution of these compounds was associated with the food habits, living patterns and trophic levels of the biota. Slightly higher levels of hydrophobic PAEs (DBP and DEHP, logKOW 4.27 and 7.33, respectively) were observed in fish species consuming benthic organisms or in demersal fish species, suggesting the importance of benthic organisms and sediment. Trophic dilution of both PAEs and MPEs implies further metabolic transformation at higher trophic levels. MPE tissue distributions in fish demonstrate that the highest concentrations were always observed in bile. Metabolism via the kidney and gill is a probable main way for the relatively less hydrophobic MPEs (logKOW = <4.73, from MMP to MEHP), whereas metabolism via the liver is likely the main way for the most hydrophobic MNOP (logKOW 5.22). Generally, higher detection frequencies of MPEs were observed than those of parent PAEs. Significant liner correlations were observed between the levels of short-branched (carbon atom per chain = <4) MPEs and the sum of PAEs and MPEs (n = 95, p < 0.01), demonstrating that short-branched MPEs can be used as biomarkers of exposure to quantitatively reflect parent PAE contamination in wild marine organisms.

Sediment samples (n = 20) were collected from Yangtze River Estuary (YRE) and the adjacent East China Sea (ECS) inner shelf to explore spatial and temporal distributions, environmental fate, sources and potential health risk of polybrominated diphenyl ethers (PBDEs). Concentrations of BDE-209 and total 7 PBDEs (without BDE-209; ∑7PBDEs) ranged from 62.3 to 1758 pg g−1 and from 36.9 to 233.6 pg g−1 dry weight, respectively; both of the highest values occurred near the city of Wenzhou. Concentrations of BDE-209 and ∑7PBDEs both indicated a decreasing trend from inshore areas toward outer shelf. Significantly positive linear correlations were only observed between logBDE-183 concentrations and TOC/grain size (r2 = 0.6734 and 0.5977 for TOC and grain size, respectively) as well as BDE-209 and TOC/grain size (r2 = 0.4137 and 0.5332 for TOC and grain size, respectively) in the north of 28°N, indicating that YR had significant influence on the distribution of higher brominated congeners only in the north part. Depth profiles of PBDEs in a sediment core P01 (n = 1, m = 11) collected from YRE showed that the input of BDE-209 gradually increased from 1930 to 2010, while the levels of ∑7PBDEs peaked in 1986 and obviously decreased in recent years. Partial Least-Squares Regression (PLSR) revealed that PBDEs in the coastal ECS were mainly from direct discharge of local anthropogenic activities (80.7%), followed by surface runoff of contaminated soils (15.1%), microbial degradation after sedimentation (2.6%) and photodegradation during atmospheric transportation (1.6%). The cancer risk of human exposure to BDE-209 at the 95% confidence level was 3.09 × 10−7, 1.67 × 10−7 and 8.86 × 10−7 for children, teens and adults, respectively, significantly lower than the threshold level (10−6). Hazard index (HI) calculated for non-cancer risk was also far less than 1 for the three groups, suggesting no non-cancer risk.

Understanding the evolution of aerosols in the atmosphere is of great importance for improving air quality and reducing aerosol-related uncertainties in global climate simulations. Here, a unique haze episode at a regional receptor site near the East China Sea was examined as a case study of the aging process of atmospheric aerosols during transport. An increase in photochemical age from 5 h to more than 25 h and a progressive increase in the fitted mean particle diameter from 70 nm to approximately 300 nm were observed. According to the pollution features and meteorology conditions involved, pollution accumulation (PA), sea breeze (SB), and land breeze (LB) periods were identified. Concentrations of black carbon (BC), hydrocarbon-like organic aerosols (HOA), semi-volatile oxidized organic aerosols (SV-OOA), and nitrate increased by 7-fold up to 39-fold when the air masses passed through Taizhou, a nearby city. In addition, nitrate and SV-OOA dominated the aerosol composition in the urban outflow plumes (52% and 18%, respectively), yet they gradually decreased in concentration during transport. In contrast, sulfate and the low-volatile oxidized organic aerosols (LV-OOA) exhibited more regional footprints and potentially have similar formation mechanisms. The atomic oxygen-to-carbon (O/C) ratio also increased from 0.45 to 0.9, thereby suggesting that rapid formation of highly oxidized secondary organic aerosols (SOA) occurred during transport. Overall, these results provide valuable insight into the evolution of the chemical and physical features of aerosol pollution during transport and also highlight the need for regulatory controls of nitrogen oxides, sulfur dioxide, and VOCs to improve air quality on different scales.

Historical records of polycyclic aromatic hydrocarbons (PAHs), organochlorine pesticides (OCPs) and polychlorinated biphenyls (PCBs) were analyzed in two dated sediment cores (DH05 and DH11) collected from the continental shelf of the East China Sea (ECS) to investigate the influence of anthropogenic activities on marine sediment over the past century. The concentrations and fluxes of 15 PAHs were in the range of 28.6–96.5 ng g−1 and 7.6–35.2 ng cm−2 yr−1 in DH05 (1920s–2009), 18.8–76.4 ng g−1 and 13.9–30.9 ng cm−2 yr−1 in DH11 (1860s–2009). The sedimentary records of PAHs in the two cores generally reflected the economic development and energy consumption change in China. Identification of sources suggested that PAHs in ECS were predominantly from petrogenic origin and various combustion sources. A change of source from low- and moderate-temperature combustion to high-temperature combustion process was observed. Although a production ban of technical HCH and DDT was imposed in China in 1983, their sedimentary fluxes display increasing trends or strong rebounds from 1980s to 1990s as recorded in the core profiles. High proportions of DDD + DDE and γ-HCH suggested those OCPs mainly derived from early residuals. Temporal trends of PCBs presented relative high levels from 1970s to 1980s and high proportions of PCB congeners with 3–6 chlorines atoms indicated industrial sources.

Hydroxylated (OH-) and methoxylated (MeO-) polybrominated diphenyl ethers (PBDEs) have caused much concern because of their potential toxicity and worldwide distribution. These compounds are recently suggested to originate from the natural process in the ocean. However, their source remains highly controversial. In this study, we analyzed the contents of nine MeO-BDEs, ten OH-BDEs, and phytoplankton biomarkers (PBs) in two sediment cores collected from the East China Sea (ECS). The detection of 6-MeO-BDE-47, 2′-MeO-BDE-68, and 6-OH-BDE-47 have been reported since the 1920s, prior to the production of PBDEs. Significant relations were found between MeO/OH-BDEs and indicators of marine organic matters. The similar down-core variations and significant correlations between MeO/OH-BDEs and PBs suggest the possibility that phytoplankton produced these natural compounds. Laboratory incubation further demonstrates that phytoplankton can produce MeO-BDEs. Comparisons between the content ratios of 6-MeO-BDE-47/2′-MeO-BDE-68 and brassicasterol/dinosterol indicate that the signature of MeO-BDEs is controlled by the phytoplankton community structure.

Carbon monoxide (CO) emissions in China in 2005–2010 were estimated by inversion, using the Green's function method from vertical CO profiles derived from MOPITT Version 5 satellite data and a tagged CO simulation, and validated with independent in situ observations from the World Data Centre for Greenhouse Gases. Modeling with a posteriori emission successfully reproduced CO outflow from the continent to the East China Sea, Sea of Japan, and Japanese islands during winter and spring, and compensated for underestimates in central and eastern China in summer. A posteriori emissions showed large seasonal variations in which December and March emissions were on average 23% larger than August emissions, consistent with other studies. Estimated Chinese CO emissions were 184.4, 173.1, 184.6, 158.4, 157.4, and 157.3 Tg/year for 2005–2010, respectively. The decrease after 2007 is partly attributed to Chinese socioeconomic conditions and improved combustion efficiency.