Sewage sludge used as agricultural fertilizer has been identified as an important source of microplastics (MPs) to the environment. However, the fate of MPs added to agricultural soils is largely unknown. This study investigated the fate of MPs in agricultural soils amended with sewage sludge and the role of surface water runoff as a mechanism driving their transfer to aquatic ecosystems. This was assessed using three experimental plots located in a semi-arid area of Central Spain, which were planted with barley. The experimental plots received the following treatments: (1) control or no sludge application; (2) historical sludge application, five years prior to the experiment; and (3) sludge application at the beginning of the experiment. MPs were analyzed in surface water runoff and in different soil layers to investigate transport and infiltration for one year. The sewage sludge used in our experiment contained 5972–7771 MPs/kg dw. Based on this, we estimated that about 16,000 MPs were added to the agricultural plot amended with sludge. As expected, the sludge application significantly increased the MP concentration in soils. The control plot contained low MP concentrations (31–120 MPs kg⁻¹ dw), potentially originating from atmospheric deposition. The plot treated five years prior to the experiment contained 226–412 and 177–235 MPs kg⁻¹ dw at the start and end of the experiment, respectively; while the recently treated plot contained 182–231 and 138–288 MPs kg⁻¹ dw. Our study shows that MP concentrations remain relatively constant in agricultural soils and that the MP infiltration capacity is very low. Surface water runoff had a negligible influence on the export of MPs from agricultural soils, mobilizing only 0.2–0.4% of the MPs added with sludge. We conclude that, in semi-arid regions, agricultural soils can be considered as long-term accumulators of MPs.

High demands for but strict regulatory measures on Organophosphorus Flame Retardants (OPFRs) have resulted in mainland China transitioning from the region that imports OPRFs to one that exports these substances. Simultaneously, large quantities of terrigenous OPFRs have been exported to adjacent seas by the major river systems, particularly the Yangtze River. This study examined the presence of ten OPFRs in China's adjacent seas. High levels of OPFRs were observed in seas south of mainland China, with Tris (2-chloroethyl) phosphate (TCEP) and Tris (1,3-dichloro-2-propyl) phosphate (TDCPP) dominant. The terrigenous OPFRs were redistributed by the ocean surface currents, with OPFRs tending to accumulate in regions with lower current speed. The producers of OPFRs are mainly distributed along the Haihe, Yellow, and Yangtze river systems. The application of OPFRs to electric vehicle charging stations, charging connectors, and 5G infrastructure in the Chinese mainland will likely drive rapid growth in OPFR related industry in the future. The diffusion trend map of OPFR indicated that the Bohai Sea and the central northern Yellow Sea are at high risk of ecological damage in the spring. The offshore region of the north of the South China Sea tended to aggregate more OPFRs in summer. Regions of the OPFR aggregation effect were at a higher risk of ecological damage.

Copper export and mobility in acid mine drainage are difficult to understand with conventional approaches. Within this context, Cu isotopes could be a powerful tool and here we have examined the relative abundance of dissolved (<0.22 μm) Cu isotopes (δ⁶⁵Cu) in the Meca River which is an outlet of the Tharsis mine, one of the largest abandoned mines of the Iberian Pyrite Belt, Spain. We followed the chemical and isotopic composition of the upstream and downstream points of the catchment during a 24-h diel cycle. Additional δ⁶⁵Cu values were obtained from the tributary stream, suspended matter (>0.22 μm) and bed sediments samples. Our goals were to 1) assess Cu sources variability at the upstream point under contrasted hydrological conditions and 2) investigate the conservative vs. non conservative Cu behavior along a stream. Average δ⁶⁵Cu values varied from −0.47 to −0.08‰ (n = 9) upstream and from −0.63 to −0.31‰ downstream (n = 7) demonstrating that Cu isotopes are heterogeneous over the diel cycle and along the Meca River. During dry conditions, at the upstream point of the Meca River the Cu isotopic composition was heavier which is in agreement with the preferential release of heavy isotopes during the oxidative dissolution of primary sulfides. The more negative values obtained during high water flow are explained by the contribution of soil and waste deposit weathering. Finally, a comparison of upstream vs. downstream Cu isotope composition is consistent with a conservative behavior of Cu, and isotope mass balance calculations estimate that 87% of dissolved Cu detected downstream originate from the Tharsis mine outlet. These interpretations were supported by thermodynamic modelling and sediment characterization data (X-ray diffraction, Raman Spectroscopy). Overall, based on contrasted hydrological conditions (dry vs flooded), and taking the advantage of isotope insensitivity to dilution, the present work demonstrates the efficiency of using the Cu isotopes approach for tracing sources and processes in the AMD regions.

Riverine carbon (C) composition and export are closely related to changes in the coastal environment and climate. Excessive C inputs from rivers to seas and their subsequent decomposition could result in harmful algal blooms and ecosystem degradation in the coastal sea. In this study, we explored the C transportation and composition in the 24 major rivers of the Bohai Sea (BS) Rim based on the investigation of dissolved organic carbon (DOC), carbon stable isotopes (δ¹³CDOC) and chromophoric dissolved organic matter (CDOM). The results showed that the riverine DOC concentrations were high (10.6 ± 6.04 mg/L) in the BS Rim compared with the DOC levels in the main rivers in Eastern China (4.98 ± 2.45 mg/L). The δ¹³CDOC ranged from −28.29‰ to −25.32‰ in the rivers of the BS Rim, suggesting that the DOC mainly originated from riverine plankton, soil organic matter mainly induced by C3 plants, and sewage. The excitation-emission matrix fluorescence spectroscopy of the CDOM indicated that a soluble, microbial by product-like material accounted for the largest proportion (approximately 40%) of CDOM in these rivers and that CDOM mainly originated from autochthonous riverine sources with high protein-like components. The rivers in the BS Rim transported approximately 0.55 Tg C of DOC to the BS each year, with more than 70% of reactive C based on the CDOM composition. The DOC yields in terms of unit drainage area transported from the small rivers to the BS were higher compared to those of the larger rivers in the world, which indicated that the small rivers in the Bohai Rim could be an important source of the C in the BS. This study would enrich our understanding of environmental evolution in coastal areas with numerous small rivers.

Plastic pollution in the natural environment is causing increasing concern at both the local and global scale. Understanding the dispersion of plastic through the environment is of key importance for the effective implementation of preventive measures and cleanup strategies. Over the past few years, various models have been developed to estimate the transport of plastics in rivers, using limited plastic observations in river systems. However, there is a large discrepancy between the amount of plastic being modelled to leave the river systems, and the amount of plastic that has been found in the seas and oceans. Here, we investigate one of the possible causes of this mismatch by performing an extensive uncertainty analysis of the riverine plastic export estimates. We examine the uncertainty from the homogenisation of observations, model parameter uncertainty, and underlying assumptions in models. To this end, we use the to-date most complete time-series of macroplastic observations (macroplastics have been found to contain most of the plastic mass transported by rivers), coming from three European rivers. The results show that model structure and parameter uncertainty causes up to four orders of magnitude, while the homogenisation of plastic observations introduces an additional three orders of magnitude uncertainty in the estimates. Additionally, most global models assume that variations in the plastic flux are primarily driven by river discharge. However, we show that correlations between river discharge (and other environmental drivers) and the plastic flux are never above 0.5, and strongly vary between catchments. Overall, we conclude that the yearly plastic load in rivers remains poorly constrained.

Riverine nitrogen loading to the continental shelf sea is important for terrestrial–marine linkage and global nitrogen cycling and leads to serious marine environmental problems. The budget and cycle of riverine nitrogen over the continental shelf in the East China Sea (ECS) are unknown. Using the tracking technique within a physical–biological coupled model, we quantified the nitrogen budgets of riverine dissolved inorganic nitrogen (DIN) and particulate organic nitrogen (PON) over seasonal to annual scales in the ECS, especially from the Changjiang River, which plays a dominant role in riverine nitrogen input. The horizontal distributions of the Changjiang DIN and PON generally followed the Changjiang diluted water and coastal currents and were affected by stratification in the vertical direction. Their inventory variations were dominated by biological fluxes and modulated by physical ones, and changed most dramatically in the inner shelf among three subregions. Less than half of DIN were converted to PON with most of the rest leaving the ECS through lateral transport pathways, among which the flux through the Tsushima Strait was dominant. With the increasing loading of the Changjiang DIN flux from the 1980s–2010s, lateral transports rather than PON production increased due to limited primary production. Approximately 60 % of the produced PON exported to the sediment and 34 % went to the Tsushima Strait. According to the export production, the DIN from the Changjiang River contributed 12–42 % to the ECS carbon sequestration.

The atmospheric circulation plays a critical role in the global transport and deposition of atmospheric pollutants such as mercury (Hg). Desert dust emissions contribute to nearly 60–95% of the global dust budget and thus, desert dust may facilitate atmospheric Hg transport and deposition to the downwind regions worldwide. The role of desert dust in biogeochemical cycling of Hg, however, has not been well recognized by the Hg research community. In this study, we measured the concentration of particulate bound Hg (HgP) in total suspended particulate (TSP) collected from China’s largest desert, Taklimakan Desert, between 2013 and 2017. The results show that HgP concentrations over the Taklimakan Desert atmosphere are remarkably higher than those observed from background sites in China and are even comparable to those measured in most of the Chinese metropolitan cities. Moreover, HgP concentrations in the Taklimakan Desert exhibit a distinct seasonal pattern peaking during dust storm outbreak periods in spring and summer (March to August). A preliminary estimation demonstrates that export of total Hg associated with atmospheric dust from the Taklimakan Desert could be 59.7 ± 60.3 (1SD) Mg yr⁻¹. The unexpectedly high HgP concentrations during duststorms, together with consistent seasonal pattern of Hg revealed from the snow/ice, clearly demonstrate that Asian desert dust could act as a significant carrier of atmospheric Hg to the cryosphere of Western China and even can have further global reach.

Decabromodiphenyl ethane (DBDPE) is an alternative to the commercial decabromodiphenyl ether (deca-BDE) mixture but has potentially similar persistence, bioaccumulation potential and toxicity. While it is widely used as a flame retardant in electrical and electronic equipment (EEE) in China, DBDPE could be distributed globally on a large scale with the international trade of EEE emanating from China. Here, we performed a dynamic substance flow analysis to estimate the time-dependent mass flows, stocks and emissions of DBDPE in China, and the global spread of DBDPE originating in China through the international trade of EEE and e-waste. Our analysis indicates that, between 2006 and 2016, ∼230 thousand tonnes (kt) of DBDPE were produced in China; production, use and disposal activities led to the release of 196 tonnes of DBDPE to the environment. By the end of 2016, ∼152 kt of the DBDPE produced resided in in-use products across China. During the period 2000–2016, ∼39 kt of DBDPE were exported from China in EEE products, most of which (>50%) ended up in North America. Based on projected trends of China's DBDPE production, use and EEE exports, we predict that, by 2026, ∼74 and ∼14 kt of DBDPE originating in China will reside in in-use and waste stocks, respectively, in regions other than mainland China, which will act as long-term emission sources of DBDPE worldwide. This study discusses the considerable impact of DBDPE originating in China and distributed globally through the international trade of EEE; this is projected to occur on a large scale in the near future, which necessitates countermeasures.

Mercury (Hg) is a global toxic pollutant and has raised the world's attention for decades. In this study, we reviewed the fish mercury levels in China (both marine and freshwater, as well as wild and farmed) documented over the past decade and their controlling environmental and biological factors. China is the largest contributor of global Hg cycling and the largest nation for the consumption and export of fish and fish product, thus Hg level in fish becomes a critical issue for food safety and public health. In China, Hg in fish is generally accumulated at a low level, but significant geographical differences were evident and formed the “hot spots” from the north to the south. For marine fish, the east (median: 70 ng g−1 ww, range: 5.0–330 ng g−1 ww) and southeast (median: 72 ng g−1 ww, range: 0.3–329 ng g−1 ww) of China have higher total Hg concentrations than the other coastal areas. For freshwater fish, Tibetan Plateau exhibited the highest total Hg levels (median: 104 ng g−1 ww, range: 5.0–868 ng g−1 ww). Risk assessment of the exposure of low-Hg-level fish to China's population deserves more attention and detailed fish consumption advisories to specific populations are urgently needed. The biokinetic model is a useful tool to characterize the underlying processes involved in Hg accumulation by fish. The diet (Hg concentration, speciation, food quality and quantity) and growth appear to be the important factors affecting the Hg levels of fish in China. The Hg biotransformation can also make contributions to Hg speciation and overall accumulation in fish. The intestinal microbes play an important role in Hg biotransformation and the potential for minimizing Hg contamination in fish deserves further investigation.

Despite the ban on new manufacture and commercial use of PCBs, municipal sewer systems continue to serve as ongoing secondary sources for contamination in receiving water bodies. Ongoing PCB sources have made it difficult to achieve desired recovery after implementation of sediment cleanup efforts. We report on a 16-month surveillance to determine the inputs, fate, and export of PCBs within a municipal waste collection/treatment system by strategic sampling of the freely-dissolved and biosolids-associated PCBs. The total PCBs entering the treatment plant was found to be 170 g/day of which 100 g/day exited the plant associated with the biosolids and 5.2 g/day was discharged in the form of freely-dissolved PCBs in the effluent. A net loss of 68 g/day was calculated for the plant, attributable to volatilization and biodegradation. Freely dissolved PCBs in the treated effluent was an order of magnitude higher than the water quality criteria for the protection of human health through fish consumption and found to be a major contributor to the dissolved concentration in the receiving river. Predicted bioaccumulation in fish from dissolved PCBs in the effluent exceeded the threshold for human consumption. The biosolids, currently land-applied as fertilizer, contained an average PCB concentration of 760 μg/kg. The sludge produced in this treatment plant is processed in large anaerobic digesters and changes to the homolog distribution point to some microbial dechlorination. Application of biosolids to clean agricultural soil resulted in a 6-fold increase in PCB levels in the earthworm E. fetida which could be eliminated by the amendment of 1% by weight of activated carbon.