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Plastic pollution in the environment has spurred debate among scientists, policymakers, and the general public over how industrialization and consumerism are wreaking havoc on our ecosystem, but some policies might assist to ameliorate the problem in the near future. In this study, the decision tree classifier and Bayesian Structural Time Series (BSTS) model was used to anticipate the possible sources of microplastics and their near future state in 26 surface sediment and a sediment core, respectively in Sansha Bay, which has been criticized for its intensive mariculture applications. An inventory of microplastics in the sediment core was estimated, and it was discovered that during the previous six decades, an average of 181.95 tons of microplastics were deposited, with an average deposition (by a layer of sediment) of 179.44 tons/cm. According to the DT classifier, mariculture was the primary source of microplastics, whereas urban and industrial areas were the primary sources of POPs. The Bayesian Structural Time Series (BSTS) model revealed a microplastic downward slope, indicating that regional and national strategies implemented might successfully reduce microplastic pollution regionally.

To mitigate mercury (Hg) pollution and reduce Hg downstream transportation, a weir was designed by a river system that had been inflicted by leachate from the slagheap of the Yanwuping Hg mine in Wanshan Hg mining area. A whole year monitoring of Hg species was conducted, and the efficiency of Hg reduction by the weir application was evaluated. The Hg concentrations in the river water were significantly higher in the wet season than in the dry season. Waterflow was confirmed to be the main driving factor for Hg mobilization and transportation, and an episode study revealed that most Hg was released in times of storms. Increased monitoring and preventive maintenance measures need to be taken on barriers in advance of storms. A large proportion of the total Hg (THg) and methylmercury (MeHg) is associated to particles. During the study period, approximately 412 g THg and 4.04 g total MeHg (TMeHg) were released from the YMM slagheap, of which 167 g THg and 1.15 g TMeHg were retained by the weir. Annually, 40.4% THg and 38.4% TMeHg was retained by the weir. Weir construction is considered as a potential cost-effective measure to mitigate Hg in river water and should be promoted and extended in the future after optimization.

The exposure to ambient fine particulate matter (PM2.5) can induce oxidative stress, contributing to global burden of diseases. The evaluation of the oxidative potential (OP) of PM2.5 is thus critical for the health risk assessment. We collected ambient PM2.5 samples in Hangzhou city, China for four consecutive quarters in the year 2017 and investigated the oxidation property of PM2.5 components by the dithiothreitol (DTT) assay. The annual mean of ambient PM2.5 mass concentrations in 2017 was 63.05 μg m−3 (median: 57.34, range: 6.67–214.33 μg m−3) with the significant seasonal variations ranking as winter > spring > summer > autumn. Secondary inorganic aerosol (SIA) species including SO42−, NO3− and NH4+ totally account for >50% of PM2.5 mass. The annual mean volume-normalized DTT activity (DTTv) showed a relatively high value of 0.62 nmol/min/m3 (median: 0.62, range: 0.11–1.66 nmol/min/m3) and DTTv of four seasons was roughly at the same level, indicating a high annual exposure level of ambient PM2.5. SIA species were correlated well with the corresponding DTTv and showed significant diurnal variations with strong or moderate correlations at day and weak correlations at night, suggesting strong secondary formation in daytime with contribution to the particulate OP. The annual mean mass-normalized DTT activity (DTTm) had a relatively low value of 6.39 pmol/min/μg (median: 5.63, range: 1.99–22.70 pmol/min/μg), indicating low intrinsic oxidative toxicity. The DTTm of four seasons ranked as autumn > winter > spring > summer, indicating seasonal variations of the DTT-active components. The PM2.5 mass concentration is more related to exposure levels than intrinsic properties of components, while OP is determined by the components rather than PM2.5 mass concentration. Our results provide an insight into reactive oxygen species-induced health risk of PM2.5 exposure and decision for subsequent emission control.

As an important factor related to the self-purification capacity (e.g. denitrification, burial rate, and downstream output) in aquatic systems, water residence time (WRT) has great impacts on the nitrogen (N) dynamics and its removal process in lakes and reservoirs. In this study, we have analysed the impacts of WRT on the change rates of total nitrogen (TN) concentrations in 50 waterbodies (including 33 lakes and 17 reservoirs) in China, with different change trends (e.g. increasing trends and decreasing trends) and TN concentrations during 2012–2016. Based on the annual ecosystem-scale N mass balance, TN input and output flux in the waterbodies are estimated. The results showed that the decreases of TN concentrations usually occur in the waterbodies with the relatively high TN concentrations in 2012, and WRT has significant impacts on the TN change rates in the waterbodies. Longer WRT could slow down the TN increasing rates in the waterbodies acting as N sinks, but could accelerate the removal from the waterbodies acting as N sources. Higher water phosphorus (P) concentrations could also be beneficial for the faster N removal from the waterbodies, which is mediated via the coupled processes regulating the N transfer from water column to anoxic sediments. China has recently issued the “lake-chief” systems, addressing the specific and flexible strategies for water pollution control in different lakes. The self-purification capacity through denitrification and burial rate, which are closely related to WRT, should be taken into consideration when making specific water management plans in the future.

Excess nutrient inputs and climate change are two of multiple stressors affecting many lakes worldwide. Lake Vansjø in southern Norway is one such eutrophic lake impacted by blooms of toxic blue-green algae (cyanobacteria), and classified as moderate ecological status under the EU Water Framework Directive. Future climate change may exacerbate the situation. Here we use a set of chained models (global climate model, hydrological model, catchment phosphorus (P) model, lake model, Bayesian Network) to assess the possible future ecological status of the lake, given the set of climate scenarios and storylines common to the EU project MARS (Managing Aquatic Ecosystems and Water Resources under Multiple Stress). The model simulations indicate that climate change alone will increase precipitation and runoff, and give higher P fluxes to the lake, but cause little increase in phytoplankton biomass or changes in ecological status. For the storylines of future management and land-use, however, the model results indicate that both the phytoplankton biomass and the lake ecological status can be positively or negatively affected. Our results also show the value in predicting a biological indicator of lake ecological status, in this case, cyanobacteria biomass with a BN model. For all scenarios, cyanobacteria contribute to worsening the status assessed by phytoplankton, compared to using chlorophyll-a alone.

To obtain the historical changes of pyrogenic sources, integrated source apportionment methods, which include PAH compositions, diagnostic ratios (DRs), Pb isotopic ratios, and positive matrix factorization (PMF) model, were developed and applied in sediments of the northern South China Sea. These methods provided a gradually clear picture of energy structural change. Spatially, Σ15PAH (11.3 to 95.5 ng/g) and Pb (10.2 to 74.6 μg/g) generally exhibited decreasing concentration gradient offshore; while the highest levels of PAHs and Pb were observed near the southern Taiwan Strait, which may be induced by accumulation of different fluvial input. Historical records of pollutants followed closely with the economic development of China, with fast growth of Σ15PAH and Pb occurring since the 1980s and 1990s, respectively. The phasing-out of leaded gasoline in China was captured with a sharp decrease of Pb after the mid-1990s. PAHs and Pb correlated well with TOC and clay content for core sediments, which was not observed for surface sediments. There was an up-core increase of high molecular PAH proportions. Coal and biomass burning were then qualitatively identified as the major sources of PAHs with DRs. Furthermore, shift toward less radiogenic signatures of Pb isotopic ratios after 1900 revealed the start and growing importance of industrial sources. Finally, a greater separation and quantification of various input was achieved by a three-factor PMF model, which made it clear that biomass burning, coal combustion, and vehicle emissions accounted for 40 ± 20%, 41 ± 13%, and 19 ± 12% of PAHs through the core. Biomass and coal combustion acted as major sources before 2000, while contributions from vehicle emission soared thereafter. The integrated multi-methodologies here improved the source apportionment by reducing biases with a step-down and cross-validation perspective, which could be similarly applied to other aquatic systems.

Identifying the sanitation efficacy in reducing contaminations entering the environment is an important step for water pollution controls and developing management strategies to further improve sanitation conditions. With continuous efforts in sanitation improvement during the past decade, reductions in discharges of aquatic nutrients are expected in China. In this study, we estimated the aquatic nitrogen discharges from human excreta in 31 provinces in China during 2006-2014. The results indicated that the nitrogen discharges entering the environment from human excreta are largely determined by both local population and sanitation conditions. In 2014, the nitrogen discharges from human excreta in the rural areas (2118(1219-3140) Gg per year) (median and 95% confidence interval) are higher than those in the urban areas (1485(626-2495) Gg per year). The significant relationship (R2=0.38, n=29) between the total nitrogen concentrations in lakes and corresponding local nitrogen discharges indicated that, the lakes might be potentially affected by the contaminant inputs from human excreta. The further calculations under two policy scenarios showed that through sanitation improvement, further reduction of nitrogen discharges from human excreta in the developed regions might be limited. The sanitation improvement in the less-developed regions, such as Tibet, Qinghai, and Ningxia, should be considered a priority due to the larger reduction potentials.

To better characterize the chemical compositions and sources of fine particulate matter (i.e. PM2.5) in Sanjiang Plain, Northeast China, total carbon (TC), organic carbon (OC), elemental carbon (EC), water-soluble organic carbon (WSOC), and inorganic ions as well as stable carbon isotopic composition (δ13C) were measured in this study. Intensively open biomass burning episodes are identified from late September to early October by satellite fire and aerosol optical depth maps. During the biomass-burning episode, concentrations of PM2.5, OC, EC, and WSOC are increased by a factor of 4-12 compared to those during the non-biomass-burning period. Non-sea-salt potassium is strongly correlated with PM2.5, OC, EC and WSOC, demonstrating an important contribution from biomass-burning emissions. The enrichment in both the non-sea-salt potassium and chlorine is significantly larger than other inorganic species, suggesting that biomass-burning aerosols in Sanjiang Plain are mostly fresh and less aged. In addition, the WSOC-to-OC ratio is lower than that reported in biomass-burning aerosols in tropical regions, further supporting that biomass-burning aerosols in Sanjiang Plain are mostly primary and secondary organic aerosols may be not significant. A lower average δ13C value (-26.2‰) is observed during the biomass-burning period, indicating a dominant contribution from combustion of C3 plants in the studied region.

Polycyclic aromatic hydrocarbons (PAHs), formed through incomplete combustion process, have adverse health effects. To investigate spatial distribution and sources of PAHs in North China, PAHs with passive sampling in 90 gridded sites during June to September in 2011 were analyzed. The average concentration of the sum of fifteen PAHs in North China is 220 ± 14 ng/m 3 , with the highest in Shanxi, followed by Shandong and Hebei, and then the Beijing-Tianjin area. Major sources of PAHs are identified for each region of North China, coke process for Shanxi, biomass burning for Hebei and Shandong, and coal combustion for Beijing-Tianjin area, respectively. Emission inventory is combined with back trajectory analysis to study the influence of emissions from surrounding areas at receptor sites. Shanxi and Beijing-Tianjin areas are more influenced by sources nearby while regional sources have more impact on Hebei and Shandong areas. Results from this study suggest the areas where local emission should be the major target for control and areas where both local and regional sources should be considered for PAH abatement in North China.

Polycyclic aromatic hydrocarbons (PAHs) have become the dominating burden in the Arctic ecosystems, but their transport pathways and relative importance of different sources in the Arctic remained unclear, and this would be further complicated by climate change. Here we interpreted 27 PAHs in 34 surface sediments from the northern Bering-Chukchi margin. We integrated source apportionment methods (including diagnostic ratios, principal component analysis, hierarchical analysis, and positive matrix factorization (PMF) model) together with geochemistry parameters, which reveal a gradually clear picture of the spatial patterns of different sources. The total PAH concentrations (50.4 to 896.0 ng/g dw) exhibited a "hilly" shape with the increase of latitude, showing the highest level of PAHs in the northeast Chukchi Sea. The total BaP toxic equivalent quotient (TEQ) for carcinogenic compounds was from 1.06 to 33.3 ng TEQ/g. Most PAHs showed positive correlations with silt content, total organic carbon, stable carbon isotopes and black carbon (p 0.01 or 0.05). Generally, source apportionment methods revealed an increasing petrogenic source of PAHs with latitudes. The PMF model further differentiated two petrogenic (36.7%), two pyrogenic (softwood and fossil fuel combustion, 35.5%) and one in-situ biogenic source (Perylene, 27.8%). An extremely high petrogenic signal was captured in the Canada Basin margin, possibly originating from the Mackenzie River via ice drifting with Beaufort Gyre, while another petrogenic source may come from coal deposit erosion by deglaciation. Softwood combustion (characterized by Retene) exhibited exclusively higher contribution in the northeast Chukchi Sea and might result from the increasing wildfire in Alaska due to climate change, whereas fossil fuel combustion exhibited similar contributions across different latitudes. Our results revealed natural PAHs as important "inside sources" in the Arctic, which are highly sensitive to global warming and deserves more attention.

High particulate matter (PM) pollution frequently occurs in winter over northern China , resulting in threats to human health. To date, there are limited studies to link source apportionments and health risk assessments in the different size-resolved PM samples during high PM events. In this study, size-segregated PM samples were collected in Linfen, a typical coal-burning city, in northern China during a wintertime haze pollution. In addition to water-soluble ions and carbon contents, metallic elements in the different size-segregated PM samples were also determined for health risk assessments by inhalation of PM. During the sampling period, the average concentration of PM10 was 274 ± 57 μg m-3 with a major fraction (73%) of organic material and secondary-related aerosols, and an insignificant portion of trace elements (TEs, ~ 3%). The size distribution showed that As and Se, markers of coal combustion, exhibited a mono-modal distribution with a major peak at 0.4-0.7 μm and the others mostly possessed mono-/bi-modal patterns with a major peak at 3.3-5.8 μm. The cancer risk (CR) resulted from PM10 metals by inhalation was estimated to be 2.91 × 10-5 for children and 7.75 × 10-5 for adults while non-cancer risk (NCR) was 2.10 for children and 0.70 for adults. Chromium (Cr) was the dominant species (~89%) of cancer risk in PM10. Road dust was a major fraction (~65%) to total metals in coarse PM (dp > 3.3 μm) whereas coal combustion was a dominant source (~55%) in submicron (dp < 1.1 μm) PM metals. However, traffic emissions (40%) and coal combustion (36%) were the dominant sources of CR since both emissions contributed major fractions (74%) to Cr, especially in submicron PM which exhibited high deposition efficiency of TEs into respiratory tracts, resulting in high CR in Linfen City.

Models for pollution exposure assessment typically adopt an overly simplistic representation of geography, climate and biogeochemical processes. This strategy is unsatisfactory when high temporal resolution simulations for sub-regional spatial domains are performed, in which parameters defining scenarios can vary interdependently in space and time. This is, for example, the case when assessing the influence of biogeochemical processing on contaminant fate. Here we present INCA-Contaminants, the Integrated Catchments model for Contaminants; a new model that simultaneously and realistically solves mass balances of water, carbon, sediments and contaminants in the soil-stream-sediment system of catchments and their river networks as a function of climate, land use/management and contaminant properties. When forced with realistic climate and contaminant input data, the model was able to predict polychlorinated biphenyls (PCBs) concentrations in multiple segments of a river network in a complex landscape. We analyzed model output sensitivity to a number of hydro-biogeochemical parameters. The rate of soil organic matter mineralization was the most sensitive parameter controlling PCBs levels in river water, supporting the hypothesis that organic matter turnover rates will influence re-mobilization of previously deposited PCBs which had accumulated in soil organic matrix. The model was also used to project the long term fate of PCB 101 under two climate scenarios. Catchment diffuse run-off and riverine transport were the major pathways of contaminant re-mobilization. Simulations show that during the next decade the investigated boreal catchment will shift from being a net atmospheric PCB sink to a net source for air and water, with future climate perturbation having little influence on this trend. Our results highlight the importance of using credible hydro-biogeochemical simulations when modeling the fate of hydrophobic contaminants.

Satellite-based mapping has been proven to be an effective method to reveal the spatiotemporal variations of PM2.5 distributions. However, most satellite AOD (aerosol optical depth) statistical models suffer from unstable accuracy over long time spans. This study thus aims to propose an accurate and stable method for PM2.5 concentration estimations in time series. Specifically, a three-step residual variance constraint method (RVCM) is developed to simulate PM2.5 concentrations from January 2013 to December 2017 with the aid of AODs and other auxiliary data. Results show that the five-year fitting R2 and cross-validation R2 of RVCMs improved from 0.77 to 0.88 and 0.71 to 0.84, respectively, compared to those models without residual variance constraint (WO-RVCM). Additionally, RVCM demonstrated more stable performance on time series simulation of PM2.5 concentrations than WO-RVCM, with the yearly fitting R2 of 0.89, 0.88, 0.85, 0.87 and 0.88, and corresponding cross validation R2 of 0.85, 0.84, 0.80, 0.82 and 0.83, respectively. Furthermore, accuracy verification of removed outliers in residual variance constraint modeling confirmed the credibility of RVCM in outliers' simulation compared to WO-RVCM models. Finally, RVCM-aided estimations of time series PM2.5 concentrations and associated premature deaths in the study area (east and southeast mainland China) revealed their total decrease rates were 35.21% and 21.57%, and excellent air quality days increased from 7% to 35%. These findings suggest that residual variance constraint is effective and could be a reliable solution to providing time series AOD-PM2.5 modeling with stable accuracy over long time spans.

This study investigates the atmospheric occurrence of persistent organic pollutants (POPs) over the Pacific Ocean near southern Taiwan and the northern Philippines. We determined sixty-six compounds, including polychlorinated dibenzo-p-dioxins and dibenzofurans (PCDD/Fs), dioxin-like polychlorinated biphenyls (DLPCBs), polybrominated diphenyl ethers (PBDEs), as well as polychlorinated diphenyl ethers (PCDEs), polybrominated dibenzo-p-dioxins and dibenzofurans (PBDD/Fs), and polybrominated biphenyls (PBBs), in air samples simultaneously collected from the offshore oceanic atmosphere (n=6) and over a rural area (n=2). We calculated the atmospheric World Health Organization 2005 toxic equivalency levels (WHO2005-TEQ), for the total dioxin-like POPs, including PCDD/Fs, DLPCBs, and PBDD/Fs, being 0.00612 pg WHO2005-TEQ/m(3) and 0.0138 pg WHO2005-TEQ/m(3) over the ocean and land, respectively. We found unexpected lower averaged atmospheric PBDE concentrations in the rural area (15.9 pg/m(3)) than over the ocean (31.1 pg/m(3)) due to higher levels of the BDE209 congener, although the difference was not statistically significant. We have compared and reported our field results with previously published datasets over the global oceans, which suggest PCBs and PBDEs are the dominant chemical contaminants in the global oceanic atmosphere among these halogenated POPs (e.g. PCBs and Σdi-hepta PBDEs could be found in the range of 0.09-48.7 and 8.07-94.0 pg/m(3), respectively, including our dataset). However, there are still very few investigations on the global atmospheric levels of PBDD/Fs, PCDEs and PBBs and our data sums to these earlier studies. Finally, we point out that the halogenated POPs originated from Taiwan or the continental East Asia which could easily reach remote ocean sites via atmospheric transport.