A probe into the acid deposition mitigation path in China over the last four decades and beyond.

China currently has the highest acid deposition globally, yet research on its status, impacts, causes and controls is lacking. Here, we compiled data and calculated critical loads regarding acid deposition. The results showed that the abatement measures in China have achieved a sharp decline in the emissions of acidifying pollutants and a continuous recovery of precipitation pH, despite the drastic growth in the economy and energy consumption. However, the risk of ecological acidification and eutrophication showed no significant decrease. With similar emission reductions, the decline in areas at risk of acidification in China (7.0%) lags behind those in Europe (20%) or the USA (15%). This was because, unlike Europe and the USA, China's abatement strategies primarily target air quality improvement rather than mitigating ecological impacts. Given that the area with the risk of eutrophication induced by nitrogen deposition remained at 13% of the country even under the scenario of achieving the dual targets of air quality and carbon dioxide mitigation in 2035, we explored an enhanced ammonia abatement pathway. With a further 27% reduction in ammonia by 2035, China could largely eliminate the impacts of acid deposition. This research serves as a valuable reference for China's future acid deposition control and for other nations facing similar challenges.

Delayed recovery of surface water chemistry from acidification in subtropical forest region of China.

The three largest acid rain regions of current earth are located in northern and western Europe, eastern North America, and East Asia. Sulfur and nitrate concentrations in headwater streams in Europe and North America decreased as atmospheric sulfur and nitrogen deposition decreased, albeit with a considerable delay. However, how water chemistry responds to the declining sulfur and nitrogen deposition in China is unclear. The regional survey of surface water chemistry during 2010 and 2018 within the Sichuan Basin in southwestern China showed that the recovery of the surface water chemistry was delayed for at least 5 years owing to the release of previously deposited sulfur and nitrogen stored in the soil. After sulfur deposition declined from its peak value, the subregions of purplish soil with low sulfate adsorption capacity still exhibited a net sulfur release in 2010, but this release was no longer evident by 2018. The subregions with the red and yellow soils, which have a high sulfate adsorption capacity, operated as sulfur sinks during 2010 and 2018, indicating a continuous immobilization process through sulfate reduction despite a decrease in sulfur deposition. Additionally, this sulfate reduction countered the release of sulfate caused by sulfur desorption. There was a substantial nitrogen sink within the Sichuan Basin. Nitrogen leaching decreased slowly with the declined nitrogen deposition, except in regions where nitrogen deposition exceeded the critical threshold. Compared to temperate forest regions in Europe, the Sichuan Basin and its surrounding areas have experienced higher decline rates in the leaching of sulfur and nitrogen, highlighting that the subtropical forest region undergoes a faster restoration of surface water chemistry.

Decreasing mercury levels in consumer fish over the three decades of increasing mercury emissions in China.

Fish consumption is the primary dietary route of human exposure to methylmercury. It has been well documented that elevated mercury concentration in fish in North America and Europe is linked to anthropogenic mercury emissions. China is the world's largest producer, consumer, and emitter of mercury, as well as the world's largest commercial fish producer and consumer. Although mercury pollution in fish in China is currently receiving much attention worldwide, its status remains largely unknown. Here, we conducted a meta-analysis on total mercury concentrations in marine and freshwater fish samples, covering 35,464 samples collected in China over the past 30 years. It is found that, opposite to the increasing emission and documented mercury contamination events, mercury levels in fish have gradually decreased in China over the past 30 years. The results were in sharp contrast to those found in North America and Europe. The mercury concentrations in fish were significantly anticorrelated with the fish catch and fish aquaculture and were inverse to trophic levels. Overfishing and the short lifecycle of aquaculture fish, both reducing the trophic level and the duration of mercury accumulation, were the most likely causes leading to the decline of mercury concentrations found in fish in China.

Critical loads of headwater streams in China using SSWC model modified by comprehensive F-factor.

In order to evaluate the potential risk of surface water acidification in regions with historically-elevated acid deposition and to measure the recovery of such ecosystems after policy changes, critical loads and their exceedances were estimated for 349 headwater streams across China using a modified SSWC model. Such a model considered the acid-neutralizing capacity derived from high base cation deposition and the robust retention of sulfate and nitrate. Results indicated that China's streams had higher critical loads (averaged at 4.7 keq·ha-1·yr-1) and were less sensitive to acid deposition as compared to Europe and North America. The proportion of surveyed streams with acid deposition exceeded critical load decreased from 40.4% in 2005 to 29.5% in 2018, indicating a significant decrease in risk of surface water acidification, and thus a benefit from the emission abatement in recent years. Nonetheless, a relatively high risk of acidification still existed in southeast China with lower critical loads and most critical load exceedances. More efforts should be put into implementing emission control policies in the future.

Improvement in municipal wastewater treatment alters lake nitrogen to phosphorus ratios in populated regions.

Large-scale and rapid improvement in wastewater treatment is common practice in developing countries, yet this influence on nutrient regimes in receiving waterbodies is rarely examined at broad spatial and temporal scales. Here, we present a study linking decadal nutrient monitoring data in lakes with the corresponding estimates of five major anthropogenic nutrient discharges in their surrounding watersheds over time. Within a continuous monitoring dataset covering the period 2008 to 2017, we find that due to different rates of change in TN and TP concentrations, 24 of 46 lakes, mostly located in China's populated regions, showed increasing TN/TP mass ratios; only 3 lakes showed a decrease. Quantitative relationships between in-lake nutrient concentrations (and their ratios) and anthropogenic nutrient discharges in the surrounding watersheds indicate that increase of lake TN/TP ratios is associated with the rapid improvement in municipal wastewater treatment. Due to the higher removal efficiency of TP compared with TN, TN/TP mass ratios in total municipal wastewater discharge have continued to increase from a median of 10.7 (95% confidence interval, 7.6 to 15.1) in 2008 to 17.7 (95% confidence interval, 13.2 to 27.2) in 2017. Improving municipal wastewater collection and treatment worldwide is an important target within the 17 sustainable development goals set by the United Nations. Given potential ecological impacts on biodiversity and ecosystem function of altered nutrient ratios in wastewater discharge, our results suggest that long-term strategies for domestic wastewater management should not merely focus on total reductions of nutrient discharges but also consider their stoichiometric balance.

Modelling Environmental Impacts of Cesium-137 Under a Hypothetical Release of Radioactive Waste.

Waste tanks at the nuclear facility located at Sellafield, UK, represent a nuclear source which could release radionuclides to the atmosphere. A model chain which combines atmospheric transport, deposition as well as riverine transport to sea has been developed to predict the riverine activity concentrations of 137Cs. The source term was estimated to be 9 × 104 TBq of 137Cs, or 1% of the assumed total 137Cs inventory of the HAL (Highly Active Liquid) storage tanks. Air dispersion modelling predicted 137Cs deposition reaching 127 kBq m-2 at the Vikedal catchment in Western Norway. Thus, the riverine transport model predicted that the activity concentration of 137Cs in water at the river outlet could reach 9000 Bq m-3 in the aqueous phase and 1000 Bq kg-1 in solid phase at peak level. The lake and river reaches showed different transport patterns due to the buffering effects caused by dilution and slowing down of water velocity.

Assessing Air-Surface Exchange and Fate of Mercury in a Subtropical Forest Using a Novel Passive Exchange-Meter Device.

A novel passive exchange meter (EM) device was developed to assess air-surface exchange and leaching of Hg in a forest floor. Flux measurements were carried out in a subtropical forest ecosystem during a full year. Over 40% of the Hg fixed in fresh forest litter was remobilized in less than 60 days in warm and humid conditions as a response to rapid turnover of labile organic matter (OM). A two-block experiment including understory and clearing showed that losses of Hg covaried with seasonal conditions and was significantly affected by forest coverage. The process controlling the bulk loss of total Hg from the litter was volatilization, which typically represented 76-96% of the loss processes (Floss). The Floss ranges were 520-1370 and 165-942 ng m-2 d-1 in the understory and clearing, respectively. On a yearly basis, deposition of airborne Hg exceeded total losses by a factor of 2.5 in the clearing and 1.5 in the understory. The vegetation litter in this subtropical forest therefore represented a net sink of atmospheric Hg. This study provided a novel approach to Hg air-soil exchange measurements and further insights on the link between Hg remobilization and OM turnover along with its environmental drivers.

Dynamic Modeling and Target Loads of Sulfur and Nitrogen for Surface Waters in Finland, Norway, Sweden, and the United Kingdom.

The target load concept is an extension of the critical load concept of air pollution inputs to ecosystems. The advantage of target loads over critical loads is that one can define the deposition and the point in time (target year) when the critical (chemical) limit is no longer violated. This information on the timing of recovery requires dynamic modeling. Using a well-documented dynamic model, target loads for acidic deposition were determined for 848 surface waters across Finland, Norway, Sweden, and the United Kingdom for the target year 2050. In the majority of sites ( n = 675), the critical ANC-limit was predicted to be achieved by 2050; however, for 127 sites, target loads were determined. In addition, 46 sites were infeasible, i.e., even a reduction of anthropogenic deposition to zero would not achieve the limit by 2050. The average maximum target load for sulfur was 38% lower than the respective critical load across the study lakes ( n = 127). Target loads on a large regional scale can inform effects-based emission reduction policies; the current assessment suggests that reductions beyond the Gothenburg Protocol are required to ensure surface water recovery from acidification by 2050.

Weir building: A potential cost-effective method for reducing mercury leaching from abandoned mining tailings.

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 organic pollutant status of rivers in Bosnia and Herzegovina as determined by a combination of active and passive sampling methods.

There is an overall lack of data concerning the pollution status of Bosnia Herzegovina, which is confounded by fragmented national environmental management. The present study aimed to provide some initial data for concentrations of priority substances in two major Bosnian Rivers, using two types of passive sampler (PS) as well as by using high volume water sampling (HVWS). Overall, concentrations of most persistent organic pollutants (POPs), including polychlorinated biphenyls (PCBs) and legacy pesticides, were shown to be low. However, around the town of Doboj on the Bosna River, concentrations of polycyclic aromatic hydrocarbons (PAH) breached European standards for several compounds and reached 67 ng L-1 for freely dissolved concentrations and 250 ng L-1 for total concentrations. In general, contamination was lower in the Neretva River compared to the Bosna, although for brominated diphenyl ethers (PBDEs), results suggested an active source of PBDEs at one location based on the ratio of congeners 47 and 99. Direct comparisons between the different sampling techniques used are not straightforward, but similar patterns of PAH contamination were shown by HVWS and PS in the Bosna River. There are both scientific and practical considerations when choosing which type of sampling technique to apply, and this should be decided based on the goals of each individual study.

Mercury in fish from Norwegian lakes: The complex influence of aqueous organic carbon.

Mercury (Hg) concentrations in water and biota are often positively correlated to organic matter (OM), typically measured as total or dissolved organic carbon (TOC/DOC). However, recent evidence suggests that higher OM concentrations inhibit bioaccumulation of Hg. Here, we test how TOC impacts the Hg accumulation in fish in a synoptic study of Methyl-Hg (MeHg) in water and total Hg (THg) in perch (Perca fluviatilis) in 34 boreal lakes in southern Norway. We found that aqueous MeHg (r2 = 0.49, p < 0.0001) and THg (r2 = 0.69, p < 0.0001), and fish THg (r2 = 0.26, p < 0.01) were all positively related with TOC. However, we found declining MeHg bioaccumulation factors (BAFMeHg) for fish with increasing TOC concentrations. The significant correlation between fish THg concentrations and aqueous TOC suggests that elevated fish Hg levels in boreal regions are associated with humic lakes. The declining BAFMeHg with increasing TOC suggest that increased OM promotes increased aqueous Hg concentrations, but lowers relative MeHg bioaccumulation. A mechanistic understanding of the response from OM on BAFMeHg might be found in the metal-complexation properties of OM, where OM complexation of metals reduces their bioavailability. Hence, suggesting that MeHg bioaccumulation becomes less effective at higher TOC, which is particularly relevant when assessing potential responses of fish Hg to predicted future changes in OM inputs to boreal ecosystems. Increased browning of waters may affect fish Hg in opposite directions: an increase of food web exposure to aqueous Hg, and reduced bioavailability of Hg species. However, the negative relationship between BAFMeHg and TOC is challenging to interpret, and carries a great deal of uncertainty, since this relationship may be driven by the underlying correlation between TOC and MeHg (i.e. spurious correlations). Our results suggest that the trade-off between Hg exposure and accumulation will have important implications for the effects of lake browning on Hg transport, bioavailability, and trophodynamics.

Monitoring Effect of SO2 Emission Abatement on Recovery of Acidified Soil and Streamwater in Southwest China.

Following Europe and North America, East Asia has become a global hotspot of acid deposition, with very high deposition of both sulfur (S) and nitrogen (N) occurring in large areas in southwest and southeast China. Great efforts have been made in reducing national emission of sulfur dioxide (SO2) since 2006 in China. However, the total emission of nitrogen oxides (NOx) continued to increase until 2011. To evaluate the effects of SO2 and NOx emission abatement on acid deposition and acidification of soil and water, we monitored the chemical composition of throughfall, soil water, and streamwater from 2001 to 2013 in a small, forested catchment near Chongqing city in Southwestern China. The deposition of S decreased significantly, whereas N deposition increased in the recent years. This clearly showed the effect of SO2 abatement but not of NOx. Overall the rate of acid deposition was reduced. However, there was delay in the recovery of soil and surface water from acidification, probably due to desorption of previously stored sulfate (SO42-) and increase in nitrate (NO3-) leaching from soil. The average acid input by N transformations has greatly exceeded the H+ input directly by atmospheric deposition. The reversal of acidification with an increase in pH of soil water, requires additional abatement of emissions of both SO2 and NOx.

Is surface water acidification a serious regional issue in China?

Acidic deposition used to cause severe surface water acidification in Europe and the North America, but no damage of surface water acidification was reported under continuous heavy acid deposition in China. We present the first detailed study on regional surface water acidification in southern and northeastern China based on a survey of 255 forested headwater streams, which were investigated during 2010-2015 to explore the status and mechanism of surface water acidification. South China has a subtropical climate with high acid deposition, whereas northeast China is located in a cold temperature zone with relatively low acid deposition. High pH and acid neutralizing capacity (ANC) were observed for almost all of the streams, indicating that surface water acidification may not be a serious regional issue in China both at present and in the future. In northeast China, where soil types are similar in low weathering rate to those in Northern Europe and North America, the ANC of surface waters was lower than that in South China, indicating a higher acid-sensitivity of the surface water. In comparison, the high pH and ANC of streams in southwest China resulted from high soil weathering and atmospheric calcium (Ca) deposition, despite elevated atmospheric acid inputs due to the high sulfur (S) and nitrogen (N) deposition. Comparison of stream nitrate (NO3-) and sulfate (SO42-) concentrations with modeled N and S deposition showed significant N and possible S sinks in the catchments in south China, probably due to denitrification of NO3- in groundwater discharge zone and SO42- adsorption by acid soils respectively, which may also buffer the acidifying effect of S and N depositions. It seems that considerable NO3- leaching to stream waters does not occur in China unless N deposition is higher than 1.8keq·ha-1·yr-1 (2.50g N·m-2·yr-1) (or greater values in certain regions).

Mercury Flows in China and Global Drivers.

Mercury (Hg) pollution control has become an urgent need at global and national scales. This study, for the first time, comprehensively examines Hg flows in Mainland China and uncovers domestic and external causal drivers of China's Hg emissions/releases. Results show that China's Hg input reaches 2643 t in 2010. China discharges 1368 t of Hg to the environment (to air, 633 t; water, 84 t; and land, 651 t). Embedded Hg transfers across production sectors via waste/byproduct flows reduce Hg releases to land, but lead to secondary Hg emissions to air. Such revelations of embedded Hg transfers adjusts China's comprehensive Hg control that would otherwise only tackle primary emitters. Domestic consumption causes 67% of China's Hg emissions/releases, and external consumption induces the remaining 33%. Besides traditional production-side Hg control measures, demand-side measures and international joint efforts are required to effectively combat Hg pollution. Uncovering embedded and embodied Hg flows within the global economy can assist a paradigm shift necessary to make real progress in global Hg control and the implementation of the Minamata Convention on Mercury.

Atmospheric S and N deposition relates to increasing riverine transport of S and N in southwest China: Implications for soil acidification.

Following Europe and North America, East Asia has become a global hotspot for acid deposition, with very high deposition of both sulfur (S) and nitrogen (N) occurring in large areas of southwest and southeast China. This study shows that the outflow flux of sulfate (SO42-) in three major tributaries of the Upper Yangtze River in the Sichuan Basin in southwest China has been increasing over the last three decades, which implies the regional soil acidification caused by increasing sulfur dioxide (SO2) emissions. Since 2005, the outflow of SO42- to the Upper Yangtze River from the Sichuan Basin has even reached the atmospheric SO2 emission from the basin. In contrast to S emissions, the rapid increase in nitrogen (N) emissions, including nitrogen oxides (NOx) and ammonia (NH3), have resulted in only a slight increase in nitrate (NO3-) concentrations in surface waters, indicating a large retention of N in the basin. Although N deposition currently contributes much less than S to soil acidification in this area, it is possible that catchments receiving a high input of N may be unable to retain a large fraction of the N deposition over long periods.

Material Flow for the Intentional Use of Mercury in China.

Intentional use of mercury (Hg) is an important contributor to the release of Hg into the environment. This study presents the first inventory of material flow for intentional use of Hg in China. The total amount of Hg used in China increased from 803 ± 95 tons in 2005 to its peak level of 1272 ± 110 tons in 2011. Vinyl chloride monomer (VCM) production is the largest user of Hg, accounting for over 60% of the total demand. As regulations on Hg content in products are tightening globally against the background of the Minamata Convention, the total demand will decrease. Medical devices will likely still use a significant amount of Hg and become the second largest user of Hg if no proactive measures are taken. Significant knowledge gaps exist in China for catalyst recycling sector. Although more than half of the Hg used is recycled, this sector has not drawn enough attention. There are also more than 200 tons of Hg that had unknown fates in 2011; very little information exists related to this issue. Among the final environmental fates, landfill is the largest receiver of Hg, followed by air, water, and soil.

Perfluoroalkyl substances (PFAS) in river and ground/drinking water of the Ganges River basin: Emissions and implications for human exposure.

Many perfluoroalkyl substances (PFAS) are ubiquitous environmental contaminants. They have been widely used in production processes and daily-use products or may result from degradation of precursor compounds in products or the environment. India, with its developing industrialization and population moving from traditional to contemporary lifestyles, represents an interesting case study to investigate PFAS emission and exposure along steep environmental and socioeconomic gradients. This study assesses PFAS concentrations in river and groundwater (used in this region as drinking water) from several locations along the Ganges River and estimates direct emissions, specifically for PFOS and PFOA. 15 PFAS were frequently detected in the river with the highest concentrations observed for PFHxA (0.4-4.7 ng L(-1)) and PFBS (

Assessment of contaminant fate in catchments using a novel integrated hydrobiogeochemical-multimedia fate model.

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.