Increased Contribution of Circumpolar Deep Water Upwelling to Methylmercury in the Upper Ocean around Antarctica: Evidence from Mercury Isotopes in the Ornithogenic Sediments.

Upwelling plays a pivotal role in supplying methylmercury (MeHg) to the upper oceans, contributing to the bioaccumulation of MeHg in the marine food web. However, the influence of the upwelling of Circumpolar Deep Water (CDW), the most voluminous water mass in the Southern Ocean, on the MeHg cycle in the surrounding oceans and marine biota of Antarctica remains unclear. Here, we study the mercury (Hg) isotopes in an ornithogenic sedimentary profile strongly influenced by penguin activity on Ross Island, Antarctica. Results indicate that penguin guano is the primary source of Hg in the sediments, and the mass-independent isotope fractionation of Hg (represented by Δ199Hg) can provide insights on the source of marine MeHg accumulated by penguin. The Δ199Hg in the sediments shows a significant decrease at ∼1550 CE, which is primarily attributed to the enhanced upwelling of CDW that brought more MeHg with lower Δ199Hg from the deeper seawater to the upper ocean. We estimate that the contribution of MeHg from the deeper seawater may reach more than 38% in order to explain the decline in Δ199Hg at ∼1550 CE. Moreover, we found that the intensified upwelling may have increased the MeHg exposure for marine organisms, highlighting the importance of CDW upwelling on the MeHg cycle in Antarctic coastal ecosystems.

The Marginal Ice Zone as a dominant source region of atmospheric mercury during central Arctic summertime.

Atmospheric gaseous elemental mercury (GEM) concentrations in the Arctic exhibit a clear summertime maximum, while the origin of this peak is still a matter of debate in the community. Based on summertime observations during the Multidisciplinary drifting Observatory for the Study of Arctic Climate (MOSAiC) expedition and a modeling approach, we further investigate the sources of atmospheric Hg in the central Arctic. Simulations with a generalized additive model (GAM) show that long-range transport of anthropogenic and terrestrial Hg from lower latitudes is a minor contribution (~2%), and more than 50% of the explained GEM variability is caused by oceanic evasion. A potential source contribution function (PSCF) analysis further shows that oceanic evasion is not significant throughout the ice-covered central Arctic Ocean but mainly occurs in the Marginal Ice Zone (MIZ) due to the specific environmental conditions in that region. Our results suggest that this regional process could be the leading contributor to the observed summertime GEM maximum. In the context of rapid Arctic warming and the observed increase in width of the MIZ, oceanic Hg evasion may become more significant and strengthen the role of the central Arctic Ocean as a summertime source of atmospheric Hg.

Positive Atlantic Multidecadal Oscillation has driven poleward redistribution of the West Antarctic Peninsula biota through a food-chain mechanism.

The West Antarctic Peninsula (WAP) has recorded a significant poleward range shift in marine biota, including Adélie penguins, Antarctic krill and phytoplankton. The ecological changes have been widely attributed to Pacific/Southern Hemisphere variabilities. However, the teleconnection from the North Atlantic Ocean, which also could induce changes in the WAP physical environments, has been overlooked. Here we combine state-of-the-art observational/modelling databases to quantify the poleward redistribution since the 1980s of three key members of the WAP biota and explored their response to several climatic oscillations. The abundance of Adélie penguins, Antarctic krill and phytoplankton in the WAP all show a decrease in the north and an increase in the south, leading to a poleward shift of their distribution centers by ~0.8-2.3°. A more positive Atlantic Multidecadal Oscillation (AMO) has contributed to the poleward redistribution of phytoplankton/krill/penguin with a time lag of 0/1/5 yr, indicating a food-chain related mechanism. +AMO in spring resulted in reduced sea ice, earlier ice retreat and enhanced winds in the northern WAP, which constrained phytoplankton blooms and krill reproduction, thereby decreasing the krill recruitment 1 yr later and consequently the penguin recruitment 5 yr later. In the southern WAP, where the sea ice cover was nearly permanent in the 1980s, reduced sea ice and earlier ice retreat promoted phytoplankton growth and krill/penguin reproduction. Our results emphasize the global nature of climate-ecological coupling; the influence of the Northern Hemisphere climate system on Antarctic/Southern Ocean biota is a non-negligible factor for the ecosystem management.

Elevated methylmercury in Antarctic surface seawater: The role of phytoplankton mass and sea ice.

Methylmercury is a neurotoxin that is biomagnified in marine food webs. Its distribution and biogeochemical cycle in Antarctic seas are still poorly understood due to scarce studies. Here, we report the total methylmercury profiles (up to 4000 m) in unfiltered seawater (MeHgT) from the Ross Sea to the Amundsen Sea. We found high MeHgT levels in oxic unfiltered surface seawater (upper 50 m depth) in these regions. It was characterized by an obviously higher maximum concentration level of MeHgT (up to 0.44 pmol/L, at a depth of 3.35 m), which is higher than other open seas (including the Arctic Ocean, the North Pacific Ocean and the equatorial Pacific), and a high MeHgT average concentration in the summer surface water (SSW, 0.16 ± 0.12 pmol/ L). Further analyses suggest that the high phytoplankton mass and sea-ice fraction are important drivers of the high MeHgT level that we observed in the surface water. For the influence of phytoplankton, the model simulation showed that the uptake of MeHg by phytoplankton would not fully explain the high levels of MeHgT, and we speculated that high phytoplankton mass may emit more particulate organic matter as microenvironments that can sustain Hg in-situ methylation by microorganisms. The presence of sea-ice may not only harbor a microbial source of MeHg to surface water but also trigger increased phytoplankton mass, facilitating elevation of MeHg in surface seawater. This study provides insight into the mechanisms that impact the content and distribution of MeHgT in the Southern Ocean.

Holocene changes in biomass burning in the boreal Northern Hemisphere, reconstructed from anhydrosugar fluxes in an Arctic sediment profile.

The rapid warming of Arctic is causing increased fire activities in the boreal Northern Hemisphere (NH), leading to unprecedent changes in the global carbon cycling, human health and ecosystems. Understanding the interaction between fire and climate in this far north region is crucial for predicting future changes of wildfires. However, fire records over geological time scales are still scarce in the high latitudes of NH to provide comprehensive pictures of the fire history in this region. Here, we used the flux of levoglucosan (Lev) and its isomers in a sediment profile YN from Svalbard, high Arctic, as proxies for the changes in biomass burning from ∼9-2 kyr BP (thousand years before present). Backward trajectories and comparison with charcoal syntheses from various regions confirmed that the Lev transport to the profile site is sourced from the fire activities in the boreal NH, especially in northern Europe and northern Siberia. The Lev flux exhibited a slight overall decreasing trend at ∼3 %/kyr (p = 0.09) over the study period, as well as centennial maxima at ∼9, 8-7, 6, 5, and 4-3 kyr BP (p = 0.06). On sub-orbital scales, the long-term decrease in fire activities corresponded to trends of summer temperature in the extratropics of the NH (p = 0.01, r = 0.42), reflecting their regulation of fuel availability and flammability. On centennial to sub-millennial time scales, high levels of biomass burning were associated with periods of increased North Atlantic ice-rafted debris (p = 0.02, r = 0.38), which were indicative of cold and dry conditions over most of the source regions, reflecting the impacts of dryness on fuel flammability. The results suggested that enhanced Arctic amplification on centennial time scales may reduce biomass burning in most of the boreal NH, although fires in some mid-latitude regions may be facilitated.

Indoor air particles in research vessel from Shanghai to Antarctic: Characteristics, influencing factors, and potential controlling pathway.

Despite millions of seafarers and passengers staying on ships each year, few studies have been conducted on the indoor air quality inside ship hulls. In this study, we investigated the levels and size distribution of indoor particulate matter during two cruises of the research vessel "Xuelong" from Shanghai to Antarctica. The results showed that the particle size less than 2.5 µm (PM2.5), and particle size less than 10 µm (PM10) concentrations in different rooms of the ship widely varied. We observed high particulate matter (PM) levels in some of the rooms. The mass concentration distribution was dominated by 1-4 µm particles, which may have been caused by the hygroscopic growth of fine particles. The dominant factors influencing PM concentrations were indoor temperature, relative humidity, and human activity. We quantified contributions of these factors to the levels of indoor particles using a generalized additive model. In clean rooms, the levels of indoor particles were controlled by temperature and relative humidity, whereas in polluted rooms, the levels of indoor particles were mainly influenced by temperature and human activity, which implied that controlling temperature and human activity would efficiently reduce the levels of indoor particles.

Spatiotemporal distribution and influencing factors of secondary organic aerosols in the summer atmosphere from the Bering Sea to the western North Pacific.

To better understand the formation process of biogenic and anthropogenic secondary organic aerosols (BSOA and ASOA) in the marine atmosphere under the background of global warming, aerosol samples were collected over three summers (i.e., 2014, 2016 and 2018) from the Bering Sea (BS) to the western North Pacific (WNP). The results showed that temporally, atmospheric concentrations of isoprene-derived SOA (SOAI) tracers were the lowest in 2014 regardless of the marine region, while atmospheric concentrations of monoterpenes-derived SOA (SOAM) tracers in this year were the highest and the aerosols were more aged than those in the other two years. In comparison, the concentrations of ß-caryophyllene-derived and toluene-derived SOA (SOAC and SOAA) tracers were relatively low overall. Spatially, the concentrations of SOA tracers were significantly higher over the WNP than over the BS, with SOA tracers over the BS mainly coming from marine sources, while the WNP was strongly influenced by terrestrial inputs. In particular, for land-influenced samples from the WNP, NOx-channel products of SOAI were more dependent on O3 and SO2 relative to HO2-channel product, and the high atmospheric oxidation capacity and SO2 could promote the formation of later-generation SOAM products. The extent of terrestrial influence was further quantified using a principal component analysis (PCA)-generalized additive model (GAM), which showed that terrestrial emissions explained more than half of the BSOA tracers' concentrations and contributed almost all of the ASOA tracer. In addition, the assessment of secondary organic carbon (SOC) highlighted the key role of anthropogenic activities in organic carbon levels in offshore areas. Our study revealed significant contributions of terrestrial natural and anthropogenic sources to different SOA over the WNP, and these relevant findings help improve knowledge about SOA in the marine atmosphere.

Which aerosol type dominate the impact of aerosols on ozone via changing photolysis rates?

The impact of aerosols on ozone via influencing photolysis rates is a combined effect of absorbing aerosols (AA) and scattering aerosols (SA). However, AA and SA show different optical properties and influence photolysis rates differently, which then cause different impacts on ozone. Till now, the dominate factor is disconfirmed, which is largely due to the impact of SA on ozone not reaching to a consistent conclusion. In this study, the WRF-Chem model was implemented to simulate the air pollutants over the North China Plain (NCP). The impacts of AA and SA on ozone via influencing photolysis rates were quantitatively isolated and analyzed. Our results also demonstrated the decreasing effect of AA on ozone within planet boundary layer (PBL) which is consistent with the conclusions of previous studies. But for SA, it decreased the ozone chemical contribution (CHEM) near surface but increased which in the upper layers of PBL, that enlarge the ozone vertical gradients. In this case, more vertical exchanges of ozone would occur with the effect of vertical mixing motion of atmosphere, then the opposite CHEM variations were counteracted with each other and finally led to very slight changes in ozone within PBL. Thus, it can be summarized that AA dominate this impact of aerosols on ozone. Reducing AA could cause a general increase in ozone (ΔO3) over the NCP. Based on the aerosol levels of this case, ΔO3 would be seen over 86 % of the areas in the NCP when reducing AA by 3/4 and ΔO3 was more significant in the megacities. Our study highlights the different relationships between ozone and aerosol types, which suggests that more attentions should be paid on aerosol types, especially AA, when making the synergetic control strategy of aerosols and ozone in China.

Molecular characteristics, sources and influencing factors of isoprene and monoterpenes secondary organic aerosol tracers in the marine atmosphere over the Arctic Ocean.

Biogenic secondary organic aerosols (BSOA) are important components of the remote marine atmosphere. However, the response of BSOA changes to sea ice reduction over the Arctic Ocean remains unclear. Here we investigated isoprene and monoterpenes secondary organic aerosol (SOAI and SOAM) tracers in three years of summer aerosol samples collected from the Arctic Ocean atmosphere. The results indicated that methyltetrols were the most abundant SOAI tracers, while the main oxidation products of monoterpenes varied over the years owing to different aerosol aging. The results of the principal component analysis (PCA)-generalized additive model (GAM) combined with correlation analysis suggested that SOAI tracers were mainly generated by the oxidation of isoprene from marine emissions, while SOAM tracers were probably more influenced by terrestrial transport. Estimation of secondary organic carbon (SOC) indicated that monoterpenes oxidation contributed more than isoprene and that sea ice changes had a relatively small effect on biogenic SOC concentration levels. Our study quantified the contribution of influencing factors to the atmospheric concentration of BSOA tracers in the Arctic Ocean, and showed that there were differences in the sources of precursors for different BSOA. Hence, our findings have contributed to a better understanding of the characteristics, sources and formation of SOA in the atmosphere of the Arctic Ocean.

Special issue on the AMAP 2021 assessment of mercury in the Arctic.

This Editorial presents an overview of the Special Issue on advances in Arctic mercury (Hg) science synthesized from the 2021 assessment of the Arctic Monitoring and Assessment Programme (AMAP). Mercury continues to travel to Arctic environments and threaten wildlife and human health in this circumpolar region. Over the last decade, progress has been achieved in addressing policy-relevant uncertainties in environmental Hg contamination. This includes temporal trends of Hg, its transport to and within the Arctic, methylmercury cycling, climate change influences, biological effects of Hg on fish and wildlife, human exposure to Hg, and forecasting of Arctic responses to different future scenarios of anthropogenic Hg emissions. In addition, important contributions of Indigenous Peoples to Arctic research and monitoring of Hg are highlighted, including through projects of knowledge co-production. Finally, policy-relevant recommendations are summarized for future study of Arctic mercury. This series of scientific articles presents comprehensive information relevant to supporting effectiveness evaluation of the United Nations Minamata Convention on Mercury.

A potential controlling approach on surface ozone pollution based upon power big data.

Surface ozone pollution has attracted extensive attention with the decreasing of haze pollution, especially in China. However, it is still difficult to efficiently control the pollution in time despite numbers of reports on mechanism of ozone pollution. Here we report a method for implementing effective control of ozone pollution through power big data. Combining the observation of surface ozone, NO2, meteorological parameters together with hourly electricity consumption data from volatile organic compounds (VOCs) emitting companies, a generalized additive model (GAM) is established for quantifying the influencing factors on the temporal and spatial distribution of surface ozone pollution from 2020 to 2021 in Anhui province, central China. The average R2 value for the modelling results of 16 cities is 0.82, indicating that the GAM model effectively captures the characteristics of ozone. The model quantifies the contribution of input variables to ozone, with both NO2 and industrial VOCs being the main contributors to ozone, contributing 33.72% and 21.12% to ozone formation respectively. Further analysis suggested the negative correlation between ozone and NO2, revealing VOCs primarily control the increase in ozone. Under scenarios controlling for a 10% and 20% reduction in electricity use in VOC-electricity sensitive industries that can be identified by power big data, ozone concentrations decreased by 9.7% and 19.1% during the pollution period. This study suggests a huge potential for controlling ozone pollution through power big data and offers specific control pathways. Supplementary Information: The online version contains supplementary material available at 10.1007/s42452-022-05045-5.

Mixing state and distribution of iodine-containing particles in Arctic Ocean during summertime.

Iodine chemistry plays a key role in ozone destruction and new aerosol formation in the marine boundary layer (MBL), especially in polar regions. We investigated iodine-containing particles (0.2-2 µm) in the Arctic Ocean using a ship-based single particle aerosol mass spectrometer from July to August 2017. Seven main particle types were identified: dust, biomass combustion particles, sea salt, organic S, aromatics, hydrocarbon-like compounds, and amines. The number fraction of iodine-containing particles was higher inside the Arctic Circle (>65°N) than outside (55-65°N). According to the air mass back trajectories, the latitudinal distribution of iodine-containing particles can be mainly attributed to iodine emissions from the sea ice edge region. Diurnal trends were found, especially during the second half of cruise, with peak iodine-containing particle number fractions during low-light conditions and relatively low number fractions at midday. These results imply that solar radiation plays a significant role in modulating particulate iodine in the Arctic atmosphere.

Latitudinal Distribution of Gaseous Elemental Mercury in Tropical Western Pacific: The Role of the Doldrums and the ITCZ.

The role of the tropical western Pacific in the latitudinal distribution of atmospheric mercury is still unclear. In this study, we conducted continuous measurements of gaseous elemental mercury (GEM) in the marine boundary layer (MBL) along a large latitudinal transect (∼60° S to ∼30° N) of the western Pacific, accompanied by measurements of dissolved gaseous mercury (DGM) in the surface seawater. We found that the GEM latitudinal gradient is the most significant in the tropical western Pacific, which to some extent might be attributed to the impact of the doldrums and the Intertropical Convergence Zone (ITCZ) in this area. For the doldrums, calm weather may delay the transport of GEM, facilitating its accumulation in the tropical western Pacific. Furthermore, the regional transport, and low O3 and sea-salt aerosol levels in this area which would not favor the oxidation of GEM in the MBL, would intensify the accumulation of GEM in the tropical western Pacific. For the ITCZ, the vast wet deposition of Hg would drive elevated DGM in the surface seawater, which can increase the evasion flux and may further influence the spatial distribution of GEM. This study provides insight into the role of the tropical western Pacific in the regional atmospheric mercury cycle.

Quantify the role of anthropogenic emission and meteorology on air pollution using machine learning approach: A case study of PM2.5 during the COVID-19 outbreak in Hubei Province, China.

Air pollution is becoming serious in developing country, and how to quantify the role of local emission and/or meteorological factors is very important for government to implement policy to control pollution. Here, we use a random forest model, a machine learning (ML) approach, combined with a de-weather method to analyze the PM2.5 level during the COVID-19 outbreak in Hubei Province. The results show that changes in anthropogenic emissions have reduced PM2.5 concentrations in February and March 2020 by about 33.3% compared to the same period in 2019, while changes in meteorological conditions have increased PM2.5 concentrations by about 8.8%. Moreover, the impact of meteorological conditions is more significant in the central region, which is likely to be related to regional transport. After excluding the contribution of meteorological conditions, the PM2.5 concentration in Hubei Province in February and March 2020 is lower than the secondary standard of China (35 µ g/m3). Our estimates also indicate that under similar meteorological conditions as in February and March 2019, an emission reduction intensity equivalent to about 48% of the emission reduction intensity during the lockdown may bring the annual average PM2.5 concentration to the standard (35 µ g/m3). Our study shows that machine learning is a powerful tool to quantify the influencing factors of PM2.5, and the results further emphasize the need for scientific emission reduction as well as joint regional control measures in future.

The impact of the aerosol reduction on the worsening ozone pollution over the Beijing-Tianjin-Hebei region via influencing photolysis rates.

Due to the implementation of the toughest-ever emission control actions across China from 2013 to present, the aerosols are decreasing annually but ozone is simultaneously increasing, especially over the Beijing-Tianjin-Hebei (BTH) region, where ozone pollution can even spread into winter. Quantifying each impact of aerosols on ozone in all seasons is urgent for the worsening ozone pollution in the improved aerosol air quality. In this study, we focused on the impact of aerosols on ozone via influencing photolysis rates. The air pollutants were simulated over the Central East China (CEC) in 2018 by using the Weather Research and Forecasting with Chemistry (WRF-Chem) model. By implementing emissions with base years of 2014 and 2018, we quantified the increase in ozone (ΔOzone_photolysis) caused by the decreasing aerosol concentrations (ΔPM2.5) by influencing photolysis rates over the BTH region in all seasons. Furthermore, combined with the ozone observations, the contribution of ΔOzone_photolysis to the total changes in ozone (ΔOzone_total) in all seasons was quantitatively discussed. Our results showed that ΔPM2.5 showed obvious seasonal variations, which PM2.5 decreased more significantly in winter and autumn than in spring and summer, although significant reductions in anthropogenic emissions were observed in all seasons. Consistent seasonal variations were also observed in ΔOzone_photolysis, and the mean increases reached 5.5 µg m-3, 2.6 µg m-3, 1.2 µg m-3, and 1.4 µg m-3 in winter, autumn, spring, spring, and summer, respectively. Compared with ΔOzone_total, ΔOzone_photolysis accounted for 36.3%, 17.2%, 3.5% and 10.6% of ΔOzone_total in winter, autumn, spring, and summer, respectively, suggesting that ΔOzone_photolysis was not the primary contributor to the current changes in ozone over the BTH region. However, the 36.3% contribution to ΔOzone_total in winter suggested that ΔOzone_photolysis is still an important contributor and should not be ignored when discussing the formation of high ozone episodes occurring in winter.

Exploring the impact of new particle formation events on PM2.5 pollution during winter in the Yangtze River Delta, China.

New particle formation (NPF) events are an increasingly interesting topic in air quality and climate science. In this study, the particle number size distributions, and the frequency of NPF events over Hefei were investigated from November 2018 to February 2019. The proportions of the nucleation mode, Aitken mode, and accumulation mode were 24.59%, 53.10%, and 22.30%, respectively, which indicates the presence of abundant ultrafine particles in Hefei. Forty-six NPF events occurred during the observation days, accounting for 41.82% of the entire observation period. Moreover, the favorable meteorological conditions, potential precursor gases, and PM2.5 range of the NPF events were analyzed. Compared to non-NPF days, the NPF events preferentially occurred on days with lower relative humidity, higher wind speeds, and higher temperatures. When the PM2.5 was 15-20, 70-80, and 105-115 µg/m3, the frequency of the NPF events was higher. Nucleation mode particles were positively related to atmospheric oxidation indicated by ozone when PM2.5 ranged from 15 to 20 µg/m3, and related to gaseous precursors like SO2 and NO2 when PM2.5 was located at 70-80 and 105-115 µg/m3. On pollution days, NPF events did not directly contribute to the increase in the PM2.5 in the daytime, however, NPF events would occur during the night and the growth of particulate matter contributes to the nighttime PM2.5 contents. This could lead to pollution that lasted into the next day. These findings are significant to the improvement of our understanding of the effects of aerosols on air quality.

Potential influence of rapid climate change on elemental geochemistry distributions in lacustrine sediments-A case study at a high Arctic site in Ny-Ålesund, Svalbard.

Metal contamination has become an increasingly severe environmental issue due to intense anthropogenic activities in recent decades. Many studies have reported a rapidly increasing trend of heavy metal contents in sedimentary records. In this study, two lacustrine sediment cores (LDL and YL) far away from scientific research stations were collected in Ny-Ålesund and analyzed for the vertical distributions of 17 elemental concentrations (Cu, Zn, Pb, Co, Ni, Cr, Sr, Ba, Mn, P, Ti, K2O, Na2O, CaO, MgO, Fe2O3, Al2O3), CIA and TOC contents. The results indicated that only the proxies Pb, P, CaO, TOC, and CIA showed an increasing trend in the upper 7 cm section of the sediment cores, while most of the elements' concentrations decreased towards the surface. The rapid increase of TOC contents is likely related to the climate warming over the past 200 years, which promotes the prosperity of vegetation and thus leads to more input of organic matter into the lakes. Moreover, a large number of seabirds live around the sampling position and the seabird guano contains high concentrations of P, which could be regarded as an important nutrient source for vegetation. Additionally, the rapid climate warming could accelerate the chemical weathering rates, and thus lead to increased CaO contents in the sediment profiles according to its geological background. Therefore, the concentrations of other elements are very likely diluted by the high contents of organic matter and CaO in the upper part of the sediment cores. It is noteworthy that the rapidly increasing trend of Pb contents are related to the gas-oil powered generators in Ny-Ålesund and long-range atmospheric transport from Europe. This study highlighted the nonnegligible influence of climate warming on the inorganic elemental geochemistry distributions in remote lakes.

Effects of heavy metals speciations in sediments on their bioaccumulation in wild fish in rivers in Liuzhou-A typical karst catchment in southwest China.

Although fish are widely confirmed to be susceptible to heavy metals (HMs) contamination in sediments, this bioconversion haven't been detailed. This is especially the case in karst areas, where HMs are less stably retained in the sediments and are more bioavailable. Therefore, we surveyed representative karst rivers in Liuzhou, China, in order to study the relationship between the speciations of seven HMs in the sediments with their bioaccumulation in wild fish. The results showed that the HMs in sediments are all below their permissible exposure limit (PEL), but Cd and Zn are significantly higher than soil basline. Most HMs are in residual fraction, while their exchangeable fractions are present in extremely low proportions. The concentration of Zn, Cr and Cd in some fish are above their maximum recommended limit (MRL). The concentrations of most of the HMs in the fish are significantly correlated with the levels in the sediments and given the higher correlation coefficients for their carbonate-bound phase, this phase can be seen to play a critical role in HMs bioconversion. However, the presence of this phase in low proportions enables other phases, especially oxidizable form, to play a greater role in HMs bioaccumulation. Apart from Do, HMs in the fish samples are significantly correlated with multiple environmental factors, demonstrating environmental fluctuations can manipulate HMs bioconversion from sediments; however, their significance depend heavily on the proportion of particular species. HMs in reducible and oxidizable fraction are more important in regulating, rather than promoting, their bioconversion during environmental fluctuations. Fluctuations in EC, TDS and pH can increase the impacts of HMs in carbonate-bound fraction on their bioconversion. Given the higher background values of EC and TDS and lower pH values during the monsoon period, careful attention should be paid to the increased bioconversion of HMs in karst rivers during this season.

Detection of organosulfates and nitrooxy-organosulfates in Arctic and Antarctic atmospheric aerosols, using ultra-high resolution FT-ICR mass spectrometry.

Organosulfates (OSs) are recognized as important secondary organic aerosols (SOAs) in recent years. Due to their amphipathy and light absorptive capacity, OSs may potentially impact climate. Moreover, OSs can serve as molecular tracers for precursors and multiple processes leading to the generation of SOA. However, studies on OSs are lacking in the polar regions which limits our understanding of both their formation pathways and impacts on the polar environment. Here we present the first investigation into OSs in both the Arctic and Antarctic. Organic compounds in aerosol samples collected from the polar regions during the 2013/2014 Chinese National Arctic/Antarctic Research Expedition (CHINARE) were analyzed by Fourier transform ion cyclotron resonance mass spectrometry (FT-ICR-MS) coupled with negative ion mode electrospray ionization (ESI(-)). Hundreds to thousands of OSs were detected at the polar sampling sites. The estimated total concentrations of OSs were in the range of 46-670 ng/m3 in the Arctic sampling area, and 47-260 ng/m3 in the Antarctic sampling area, accounting for 1-16% of total OM. OSs were found to have undergone a high degree of oxidation in the aerosol samples, which might be due to the combined effects of enhanced photo-oxidation in summertime or continuous oxidation during transport to the polar region. The potential appointment of OS precursors highlights the important role of long-range air-mass transport on the OSs derived from biogenic precursors and a notably large contribution from anthropogenic emissions, suggesting that human activities have significant impacts in remote polar environments. The results of this study provide important insights into the characteristics of OSs in the polar atmosphere. However, the need for further research focusing on the quantification, formation mechanisms and impacts of OSs on climate is emphasized.

Volatilization of polycyclic aromatic hydrocarbons (PAHs) over the North Pacific and adjacent Arctic Ocean: The impact of offshore oil drilling.

Air and seawater samples were collected in 2016 over the North Pacific Ocean (NPO) and adjacent Arctic Ocean (AO), and Polycyclic Aromatic Hydrocarbons (PAHs) were quantified in them. Atmospheric concentrations of ∑15 PAHs (gas + particle phase) were 0.44-7.0 ng m-3 (mean = 2.3 ng m-3), and concentrations of aqueous ∑15 PAHs (dissolved phase) were 0.82-3.7 ng L-1 (mean = 1.9 ng L-1). Decreasing latitudinal trends were observed for atmospheric and aqueous PAHs. Results of diagnostic ratios suggested that gaseous and aqueous PAHs were most likely to be related to the pyrogenic and petrogenic sources, respectively. Three sources, volatilization, coal and fuel oil combustion, and biomass burning, were determined by the PMF model for gaseous PAHs, with percent contributions of 10%, 44%, and 46%, respectively. The 4- ring PAHs underwent net deposition during the cruise, while some 3- ring PAHs were strongly dominated by net volatilization, even in the high latitude Arctic region. Offshore oil/gas production activities might result in the sustained input of low molecular weight 3- ring PAHs to the survey region, and further lead to the volatilization of them. Compared to the gaseous exchange fluxes, fluxes of atmospheric dry deposition and gaseous degradation were negligible. According to the extrapolated results, the gaseous exchange of semivolatile aromatic-like compounds (SALCs) may have a significant influence on the carbon cycling in the low latitude oceans, but not for the high latitude oceans.