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Atmospheric gaseous elemental mercury (GEM), particulate bound mercury (PBM), and gaseous oxidized mercury (GOM) were continuously measured at a remote site in northeastern China from July 2013 to July 2014. Mean (±1SD) concentrations of the hourly data of GEM, PBM, and GOM were 1.68 ± 0.47 ng m−3, 16.6 ± 15.2 pg m−3, and 5.4 ± 6.4 pg m−3, respectively. Concentration-weighted trajectory (CWT) analysis suggested that the potential source regions of GEM and GOM observed at this site were northern and eastern China. GEM and GOM CWT values significantly correlated with anthropogenic Hg emissions, suggesting that long-range transport of anthropogenic Hg emissions played an important role in GEM and GOM pollutions in remote areas of northeastern China. On the other hand, long-range transport of anthropogenic PBM emissions from eastern and northeastern China combined with large-scale biomass burning in Northeast Asia likely dominated PBM pollution. Principal component analysis (PCA) results, making use of the combined data sets of speciated atmospheric Hg, trace elements, and meteorological parameters, suggested that coal combustion and non-ferrous metal smelting contributed significantly to all the Hg species at this site, while the other anthropogenic sources in China also had a major impact on GEM. Forward air mass trajectory analysis revealed that outflows of GEM from northeastern China may have a potential impact on GEM pollutions in remote and oceanic areas in Northeast Asia.

Isotopic composition of atmospheric particulate bound mercury (PBM) was obtained at four remote sites in different geographical regions of China for three to 12 month periods. Mean (±1σ) Δ199HgPBM was the highest at the site in southwestern China (0.66 ± 0.32‰), followed by the site in northeastern China (0.36 ± 0.34‰), the site in the marine boundary layer of East China Sea (0.35 ± 0.33‰), and was the lowest at the site in northwestern China (0.27 ± 0.22‰). Δ199HgPBM was relatively higher in cold than warm season at the sites in northwestern and southwestern China, whereas the opposite was found at the site in northeastern China. We propose that the seasonal variations of Δ199HgPBM were influenced by the exposure of air masses to regional (e.g., anthropogenic and dust related) and long-range (e.g., anthropogenic and oceanic) sources in the preceding several days, with the former characterized by lower Δ199HgPBM and the latter characterized by more positive Δ199HgPBM due to sufficient atmospheric transformations. Modeling results from Potential Source Contribution Function suggested that domestic anthropogenic emission was the major contributor to PBM pollution at the sites in northeastern and eastern China, whereas long-range transboundary transport of PBM from South Asia played a more important role at the sites in southwestern and northwestern China.

Fine particle (PM 2.5 ) samples were collected simultaneously at three urban sites (Shanghai, Nanjing, and Hangzhou) and one rural site near Ningbo in the Yangtze River Delta (YRD) region, China, on a weekly basis from September 2013 to August 2014. In addition, high-frequency daily sampling was conducted in Shanghai and Nanjing for one month during each season. Severe regional PM 2.5 pollution episodes were frequently observed in the YRD, with annual mean concentrations of 94.6 ± 55.9, 97.8 ± 40.5, 134 ± 54.3, and 94.0 ± 57.6 μg m −3 in Shanghai, Nanjing, Hangzhou, and Ningbo, respectively. The concentrations of PM 2.5 and ambient trace metals at the four sites showed clear seasonal trends, with higher concentrations in winter and lower concentrations in summer. In Shanghai, similar seasonal patterns were found for organic carbon (OC), elemental carbon (EC), and water-soluble inorganic ions (K + , NH 4 + , Cl − , NO 3 − , and SO 4 2- ). Air mass backward trajectory and potential source contribution function (PSCF) analyses implied that areas of central and northern China contributed significantly to the concentration and chemical compositions of PM 2.5 in Shanghai during winter. Three heavy pollution events in Shanghai were observed during autumn and winter. The modelling results of the Nested Air Quality Prediction Modeling System (NAQPMS) showed the sources and transport of PM 2.5 in the YRD during the three pollution processes. The contribution of secondary species (SOC, NH 4 + , NO 3 − , and SO 4 2- ) in pollution event (PE) periods was much higher than in BPE (before pollution event) and APE (after pollution event) periods, suggesting the importance of secondary aerosol formation during the three pollution events. Furthermore, the bioavailability of Cu, and Zn in the wintertime PM 2.5 samples from Shanghai was much higher during the pollution days than during the non-pollution days.

Characterizing the speciation and isotope signatures of atmospheric mercury (Hg) downwind of mainland China is critical to understanding the outflow of Hg emission and the contributing sources. In this study, we measured the concentrations of gaseous elemental mercury (GEM), particulate bound mercury, gaseous oxidized mercury, and the GEM isotopic composition in the marine boundary layer of East China Sea from October 2013 to January 2014. Mean (+/- 1 sigma) GEM, particulate bound mercury, and gaseous oxidized mercury concentrations were 2.25 +/- 1.03 ng/m(3), 26 +/- 38 pg/m(3), and 8 +/- 10 pg/m(3) respectively. Most events of elevated GEM are associated with the outflow of Hg emissions in mainland China. The 24- and 48-hr integrated GEM samples showed large variations in both delta Hg-202 (-1.63 parts per thousand to 0.34 parts per thousand) and Delta Hg-199 (-0.26 parts per thousand to -0.02 parts per thousand). GEM delta Hg-202 and Delta Hg-199 were negatively and positively correlated to its atmospheric concentrations, respectively, suggesting a binary physical mixing of regional background GEM and Hg emissions in mainland China. Using a binary mixing model, highly negative delta Hg-202 (-1.79 +/- 0.24 parts per thousand, 1 sigma) and near-zero Delta Hg-199 (0.02 +/- 0.04 parts per thousand,1 sigma) signatures for China GEM emissions are predicted. Such isotopic signatures are significantly different from those found in North America and Europe and the background global/regional atmospheric GEM pool. It is likely that emissions from industrial and residential coal combustion (lacking conventional air pollutant control devices), cement and mercury production, biomass burning, and soil emissions contributed significantly to the estimated isotope signatures of GEM emissions in China.

We measured the concentrations and profiles of polycyclic aromatic hydrocarbons (PAHs) in the soil, water, and rice tissues from a typical subtropical paddy system at various stages of rice growth over two growing seasons. Rice growth had a significant impact on the distribution and dissipation of PAHs in the paddy field. While rice was growing, the concentrations of PAHs in the soils decreased at an average decline rate of 5.3±2.9 ng PAHs g(-1) soild(-1), whereas, the concentrations of PAHs in rice tissues increased with growth time. However, the concentrations of PAHs in the rice leaves decreased during the heading stage of both two growing seasons. PAH profiles in soil, water, and different rice tissues also showed different patterns with the growing time of rice. Irrigation water was a significant source of PAHs to the paddy field. Rice growth enhanced the dissipation and transport of PAHs in the paddy system, while the sewage irrigation and straw burning after harvest added or returned PAHs to the system. For food safety precaution, sewage irrigation and straw burning should be well monitored and controlled.

Global warming has induced visible glacier retreat on many high mountains. The glacier forelands with the chronosequence and vegetation succession offer a good opportunity to assess natural (e.g., mineral weathering) and anthropogenic influence on trace element geochemical cycling in high mountain ecosystems. In the present study, the concentrations and isotope composition of lead (Pb) in soil profiles and mosses from the Hailuogou Glacier foreland in eastern Tibetan Plateau were investigated. The enrichment of Pb in the 0 and A horizons of soil layers and mosses indicated the influence from recently atmospheric deposition, while the local soil parent materials mainly affected the C horizon of soils. The lower Pb-206/Pb-207 (1.160-1.180) and higher Pb-208/Pb-206 (2.092-2.120) ratios were observed in the O horizon in comparison with the A (1.171-1.209 and 2.042-2.108, respectively) and C (1.183-1.206 and 2.070-2.130, respectively) horizons. The Pb isotope composition in the mosses was similar to those of the O horizon. The Pb-ore-involved industries and coal combustion in southwest China and South Asia were identified as the major sources of anthropogenic Pb at the glacier foreland. The estimations using binary mixing model indicated that the anthropogenic Pb contribution was about 45.2-61.3% for the O horizon, 8.6-34.8% for the A horizon, and 41.6-65.9% for the mosses. The results indicated that the anthropogenic Pb could reach the remote high mountains of eastern Tibetan Plateau through long distance atmospheric transport. (C) 2014 Elsevier Ltd. All rights reserved.

A new passive exchange meter (PEM) to measure inter-compartment fluxes of persistent organic pollutants (POPs) at the interface between soil and the atmosphere is described. The PEM uses labeled reference compounds (RC) added in-situ to vegetation litter deployed in open cylinders designed to trap the vertical downward export of the RCs while allowing free exchange of POPs between litter and air. Fluxes of native compounds (bulk deposition, volatilization and downward export) are quantitatively tracked. One scope of the PEM is to investigate the influence of biogeochemical controls on contaminant re-mobilization. The PEM performance was tested in a subtropical forest by comparing measurements under dense canopy and in a canopy gap; conditions in which deposition and turn-over of organic matter (OM) occur at different rates. Significant differences in fate processes were successfully detected. Surprisingly, mobilization by leaching of more hydrophobic compounds was higher under canopy, possibly as a result of canopy mediated enhancement of OM degradation.

The Chinese Gridded Pesticide Emission and Residue Model was applied to simulate long-term environmental fate of -hexachlorocyclohexane (HCH) in Asia spanning 1948 to 2008. The simulation identifies the southern Tibetan Plateau and the margin of the Asian monsoon regime from the northeast area of the Tibetan Plateau to the Northeast China as sink areas. This spatial pattern of sink distribution is closely related to the summer monsoon activities in Asia. Wet deposition associated with the summer monsoon (June to August) is responsible for at least half of the -HCH mass entering into the sink areas. After deposition, relatively low temperature and high soil organic matter in the sink areas are favorable for -HCH detention. Chinese and Indian sources are the major contributors to -HCH contamination over the monsoon margin and the Tibetan Plateau, driven by the East Asian summer monsoon and South Asian summer monsoon, respectively.

Fine particle (PM

Rice, one of the most widely cultivated crops, has received great attention in contaminant uptake from soil and air, especially for the special approaches used for its cultivation. The dry-wet alternation method can influence the air-soil partitioning of semivolatile organic compounds (SVOCs) in the paddy ecosystem. Here, we modified a fugacity sampler to investigate the air-surface in situ partitioning of ubiquitous polycyclic aromatic hydrocarbons (PAHs) at different growth stages in a suburban paddy field in South China. The canopy of rice can form a closed space, which acts like a chamber that can force the air under the canopy to equilibrate with the field surface. When we compared the fugacities calculated using a fugacity model of the partition coefficients to the measured fugacities, we observed similar trends in the variation, but significantly different values between different growing stages, especially during the flooding stages. However, the measured and calculated fugacity fractions were comparable when uncertainties in our calculations were considered, with the exception of the high molecular weight (HMW) PAHs. The measured fugacity fractions suggested that the HMW PAHs were also closed to equilibrium between the paddy field and atmosphere. The modified fugacity sampler provided a novel way of accurately determining the in situ air-soil partitioning of SVOCs in a wet paddy field.

The rice canopy in paddy fields can influence the air–soil exchange of organic chemicals. We used paired passive air samplers to assess the exchange of polycyclic aromatic hydrocarbons (PAHs) and organochlorine pesticides (OCPs) in a paddy field, South China. Levels of OCPs and light PAHs were generally higher under the canopy than above it. We found that the rice canopy can physically obstruct the evaporation of most OCPs and light PAHs, and can also act as a barrier to the gaseous deposition of p , p' -DDT and heavy PAHs. Paddy fields can behave as a secondary source of OCPs and light PAHs. The homolog patterns of these two types of chemical varied slightly between the air below and above the rice canopy, implying contributions of different sources. Paired passive air samplers can be used effectively to assess the in situ air–soil exchange of PAHs and OCPs in subtropical paddy fields.

Chinese Gridded Pesticide Emission and Residue Model was applied to simulate long-term environmental fate of beta-HCH in Asia spanning 1948-2009. The model captured well the spatiotemporal variation of beta-HCH soil concentrations across the model domain. beta-HCH use in different areas within the model domain was simulated respectively to assess the influence of the different sources of beta-HCH on its environment fate. A mass center of soil residue (MCSR) was introduced and used to explore environmental factors contributing to the spatiotemporal variation of beta-HCH soil residue. Results demonstrate that the primary emission dominates beta-HCH soil residues during the use of this pesticide. After phase-out of the pesticide in 1999, the change in beta-HCH soil residues has been associated with the Asian summer monsoon, featured by northward displacement of the MCSR. The displacement from several major sources in China and northeastern Asia shows a downward trend at a 95% confidence level, largely caused by environmental degradation and northward delivery of beta-HCH under cold condition in northern area. The MCSRs away from the India and southern and southeastern Asia sources show a rapid northward displacement at a 99% confidence level, featuring the cold trapping effect of the Tibetan Plateau.

Branched glycerol dialkyl glycerol tetraethers (GDGTs) were analyzed in peat samples taken from the Zoige grassland, located on the eastern margin of the Qinghai-Tibetan Plateau. The mean annual air temperature (MAAT) and pH in the 210Pb-dating peat core were reconstructed based on the cyclization of branched tetraethers (CBT) and methylation of branched tetraethers (MBT) indices for the last 150 years. The results showed that the MAAT and pH values involved three stages of variation over the last 150 years. The pH was stable and the MAAT decreased slowly by about 1°C from 1851 to 1927. The pH decreased rapidly by 0.6 and the MAAT decreased significantly by 2.5°C between 1927 and 1979. The pH and MAAT increased by 0.8 and 5°C, respectively, since the 1980s. The reconstructed temperatures correspond well to the mean winter temperatures reconstructed using tree-rings from the Jiuzhaigou Valley, situated at the boundary between the Qinghai-Tibetan Plateau and the Sichuan Basin. The estimated MAAT was similar to the temperatures reconstructed using tree-rings, indicating an increasing trend, as shown by local instrumental records from 1957 to 2001. These results provide further confidence in the application of proxies based on glycerol dialkyl glycerol tetraethers in peat records for continental paleoclimate reconstruction.

High-precision 210Pb dating technology was applied to a peat core with a time span of about 150 years that was taken from Hongyuan, Sichuan Province, China. The concentrations of total mercury (Hg) and stable isotope compositions of mercury in the peat core were measured using a LUMEX 915 instrument and multi-collector inductively coupled plasma mass spectrometer, respectively. Total mercury (Hg) concentrations in the peat core had a clearly increasing trend from the bottom to top of the core while δ202Hg values (relative to NIST 3133) of peat had a decreasing trend. The total mercury (Hg) concentration varied from 16.7 to 101.3 ng/g and the δ202Hg values ranged from −0.44‰ ± 0.14‰ to −1.45‰ ± 0.22‰. We clearly show that the study area experienced mercury pollution after the industrial revolution, and the mercury emitted from natural sources and anthropogenic sources had different Hg isotope signatures.