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We apply the regional chemistry-transport model WRF-Chem to investigate the air pollution characteristics in three Chinese metropolitan areas (Beijing, Shanghai and Guangzhou) and assess the model performance in wintertime (January 2010) and summertime (July 2010) conditions. Three simulations utilizing the HTAPv2, REASv2 and MACCity anthropogenic emission inventories are conducted and compared with satellite and ground-based measurements to assess the sensitivity of the model predictions to anthropogenic emissions. Model-predicted surface meteorological fields are overall in good agreement with surface observations. However, the model tends to overestimate maximum surface wind speed, a feature also found in previous WRF-Chem modelling studies. Large discrepancies between the three emission inventories are found, specifically in the spatial distribution and the magnitude of the emissions (e.g. over 98%, 86% and 85% differences in some regions for carbon monoxide (CO), nitrogen oxide (NO) and organic carbon (OC) emissions, respectively). As a result, we find large differences between the simulations. When compared to satellite and surface observations, the HTAPv2-and REASv2-based simulations better reproduce the magnitude and spatial patterns of CO total columns and NO2 tropospheric columns derived from MOPITTv6 and GOME2 satellite observations, respectively. The simulations satisfactorily reproduce the air pollution characteristics in January 2010 as observed at surface monitoring stations in Beijing and Shanghai. The HTAPv2-based simulation better captures the pollution episode that occurred in Beijing in mid-January 2010, which is found to be related to a combination of different meteorological factors that led to the build-up of pollution. The high photochemical activity and convective turbulence in July 2010, in addition to differences in the emissions used, led to more pronounced differences between the simulations and lower statistical skills in particular for trace gases. This study shows that a considerable part of uncertainties in air quality model predictions for China can be attributed to uncertainties in current anthropogenic emission inventories. It highlights the need for more accurate and highly resolved emissions in order to improve the accuracy of model predictions. However, this study reveals that in some cases, model-observation discrepancies cannot be attributed only to inaccuracies in the emissions. For example, we found that regardless of the adopted emissions, all of the simulations fail to capture the temporal variability of particulate matter in Guangzhou during January 2010, indicating that factors other than emissions have a considerable influence on the atmospheric composition in this region. This work shows that inaccuracies in the predicted meteorological parameters (e.g. wind speed/direction, relative humidity, etc.) significantly affect the model performance, as found for example in the model predictions for Shanghai for July 2010, which show high and abrupt increases of NOx and particulates due to rapid decreases in wind speed in the model.

International audience; Increasing use of emerging per- and polyfluoroalkyl substances (PFASs) has caused extensive concerns around the world. Effective detection methods to trace their pollution characteristics and environmental behaviors in complex soil-crop systems are urgently needed. In this study, a reliable and matrix effect (ME)-free method was developed for simultaneous determination of 14 legacy and emerging PFASs, including perfluorooctanoic acid, perfluorooctane sulfonate, 6 hydrogenous PFASs, 3 chlorinated PFASs, and 3 hexafluoropropylene oxide homologues, in 6 crop (the edible parts) and 5 soil matrices using ultrasonic extraction combined with solid-phase extraction and ultraperformance liquid chromatography-mass spectrometry (MS)/MS. The varieties of extractants and cleanup cartridges, the dosage of ammonia hydroxide, and the ME were studied to obtain an optimal pretreatment procedure. The developed method had high sensitivity and accuracy with satisfactory method detection limits (2.40-83.03 pg/g dry weight) and recoveries (72-117%) of all target analytes in matrices at five concentrations, that is, 0.1, 1, 10, 100, and 1000 ng/g. In addition, the ME of this method (0.82-1.15) was negligible for all PFASs, even considering 11 different matrices. The successful application of the ME-free method to simultaneously determine the legacy and emerging PFASs in crop and soil samples has demonstrated its excellent practicability for monitoring emerging PFASs in soil-crop systems.

The fern Dicranopteris linearis (Gleicheniaceae) from China is a hyperaccumulator of rare earth element (REE), but little is known about the ecophysiology of REE in this species. This study aimed to clarify tissue-level and organ-level distribution of REEs via synchrotron-based X-ray fluorescence microscopy (XFM). The results show that REEs (La + Ce) are mainly colocalized with Mn in the pinnae and pinnules, with the highest concentrations in necrotic lesions and lower concentrations in veins. In the cross sections of the pinnules, midveins, rachis, and stolons, La + Ce and Mn are enriched in the epidermis, vascular bundles, and pericycle (midvein). In these tissues, Mn is localized mainly in the cortex and mesophyll. We hypothesize that the movement of REEs in the transpiration flow in the veins is initially restricted in the veins by the pericycle between vascular bundle and cortex, while excess REEs are transported by evaporation and cocompartmentalized with Mn in the necrotic lesions and epidermis in an immobile form, possibly a Si-coprecipitate. The results presented here provide insights on how D. linearis regulates high concentrations of REEs in vivo, and this knowledge is useful for developing phytotechnological applications (such as REE agromining) using this fern in REE-contaminated sites in China.

The OceanGliders program started in 2016 to support active coordination and enhancement of global glider activity. OceanGliders contributes to the international efforts of the Global Ocean Observation System (GOOS) for Climate, Ocean Health, and Operational Services. It brings together marine scientists and engineers operating gliders around the world: (1) to observe the long-term physical, biogeochemical, and biological ocean processes and phenomena that are relevant for societal applications; and, (2) to contribute to the GOOS through real-time and delayed mode data dissemination. The OceanGliders program is distributed across national and regional observing systems and significantly contributes to integrated, multi-scale and multi-platform sampling strategies. OceanGliders shares best practices, requirements, and scientific knowledge needed for glider operations, data collection and analysis. It also monitors global glider activity and supports the dissemination of glider data through regional and global databases, in real-time and delayed modes, facilitating data access to the wider community. OceanGliders currently supports national, regional and global initiatives to maintain and expand the capabilities and application of gliders to meet key global challenges such as improved measurement of ocean boundary currents, water transformation and storm forecast.

A large fraction of fossil fuel CO2 emissions emanate from “hotspots”, such as cities (where direct CO2 emissions related to fossil fuel combustion in transport, residential, commercial sectors, etc., excluding emissions from electricity-producing power plants, occur), isolated power plants, and manufacturing facilities, which cover a small fraction of the land surface. The coverage of all high-emitting cities and point sources across the globe by bottom-up inventories is far from complete, and for most of those covered, the uncertainties in CO2 emission estimates in bottom-up inventories are too large to allow continuous and rigorous assessment of emission changes (Gurney et al., 2019). Space-borne imagery of atmospheric CO2 has the potential to provide independent estimates of CO2 emissions from hotspots. But first, what a hotspot is needs to be defined for the purpose of satellite observations. The proposed space-borne imagers with global coverage planned for the coming decade have a pixel size on the order of a few square kilometers and a XCO2 accuracy and precision of  ppm for individual measurements of vertically integrated columns of dry-air mole fractions of CO2 (XCO2). This resolution and precision is insufficient to provide a cartography of emissions for each individual pixel. Rather, the integrated emission of diffuse emitting areas and intense point sources is sought. In this study, we characterize area and point fossil fuel CO2 emitting sources which generate coherent XCO2 plumes that may be observed from space. We characterize these emitting sources around the globe and they are referred to as “emission clumps” hereafter. An algorithm is proposed to identify emission clumps worldwide, based on the ODIAC global high-resolution 1 km fossil fuel emission data product. The clump algorithm selects the major urban areas from a GIS (geographic information system) file and two emission thresholds. The selected urban areas and a high emission threshold are used to identify clump cores such as inner city areas or large power plants. A low threshold and a random walker (RW) scheme are then used to aggregate all grid cells contiguous to cores in order to define a single clump. With our definition of the thresholds, which are appropriate for a space imagery with 0.5 ppm precision for a single XCO2 measurement, a total of 11 314 individual clumps, with 5088 area clumps, and 6226 point-source clumps (power plants) are identified. These clumps contribute 72 % of the global fossil fuel CO2 emissions according to the ODIAC inventory. The emission clumps is a new tool for comparing fossil fuel CO2 emissions from different inventories and objectively identifying emitting areas that have a potential to be detected by future global satellite imagery of XCO2. The emission clump data product is distributed from https://doi.org/10.6084/m9.figshare.7217726.v1.

International audience

Thallium (Tl) is a toxic trace metal, whose geochemical behavior and biological effects are closely controlled by its chemical speciation in the environment. However, little tends to be known about this speciation of Tl in soil and plant systems that directly affect the safety of food supplies. In this context, the objective of the present study was to elaborate an efficient method to separate and detect Tl(I) and Tl(III) species for soil and plant samples. This method involves the selective adsorption of Tl(I) on microcolumns filled with immobilized oxine, in the presence of DTPA (diethylenetriaminepentaacetic acid), followed by DTPA-enhanced ultrasonic and heating-induced extraction, coupled with ICP-MS detection. The method was characterized by a LOD of 0.037 μg/L for Tl(I) and 0.18 μg/L for Tl(III) in 10 mL samples. With this method, a second objective of the research was to assess the speciation of Tl in pot and field soils and in green cabbage crops. Experimental results suggest that DTPA extracted Tl was mainly present as Tl(I) in soils (>95%). Tl in hyperaccumulator plant green cabbage was also mainly present as Tl(I) (>90%). With respect to Tl uptake in plants, this study provides direct evidence that green cabbage mainly takes up Tl(I) from soil, and transports it into the aboveground organs. In soils, Tl(III) is reduced to Tl(I) even at the surface where the chemical environment promotes oxidation. This observation is conducive to understanding the mechanisms of Tl isotope fractionation in the soil-plant system. Based on geochemical fraction studies, the reducible fraction was the main source of Tl getting accumulated by plants. These results indicate that the improved analytical method presented in this study offers an economical, simple, fast, and sensitive approach for the separation of Tl species present in soils at trace levels.

The well-documented energy balance dynamics within forest ecosystems are poorly implemented in studies of the biophysical effects of forests. This results in limitations to the accurate quantification of forest cooling/warming on local air temperature. Taking into consideration the forest air space, this study proposes a three-layered (canopy, forest air space and soil [CAS]) land surface energy balance model to simulate air temperature within forest spaces (Taf) and subsequently to evaluate its biophysical effects on forest cooling/warming, i.e., the air temperature gradient (∆Ta) between the Taf and air temperature of open spaces (Tao) (∆Ta = Taf − Tao). We test the model using field data for 23 sites across 10 cities worldwide; the model shows satisfactory performance with the test data. High-latitude forests show greater seasonal dynamics of ∆Ta, generating considerable cooling of local air temperatures in warm seasons but minimal cooling or even warming effects during cool seasons, while low-latitude tropical forests always exert cooling effects with less interannual variability. The interannual dynamics of ∆Ta are significantly related to the seasonality of solar geometry and canopy leaf phenology. The differences between forest canopy temperature (Tc) and Tao, which are the two most important terms attributed by the CAS model in impacting Taf, explain a large part of forest cooling and warming (May–July: R2 = 0.35; November–January: R2 = 0.51). The novel CAS model provides a feasible way to represent the energy balance within forest ecosystems and to assess its impacts on local air temperatures globally. Keywords: Forest cooling/warming, Forest biophysical effects, Radiative transfer equation, Land-atmosphere model, Local environmental health, Climate warming mitigation

Metals can be immobilized on biochars by precipitation with carbonate. The distribution of metal-carbonate phases at the surface of biochars and the conditions of their formation, however, are unknown. Electron microscopy and X-photon spectroscopy were used to characterize carbonate phases in various morphological groups of particles of a wood-derived biochar, both before and after a metal-sorption experiment. Our results showed that the distribution of metals at the surface of biochar particles depended on the corresponding wood tissues and the presence of carbonate phases. Metals were particularly concentrated (i) within calcium carbonate crystals in bark-derived particles, which originated from calcium oxalate crystals formed prior to pyrolysis, and (ii) as new phases formed by the reprecipitation of carbonate on specific tissues of biochar. The formation of biochar carbonate phases and their redistribution by dissolution-precipitation mechanisms may primarily control the localization of metals on biochar particles and the durability of metals immobilization.

Dissolved organic matter (DOM) released from forest leaf litter is potentially effective for the degradation of polycyclic aromatic hydrocarbons (PAHs), yet the inherent mechanism remains insufficiently elucidated.[br/] In this study, we investigated the effects of DOM derived from Pinus elliottii and Schima superba leaf litter on the degradation of phenanthrene by the phenanthrene degrading bacterium Sphingobium sp. Phe-1. DOM from different origins and at a large range of concentrations enhanced the degradation rate of phenanthrene. DOM derived from P. elliottii leaf litter decomposed for 12 months used at a concentration of 100mg/L yielded the highest degradation rate (16.9% in 36h) and shortened the degradation time from 48h to 24h.[br/] Changes in the composition of DOM during degradation as measured by EEMs-FRI showed that proteins and tyrosine in the DOM supplied readily available nutrients that stimulated biological activity of Phe-1, increasing its growth rate and catechol 2,3-dioxygenase activity. Simultaneously, fulvic acid and humic acid in the DOM enhanced phenanthrene bioavailability by increasing the solubility and mass transfer of phenanthrene, enhancing the uptake kinetics of Phe-1, and increasing the bacteria's direct access to DOM-associated phenanthrene.[br/] Humic acid was co-metabolized by Phe-1, resulting in further stimulation of phenanthrene degradation.

Pyrolyzing sludge into biochar is a potentially promising recycling/disposal solution for municipal wastewater sludge, and the sludge-derived biochar (SDBC) presents an excellent sorbent for metal immobilization. As SDBC is composed of both mineral oxides and carbonized organic compartment, this study therefore compared the sorption behaviour of Pb and Zn on SDBC to those of individual and mixture of activated carbon (AC) and amorphous aluminium oxide (Al2O3). Batch experiments were conducted at 25 and 45 °C, and the metal-loaded sorbents were artificially aged in the atmosphere for 1–60 days followed by additional sorption experiments. The Pb sorption was generally higher than Zn sorption, and the co-presence of Pb reduced Zn sorption on each studied sorbent. Higher sorption capacities were observed at 45 °C than 25 °C for SDBC and AC, while the opposite was shown for Al2O3, indicating the significance of temperature-dependent diffusion processes in SDBC and AC. Nevertheless, metal sorption was more selective on Al2O3 that showed a greater affinity towards Pb over Zn under competition, correlating with the reducible fraction of sequential extraction. Furthermore, significant amounts of Pb and Zn were additionally sorbed on SDBC following 30-day ageing. The X-ray diffraction revealed the formation of metal-phosphate precipitates, while the X-ray photoelectron spectroscopy showed a larger quantity of metal–oxygen bonding after 30-day ageing of metal-loaded SDBC. The results may imply favourable long-term transformation and additional sorption capacity of SDBC. In conclusion, SDBC resembles the sorption characteristics of both organic and mineral sorbents in different aspects, presenting an appropriate material for metal immobilization during soil amendment.

International audience; With fast economic growth and development China is experiencing severe air pollution episodes related to rapid industrialization and urbanization since more than three decades. Through collaboration between 7 European and 7 Chinese research universities and institutes, the PANDA (Partnership with China on Space Data) EU-funded project aims to improve our understanding of the processes responsible for the formation, dispersion and destruction of air pollutants in East Asia. By combining space and in-situ observations and surface emissions of chemical pollutants with global and regional models of atmospheric composition, detailed analyses and reliable forecasts of regional air quality are produced with the aim of improving methods for monitoring and forecasting air quality in East Asia.Using a multi-model approach based on several global and regional state-of the art model simulations, we present detailed modeling studies of recent notorious haze events in East Asia (winter 2010 and 2013 haze events). We will demonstrate the effect of uncertainties and differences in current emission inventories for China and their resolution and temporal variation on model performance. We will focus especially on major city clusters that have experienced intense urbanization and population growth. The importance of using a downscaling approach to better reproduce and predict air pollution events that occur in East Asia will be discussed. The relation between the performance of the models and the complexity of their chemistry and aerosol schemes and choice of boundary and atmospheric forcing will be assessed. We will also present results of the air quality forecasting system being developed within PANDA and in collaboration with the EU project MarcoPolo.

Mechanisms of cadmium (Cd)-induced inhibition of photosynthesis in the Zn/Cd hyperaccumulator Picris divaricata were investigated using photosynthesis limitation analysis. P. divaricata seedlings were grown in nutrient solution containing 0, 5, 10, 25, 50, or 75 μM Cd for 2 weeks. Total limitations to photosynthesis (TL) increased from 0% at 5 μM Cd to 68.8% at 75 μM Cd. CO2 diffusional limitation (DL) made the largest contribution to TL, accounting for 93-98% of TL in the three highest Cd treatments, compared to just 2-7% of TL attributable to biochemical limitation (BL). Microscopic imaging revealed significantly decreased stomatal density and mesophyll thickness in the three highest Cd treatments. Chlorophyll fluorescence parameters related to photosynthetic biochemistry (Fv/Fm, NPQ, ΦPSII, and qP) were not significantly decreased by increased Cd supply. Our results suggest that increased DL in leaves is the main cause of Cd-induced inhibition of photosynthesis in P. divaricata, possibly due to suppressed function of mesophyll and stomata. Analysis of chlorophyll fluorescence showed that Cd supply had little effect on photochemistry parameters, suggesting that the PSII reaction centers are not a main target of Cd inhibition of photosynthesis in P. divaricata.

The development and implementation of a three-dimensional ocean modeling system for the Prince William Sound (PWS) is described. The system consists of a regional ocean model component (ROMS) forced by output from a regional atmospheric model component (the Weather Research and Forecasting Model, WRF). The ROMS ocean model component has a horizontal resolution of 1 km within PWS and utilizes a recently-developed multi-scale 3DVAR data assimilation methodology along with freshwater runoff from land obtained via real-time execution of a digital elevation model. During the Sound Predictions Field Experiment (July 19–August 3, 2009) the system was run in real-time to support operations and incorporated all available real-time streams of data. Nowcasts were produced every 6 h and a 48-h forecast was performed once a day. In addition, a sixteen-member ensemble of forecasts was executed on most days. All results were published at a web portal ( http://ourocean.jpl.nasa.gov/PWS ) in real time to support decision making. The performance of the system during Sound Predictions 2009 is evaluated. The ROMS results are first compared with the assimilated data as a consistency check. RMS differences of about 0.7 °C were found between the ROMS temperatures and the observed vertical profiles of temperature that are assimilated. The ROMS salinities show greater discrepancies, tending to be too salty near the surface. The overall circulation patterns observed throughout the Sound are qualitatively reproduced, including the following evolution in time. During the first week of the experiment, the weather was quite stormy with strong southeasterly winds. This resulted in strong north to northwestward surface flow in much of the central PWS. Both the observed drifter trajectories and the ROMS nowcasts showed strong surface inflow into the Sound through the Hinchinbrook Entrance and strong generally northward to northwestward flow in the central Sound that was exiting through the Knight Island Passage and Montague Strait entrance. During the latter part of the second week when surface winds were light and southwesterly, the mean surface flow at the Hinchinbrook Entrance reversed to weak outflow and a cyclonic eddy formed in the central Sound. Overall, RMS differences between ROMS surface currents and observed HF radar surface currents in the central Sound were generally between 5 and 10 cm/s, about 20–40% of the time mean current speeds. The ROMS reanalysis is then validated against independent observations. A comparison of the ROMS currents with observed vertical current profiles from moored ADCPs in the Hinchinbrook Entrance and Montague Strait shows good qualitative agreement and confirms the evolution of the near surface inflow/outflow at these locations described above. A comparison of the ROMS surface currents with drifter trajectories provided additional confirmation that the evolution of the surface flow described above was realistic. Forecasts of drifter locations had RMS errors of less than 10 km for up to 36 h. One and two-day forecasts of surface temperature, salinity and current fields were more skillful than persistence forecasts. In addition, ensemble mean forecasts were found to be slightly more skillful than single forecasts. Two case studies demonstrated the system’s qualitative skill in predicting subsurface changes within the mixed layer measured by ships and autonomous underwater vehicles. In summary, the system is capable of producing a realistic evolution of the near-surface circulation within PWS including forecasts of up to two days of this evolution. Use of the products provided by the system during the experiment as part of the asset deployment decision making process demonstrated the value of accurate regional ocean forecasts in support of field experiments.

International audience; We examine the characteristics of the spatial distribution and variability of tropospheric ozone (O3) by analysis of 93 ozonesonde profiles obtained at five stations over south China (18-30°N) during a field campaign in April-May 2004. We use a global 3-D chemical transport model (GEOS-Chem) to interpret these characteristics and to quantify the sources of tropospheric O3 over south China during this period. The observed tropospheric O3 mixing ratios showed strong spatiotemporal variability due to a complex interplay of various dynamical and chemical processes. A prominent feature in the upper and middle troposphere (UT/MT) was the frequent occurrence of high O3 mixing ratios shown as tongues extending down from the lower stratosphere or as isolated layers at all stations. The model largely captured the observed pattern of day-to-day variability in tropospheric O3 mixing ratios at all stations, but often underestimated those tongues or isolated layers of O3 enhancements observed in the UT/MT, especially at low-latitude stations. We found that tropospheric O3 along the southeast China coast was mainly produced within Asia. Lightning NOx emissions (over South Asia and equatorial Africa) and/or stratospheric influences were responsible for major events of high O3 observed in the UT/MT at all stations. Underestimated contributions of these sources likely led to the model's underestimate in the low-latitude UT/MT O3. This study emphasizes the need for improved understanding of lightning NOx emissions and stratospheric influences over the Eurasian and African continents and for better representation of these processes in current global models.

International audience; This paper presents a review of soil contamination resulting from e-waste recycling activities, with a special focus on China, where many data have been collected for a decade. Soils in the e-waste areas are often contaminated by heavy metals and organic compounds, mainly polycyclic aromatic hydrocarbons (PAHs), polybrominated diphenyl ethers (PBDEs), polychlorinated and polybrominated biphenyls (PCBs and PBBs), dechlorane plus (DP), hexabromocyclododecanes (HBCDs), polychlorinated and polybrominated dibenzo- p-dioxins (PCDDs and PBDDs), and polychlorinated and polybrominated dibenzofurans (PCDFs and PBDFs), while other compounds, not systematically monitored, can be found as well. Pollutants are generally present in mixtures, so pollution situations are complex and diversi¯ed with a gradient of contamination from agricultural soils to hot spots at e-waste sites and mainly in open burning areas. It has been proved that pollutants were transferred to the food chain via rice in China, and that the population was threatened since high levels of various pollutants were detected in blood, placentas, hair, etc., of residents of e-waste sites. Eventually, soil remediation techniques are reviewed. Although there are many available techniques devoted to heavy metals and persistent organic pollutants, the current techniques for the e-waste sites, where these contaminants coexist, are very sparse. Phytoremediation has been investigated and co-cropping appears as a promising approach for the slightly contaminated agricultural soils. In some cases, di®erent remediation techniques should be combined or trained, while the in°uence of coexisting contaminants and the removal sequence of contaminants should be considered. In hot spots, physical and chemical techniques should be used to reduce high pollution levels to prevent further pollutant dissemination. This review highlights the urgent needs for 1) characterization of pollution status in all the countries where e-wastes are recycled, 2) research on fate and toxicity of pollutant mixtures, and 3) development of combined techniques and strategies to remediate agricultural ¯elds and hot spots of pollution