State Key Laboratory of Environmental Geochemistry

A panel of international experts was convened in Madison, Wisconsin, in 2005, as part of the 8th International Conference on Mercury as a Global Pollutant. Our charge was to address the state of science pertinent to source attribution, specifically our key question was: "For a given location, can we ascertain with confidence the relative contributions of local, regional, and global sources, and of natural versus anthropogenic emissions to mercury deposition?" The panel synthesized new research pertinent to this question published over the past decade, with emphasis on four major research topics: long-term anthropogenic change, current emission and deposition trends, chemical transformations and cycling, and modeling and uncertainty. Within each topic, the panel drew a series of conclusions, which are presented in this paper. These conclusions led us to concur that the answer to our question is a "qualified yes," with the qualification being dependent upon the level of uncertainty one is willing to accept. We agreed that the uncertainty is strongly dependent upon scale and that our question as stated is answerable with greater confidence both very near and very far from major point sources, assuming that the "global pool" is a recognizable "source." Many regions of interest from an ecosystem-exposure standpoint lie in between, where source attribution carries the greatest degree of uncertainty.

The accurate determination of the carbon neutrality capacity (CNC) of a region is crucial for developing policies related to emissions and climate change. However, a systematic diagnostic method for determining the CNC that considers the rock chemical weathering carbon sink (RCS) is lacking. Moreover, it is challenging but indispensable to establish a fast and practical index model to determine the CNC. Here, we selected Guizhou as the study area, used the methods for different types of carbon sinks, and constructed a CNC index (CNCI) model. We found that: (1) the carbonate rock chemical weathering carbon sink flux was 30.3 t CO2 km−2 yr−1. Guizhou accounted for 1.8% of the land area and contributed 5.4% of the carbonate chemical weathering carbon sink; (2) the silicate rock chemical weathering carbon sink and its flux were 1.44 × 103 t CO2 and 2.43 t CO2 km−2 yr−1, respectively; (3) the vegetation-soil ecosystem carbon sink and its flux were 1.37 × 108 t CO2 and 831.70 t CO2 km−2 yr−1, respectively; (4) the carbon emissions (CEs) were 280 Tg CO2, about 2.8% of the total for China; and (5) the total carbon sinks in Guizhou were 160 Tg CO2, with a CNCI of 57%, which is 4.8 times of China and 2.1 times of the world. In summary, we conducted a systematic diagnosis of the CNC considering the RCS and established a CNCI model. The results of this study have a strong implication and significance for national and global CNC determination and gap analysis.

The Hg isotopic signature may provide insight into tracking the sources and pathways of both airborne particulate matter (PM) and particle-bound Hg (PHg) in the atmosphere.

, methylmercury (MeHg)), are responsible for many adverse health effects, such as neurological and cardiovascular effects. The main source of Hg is from natural release. Nevertheless, with the development of industrialization and urbanization, Hg-contaminated soil mainly influenced by human activities (especially near mercury mining areas) has become a problem. Therefore, much more attention has been paid to the development and selection of various treatment methods to remediate Hg-contaminated soils. This paper presented a systematical review of the recent developments for the remediation of Hg-contaminated soils. Firstly, we briefly introduced the Hg chemistry, toxicity and the main human activity-related sources of mercury in soil. Then the advances in remediation technologies for removing Hg pollution from the soil were summarized. Usually, the remediation technology includes physical, chemical and biological remediation technology. Depending on this, we further classified these remediation technologies into six techniques, including thermal desorption, electrokinetic extraction, soil washing, chemical stabilization, phytoremediation and microbial technology. Finally, we also discussed the challenges and future perspectives of remediating Hg-contaminated soils.

Biochar-supported CNT and GO nanocomposites have provided new solutions for the removal of various environmental contaminants.

Abstract. Dynamic global vegetation models (DGVMs) typically rely on plant functional types (PFTs), which are assigned distinct environmental tolerances and replace one another progressively along environmental gradients. Fixed values of traits are assigned to each PFT; modelled trait variation along gradients is thus driven by PFT replacement. But empirical studies have revealed "universal" scaling relationships (quantitative trait variations with climate that are similar within and between species, PFTs and communities); and continuous, adaptive trait variation has been proposed to replace PFTs as the basis for next-generation DGVMs. Here we analyse quantitative leaf-trait variation on long temperature and moisture gradients in China with a view to understanding the relative importance of PFT replacement vs. continuous adaptive variation within PFTs. Leaf area (LA), specific leaf area (SLA), leaf dry matter content (LDMC) and nitrogen content of dry matter were measured on all species at 80 sites ranging from temperate to tropical climates and from dense forests to deserts. Chlorophyll fluorescence traits and carbon, phosphorus and potassium contents were measured at 47 sites. Generalized linear models were used to relate log-transformed trait values to growing-season temperature and moisture indices, with or without PFT identity as a predictor, and to test for differences in trait responses among PFTs. Continuous trait variation was found to be ubiquitous. Responses to moisture availability were generally similar within and between PFTs, but biophysical traits (LA, SLA and LDMC) of forbs and grasses responded differently from woody plants. SLA and LDMC responses to temperature were dominated by the prevalence of evergreen PFTs with thick, dense leaves at the warm end of the gradient. Nutrient (N, P and K) responses to climate gradients were generally similar within all PFTs. Area-based nutrients generally declined with moisture; Narea and Karea declined with temperature, but Parea increased with temperature. Although the adaptive nature of many of these trait-climate relationships is understood qualitatively, a key challenge for modelling is to predict them quantitatively. Models must take into account that community-level responses to climatic gradients can be influenced by shifts in PFT composition, such as the replacement of deciduous by evergreen trees, which may run either parallel or counter to trait variation within PFTs. The importance of PFT shifts varies among traits, being important for biophysical traits but less so for physiological and chemical traits. Finally, models should take account of the diversity of trait values that is found in all sites and PFTs, representing the "pool" of variation that is locally available for the natural adaptation of ecosystem function to environmental change.

Methylmercury (MeHg) is recognized as one of the major water quality concerns in the Florida Everglades. Degradation of MeHg in the water is thought to be one of the most important processes to the cycling of MeHg, but there is a lack of quantitative estimations of its effect on the distribution and cycling of MeHg in this ecosystem. Stable isotope (Me201Hg) addition method was implemented to investigate the degradation of MeHg in the Everglades. By combining these results with the field monitoring data, effects of photodegradation on MeHg distribution and its contribution to MeHg cycling were estimated. The results indicate that degradation of MeHg in Everglades water is mediated by sunlight and that UV-A and UV-B radiations are the principal driver. The spatial pattern of MeHg photodegradation potential (PPD) generally illustrated an increasing trend from north to south in the Everglades, which was opposite to the distribution of MeHg in water column. Correlation analysis shows that MeHg concentration in the water had a significant negative relation to PPD, suggesting that photodegradation could play an important role in controlling the distribution of MeHg in Everglades water. Furthermore, about 31.4% of MeHg input into the water body was removed by photodegradation, indicating its importance in the biogeochemical cycling of MeHg in the Everglades. This percent reduction is much lower than that reported for other ecosystems, which could be caused by the higher concentration of DOC in the Everglades. The relatively slower degradation of MeHg could be one of the main reasons for the high ratio of MeHg to total mercury (THg) in this ecosystem.

Providing quantitative information on the sources of PM2.5-bound polycyclic aromatic hydrocarbons (PAHs) in urban regions is vital to establish effective abatement strategies for air pollution in a megacity. In this study, based on a year data set from October 2011 to August 2012, the sources of PM2.5-bound 16 USEPA priority PAHs (16 PAHs) in Shanghai, a megacity in China, were apportioned by positive matrix factorization (PMF) modeling. The average concentrations (in ng m(-3)) of 16 PAHs in PM2.5 in the fall, winter, spring and summer were 20.5 ± 18.2, 27.2 ± 24.0, 13.7 ± 7.7 and 6.4 ± 8.1, respectively, with an annual average of 16.9 ± 9.0. The source apportionment by PMF indicated that coal burning (30.5%) and gasoline engine emission (29.0%) were the two major sources of PAHs in the PM2.5 in Shanghai, followed by diesel engine emission (17.5%), air-surface exchange (11.9%) and biomass burning (11.1%). The highest source contributor for PAHs in the fall and winter was gasoline engine emission (36.7%) and coal burning (41.9%), respectively; while in the spring and summer, it was diesel engine emission that contributed the most (52.1% and 43.5%, respectively). It was suggested that there was a higher contribution of PAHs from engine emissions in 2011-2012 compared with those in 2002-2003. The major sources apportioned by PMF complemented well with this of using diagnostic ratios, suggesting a convincing identification of sources for the PM2.5-bound 16 PAHs in a megacity.

The accuracy and precision of Cd isotope measurement at different injecting sample sizes.

Maple wood biochars were produced at different pyrolysis temperatures and residence times to investigate the effects of pyrolysis conditions and oxidation on the retention of ammonium in aqueous solution and adsorption and desorption was determined.

This study examined for the first time the Hg isotope composition in rain samples from a single precipitation event at Lhasa City (China) on the Tibetan Plateau, the “world's third pole”. Large variations of both mass-dependent fractionation (MDF, δ202Hg from -0.80‰ to -0.42‰) and mass-independent fractionation (MIF, Δ199Hg from 0.38‰ to 0.76‰) were observed, with the latter increasing with time. Our results demonstrated that the large variation of Hg isotope ratios likely resulted from mixing of locally emitted Hg and long-term transported Hg, which were characterized by different Hg isotope signatures and mainly leached by below-cloud scavenging and in-cloud scavenging processes, respectively. Our findings demonstrated that Hg isotopes are a powerful tool for investigating the dynamics of precipitation events and emphasized the importance of systematic monitoring studies of the chemical and isotope variability of Hg and other elements during rainfall events.

Abstract In contrast to larger river systems that drain relatively pristine basins, little is known about the sediment geochemistry of rivers impacted by intense human activities. In this paper, we present a systematic investigation of the anthropogenic overprints on element geochemistry in sediments of the human‐impacted Seine River, France. Most elements are fractionated by grain size, as shown by the comparison between suspended particulate matter (SPM) and riverbank deposits (RBD). The RBD are particularly coarse and enriched in carbonates and heavy minerals and thus in elements such as Ba, Ca, Cr, Hf, Mg, Na, REEs, Sr, Ti, Th, and Zr. Although the enrichment/depletion pattern of some elements (e.g., K, REEs, and Zr) can largely be explained by a binary mixture between two sources, other elements such as Ag, Bi, Cr, Cd, Co, Cu, Fe, Mo, Ni, Pb, Sb, Sn, W, and Zn in SPM in Paris show that a third end‐member having anthropogenic characteristics is needed to account for their enrichment at low water stage. These “anthropophile” elements, with high enrichment factors (EFs) relative to the upper continental crust (UCC), display a progressive enrichment downstream and different geochemical behaviors with respect to the hydrodynamic conditions (e.g., grain size) compared to elements having mainly a natural origin. Our findings emphasize the need for systematic studies of these anthropophile elements in other human‐impacted rivers using geochemical normalization techniques, and stress the importance of studying the chemical variability associated with hydrodynamic conditions when characterizing riverine element geochemistry and assessing their flux to the ocean.

Paddy soils from mercury (Hg)-contaminated rice fields in Guizhou, China were studied with respect to total mercury (THg) and methylmercury (MeHg) concentrations as well as Bacterial and Archaeal community composition. Total Hg (0.25-990 μg g-1) and MeHg (1.3-30.5 ng g-1) varied between samples. Pyrosequencing (454 FLX) of the hypervariable v1-v3 regions of the 16S rRNA genes showed that Proteobacteria, Actinobacteria, Chloroflexi, Acidobacteria, Euryarchaeota, and Crenarchaeota were dominant in all samples. The Bacterial α-diversity was higher in samples with relatively Low THg and MeHg and decreased with increasing THg and MeHg concentrations. In contrast, Archaeal α-diversity increased with increasing of MeHg concentrations but did not correlate with changes in THg concentrations. Overall, the methylation gene hgcAB copy number increased with both increasing THg and MeHg concentrations. The microbial communities at High THg and High MeHg appear to be adapted by species that are both Hg resistant and carry hgcAB genes for MeHg production. The relatively high abundance of both sulfate-reducing δ-Proteobacteria and methanogenic Archaea, as well as their positive correlations with increasing THg and MeHg concentrations, suggests that these microorganisms are the primary Hg-methylators in the rice paddy soils in Guizhou, China.

A flexible, easy and highly efficient Cr purification method was developed for high-precision measurement of Cr isotopes by double-spike MC-ICP-MS.

The study of heavy metal speciation is of interest for the evaluation of their ecotoxicological risk. Free heavy metal ion concentrations of Cu2+, Zn2+, Ni2+ and Cd2+ were studied at different soil to soil solution ratio (SSR) to discuss metal bioavailability and toxicity in circumstance. The samples were collected from two farmed soils, impacted by a cadmium rich zinc deposit, Guizhou, China. One is near a bridge (QBT for short), which is 15 km away from smelter and is regarded as polluted by fly ash from smelter, the other is located 300 m away from a smelting factory (BXT for short), and it is polluted badly by waste water from smelter. To determine the free heavy metal ion concentration, Donnan Membrane Technique (DMT) and ECOSAT program were used. The concentrations of free copper and zinc ions in QBT and all studied metal ions in BXT were nearly in direct ratio with the soil to soil solution ratio, and they increased with the increasing of SSR. The variational trends of the concentrations of free nickel and cadmium ions in QBT were contrary to those of copper and zinc ions. The measured and predicted results were compared and they agreed with each other. Individual sorbents contribution to metal binding was also predicted. The results suggest soil organic matter is the most important sorbents in the two soils, and hydrous ferric oxide takes the second place.

An inexpensive, simple and low-blank Ni purification method is presented for the high-precision measurement of Ni isotopes by double-spike MC-ICP-MS.

A new method is developed to meet the criteria for precise and efficient measurements of mercury isotopic composition in various water samples.

This study proposes a “waste-to-resource” strategy by reusing the incineration ash of municipal wastewater sludge as a ceramic material to immobilize copper.

Abstract. A process-oriented niche specification (PONS) model was constructed to quantify climatic controls on the distribution of ecosystems, based on the vegetation map of China. PONS uses general hypotheses about bioclimatic controls to provide a "bridge" between statistical niche models and more complex process-based models. Canonical correspondence analysis provided an overview of relationships between the abundances of 55 plant communities in 0.1° grid cells and associated mean values of 20 predictor variables. Of these, GDD0 (accumulated degree days above 0 °C), Cramer–Prentice α (an estimate of the ratio of actual to equilibrium evapotranspiration) and mGDD5 (mean temperature during the period above 5 °C) showed the greatest predictive power. These three variables were used to develop generalized linear models for the probability of occurrence of 16 vegetation classes, aggregated from the original 55 types by k-means clustering according to bioclimatic similarity. Each class was hypothesized to possess a unimodal relationship to each bioclimate variable, independently of the other variables. A simple calibration was used to generate vegetation maps from the predicted probabilities of the classes. Modelled and observed vegetation maps showed good to excellent agreement (κ = 0.745). A sensitivity study examined modelled responses of vegetation distribution to spatially uniform changes in temperature, precipitation and [CO2], the latter included via an offset to α (based on an independent, data-based light use efficiency model for forest net primary production). Warming shifted the boundaries of most vegetation classes northward and westward while temperate steppe and desert replaced alpine tundra and steppe in the southeast of the Tibetan Plateau. Increased precipitation expanded mesic vegetation at the expense of xeric vegetation. The effect of [CO2] doubling was roughly equivalent to increasing precipitation by ~ 30%, favouring woody vegetation types, particularly in northern China. Agricultural zones in northern China responded most strongly to warming, but also benefited from increases in precipitation and [CO2]. These results broadly conform to previously published findings made with the process-based model BIOME4, but they add regional detail and realism and extend the earlier results to include cropping systems. They provide a potential basis for a broad-scale assessment of global change impacts on natural and managed ecosystems.

A new purification approach is reported for the highly precise and accurate determination of Sb isotope ratios in geological samples.