Coastal marine atmospheric fog has recently been implicated as a potential source of ocean-derived monomethylmercury (MMHg) to coastal terrestrial ecosystems through the process of sea-to-land advection of foggy air masses followed by wet deposition. This study examined whether pumas (
- NSF-PAR ID:
- 10153770
- Publisher / Repository:
- Nature Publishing Group
- Date Published:
- Journal Name:
- Scientific Reports
- Volume:
- 9
- Issue:
- 1
- ISSN:
- 2045-2322
- Format(s):
- Medium: X
- Sponsoring Org:
- National Science Foundation
More Like this
-
Mercury (Hg), a neurotoxic heavy metal, is transferred to marine and terrestrial ecosystems through atmospheric transport. Recent studies have highlighted the role of vegetation uptake as a sink for atmospheric elemental mercury (Hg0) and a source of Hg to soils. However, the global magnitude of the Hg0 vegetation uptake flux is highly uncertain, with estimates ranging 1000–4000 Mg per year. To constrain this sink, we compare simulations in the chemical transport model GEOS-Chem with a compiled database of litterfall, throughfall, and flux tower measurements from 93 forested sites. The prior version of GEOS-Chem predicts median Hg0 dry deposition velocities similar to litterfall measurements from Northern hemisphere temperate and boreal forests (~0.03 cm s-1 yet it underestimates measurements from a flux tower study (0.04 cm s-1 vs. 0.07 cm s-1and Amazon litterfall (0.05 cm s-1 vs. 0.17 cm s-1). After revising the Hg0 reactivity within the dry deposition parametrization to match flux tower and Amazon measurements, GEOS-Chem displays improved agreement with the seasonality of atmospheric Hg0 observations in the Northern midlatitudes. Additionally, the modelled bias in Hg0 concentrations in South America decreases from +0.21 ng m-3 +0.05 ng m-3. We calculate a global flux of Hg0 dry deposition to land of 2276 Mg per year, approximately double previous model estimates. The Amazon rainforest contributes 29% of the total Hg0 land sink, yet continued deforestation and climate change threatens the rainforest's stability and thus its role as an important Hg sink. In an illustrative worst-case scenario where the Amazon is completely converted to savannah, GEOS-Chem predicts that an additional 283 Mg Hg per year would deposit to the ocean, where it can bioaccumulate in the marine food chain. Biosphere–atmosphere interactions thus play a crucial role in global Hg cycling and should be considered in assessments of future Hg pollution.more » « less
-
Abstract Torrential rain and extreme flooding caused by Atlantic hurricanes mobilize a large pool of organic matter (OM) from coastal forested watersheds in the southeastern United States. However, the mobilization of toxic metals such as mercury (Hg) that are associated with this vast pool of OM are rarely measured. This study aims to assess the variations of total Hg (THg) and methylmercury (MeHg) levels and the isotopic compositions of Hg in a blackwater river (Waccamaw River, SC, U.S.A.) during two recent extreme flooding events induced by Hurricane Joaquin (October 2015) and Hurricane Matthew (October 2016). We show that extreme flooding considerably increased filtered THg and MeHg concentrations associated with aromatic dissolved organic matter. During a 2‐month sampling window each year (October–November), we estimate that about 27% (2015) and 78% (2016) of the average amount of Hg deposited atmospherically during these 2 months was exported via the river. The isotopic composition of Hg in the river waters was changed only slightly by the substantial inputs of runoff from surrounding landscapes, in which mass‐dependent fractionation (as δ202Hg) decreased from −1.47 to −1.67‰ and mass‐independent fractionation (as ∆199Hg) decreased from −0.15 to −0.37‰. The slight variations in Hg isotopic composition during such extreme flooding events imply that sources of Hg in the river are nearly unchanged even under the very high wet deposition of Hg derived from the intensive rainfall. The majority of Hg exported by the river (74–85%) is estimated to have been derived from dry deposition to the watersheds. An increase in frequency and intensity of Atlantic hurricanes is expected in the next few decades due to further warming of ocean surface waters. We predict that increased hurricanes will mobilize more dry‐deposited Hg and in situ produced MeHg from these coastal watersheds where MeHg can be extensively bioaccumulated and biomagnified in the downstream aquatic food webs.
-
Abstract. Mercury (Hg) is emitted to the atmosphere mainly as volatile elemental Hg0. Oxidation to water-soluble HgII plays a major role in Hg deposition to ecosystems. Here, we implement a new mechanism for atmospheric Hg0∕HgII redox chemistry in the GEOS-Chem global model and examine the implications for the global atmospheric Hg budget and deposition patterns. Our simulation includes a new coupling of GEOS-Chem to an ocean general circulation model (MITgcm), enabling a global 3-D representation of atmosphere–ocean Hg0∕HgII cycling. We find that atomic bromine (Br) of marine organobromine origin is the main atmospheric Hg0 oxidant and that second-stage HgBr oxidation is mainly by the NO2 and HO2 radicals. The resulting chemical lifetime of tropospheric Hg0 against oxidation is 2.7 months, shorter than in previous models. Fast HgII atmospheric reduction must occur in order to match the ∼ 6-month lifetime of Hg against deposition implied by the observed atmospheric variability of total gaseous mercury (TGM ≡ Hg0+HgII(g)). We implement this reduction in GEOS-Chem as photolysis of aqueous-phase HgII–organic complexes in aerosols and clouds, resulting in a TGM lifetime of 5.2 months against deposition and matching both mean observed TGM and its variability. Model sensitivity analysis shows that the interhemispheric gradient of TGM, previously used to infer a longer Hg lifetime against deposition, is misleading because Southern Hemisphere Hg mainly originates from oceanic emissions rather than transport from the Northern Hemisphere. The model reproduces the observed seasonal TGM variation at northern midlatitudes (maximum in February, minimum in September) driven by chemistry and oceanic evasion, but it does not reproduce the lack of seasonality observed at southern hemispheric marine sites. Aircraft observations in the lowermost stratosphere show a strong TGM–ozone relationship indicative of fast Hg0 oxidation, but we show that this relationship provides only a weak test of Hg chemistry because it is also influenced by mixing. The model reproduces observed Hg wet deposition fluxes over North America, Europe, and China with little bias (0–30%). It reproduces qualitatively the observed maximum in US deposition around the Gulf of Mexico, reflecting a combination of deep convection and availability of NO2 and HO2 radicals for second-stage HgBr oxidation. However, the magnitude of this maximum is underestimated. The relatively low observed Hg wet deposition over rural China is attributed to fast HgII reduction in the presence of high organic aerosol concentrations. We find that 80% of HgII deposition is to the global oceans, reflecting the marine origin of Br and low concentrations of organic aerosols for HgII reduction. Most of that deposition takes place to the tropical oceans due to the availability of HO2 and NO2 for second-stage HgBr oxidation.
-
null (Ed.)A method was developed to measure gaseous oxidized mercury (GOM) air-surface exchange using 2 replicated dynamic flux chambers (DFCs) in conjunction with cation exchange membrane (CEM) filters. The experimental design and method was developed and tested in a laboratory setting, using materials collected from industrial scale open pit gold mines in central Nevada, USA. Materials used included waste rock, heap leach ore, and tailings, with substrate concentrations ranging from 100 to 40000 ng g-1 total mercury (THg). CEM filters were used to capture GOM from the DFC sample lines while a Tekran® 2537A analyzer measured GEM concurrently. Previous and ongoing work has demonstrated that CEM do not collect GEM and efficiently collect multiple compounds of GOM. GOM emission rates up to 4000 pg m- 2 h-1 were measured from tailings materials with high Hg substrate concentrations, and this has significant implication with respect to air-Hg surface exchange. GOM flux was variable for lower Hg concentration substrates, with both emission and deposition observed, and this was affected by ambient air GOM concentrations. For substrates that experienced GOM deposition, deposition velocities were in the range 0.01 – 0.07 cm s-1.more » « less
-
Abstract Wetlands play an important role in regulating the atmospheric carbon dioxide (
CO 2) concentrations and thus affecting the climate. However, there is still lack of quantitative evaluation of such a role across different wetland types, especially at the global scale. Here, we conducted a meta‐analysis to compare ecosystemCO 2fluxes among various types of wetlands using a global database compiled from the literature. This database consists of 143 site‐years of eddy covariance data from 22 inland wetland and 21 coastal wetland sites across the globe. Coastal wetlands had higher annual gross primary productivity (GPP ), ecosystem respiration (R e), and net ecosystem productivity (NEP ) than inland wetlands. On a per unit area basis, coastal wetlands provided largeCO 2sinks, while inland wetlands provided smallCO 2sinks or were nearlyCO 2neutral. The annualCO 2sink strength was 93.15 and 208.37 g C m−2for inland and coastal wetlands, respectively. AnnualCO 2fluxes were mainly regulated by mean annual temperature (MAT ) and mean annual precipitation (MAP ). For coastal and inland wetlands combined,MAT andMAP explained 71%, 54%, and 57% of the variations inGPP ,R e, andNEP , respectively. TheCO 2fluxes of wetlands were also related to leaf area index (LAI ). TheCO 2fluxes also varied with water table depth (WTD ), although the effects ofWTD were not statistically significant.NEP was jointly determined byGPP andR efor both inland and coastal wetlands. However, theNEP /R eandNEP /GPP ratios exhibited little variability for inland wetlands and decreased for coastal wetlands with increasing latitude. The contrasting ofCO 2fluxes between inland and coastal wetlands globally can improve our understanding of the roles of wetlands in the global C cycle. Our results also have implications for informing wetland management and climate change policymaking, for example, the efforts being made by international organizations and enterprises to restore coastal wetlands for enhancing blue carbon sinks.