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1.
Proc Natl Acad Sci U S A ; 120(2): e2202488120, 2023 01 10.
Artículo en Inglés | MEDLINE | ID: mdl-36595667

RESUMEN

Human exposure to monomethylmercury (CH3Hg), a potent neurotoxin, is principally through the consumption of seafood. The formation of CH3Hg and its bioaccumulation in marine food webs experience ongoing impacts of global climate warming and ocean biogeochemistry alterations. Employing a series of sensitivity experiments, here we explicitly consider the effects of climate change on marine mercury (Hg) cycling within a global ocean model in the hypothesized twenty-first century under the business-as-usual scenario. Even though the overall prediction is subjected to significant uncertainty, we identify several important climate change impact pathways. Elevated seawater temperature exacerbates elemental Hg (Hg0) evasion, while decreased surface wind speed reduces air-sea exchange rates. The reduced export of particulate organic carbon shrinks the pool of potentially bioavailable divalent Hg (HgII) that can be methylated in the subsurface ocean, where shallower remineralization depth associated with lower productivity causes impairment of methylation activity. We also simulate an increase in CH3Hg photodemethylation potential caused by increased incident shortwave radiation and less attenuation by decreased sea ice and chlorophyll. The model suggests that these impacts can also be propagated to the CH3Hg concentration in the base of the marine food web. Our results offer insight into synergisms/antagonisms in the marine Hg cycling among different climate change stressors.


Asunto(s)
Mercurio , Contaminantes Químicos del Agua , Humanos , Mercurio/análisis , Agua de Mar , Cadena Alimentaria , Cambio Climático , Metilación , Contaminantes Químicos del Agua/análisis
2.
Environ Sci Technol ; 2024 May 29.
Artículo en Inglés | MEDLINE | ID: mdl-38810222

RESUMEN

The redox chemistry of mercury (Hg) in the atmosphere exerts a significant influence on its global cycle. However, our understanding of this important process remains shrouded in uncertainty. In this study, we utilize three-dimensional atmospheric Hg isotope modeling to evaluate the isotopic composition of particle-bound mercury [HgII(P)] in the global atmosphere. We investigate various chemistry mechanisms and find that they induce remarkably disparate odd-number mass-independent fractionation (odd-MIF) in HgII(P) on a global scale. The observed odd-MIF data identify the essential role of sea salt aerosol debromination in the redox chemistry of atmospheric Hg and underscore the predominant influence of Br oxidation in the marine boundary layer. The odd-MIF signatures significantly narrow the uncertainty range of redox chemistry rates and constrain the photoreduction of HgII(P) at a magnitude of 10-3 JNO2 (local photolysis frequency of NO2) in the global atmosphere. This study advances our understanding of atmospheric Hg chemistry processes and provides insights into the potential impacts of climate change on Hg cycling.

3.
Proc Natl Acad Sci U S A ; 118(47)2021 11 23.
Artículo en Inglés | MEDLINE | ID: mdl-34751160

RESUMEN

The COVID-19 pandemic has led to an increased demand for single-use plastics that intensifies pressure on an already out-of-control global plastic waste problem. While it is suspected to be large, the magnitude and fate of this pandemic-associated mismanaged plastic waste are unknown. Here, we use our MITgcm ocean plastic model to quantify the impact of the pandemic on plastic discharge. We show that 8.4 ± 1.4 million tons of pandemic-associated plastic waste have been generated from 193 countries as of August 23, 2021, with 25.9 ± 3.8 thousand tons released into the global ocean representing 1.5 ± 0.2% of the global total riverine plastic discharge. The model projects that the spatial distribution of the discharge changes rapidly in the global ocean within 3 y, with a significant portion of plastic debris landing on the beach and seabed later and a circumpolar plastic accumulation zone will be formed in the Arctic. We find hospital waste represents the bulk of the global discharge (73%), and most of the global discharge is from Asia (72%), which calls for better management of medical waste in developing countries.


Asunto(s)
COVID-19/terapia , Océanos y Mares , Plásticos , SARS-CoV-2 , Contaminantes del Agua , Países en Desarrollo , Salud Global , Humanos
4.
Environ Sci Technol ; 57(16): 6563-6572, 2023 04 25.
Artículo en Inglés | MEDLINE | ID: mdl-37045790

RESUMEN

Marine fish is an excellent source of nutrition but also contributes the most to human exposure to methylmercury (MMHg), a neurotoxicant that poses significant risks to human health on a global scale and is regulated by the Minamata Convention. To better predict human exposure to MMHg, it is important to understand the trophic transfer of MMHg in the global marine food webs, which remains largely unknown, especially in the upper trophic level (TL) biota that is more directly relevant to human exposure. In this study, we couple a fish ecological model and an ocean methylmercury model to explore the influencing factors and mechanisms of MMHg transfer in marine fish food webs. Our results show that available MMHg in the zooplankton strongly determines the MMHg in fish. Medium-sized fish are critical intermediaries that transfer more than 70% of the MMHg circulating in food webs. Grazing is the main factor to control MMHg concentrations in different size categories of fish. Feeding interactions affected by ecosystem structures determine the degree of MMHg biomagnification. We estimate a total of 6.1 metric tons of MMHg potentially digested by the global population per year through marine fish consumption. The model provides a useful tool to quantify human exposure to MMHg through marine fish consumption and thus fills a critical gap in the effectiveness evaluation of the convention.


Asunto(s)
Compuestos de Metilmercurio , Contaminantes Químicos del Agua , Animales , Humanos , Cadena Alimentaria , Ecosistema , Bioacumulación , Zooplancton , Peces , Contaminantes Químicos del Agua/análisis , Monitoreo del Ambiente/métodos
5.
Environ Sci Technol ; 57(39): 14589-14601, 2023 Oct 03.
Artículo en Inglés | MEDLINE | ID: mdl-37585923

RESUMEN

Sea ice (including overlying snow) is a dynamic interface between the atmosphere and the ocean, influencing the mercury (Hg) cycling in polar oceans. However, a large-scale and process-based model for the Hg cycle in the sea ice environment is lacking, hampering our understanding of regional Hg budget and critical processes. Here, we develop a comprehensive model for the Hg cycle at the ocean-sea ice-atmosphere interface with constraints from observational polar cryospheric data. We find that seasonal patterns of average total Hg (THg) in snow are governed by snow thermodynamics and deposition, peaking in springtime (Arctic: 5.9 ng/L; Antarctic: 5.3 ng/L) and minimizing during ice formation (Arctic: 1.0 ng/L, Antarctic: 0.5 ng/L). Arctic and Antarctic sea ice exhibited THg concentration peaks in summer (0.25 ng/L) and spring (0.28 ng/L), respectively, governed by different snow Hg transmission pathways. Antarctic snow-ice formation facilitates Hg transfer to sea ice during spring, while in the Arctic, snow Hg is primarily moved through snowmelt. Overall, first-year sea ice acts as a buffer, receiving atmospheric Hg during ice growth and releasing it to the ocean in summer, influencing polar atmospheric and seawater Hg concentrations. Our model can assess climate change effects on polar Hg cycles and evaluate the Minamata Convention's effectiveness for Arctic populations.

6.
Environ Sci Technol ; 56(5): 2968-2976, 2022 03 01.
Artículo en Inglés | MEDLINE | ID: mdl-35143172

RESUMEN

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.


Asunto(s)
Contaminantes Atmosféricos , Mercurio , Contaminantes Atmosféricos/análisis , Monitoreo del Ambiente , Gases , Mercurio/análisis , Oxidación-Reducción , Agua de Mar
7.
Environ Sci Technol ; 55(10): 7145-7156, 2021 05 18.
Artículo en Inglés | MEDLINE | ID: mdl-33929202

RESUMEN

Air-sea exchange of gaseous elemental mercury (Hg(0)) is influenced by different meteorological factors and the availability of Hg in seawater. Here, we use the MITgcm ocean model to explore the interannual variability of this flux and the influence of oceanographic and atmospheric dynamics. We apply the GEOS-Chem model to further simulate the potential impact of the evasion variability on the atmospheric Hg levels. We find a latitudinal pattern in Hg(0) evasion with a relatively small variability in mid-latitudes (3.1-6.7%) and a large one in the high latitudes and Equator (>10%). Different factors dominate the patterns in the equatorial (wind speed), mid- (oceanic flow and temperature), and high-latitudinal (sea-ice, temperature, and dynamic processes) oceans. A seesaw pattern of Hg(0) evasion anomaly (±5-20%) in the equatorial Pacific is found from November to next January between El Niño and La Niña years, owing to the anomalies in wind speed, temperature, and vertical mixing. Higher atmospheric Hg level (2%-5%) are simulated for Hg(0) evasion fluxes with three-month lag, associated with the suppression of upwelling in the beginning of the El Niño event. Despite of the uncertainties, this study elucidates the spatial patterns of the interannual variability of the ocean Hg(0) evasion flux and its potential impact on atmospheric Hg levels.


Asunto(s)
Mercurio , Atmósfera , Monitoreo del Ambiente , Mercurio/análisis , Océanos y Mares , Agua de Mar
8.
Environ Sci Technol ; 55(22): 15476-15483, 2021 11 16.
Artículo en Inglés | MEDLINE | ID: mdl-34738802

RESUMEN

Methylmercury (CH3Hg+, MMHg) in the phytoplankton and zooplankton, which form the bottom of marine food webs, is a good predictor of MMHg in top predators, including humans. Therefore, evaluating the potential exposure of MMHg to higher trophic levels (TLs) requires a better understanding of relationships between MMHg biomagnification and plankton dynamics. In this study, a coupled ecological/physical model with 366 plankton types of different sizes, biogeochemical functions, and temperature tolerance is used to simulate the relationships between MMHg biomagnification and the ecosystem structure. The study shows that the MMHg biomagnification becomes more significant with increasing TLs. Trophic magnification factors (TMFs) in the lowest two TLs show the opposite spatial pattern to TMFs in higher TLs. The low TMFs are usually associated with a short food-chain length. The less bottom-heavy trophic pyramids in the oligotrophic oceans enhance the MMHg trophic transfer. The global average TMF is increased from 2.3 to 2.8 in the warmer future with a medium climate sensitivity of 2.5 °C. Our study suggests that if there are no mitigation measures for Hg emission, MMHg in the high-trophic-level plankton is increased more dramatically in the warming future, indicating greater MMHg exposure for top predators such as humans.


Asunto(s)
Compuestos de Metilmercurio , Bioacumulación , Ecosistema , Monitoreo del Ambiente , Humanos , Plancton
9.
Environ Sci Technol ; 54(9): 5446-5455, 2020 05 05.
Artículo en Inglés | MEDLINE | ID: mdl-32054263

RESUMEN

Methylmercury is greatly bioconcentrated and biomagnified in marine plankton ecosystems, and these communities form the basis of marine food webs. Therefore, the evaluation of the potential exposure of methylmercury to higher trophic levels, including humans, requires a better understanding of its distribution in the ocean and the factors that control its biomagnification. In this study, a coupled physical/ecological model is used to simulate the trophic transfer of monomethylmercury (MMHg) in a marine plankton ecosystem. The model includes phytoplankton, a microbial community, herbivorous zooplankton (HZ), and carnivorous zooplankton (CZ). The model captures both shorter food chains in oligotrophic regions, with small HZ feeding on small phytoplankton, and longer chains in higher nutrient conditions, with larger HZ feeding on larger phytoplankton and larger CZ feeding on larger HZ. In the model, trophic dilution occurs in the food webs that involve small zooplankton, as the grazing fluxes of small zooplankton are insufficient to accumulate more MMHg in themselves than in their prey. The model suggests that biomagnification is more prominent in large zooplankton and that the microbial community plays an important role in the trophic transfer of MMHg. Sensitivity analyses show that with increasing body size, the sensitivity of the trophic magnification ratio to grazing, mortality rates, and food assimilation efficiency (AEC) increases, while the sensitivity to excretion rates decreases. More predation or a longer zooplankton lifespan may lead to more prominent biomagnification, especially for large species. Because lower AEC results in more predation, modeled ratios of MMHg concentrations between large plankton are doubled or even tripled when the AEC decreases from 50% to 10%. This suggests that the biomagnification of large zooplankton is particularly sensitive to food assimilation efficiency.


Asunto(s)
Compuestos de Metilmercurio , Animales , Bioacumulación , Ecosistema , Cadena Alimentaria , Fitoplancton , Plancton , Zooplancton
10.
Environ Sci Technol ; 53(9): 5052-5061, 2019 05 07.
Artículo en Inglés | MEDLINE | ID: mdl-30946578

RESUMEN

Air-sea exchange of mercury (Hg) is the largest flux between Earth system reservoirs. Global models simulate air-sea exchange based either on an atmospheric or ocean model simulation and treat the other media as a boundary condition. Here we develop a new modeling capability (NJUCPL) that couples GEOS-Chem (atmospheric model) and MITgcm (ocean model) at the native hourly model time step. The coupled model is evaluated against high-frequency simultaneous measurements of elemental mercury (Hg0) in both the atmosphere and surface ocean obtained during five published cruises in the Atlantic, Pacific, and Southern Oceans. Results indicate that the calculated global Hg net evasion flux is 12% higher for the online model than the offline model. We find that the coupled online model captures the spatial pattern of the observations; specifically, it improves the representation of peak seawater Hg0 (Hg0aq) concentration associated with enhanced precipitation in the intertropical convergence zone in both the Atlantic and the Pacific Oceans. We investigate the causes of the observed Hg0aq peaks with two sensitivity simulations and show that the high Hg0aq concentrations are associated with elevated convective cloud mass flux and bromine concentrations in the tropical upper troposphere. Observations of elevated Hg0aq concentrations in the western tropical Pacific Ocean merit further study involving BrO vertical distribution and cloud resolving models.


Asunto(s)
Contaminantes Atmosféricos , Mercurio , Atmósfera , Monitoreo del Ambiente , Océanos y Mares , Oxidación-Reducción , Océano Pacífico
11.
Proc Natl Acad Sci U S A ; 113(3): 526-31, 2016 Jan 19.
Artículo en Inglés | MEDLINE | ID: mdl-26729866

RESUMEN

Observations of elemental mercury (Hg(0)) at sites in North America and Europe show large decreases (∼ 1-2% y(-1)) from 1990 to present. Observations in background northern hemisphere air, including Mauna Loa Observatory (Hawaii) and CARIBIC (Civil Aircraft for the Regular Investigation of the atmosphere Based on an Instrument Container) aircraft flights, show weaker decreases (<1% y(-1)). These decreases are inconsistent with current global emission inventories indicating flat or increasing emissions over that period. However, the inventories have three major flaws: (i) they do not account for the decline in atmospheric release of Hg from commercial products; (ii) they are biased in their estimate of artisanal and small-scale gold mining emissions; and (iii) they do not properly account for the change in Hg(0)/Hg(II) speciation of emissions from coal-fired utilities after implementation of emission controls targeted at SO2 and NOx. We construct an improved global emission inventory for the period 1990 to 2010 accounting for the above factors and find a 20% decrease in total Hg emissions and a 30% decrease in anthropogenic Hg(0) emissions, with much larger decreases in North America and Europe offsetting the effect of increasing emissions in Asia. Implementation of our inventory in a global 3D atmospheric Hg simulation [GEOS-Chem (Goddard Earth Observing System-Chemistry)] coupled to land and ocean reservoirs reproduces the observed large-scale trends in atmospheric Hg(0) concentrations and in Hg(II) wet deposition. The large trends observed in North America and Europe reflect the phase-out of Hg from commercial products as well as the cobenefit from SO2 and NOx emission controls on coal-fired utilities.


Asunto(s)
Contaminantes Atmosféricos/análisis , Contaminación del Aire/análisis , Atmósfera/química , Actividades Humanas , Internacionalidad , Mercurio/análisis , Carbón Mineral , Humanos , Estados Unidos
12.
Environ Sci Technol ; 52(23): 13792-13800, 2018 12 04.
Artículo en Inglés | MEDLINE | ID: mdl-30372053

RESUMEN

Mercury (Hg) is characterized by its ability to migrate between continents and its adverse effects on human health, arousing great concern around the world. The transboundary transport of large anthropogenic Hg emissions from China has attracted particular attention, especially from neighboring countries. Here, we combine an atmospheric transport model, a mass budget analysis, and a multiregional input-output model to simulate the atmospheric Hg outflow from China and investigate the impacts of Chinese interprovincial trade on the outflow. The results show outflows of 423.0 Mg of anthropogenic Hg, consisting of 65.9% of the total Chinese anthropogenic emissions, from China in 2010. Chinese interprovincial trade promotes the transfer of atmospheric outflow from the eastern terrestrial boundary (-6.4 Mg year-1) to the western terrestrial boundary (+4.5 Mg year-1) and a net decrease in the atmospheric outflow for the whole boundary, reducing the chance of risks to foreign countries derived from transboundary Hg pollution from China. These impacts of interprovincial trade will be amplified due to the expected strengthened interprovincial trade in the future. The synergistic promotional effects of interprovincial trade versus Hg controls should be considered to reduce the transboundary Hg pollution from China.


Asunto(s)
Contaminantes Atmosféricos , Mercurio , China , Monitoreo del Ambiente , Humanos , Internacionalidad
13.
J Immunol ; 197(3): 824-33, 2016 08 01.
Artículo en Inglés | MEDLINE | ID: mdl-27354218

RESUMEN

The H5N1 avian influenza virus causes severe disease and high mortality, making it a major public health concern worldwide. The virus uses the host cellular machinery for several steps of its life cycle. In this report, we observed overexpression of the ubiquitin-like protein FAT10 following live H5N1 virus infection in BALB/c mice and in the human respiratory epithelial cell lines A549 and BEAS-2B. Further experiments demonstrated that FAT10 increased H5N1 virus replication and decreased the viability of infected cells. Total RNA extracted from H5N1 virus-infected cells, but not other H5N1 viral components, upregulated FAT10, and this process was mediated by the retinoic acid-induced protein I-NF-κB signaling pathway. FAT10 knockdown in A549 cells upregulated type I IFN mRNA expression and enhanced STAT1 phosphorylation during live H5N1 virus infection. Taken together, our data suggest that FAT10 was upregulated via retinoic acid-induced protein I and NF-κB during H5N1 avian influenza virus infection. And the upregulated FAT10 promoted H5N1 viral replication by inhibiting type I IFN.


Asunto(s)
Interferón Tipo I/biosíntesis , Infecciones por Orthomyxoviridae/metabolismo , Ubiquitinas/metabolismo , Replicación Viral/fisiología , Animales , Western Blotting , Línea Celular , Técnicas de Silenciamiento del Gen , Humanos , Subtipo H5N1 del Virus de la Influenza A , Ratones , Ratones Endogámicos BALB C , Análisis de Secuencia por Matrices de Oligonucleótidos , Infecciones por Orthomyxoviridae/inmunología , Reacción en Cadena de la Polimerasa , Mucosa Respiratoria/inmunología , Mucosa Respiratoria/metabolismo , Mucosa Respiratoria/virología , Regulación hacia Arriba
14.
J Virol ; 89(20): 10347-58, 2015 Oct.
Artículo en Inglés | MEDLINE | ID: mdl-26246576

RESUMEN

UNLABELLED: As a recycling center, lysosomes are filled with numerous acid hydrolase enzymes that break down waste materials and invading pathogens. Recently, lysosomal cell death has been defined as "lysosomal membrane permeabilization and the consequent leakage of lysosome contents into cytosol." Here, we show that the neuraminidase (NA) of H5N1 influenza A virus markedly deglycosylates and degrades lysosome-associated membrane proteins (LAMPs; the most abundant membrane proteins of lysosome), which induces lysosomal rupture, and finally leads to cell death of alveolar epithelial carcinoma A549 cells and human tracheal epithelial cells. The NA inhibitors peramivir and zanamivir could effectively block the deglycosylation of LAMPs, inhibit the virus cell entry, and prevent cell death induced by the H5N1 influenza virus. The NA of seasonal H1N1 virus, however, does not share these characteristics. Our findings not only reveal a novel role of NA in the early stage of the H5N1 influenza virus life cycle but also elucidate the molecular mechanism of lysosomal rupture crucial for influenza virus induced cell death. IMPORTANCE: The integrity of lysosomes is vital for maintaining cell homeostasis, cellular defense and clearance of invading pathogens. This study shows that the H5N1 influenza virus could induce lysosomal rupture through deglycosylating lysosome-associated membrane proteins (LAMPs) mediated by the neuraminidase activity of NA protein. NA inhibitors such as peramivir and zanamivir could inhibit the deglycosylation of LAMPs and protect lysosomes, which also further interferes with the H5N1 influenza virus infection at early stage of life cycle. This work is significant because it presents new concepts for NA's function, as well as for influenza inhibitors' mechanism of action, and could partially explain the high mortality and high viral load after H5N1 virus infection in human beings and why NA inhibitors have more potent therapeutic effects for lethal avian influenza virus infections at early stage.


Asunto(s)
Membrana Celular/enzimología , Proteínas de Membrana de los Lisosomas/metabolismo , Lisosomas/enzimología , Neuraminidasa/metabolismo , Proteínas Virales/metabolismo , Ácidos Carbocíclicos , Muerte Celular/efectos de los fármacos , Línea Celular Tumoral , Membrana Celular/química , Ciclopentanos/farmacología , Citosol/efectos de los fármacos , Citosol/enzimología , Citosol/virología , Inhibidores Enzimáticos/farmacología , Células Epiteliales/efectos de los fármacos , Células Epiteliales/virología , Guanidinas/farmacología , Humanos , Hidrólisis , Subtipo H1N1 del Virus de la Influenza A/química , Subtipo H1N1 del Virus de la Influenza A/enzimología , Subtipo H5N1 del Virus de la Influenza A/química , Subtipo H5N1 del Virus de la Influenza A/enzimología , Proteínas de Membrana de los Lisosomas/química , Lisosomas/efectos de los fármacos , Lisosomas/virología , Unión Proteica , Proteolisis , Mucosa Respiratoria/efectos de los fármacos , Mucosa Respiratoria/virología , Especificidad de la Especie , Internalización del Virus/efectos de los fármacos , Zanamivir/farmacología
15.
Environ Sci Technol ; 49(15): 9185-93, 2015 Aug 04.
Artículo en Inglés | MEDLINE | ID: mdl-26110215

RESUMEN

We quantitatively examine the relative importance of uncertainty in emissions and physicochemical properties (including reaction rate constants) to Northern Hemisphere (NH) and Arctic polycyclic aromatic hydrocarbon (PAH) concentrations, using a computationally efficient numerical uncertainty technique applied to the global-scale chemical transport model GEOS-Chem. Using polynomial chaos (PC) methods, we propagate uncertainties in physicochemical properties and emissions for the PAHs benzo[a]pyrene, pyrene and phenanthrene to simulated spatially resolved concentration uncertainties. We find that the leading contributors to parametric uncertainty in simulated concentrations are the black carbon-air partition coefficient and oxidation rate constant for benzo[a]pyrene, and the oxidation rate constants for phenanthrene and pyrene. NH geometric average concentrations are more sensitive to uncertainty in the atmospheric lifetime than to emissions rate. We use the PC expansions and measurement data to constrain parameter uncertainty distributions to observations. This narrows a priori parameter uncertainty distributions for phenanthrene and pyrene, and leads to higher values for OH oxidation rate constants and lower values for European PHE emission rates.


Asunto(s)
Contaminantes Ambientales/análisis , Hidrocarburos Policíclicos Aromáticos/análisis , Incertidumbre , Regiones Árticas , Benzo(a)pireno/análisis , Simulación por Computador , Modelos Químicos , Modelos Teóricos , Fenantrenos/análisis , Pirenos/análisis
16.
Environ Sci Technol ; 48(1): 429-37, 2014.
Artículo en Inglés | MEDLINE | ID: mdl-24279957

RESUMEN

We investigate effects of 2000-2050 emissions and climate changes on the atmospheric transport of three polycyclic aromatic hydrocarbons (PAHs): phenanthrene (PHE), pyrene (PYR), and benzo[a]pyrene (BaP). We use the GEOS-Chem model coupled to meteorology from a general circulation model and focus on impacts to northern hemisphere midlatitudes and the Arctic. We project declines in anthropogenic emissions (up to 20%) and concentrations (up to 37%), with particle-bound PAHs declining more, and greater declines in midlatitudes versus the Arctic. Climate change causes relatively minor increases in midlatitude concentrations for the more volatile PHE and PYR (up to 4%) and decreases (3%) for particle-bound BaP. In the Arctic, all PAHs decline slightly under future climate (up to 2%). Overall, we observe a small 2050 "climate penalty" for volatile PAHs and "climate benefit" for particle-bound PAHs. The degree of penalty or benefit depends on competition between deposition and surface-to-air fluxes of previously deposited PAHs. Particles and temperature have greater impacts on future transport than oxidants, with particle changes alone accounting for 15% of BaP decline under 2050 emissions. Higher temperatures drive increasing surface-to-air fluxes that cause PHE and PYR climate penalties. Simulations suggest ratios of more-to-less volatile species can be used to diagnose signals of climate versus emissions and that these signals are best observed in the Arctic.


Asunto(s)
Contaminantes Atmosféricos/análisis , Benzo(a)pireno/análisis , Cambio Climático , Fenantrenos/análisis , Pirenos/análisis , Regiones Árticas , Monitoreo del Ambiente , Industria Procesadora y de Extracción , Modelos Teóricos , Petróleo , Navíos
17.
Environ Sci Technol ; 48(19): 11312-9, 2014 Oct 07.
Artículo en Inglés | MEDLINE | ID: mdl-25171182

RESUMEN

Air-sea exchange of elemental mercury (Hg(0)) is a critical component of the global biogeochemical Hg cycle. To better understand variability in atmospheric and oceanic Hg(0), we collected high-resolution measurements across large gradients in seawater temperature, salinity, and productivity in the Pacific Ocean (20°N-15°S). We modeled surface ocean Hg inputs and losses using an ocean general circulation model (MITgcm) and an atmospheric chemical transport model (GEOS-Chem). Observed surface seawater Hg(0) was much more variable than atmospheric concentrations. Peak seawater Hg(0) concentrations (∼ 130 fM) observed in the Pacific intertropical convergence zone (ITCZ) were ∼ 3-fold greater than surrounding areas (∼ 50 fM). This is similar to observations from the Atlantic Ocean. Peak evasion in the northern Pacific ITCZ was four times higher than surrounding regions and located at the intersection of high wind speeds and elevated seawater Hg(0). Modeling results show that high Hg inputs from enhanced precipitation in the ITCZ combined with the shallow ocean mixed layer in this region drive elevated seawater Hg(0) concentrations. Modeled seawater Hg(0) concentrations reproduce observed peaks in the ITCZ of both the Atlantic and Pacific Oceans but underestimate its magnitude, likely due to insufficient deep convective scavenging of oxidized Hg from the upper troposphere. Our results demonstrate the importance of scavenging of reactive mercury in the upper atmosphere driving variability in seawater Hg(0) and net Hg inputs to biologically productive regions of the tropical ocean.


Asunto(s)
Contaminantes Atmosféricos/análisis , Mercurio/análisis , Contaminantes Químicos del Agua/análisis , Océano Atlántico , Atmósfera , Monitoreo del Ambiente , Modelos Teóricos , Océano Pacífico , Salinidad , Agua de Mar/química , Temperatura , Clima Tropical
18.
Environ Sci Technol ; 48(16): 9514-22, 2014 Aug 19.
Artículo en Inglés | MEDLINE | ID: mdl-25066365

RESUMEN

Rivers are an important source of mercury (Hg) to marine ecosystems. Based on an analysis of compiled observations, we estimate global present-day Hg discharges from rivers to ocean margins are 27 ± 13 Mmol a(-1) (5500 ± 2700 Mg a(-1)), of which 28% reaches the open ocean and the rest is deposited to ocean margin sediments. Globally, the source of Hg to the open ocean from rivers amounts to 30% of atmospheric inputs. This is larger than previously estimated due to accounting for elevated concentrations in Asian rivers and variability in offshore transport across different types of estuaries. Riverine inputs of Hg to the North Atlantic have decreased several-fold since the 1970s while inputs to the North Pacific have increased. These trends have large effects on Hg concentrations at ocean margins but are too small in the open ocean to explain observed declines of seawater concentrations in the North Atlantic or increases in the North Pacific. Burial of Hg in ocean margin sediments represents a major sink in the global Hg biogeochemical cycle that has not been previously considered. We find that including this sink in a fully coupled global biogeochemical box model helps to balance the large anthropogenic release of Hg from commercial products recently added to global inventories. It also implies that legacy anthropogenic Hg can be removed from active environmental cycling on a faster time scale (centuries instead of millennia). Natural environmental Hg levels are lower than previously estimated, implying a relatively larger impact from human activity.


Asunto(s)
Sedimentos Geológicos/análisis , Mercurio/análisis , Ríos , Contaminantes Químicos del Agua/análisis , Ecosistema , Estuarios , Humanos , Modelos Teóricos , Océanos y Mares , Agua de Mar
19.
Environ Pollut ; 344: 123371, 2024 Mar 01.
Artículo en Inglés | MEDLINE | ID: mdl-38266694

RESUMEN

Accurately predicting air pollutants, especially in urban areas with well-defined spatial structures, is crucial. Over the past decade, machine learning techniques have been widely used to forecast urban air quality. However, traditional machine learning approaches have limitations in accuracy and interpretability for predicting pollutants. In this study, we propose a convolutional neural network (CNN) model to predict the spatial distribution of CO concentration in Nanjing urban area at 10 m resolution. Our model incorporates various factors as input, such as building height, topography, emissions, and is trained against the outputs simulated by the parallelized large-eddy simulation model (PALM). The PALM model has 48 different scenarios that varied in emissions, wind speeds, and wind directions. The results display a strong consistency between the two models. Furthermore, we evaluate the performance of our model using a 10-fold cross-validation and out-of-sample cross-validation approach. This yields a robust correlation (with both R2 > 0.8) and a low RMSE between the CO predicted by the PALM and CNN models, which demonstrates the generalization capability of our CNN model. The CNN can extract crucial features from the resulted weight contribution map. This map indicates that the CO concentration at a location is more influenced by nearby buildings and emissions than distant ones. The interpretable patterns uncovered by our model are related to neighborhood effects, wind speeds, directions, and the impact of orientation on urban CO distribution. The model also shows high prediction accuracy (R > 0.8) when applied to another city. Overall, the integration of our CNN framework with the PALM model enhances the accuracy of air quality predictions, while enabling a fluid dynamic laws interpretation, providing effective tools for air quality management.


Asunto(s)
Contaminantes Atmosféricos , Contaminación del Aire , Contaminación del Aire/análisis , Contaminantes Atmosféricos/análisis , Ciudades , Simulación por Computador , Aprendizaje Automático
20.
Nat Commun ; 15(1): 4837, 2024 Jun 06.
Artículo en Inglés | MEDLINE | ID: mdl-38844454

RESUMEN

The vertical settling of plastic debris in oceans is poorly understood. A large share of low-density microplastics (LDMPs) are largely absent from sea surfaces. The present study employs a model that considers the potential of an overlooked microbially induced calcium carbonate precipitation (MICP) process and new motion equations for irregular LDMPs. Here we show that the motion of LDMPs in the present model, exhibiting a damped oscillation pattern, is quite different from that in biofouling models. Furthermore, LDMPs in the size range of 10-200 µm are most likely to gain sufficient density at the biofouling/MICP stage to independently sink to the ocean floor with relatively small drag coefficients, potentially explaining the selective enrichment of LDMPs in the oceanic sediment. The size and shape exhibit strong non-linear effects on the settling patterns of LDMPs. Overall, the present study highlights the importance of calcite-mediated sinking of LDMPs in open oceans.

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