Articles | Volume 16, issue 19
© Author(s) 2016. This work is distributed under
the Creative Commons Attribution 3.0 License.
the Creative Commons Attribution 3.0 License.
© Author(s) 2016. This work is distributed under
the Creative Commons Attribution 3.0 License.
the Creative Commons Attribution 3.0 License.
Current and future levels of mercury atmospheric pollution on a global scale
Jozef M. Pacyna
NILU – Norwegian Institute for Air Research, Instituttveien 18, P.O. Box 100, 2027 Kjeller, Norway
AGH University of Science and Technology, al. Mickiewicza 30, 30-059 Krakow, Poland
Meteorological Synthesizing Centre – East of EMEP, 2nd Roshchinsky proezd, 8/5, office 207, 115419 Moscow, Russia
Francesco De Simone
CNR – Institute of Atmospheric Pollution Research, Division of Rende, UNICAL-Polifunzionalie, Rende 87036, Italy
Ian M. Hedgecock
CNR – Institute of Atmospheric Pollution Research, Division of Rende, UNICAL-Polifunzionalie, Rende 87036, Italy
NILU – Norwegian Institute for Air Research, Instituttveien 18, P.O. Box 100, 2027 Kjeller, Norway
Elisabeth G. Pacyna
NILU – Norwegian Institute for Air Research, Instituttveien 18, P.O. Box 100, 2027 Kjeller, Norway
University of Groningen, Arctic Centre, Aweg 30, 9718 CW Groningen, the Netherlands
CNR – Institute of Atmospheric Pollution Research, Area della Ricerca Roma 1, Via Salaria Km 29 300, 00015 Monterotondo (Rome), Italy
IVL Swedish Environmental Research Institute, P.O. Box 53201, 400 14 Gothenburg, Sweden
IVL Swedish Environmental Research Institute, P.O. Box 53201, 400 14 Gothenburg, Sweden
No articles found.
Håkan Pleijel, Jenny Klingberg, Michelle Nerentorp, Malin C. Broberg, Brigitte Nyirambangutse, John Munthe, and Göran Wallin
Biogeosciences, 18, 6313–6328,Short summary
Mercury is a problematic metal in the environment. It is crucial to understand the Hg circulation in ecosystems. We explored the mercury concentration in foliage from a diverse set of plants, locations and sampling periods to study the accumulation of Hg in leaves–needles over time. Mercury was always higher in older tissue: in broadleaved trees, conifers and wheat. Specific leaf area, the leaf area per unit leaf mass, turned out to be critical for Hg accumulation in leaves–needles.
Attilio Naccarato, Antonella Tassone, Maria Martino, Sacha Moretti, Antonella Macagnano, Emiliano Zampetti, Paolo Papa, Joshua Avossa, Nicola Pirrone, Michelle Nerentorp, John Munthe, Ingvar Wängberg, Geoff W. Stupple, Carl P. J. Mitchell, Adam R. Martin, Alexandra Steffen, Diana Babi, Eric M. Prestbo, Francesca Sprovieri, and Frank Wania
Atmos. Meas. Tech., 14, 3657–3672,Short summary
Mercury monitoring in support of the Minamata Convention requires effective and reliable analytical tools. Passive sampling is a promising approach for creating a sustainable long-term network for atmospheric mercury with improved spatial resolution and global coverage. In this study the analytical performance of three passive air samplers (CNR-PAS, IVL-PAS, and MerPAS) was assessed over extended deployment periods and the accuracy of concentrations was judged by comparison with active sampling.
Shaojie Song, Hélène Angot, Noelle E. Selin, Hubert Gallée, Francesca Sprovieri, Nicola Pirrone, Detlev Helmig, Joël Savarino, Olivier Magand, and Aurélien Dommergue
Atmos. Chem. Phys., 18, 15825–15840,Short summary
Mercury is a trace metal with adverse health effects on human and wildlife. Its unique property makes it undergo long-range transport, and even remote Antarctica receives significant inputs. This paper presents the first model that aims to understand mercury behavior over the Antarctic Plateau. We find that mercury is quickly cycled between snow and air in the sunlit period, likely driven by bromine chemistry, and that several uncertain processes contribute to its behavior in the dark period.
Luca Naitza, Davide Putero, Angela Marinoni, Francescopiero Calzolari, Fabrizio Roccato, Maurizio Busetto, Damiano Sferlazzo, Eleonora Aruffo, Piero Di Carlo, Mariantonia Bencardino, Francesco D'Amore, Francesca Sprovieri, Nicola Pirrone, Federico Dallo, Jacopo Gabrieli, Massimiliano Vardè, Carlo Barbante, Paolo Bonasoni, and Paolo Cristofanelli
Atmos. Meas. Tech. Discuss.,
Revised manuscript not acceptedShort summary
We implemented a prototype of a centralized system to support atmospheric observatories in data production and submission. By using the “R” Language, for several near-surface ECVs, we developed specific routines for data filtering, flagging, formatting, and creation of data products for detecting instrumental problems or special atmospheric events. Our effort would improve atmospheric data quality, accelerate the process of data submission and make the data flagging more “objective".
Qing Mu, Gerhard Lammel, Christian N. Gencarelli, Ian M. Hedgecock, Ying Chen, Petra Přibylová, Monique Teich, Yuxuan Zhang, Guangjie Zheng, Dominik van Pinxteren, Qiang Zhang, Hartmut Herrmann, Manabu Shiraiwa, Peter Spichtinger, Hang Su, Ulrich Pöschl, and Yafang Cheng
Atmos. Chem. Phys., 17, 12253–12267,Short summary
Polycyclic aromatic hydrocarbons (PAHs) are hazardous pollutants with the largest emissions in East Asia. The regional WRF-Chem-PAH model has been developed to reflect the state-of-the-art understanding of current PAHs studies with several new or updated features. It is able to reasonably well simulate the concentration levels and particulate mass fractions of PAHs near the sources and at a remote outflow region of East Asia, in high spatial and temporal resolutions.
Johannes Bieser, Franz Slemr, Jesse Ambrose, Carl Brenninkmeijer, Steve Brooks, Ashu Dastoor, Francesco DeSimone, Ralf Ebinghaus, Christian N. Gencarelli, Beate Geyer, Lynne E. Gratz, Ian M. Hedgecock, Daniel Jaffe, Paul Kelley, Che-Jen Lin, Lyatt Jaegle, Volker Matthias, Andrei Ryjkov, Noelle E. Selin, Shaojie Song, Oleg Travnikov, Andreas Weigelt, Winston Luke, Xinrong Ren, Andreas Zahn, Xin Yang, Yun Zhu, and Nicola Pirrone
Atmos. Chem. Phys., 17, 6925–6955,Short summary
We conducted a multi model study to investigate our ability to reproduce the vertical distribution of mercury in the atmosphere. For this, we used observational data from over 40 aircraft flights in EU and US. We compared observations to the results of seven chemistry transport models and found that the models are able to reproduce vertical gradients of total and elemental Hg. Finally, we found that different chemical reactions seem responsible for the oxidation of Hg depending on altitude.
Antonella Macagnano, Viviana Perri, Emiliano Zampetti, Andrea Bearzotti, Fabrizio De Cesare, Francesca Sprovieri, and Nicola Pirrone
Atmos. Chem. Phys., 17, 6883–6893,Short summary
By exploiting the photocatalytic properties of electrospun titania nanofibers, a novel conductometric sensor was designed and fabricated to entrap and detect GEM in air. Such a sensor was able to work at room temperature and was highly sensitive to elemental mercury. Since it is composed of titania and gold nanoparticles, it seems to be robust and resistant to common solvents and VOCs in the air.
Oleg Travnikov, Hélène Angot, Paulo Artaxo, Mariantonia Bencardino, Johannes Bieser, Francesco D'Amore, Ashu Dastoor, Francesco De Simone, María del Carmen Diéguez, Aurélien Dommergue, Ralf Ebinghaus, Xin Bin Feng, Christian N. Gencarelli, Ian M. Hedgecock, Olivier Magand, Lynwill Martin, Volker Matthias, Nikolay Mashyanov, Nicola Pirrone, Ramesh Ramachandran, Katie Alana Read, Andrei Ryjkov, Noelle E. Selin, Fabrizio Sena, Shaojie Song, Francesca Sprovieri, Dennis Wip, Ingvar Wängberg, and Xin Yang
Atmos. Chem. Phys., 17, 5271–5295,Short summary
The study provides a complex analysis of processes governing Hg fate in the atmosphere involving both measurement data and simulation results of chemical transport models. Evaluation of the model simulations and numerical experiments against observations allows explaining spatial and temporal variations of Hg concentration in the near-surface atmospheric layer and shows possibility of multiple pathways of Hg oxidation occurring concurrently in various parts of the atmosphere.
Francesca Sprovieri, Nicola Pirrone, Mariantonia Bencardino, Francesco D'Amore, Helene Angot, Carlo Barbante, Ernst-Günther Brunke, Flor Arcega-Cabrera, Warren Cairns, Sara Comero, María del Carmen Diéguez, Aurélien Dommergue, Ralf Ebinghaus, Xin Bin Feng, Xuewu Fu, Patricia Elizabeth Garcia, Bernd Manfred Gawlik, Ulla Hageström, Katarina Hansson, Milena Horvat, Jože Kotnik, Casper Labuschagne, Olivier Magand, Lynwill Martin, Nikolay Mashyanov, Thumeka Mkololo, John Munthe, Vladimir Obolkin, Martha Ramirez Islas, Fabrizio Sena, Vernon Somerset, Pia Spandow, Massimiliano Vardè, Chavon Walters, Ingvar Wängberg, Andreas Weigelt, Xu Yang, and Hui Zhang
Atmos. Chem. Phys., 17, 2689–2708,Short summary
The results on total mercury (THg) wet deposition flux obtained within the GMOS network have been presented and discussed to understand the atmospheric Hg cycling and its seasonal depositional patterns over the 2011–2015 period. The data set provides new insight into baseline concentrations of THg concentrations in precipitation particularly in regions where wet deposition and atmospheric Hg species were not investigated before, opening the way for additional measurements and modeling studies.
Francesco De Simone, Paulo Artaxo, Mariantonia Bencardino, Sergio Cinnirella, Francesco Carbone, Francesco D'Amore, Aurélien Dommergue, Xin Bin Feng, Christian N. Gencarelli, Ian M. Hedgecock, Matthew S. Landis, Francesca Sprovieri, Noriuki Suzuki, Ingvar Wängberg, and Nicola Pirrone
Atmos. Chem. Phys., 17, 1881–1899,Short summary
Biomass burning (BB) releases of Hg, usually considered to be Hg(0), are a significant global source of atmospheric Hg. However there is experimental evidence that a fraction of this Hg is bound to particulate matter, Hg(P). This modelling study shows how increasing fractions of Hg(P) reduce the availability of Hg to the global pool, raising Hg exposure for those regions characterized by high BB, with implications for the sub-Arctic and also rice-growing areas in South-East Asia.
Christian N. Gencarelli, Johannes Bieser, Francesco Carbone, Francesco De Simone, Ian M. Hedgecock, Volker Matthias, Oleg Travnikov, Xin Yang, and Nicola Pirrone
Atmos. Chem. Phys., 17, 627–643,Short summary
Atmospheric deposition is an important pathway by which Hg reaches marine ecosystems, where it can be methylated and enter the base of food chain. High resolution numerical experiments has been performed in order to investigate the contributions (sensitivity) of the Hg anthtropogenic emissions, speciation and atmospherical chemical reactions on Hg depositions over Europe. The comparison of wet deposition fluxes and concentrations measured on 28 monitioring sites were used to support the analysis.
Allison H. Baker, Dorit M. Hammerling, Sheri A. Mickelson, Haiying Xu, Martin B. Stolpe, Phillipe Naveau, Ben Sanderson, Imme Ebert-Uphoff, Savini Samarasinghe, Francesco De Simone, Francesco Carbone, Christian N. Gencarelli, John M. Dennis, Jennifer E. Kay, and Peter Lindstrom
Geosci. Model Dev., 9, 4381–4403,Short summary
We apply lossy data compression to output from the Community Earth System Model Large Ensemble Community Project. We challenge climate scientists to examine features of the data relevant to their interests and identify which of the ensemble members have been compressed, and we perform direct comparisons on features critical to climate science. We find that applying lossy data compression to climate model data effectively reduces data volumes with minimal effect on scientific results.
Andreas Weigelt, Franz Slemr, Ralf Ebinghaus, Nicola Pirrone, Johannes Bieser, Jan Bödewadt, Giulio Esposito, and Peter F. J. van Velthoven
Atmos. Chem. Phys., 16, 13653–13668,Short summary
Hg ∕ SO2, Hg ∕ CO, and NOx ∕ SO2 emission ratios (ERs) in the plume of the coal-fired power plant (CFPP), Lippendorf, near Leipzig in Germany, were determined in August 2013. GOM fraction of mercury emissions was also assessed. Measured Hg ∕ SO2 and Hg ∕ CO ERs were consistent with the ratios calculated from annual emissions in 2013 reported by the CFPP operator. The NOx ∕ SO2 ER was somewhat lower. GOM fractions of ~ 40 % of CFPP mercury emissions in current emission inventories are overestimated.
Ingvar Wängberg, Michelle G. Nerentorp Mastromonaco, John Munthe, and Katarina Gårdfeldt
Atmos. Chem. Phys., 16, 13379–13387,Short summary
Within the EU-funded project, Global Mercury Observation System (GMOS) airborne mercury has been monitored at the background Råö measurement site on the western coast of Sweden from May 2012 to the end of May 2015, the following mercury species/fractions were measured: gaseous elemental mercury (GEM), particulate bound mercury (PBM) and gaseous oxidised mercury (GOM). Evidence that a significant part of the GOM measured at the Råö site has been formed in the free tropospheric air is presented.
Francesca Sprovieri, Nicola Pirrone, Mariantonia Bencardino, Francesco D'Amore, Francesco Carbone, Sergio Cinnirella, Valentino Mannarino, Matthew Landis, Ralf Ebinghaus, Andreas Weigelt, Ernst-Günther Brunke, Casper Labuschagne, Lynwill Martin, John Munthe, Ingvar Wängberg, Paulo Artaxo, Fernando Morais, Henrique de Melo Jorge Barbosa, Joel Brito, Warren Cairns, Carlo Barbante, María del Carmen Diéguez, Patricia Elizabeth Garcia, Aurélien Dommergue, Helene Angot, Olivier Magand, Henrik Skov, Milena Horvat, Jože Kotnik, Katie Alana Read, Luis Mendes Neves, Bernd Manfred Gawlik, Fabrizio Sena, Nikolay Mashyanov, Vladimir Obolkin, Dennis Wip, Xin Bin Feng, Hui Zhang, Xuewu Fu, Ramesh Ramachandran, Daniel Cossa, Joël Knoery, Nicolas Marusczak, Michelle Nerentorp, and Claus Norstrom
Atmos. Chem. Phys., 16, 11915–11935,Short summary
This work presents atmospheric Hg concentrations recorded within the GMOS global network analyzing Hg measurement results in terms of temporal trends, seasonality and comparability within the network. The over-arching beneﬁt of this coordinated Hg monitoring network would clearly be the production of high-quality measurement datasets on a global scale useful in developing and validating models on different spatial and temporal scales.
Hélène Angot, Ashu Dastoor, Francesco De Simone, Katarina Gårdfeldt, Christian N. Gencarelli, Ian M. Hedgecock, Sarka Langer, Olivier Magand, Michelle N. Mastromonaco, Claus Nordstrøm, Katrine A. Pfaffhuber, Nicola Pirrone, Andrei Ryjkov, Noelle E. Selin, Henrik Skov, Shaojie Song, Francesca Sprovieri, Alexandra Steffen, Kenjiro Toyota, Oleg Travnikov, Xin Yang, and Aurélien Dommergue
Atmos. Chem. Phys., 16, 10735–10763,Short summary
This is a synthesis of the atmospheric mercury (Hg) monitoring data available in recent years (2011–2015) in the Arctic and in Antarctica along with a comparison of these observations with numerical simulations using four cutting-edge global models. Based on this comparison, we discuss whether the processes that affect atmospheric Hg seasonality and interannual variability are appropriately represented in the models, and identify remaining research gaps.
N. Pirrone, S. Cinnirella, S. Nativi, F. Sprovieri, and I. M. Hedgecock
Int. Arch. Photogramm. Remote Sens. Spatial Inf. Sci., XLI-B8, 1349–1355,
N. Batrakova, O. Travnikov, and O. Rozovskaya
Ocean Sci., 10, 1047–1063,
Related subject area
Subject: Gases | Research Activity: Atmospheric Modelling and Data Analysis | Altitude Range: Troposphere | Science Focus: Chemistry (chemical composition and reactions)Atmospheric CO2 inversion reveals the Amazon as a minor carbon source caused by fire emissions, with forest uptake offsetting about half of these emissionsRapid O3 assimilations – Part 2: Tropospheric O3 changes accompanied by declining NOx emissions in the USA and Europe in 2005–2020High-resolution air quality simulations of ozone exceedance events during the Lake Michigan Ozone StudySimulations of winter ozone in the Upper Green River basin, Wyoming, using WRF-ChemMeasurement report: Assessment of Asian emissions of ethane and propane with a chemistry transport model based on observations from the island of HaterumaSensitivity of northeastern US surface ozone predictions to the representation of atmospheric chemistry in the Community Regional Atmospheric Chemistry Multiphase Mechanism (CRACMMv1.0)Daytime isoprene nitrates under changing NOx and O3Atmospheric data support a multi-decadal shift in the global methane budget towards natural tropical emissionsAir quality and related health impact in the UNECE region: source attribution and scenario analysisEast Asian methane emissions inferred from high-resolution inversions of GOSAT and TROPOMI observations: a comparative and evaluative analysisTowards near-real-time air pollutant and greenhouse gas emissions: lessons learned from multiple estimates during the COVID-19 pandemicSpatiotemporal variation of radionuclide dispersion from nuclear power plant accidents using FLEXPART mini-ensemble modelingContinuous weekly monitoring of methane emissions from the Permian Basin by inversion of TROPOMI satellite observationsWestern European emission estimates of CFC-11, CFC-12 and CCl4 derived from atmospheric measurements from 2008 to 2021Estimating methane emissions in the Arctic nations using surface observations from 2008 to 2019Background nitrogen dioxide (NO2) over the United States and its implications for satellite observations and trends: effects of nitrate photolysis, aircraft, and open firesSeasonal, interannual and decadal variability of tropospheric ozone in the North Atlantic: comparison of UM-UKCA and remote sensing observations for 2005–2018Quantification of oil and gas methane emissions in the Delaware and Marcellus basins using a network of continuous tower-based measurementsGlobal sensitivities of reactive N and S gas and particle concentrations and deposition to precursor emissions reductionsLarge simulated future changes in the nitrate radical under the CMIP6 SSP scenarios: implications for oxidation chemistryImpact of HO2 aerosol uptake on radical levels and O3 production during summertime in BeijingSource attribution of near-surface ozone trends in the United States during 1995–2019What controls ozone sensitivity in the upper tropical troposphere?Exploring the drivers of tropospheric hydroxyl radical trends in the Geophysical Fluid Dynamics Laboratory AM4.1 atmospheric chemistry–climate modelImpacts of land cover changes on biogenic emission and its contribution to ozone and secondary organic aerosol in ChinaHigh-resolution regional emission inventory contributes to the evaluation of policy effectiveness: a case study in Jiangsu Province, ChinaWhy is ozone in South Korea and the Seoul metropolitan area so high and increasing?Vehicular ammonia emissions: an underappreciated emission source in densely populated areasImproving ozone simulations in Asia via multisource data assimilation: results from an observing system simulation experiment with GEMS geostationary satellite observationsA three-dimensional simulation and process analysis of tropospheric ozone depletion events (ODEs) during the springtime in the Arctic using CMAQ (Community Multiscale Air Quality Modeling System)A high-resolution satellite-based map of global methane emissions reveals missing wetland, fossil fuel, and monsoon sourcesGlobal impact of the COVID-19 lockdown on surface concentration and health risk of atmospheric benzeneModelling the impacts of emission changes on O3 sensitivity, atmospheric oxidation capacity and pollution transport over the Catalonia regionVariable effects of spatial resolution on modeling of nitrogen oxidesAtmospheric composition and climate impacts of a future hydrogen economyTropospheric NO2 vertical profiles over South Korea and their relation to oxidant chemistry: implications for geostationary satellite retrievals and the observation of NO2 diurnal variation from spaceA regional modelling study of halogen chemistry within a volcanic plume of Mt Etna’s Christmas 2018 eruptionAssessment of isoprene and near surface ozone sensitivities to water stress over the Euro-Mediterranean regionSimulating impacts on UK air quality from net-zero forest planting scenariosPotential impact of shipping on air pollution in the Mediterranean region – a multimodel evaluation: comparison of photooxidants NO2 and O3Summertime ozone pollution in China affected by stratospheric quasi-biennial oscillationDeclining, seasonal-varying emissions of sulfur hexafluoride from the United StatesNitrogen oxides in the free troposphere: implications for tropospheric oxidants and the interpretation of satellite NO2 measurementsClimate-driven deterioration of future ozone pollution in Asia predicted by machine learning with multi-source dataReconciling the bottom-up and top-down estimates of the methane chemical sink using multiple observationsArctic tropospheric ozone: assessment of current knowledge and model performanceChloride (HCl ∕ Cl−) dominates inorganic aerosol formation from ammonia in the Indo-Gangetic Plain during winter: modeling and comparison with observationsInferring and evaluating satellite-based constraints on NOx emissions estimates in air quality simulationsHow do Cl concentrations matter for the simulation of CH4 and δ13C(CH4) and estimation of the CH4 budget through atmospheric inversions?Cluster-based characterization of multi-dimensional tropospheric ozone variability in coastal regions: an analysis of lidar measurements and model results
Luana S. Basso, Chris Wilson, Martyn P. Chipperfield, Graciela Tejada, Henrique L. G. Cassol, Egídio Arai, Mathew Williams, T. Luke Smallman, Wouter Peters, Stijn Naus, John B. Miller, and Manuel Gloor
Atmos. Chem. Phys., 23, 9685–9723,Short summary
The Amazon’s carbon balance may have changed due to forest degradation, deforestation and warmer climate. We used an atmospheric model and atmospheric CO2 observations to quantify Amazonian carbon emissions (2010–2018). The region was a small carbon source to the atmosphere, mostly due to fire emissions. Forest uptake compensated for ~ 50 % of the fire emissions, meaning that the remaining forest is still a small carbon sink. We found no clear evidence of weakening carbon uptake over the period.
Rui Zhu, Zhaojun Tang, Xiaokang Chen, Xiong Liu, and Zhe Jiang
Atmos. Chem. Phys., 23, 9745–9763,Short summary
Ozone Monitoring Instrument (OMI) and surface O3 observations are used to investigate the changes in tropospheric O3 in the USA and Europe in 2005–2020. The surface-based assimilations show limited changes in surface and tropospheric column O3. The OMI-based assimilations show larger decreases in tropospheric O3 columns in 2010–2014, related to a decline in free-tropospheric NO2. Analysis suggests limited impacts of local emissions decline on tropospheric O3 over the USA and Europe in 2005–2020.
R. Bradley Pierce, Monica Harkey, Allen Lenzen, Lee M. Cronce, Jason A. Otkin, Jonathan L. Case, David S. Henderson, Zac Adelman, Tsengel Nergui, and Christopher R. Hain
Atmos. Chem. Phys., 23, 9613–9635,Short summary
We evaluate two high-resolution model simulations with different meteorological inputs but identical chemistry and anthropogenic emissions, with the goal of identifying a model configuration best suited for characterizing air quality in locations where lake breezes commonly affect local air quality along the Lake Michigan shoreline. This analysis complements other studies in evaluating the impact of meteorological inputs and parameterizations on air quality in a complex environment.
Shreta Ghimire, Zachary J. Lebo, Shane Murphy, Stefan Rahimi, and Trang Tran
Atmos. Chem. Phys., 23, 9413–9438,Short summary
High wintertime ozone levels have occurred often in recent years in mountain basins with oil and gas production facilities. Photochemical modeling of ozone production serves as a basis for understanding the mechanism by which it occurs and for predictive capability. We present photochemical model simulations of ozone formation and accumulation in the Upper Green River basin, Wyoming, demonstrating the model's ability to simulate wintertime ozone and the sensitivity of ozone to its precursors.
Adedayo R. Adedeji, Stephen J. Andrews, Matthew J. Rowlinson, Mathew J. Evans, Alastair C. Lewis, Shigeru Hashimoto, Hitoshi Mukai, Hiroshi Tanimoto, Yasunori Tohjima, and Takuya Saito
Atmos. Chem. Phys., 23, 9229–9244,Short summary
We use the GEOS-Chem model to interpret observations of CO, C2H6, C3H8, NOx, NOy and O3 made from Hateruma Island in 2018. The model captures many synoptic-scale events and the seasonality of most pollutants at the site but underestimates C2H6 and C3H8 during the winter. These underestimates are unlikely to be reconciled by increases in biomass burning emissions but could be reconciled by increasing the Asian anthropogenic source of C2H6 and C3H8 by factors of around 2 and 3, respectively.
Bryan K. Place, William T. Hutzell, K. Wyat Appel, Sara Farrell, Lukas Valin, Benjamin N. Murphy, Karl M. Seltzer, Golam Sarwar, Christine Allen, Ivan R. Piletic, Emma L. D'Ambro, Emily Saunders, Heather Simon, Ana Torres-Vasquez, Jonathan Pleim, Rebecca H. Schwantes, Matthew M. Coggon, Lu Xu, William R. Stockwell, and Havala O. T. Pye
Atmos. Chem. Phys., 23, 9173–9190,Short summary
Ground-level ozone is a pollutant with adverse human health and ecosystem effects. Air quality models allow scientists to understand the chemical production of ozone and demonstrate impacts of air quality management plans. In this work, the role of multiple systems in ozone production was investigated for the northeastern US in summer. Model updates to chemical reaction rates and monoterpene chemistry were most influential in decreasing predicted ozone and improving agreement with observations.
Alfred W. Mayhew, Peter M. Edwards, and Jaqueline F. Hamilton
Atmos. Chem. Phys., 23, 8473–8485,Short summary
Isoprene nitrates are chemical species commonly found in the atmosphere that are important for their impacts on air quality and climate. This paper investigates modelled changes to daytime isoprene nitrate concentrations resulting from changes in NOx and O3. The results highlight the complex, nonlinear chemistry of this group of species under typical conditions for megacities such as Beijing, with many species showing increased concentrations when NOx is decreased and/or ozone is increased.
Alice Drinkwater, Paul I. Palmer, Liang Feng, Tim Arnold, Xin Lan, Sylvia E. Michel, Robert Parker, and Hartmut Boesch
Atmos. Chem. Phys., 23, 8429–8452,Short summary
Changes in atmospheric methane over the last few decades are largely unexplained. Previous studies have proposed different hypotheses to explain short-term changes in atmospheric methane. We interpret observed changes in atmospheric methane and stable isotope source signatures (2004–2020). We argue that changes over this period are part of a large-scale shift from high-northern-latitude thermogenic energy emissions to tropical biogenic emissions, particularly from North Africa and South America.
Claudio A. Belis and Rita Van Dingenen
Atmos. Chem. Phys., 23, 8225–8240,Short summary
The study assesses the influence that abating emissions in the rest of the world have on exposure and mortality due to ozone and fine particulate matter in the region covered by the Gothenburg protocol (UNECE, mainly Europe and North America). To that end, the impacts of pollutants derived from different geographic areas and anthropogenic sources are analysed in a series of scenarios including measures to abate air pollutants and greenhouse gas emissions with different levels of ambition.
Ruosi Liang, Yuzhong Zhang, Wei Chen, Peixuan Zhang, Jingran Liu, Cuihong Chen, Huiqin Mao, Guofeng Shen, Zhen Qu, Zichong Chen, Minqiang Zhou, Pucai Wang, Robert J. Parker, Hartmut Boesch, Alba Lorente, Joannes D. Maasakkers, and Ilse Aben
Atmos. Chem. Phys., 23, 8039–8057,Short summary
We compare and evaluate East Asian methane emissions inferred from different satellite observations (GOSAT and TROPOMI). The results show discrepancies over northern India and eastern China. Independent ground-based observations are more consistent with TROPOMI-derived emissions in northern India and GOSAT-derived emissions in eastern China.
Marc Guevara, Hervé Petetin, Oriol Jorba, Hugo Denier van der Gon, Jeroen Kuenen, Ingrid Super, Claire Granier, Thierno Doumbia, Philippe Ciais, Zhu Liu, Robin D. Lamboll, Sabine Schindlbacher, Bradley Matthews, and Carlos Pérez García-Pando
Atmos. Chem. Phys., 23, 8081–8101,Short summary
This study provides an intercomparison of European 2020 emission changes derived from official inventories, which are reported by countries under the framework of several international conventions and directives, and non-official near-real-time estimates, the use of which has significantly grown since the COVID-19 outbreak. The results of the work are used to produce recommendations on how best to approach and make use of near-real-time emissions for modelling and monitoring applications.
Seyed Omid Nabavi, Theodoros Christoudias, Yiannis Proestos, Christos Fountoukis, Huda Al-Sulaiti, and Jos Lelieveld
Atmos. Chem. Phys., 23, 7719–7739,Short summary
The objective of our study is to comprehensively assess the timing of radioactive material transportation and deposition, along with the associated population exposure in the designated region. We employed diverse meteorological inputs, emission specifics, and simulation codes, aiming to quantify the level of uncertainty.
Daniel J. Varon, Daniel J. Jacob, Benjamin Hmiel, Ritesh Gautam, David R. Lyon, Mark Omara, Melissa Sulprizio, Lu Shen, Drew Pendergrass, Hannah Nesser, Zhen Qu, Zachary R. Barkley, Natasha L. Miles, Scott J. Richardson, Kenneth J. Davis, Sudhanshu Pandey, Xiao Lu, Alba Lorente, Tobias Borsdorff, Joannes D. Maasakkers, and Ilse Aben
Atmos. Chem. Phys., 23, 7503–7520,Short summary
We use TROPOMI satellite observations to quantify weekly methane emissions from the US Permian oil and gas basin from May 2018 to October 2020. We find that Permian emissions are highly variable, with diverse economic and activity drivers. The most important drivers during our study period were new well development and natural gas price. Permian methane intensity averaged 4.6 % and decreased by 1 % per year.
Alison L. Redington, Alistair J. Manning, Stephan Henne, Francesco Graziosi, Luke M. Western, Jgor Arduini, Anita L. Ganesan, Christina M. Harth, Michela Maione, Jens Mühle, Simon O'Doherty, Joseph Pitt, Stefan Reimann, Matthew Rigby, Peter K. Salameh, Peter G. Simmonds, T. Gerard Spain, Kieran Stanley, Martin K. Vollmer, Ray F. Weiss, and Dickon Young
Atmos. Chem. Phys., 23, 7383–7398,Short summary
Chlorofluorocarbons (CFCs) were used in Europe pre-1990, damaging the stratospheric ozone layer. Legislation has controlled production and use, and global emissions have decreased sharply. The global rate of decline in CFC-11 recently slowed and was partly attributed to illegal emission in eastern China. This study concludes that emissions of CFC-11 in western Europe have not contributed to the unexplained part of the global increase in CFC-11 observed in the last decade.
Sophie Wittig, Antoine Berchet, Isabelle Pison, Marielle Saunois, Joël Thanwerdas, Adrien Martinez, Jean-Daniel Paris, Toshinobu Machida, Motoki Sasakawa, Douglas E. J. Worthy, Xin Lan, Rona L. Thompson, Espen Sollum, and Mikhail Arshinov
Atmos. Chem. Phys., 23, 6457–6485,Short summary
Here, an inverse modelling approach is applied to estimate CH4 sources and sinks in the Arctic from 2008 to 2019. We study the magnitude, seasonal patterns and trends from different sources during recent years. We also assess how the current observation network helps to constrain fluxes. We find that constraints are only significant for North America and, to a lesser extent, West Siberia, where the observation network is relatively dense. We find no clear trend over the period of inversion.
Ruijun Dang, Daniel J. Jacob, Viral Shah, Sebastian D. Eastham, Thibaud M. Fritz, Loretta J. Mickley, Tianjia Liu, Yi Wang, and Jun Wang
Atmos. Chem. Phys., 23, 6271–6284,Short summary
We use the GEOS-Chem model to better understand the magnitude and trend in free tropospheric NO2 over the contiguous US. Model underestimate of background NO2 is largely corrected by considering aerosol nitrate photolysis. Increase in aircraft emissions affects satellite retrievals by altering the NO2 shape factor, and this effect is expected to increase in future. We show the importance of properly accounting for the free tropospheric background in interpreting NO2 observations from space.
Maria Rosa Russo, Brian John Kerridge, Nathan Luke Abraham, James Keeble, Barry Graham Latter, Richard Siddans, James Weber, Paul Thomas Griffiths, John Adrian Pyle, and Alexander Thomas Archibald
Atmos. Chem. Phys., 23, 6169–6196,Short summary
Tropospheric ozone is an important component of the Earth system as it can affect both climate and air quality. In this work we use observed tropospheric ozone derived from satellite observations and compare it to tropospheric ozone from model simulations. Our aim is to investigate recent changes (2005–2018) in tropospheric ozone in the North Atlantic region and to understand what factors are driving such changes.
Zachary Barkley, Kenneth Davis, Natasha Miles, Scott Richardson, Aijun Deng, Benjamin Hmiel, David Lyon, and Thomas Lauvaux
Atmos. Chem. Phys., 23, 6127–6144,Short summary
Using methane monitoring instruments attached to towers, we measure methane concentrations and quantify methane emissions coming from the Marcellus and Permian oil and gas basins. In the Marcellus, emissions were 3 times higher than the state inventory across the entire monitoring period. In the Permian, we see a sharp decline in emissions aligning with the onset of the COVID-19 pandemic. Tower observational networks can be utilized in other basins for long-term monitoring of emissions.
Yao Ge, Massimo Vieno, David S. Stevenson, Peter Wind, and Mathew R. Heal
Atmos. Chem. Phys., 23, 6083–6112,Short summary
The sensitivity of fine particles and reactive N and S species to reductions in precursor emissions is investigated using the EMEP MSC-W (European Monitoring and Evaluation Programme Meteorological Synthesizing Centre – West) atmospheric chemistry transport model. This study reveals that the individual emissions reduction has multiple and geographically varying co-benefits and small disbenefits on different species, demonstrating the importance of prioritizing regional emissions controls.
Scott Archer-Nicholls, Rachel Allen, Nathan L. Abraham, Paul T. Griffiths, and Alex T. Archibald
Atmos. Chem. Phys., 23, 5801–5813,Short summary
The nitrate radical is a major oxidant at nighttime, but much less is known about it than about the other oxidants ozone and OH. We use Earth system model calculations to show how the nitrate radical has changed in abundance from 1850–2014 and to 2100 under a range of different climate and emission scenarios. Depending on the emissions and climate scenario, significant increases are projected with implications for the oxidation of volatile organic compounds and the formation of fine aerosol.
Joanna E. Dyson, Lisa K. Whalley, Eloise J. Slater, Robert Woodward-Massey, Chunxiang Ye, James D. Lee, Freya Squires, James R. Hopkins, Rachel E. Dunmore, Marvin Shaw, Jacqueline F. Hamilton, Alastair C. Lewis, Stephen D. Worrall, Asan Bacak, Archit Mehra, Thomas J. Bannan, Hugh Coe, Carl J. Percival, Bin Ouyang, C. Nicholas Hewitt, Roderic L. Jones, Leigh R. Crilley, Louisa J. Kramer, W. Joe F. Acton, William J. Bloss, Supattarachai Saksakulkrai, Jingsha Xu, Zongbo Shi, Roy M. Harrison, Simone Kotthaus, Sue Grimmond, Yele Sun, Weiqi Xu, Siyao Yue, Lianfang Wei, Pingqing Fu, Xinming Wang, Stephen R. Arnold, and Dwayne E. Heard
Atmos. Chem. Phys., 23, 5679–5697,Short summary
The hydroxyl (OH) and closely coupled hydroperoxyl (HO2) radicals are vital for their role in the removal of atmospheric pollutants. In less polluted regions, atmospheric models over-predict HO2 concentrations. In this modelling study, the impact of heterogeneous uptake of HO2 onto aerosol surfaces on radical concentrations and the ozone production regime in Beijing in the summertime is investigated, and the implications for emissions policies across China are considered.
Pengwei Li, Yang Yang, Hailong Wang, Su Li, Ke Li, Pinya Wang, Baojie Li, and Hong Liao
Atmos. Chem. Phys., 23, 5403–5417,Short summary
We use a novel technique that can attribute O3 to precursors to investigate O3 changes in the United States during 1995–2019. We found that the US domestic energy and surface transportation emission reductions are primarily responsible for the O3 decrease in summer. In winter, factors such as nitrogen oxide emission reduction in the context of its inhibition of ozone production, increased aviation and shipping activities, and large-scale circulation changes contribute to the O3 increases.
Clara M. Nussbaumer, Horst Fischer, Jos Lelieveld, and Andrea Pozzer
Ozone is a greenhouse gas and contributes to the earth’s radiative energy budget and therefore to global warming. This effect is largest in the upper troposphere. In this study, we investigate the processes controlling ozone formation and the sensitivity to its precursors in the upper tropical troposphere based on model simulations by the ECHAM5/MESSy2 Atmospheric Chemistry (EMAC) model. We find that NOx emissions from lightning most importantly affect ozone chemistry at these altitudes.
Glen Chua, Vaishali Naik, and Larry Wayne Horowitz
Atmos. Chem. Phys., 23, 4955–4975,Short summary
The hydroxyl radical (OH) is an atmospheric
detergent, removing air pollutants and greenhouse gases like methane from the atmosphere. Thus, understanding how it is changing and responding to its various drivers is important for air quality and climate. We found that OH has increased by about 5 % globally from 1980 to 2014 in our model, mostly driven by increasing nitrogen oxide (NOx) emissions. This suggests potential climate tradeoffs from air quality policies solely targeting NOx emissions.
Jinlong Ma, Shengqiang Zhu, Siyu Wang, Peng Wang, Jianmin Chen, and Hongliang Zhang
Atmos. Chem. Phys., 23, 4311–4325,Short summary
An updated version of the CMAQ model with biogenic volatile organic compound (BVOC) emissions from MEGAN was applied to study the impacts of different land cover inputs on O3 and secondary organic aerosol (SOA) in China. The estimated BVOC emissions ranged from 25.42 to 37.39 Tg using different leaf area index (LAI) and land cover (LC) inputs. Those differences further induced differences of 4.8–6.9 ppb in O3 concentrations and differences of 5.3–8.4 µg m−3 in SOA concentrations in China.
Chen Gu, Lei Zhang, Zidie Xu, Sijia Xia, Yutong Wang, Li Li, Zeren Wang, Qiuyue Zhao, Hanying Wang, and Yu Zhao
Atmos. Chem. Phys., 23, 4247–4269,Short summary
We demonstrated the development of a high-resolution emission inventory and its application to evaluate the effectiveness of emission control actions, by incorporating the improved methodology, the best available data, and air quality modeling. We show that substantial efforts for emission controls indeed played an important role in air quality improvement even with worsened meteorological conditions and that the contributions of individual measures to emission reduction were greatly changing.
Nadia K. Colombi, Daniel J. Jacob, Laura Hyesung Yang, Shixian Zhai, Viral Shah, Stuart K. Grange, Robert M. Yantosca, Soontae Kim, and Hong Liao
Atmos. Chem. Phys., 23, 4031–4044,Short summary
Surface ozone, detrimental to human and ecosystem health, is very high and increasing in South Korea. Using a global model of the atmosphere, we found that emissions from South Korea and China contribute equally to the high ozone observed. We found that in the absence of all anthropogenic emissions over East Asia, ozone is still very high, implying that the air quality standard in South Korea is not practically achievable unless this background external to East Asia can be decreased.
Yifan Wen, Shaojun Zhang, Ye Wu, and Jiming Hao
Atmos. Chem. Phys., 23, 3819–3828,Short summary
This study established a high-resolution vehicular NH3 emission inventory for mainland China to quantify the absolute value and relative importance of on-road NH3 emissions for different regions, seasons and population densities. Our results indicate that the significant role of on-road NH3 emissions in populated urban areas may have been underappreciated, suggesting the control of vehicular NH3 emission can be a feasible and cost-effective way of mitigating haze pollution in urban areas.
Lei Shu, Lei Zhu, Juseon Bak, Peter Zoogman, Han Han, Song Liu, Xicheng Li, Shuai Sun, Juan Li, Yuyang Chen, Dongchuan Pu, Xiaoxing Zuo, Weitao Fu, Xin Yang, and Tzung-May Fu
Atmos. Chem. Phys., 23, 3731–3748,Short summary
We quantify the benefit of multisource observations (GEMS, LEO satellite, and surface) on ozone simulations in Asia. Data assimilation improves the monitoring of exceedance, spatial pattern, and diurnal variation of surface ozone, with the regional mean bias reduced from −2.1 to −0.2 ppbv. Data assimilation also better represents ozone vertical distributions in the middle to upper troposphere at low latitudes. Our results offer a valuable reference for future ozone simulations.
Le Cao, Simeng Li, Yicheng Gu, and Yuhan Luo
Atmos. Chem. Phys., 23, 3363–3382,Short summary
We performed a 3-D mesoscale model study on ozone depletion events (ODEs) occurring in the spring of 2019 at Barrow using an air quality model, CMAQ. Many ODEs observed at Barrow were captured by the model, and the contribution from each physical or chemical process to ozone and bromine species during ODEs was quantitatively evaluated. We found the ODEs at Barrow to be strongly influenced by horizontal transport. In contrast, over the sea, local chemistry significantly reduced the surface ozone.
Xueying Yu, Dylan B. Millet, Daven K. Henze, Alexander J. Turner, Alba Lorente Delgado, A. Anthony Bloom, and Jianxiong Sheng
Atmos. Chem. Phys., 23, 3325–3346,Short summary
We combine satellite measurements with a novel downscaling method to map global methane emissions at 0.1°×0.1° resolution. These fine-scale emission estimates reveal unreported emission hotspots and shed light on the roles of agriculture, wetlands, and fossil fuels for regional methane budgets. The satellite-derived emissions point in particular to missing fossil fuel emissions in the Middle East and to a large emission underestimate in South Asia that appears to be tied to monsoon rainfall.
Chaohao Ling, Lulu Cui, and Rui Li
Atmos. Chem. Phys., 23, 3311–3324,Short summary
An ensemble machine-learning model coupled with chemical transport models (CTMs) was applied to assess the impact of COVID-19 on ambient benzene. The change ratio of the deweathered benzene concentration from the pre-lockdown to lockdown period was in the order of India (−23.6 %) > Europe (−21.9 %) > the United States (−16.2 %) > China (−15.6 %), which might be associated with local serious benzene pollution and substantial emission reduction in the industrial and transportation sectors.
Alba Badia, Veronica Vidal, Sergi Ventura, Roger Curcoll, Ricard Segura, and Gara Villalba
Improving air quality is a top priority in urban areas. In this study, we used an air quality model to analyse the air quality changes occurring over the Metropolitan Area of Barcelona and other rural areas affected by transport of the atmospheric plume from the city during mobility restrictions. Our results show that mitigation strategies intended to reduce O3 should be designed according to the local meteorology, air transport, particular ozone chemistry of the urban area.
Chi Li, Randall V. Martin, Ronald C. Cohen, Liam Bindle, Dandan Zhang, Deepangsu Chatterjee, Hongjian Weng, and Jintai Lin
Atmos. Chem. Phys., 23, 3031–3049,Short summary
Models are essential to diagnose the significant effects of nitrogen oxides (NOx) on air pollution. We use an air quality model to illustrate the variability of NOx resolution-dependent simulation biases; how these biases depend on specific chemical environments, driving mechanisms, and vertical variabilities; and how these biases affect the interpretation of satellite observations. High-resolution simulations are thus critical to accurately interpret NOx and its relevance to air quality.
Nicola J. Warwick, Alex T. Archibald, Paul T. Griffiths, James Keeble, Fiona M. O'Connor, John A. Pyle, and Keith P. Shine
Atmos. Chem. Phys. Discuss.,
Preprint under review for ACPShort summary
We have used a chemistry-climate model to explore the atmospheric response to changes in emissions of hydrogen and other species associated with a shift from fossil fuel to hydrogen use. We find that leakage of hydrogen results in an indirect global warming, offsetting greenhouse gas emission reductions from reduced fossil fuel use. To maximise the benefit of hydrogen as an energy source, hydrogen leakage and emissions of methane, carbon monoxide and nitrogen oxides should be minimised.
Laura Hyesung Yang, Daniel J. Jacob, Nadia K. Colombi, Shixian Zhai, Kelvin H. Bates, Viral Shah, Ellie Beaudry, Robert M. Yantosca, Haipeng Lin, Jared F. Brewer, Heesung Chong, Katherine R. Travis, James H. Crawford, Lok N. Lamsal, Ja-Ho Koo, and Jhoon Kim
Atmos. Chem. Phys., 23, 2465–2481,Short summary
A geostationary satellite can now provide hourly NO2 vertical columns, and obtaining the NO2 vertical columns from space relies on NO2 vertical distribution from the chemical transport model (CTM). In this work, we update the CTM to better represent the chemistry environment so that the CTM can accurately provide NO2 vertical distribution. We also find that the changes in NO2 vertical distribution driven by a change in mixing depth play an important role in the NO2 column's diurnal variation.
Herizo Narivelo, Paul David Hamer, Virginie Marécal, Luke Surl, Tjarda Roberts, Sophie Pelletier, Béatrice Josse, Jonathan Guth, Mickaël Bacles, Simon Warnach, Thomas Wagner, Stefano Corradini, Giuseppe Salerno, and Lorenzo Guerrieri
Volcanic emissions provide large amounts of gases and particles that can have important effects on the atmosphere. This is why the paper presents a study of the fate of the volcanic emissions from the Mt Etna’s eruption from 24 to 30 December 2018. Using a numerical model and satellite observations, we analyse the impact of the volcanic plume as it travels and how it modifies the air composition over the whole Mediterranean basin.
Susanna Strada, Andrea Pozzer, Filippo Giorgi, Graziano Giuliani, Erika Coppola, Fabien Solmon, Xiaoyan Jiang, and Alex Guenther
Water deficit modifies emissions of isoprene, an aromatic compound released by plants that influence the production of a pollutant such as surface ozone. Numerical modeling shows that, during the warmest and driest summers, isoprene decreases between −20 to −60 % over the Euro-Mediterranean region, while surface ozone only diminishes by few percents. Decreases in isoprene emissions not only happen simultaneously of dry conditions, but could also occur after prolonged or repeated water deficit.
Gemma Purser, Mathew R. Heal, Edward J. Carnell, Stephen Bathgate, Julia Drewer, James I. L. Morison, and Massimo Vieno
Atmos. Chem. Phys. Discuss.,
Revised manuscript accepted for ACPShort summary
Forest expansion is a ‘net zero’ pathway, but change in landcover alters air quality in many ways. This study combines data on tree planting suitability with UK-specific emissions of biogenic volatile organic compound to simulate spatial and temporal changes in atmospheric composition for planting scenarios of four species. Decreases in fine particulate matter are relatively larger than increases in ozone which may indicate a net benefit of tree planting on human health aspects of air quality.
Lea Fink, Matthias Karl, Volker Matthias, Sonia Oppo, Richard Kranenburg, Jeroen Kuenen, Jana Moldanova, Sara Jutterström, Jukka-Pekka Jalkanen, and Elisa Majamäki
Atmos. Chem. Phys., 23, 1825–1862,Short summary
Potential ship impact on air pollution in the Mediterranean Sea was simulated with five chemistry transport models. An evaluation of the results for NO2 and O3 air concentrations and dry deposition is presented. Emission data, modeled year and domain were the same. Model run outputs were compared to measurements from background stations. We focused on comparing model outputs regarding the concentration of regulatory pollutants and the relative ship impact on total air pollution concentrations.
Mengyun Li, Yang Yang, Hailong Wang, Huimin Li, Pinya Wang, and Hong Liao
Atmos. Chem. Phys., 23, 1533–1544,Short summary
Using the GEOS-Chem model, the impact of the quasi-biennial oscillation (QBO) on summertime tropospheric O3 in China is investigated. In the warm phases of sea surface temperature anomalies over the eastern tropical Pacific, the QBO has a significant positive correlation with near-surface O3 concentrations over central China. The QBO impacts on O3 pollution in China are mainly a result of changing vertical transport of O3.
Lei Hu, Deborah Ottinger, Stephanie Bogle, Stephen A. Montzka, Philip L. DeCola, Ed Dlugokencky, Arlyn Andrews, Kirk Thoning, Colm Sweeney, Geoff Dutton, Lauren Aepli, and Andrew Crotwell
Atmos. Chem. Phys., 23, 1437–1448,Short summary
Effective mitigation of greenhouse gas (GHG) emissions relies on an accurate understanding of emissions. Here we demonstrate the added value of using inventory- and atmosphere-based approaches for estimating US emissions of SF6, the most potent GHG known. The results suggest a large decline in US SF6 emissions, shed light on the possible processes causing the differences between the independent estimates, and identify opportunities for substantial additional emission reductions.
Viral Shah, Daniel J. Jacob, Ruijun Dang, Lok N. Lamsal, Sarah A. Strode, Stephen D. Steenrod, K. Folkert Boersma, Sebastian D. Eastham, Thibaud M. Fritz, Chelsea Thompson, Jeff Peischl, Ilann Bourgeois, Ilana B. Pollack, Benjamin A. Nault, Ronald C. Cohen, Pedro Campuzano-Jost, Jose L. Jimenez, Simone T. Andersen, Lucy J. Carpenter, Tomás Sherwen, and Mat J. Evans
Atmos. Chem. Phys., 23, 1227–1257,Short summary
NOx in the free troposphere (above 2 km) affects global tropospheric chemistry and the retrieval and interpretation of satellite NO2 measurements. We evaluate free tropospheric NOx in global atmospheric chemistry models and find that recycling NOx from its reservoirs over the oceans is faster than that simulated in the models, resulting in increases in simulated tropospheric ozone and OH. Over the U.S., free tropospheric NO2 contributes the majority of the tropospheric NO2 column in summer.
Huimin Li, Yang Yang, Jianbing Jin, Hailong Wang, Ke Li, Pinya Wang, and Hong Liao
Atmos. Chem. Phys., 23, 1131–1145,Short summary
Future climate change will aggravate ozone pollution in Asia, especially in high-forcing scenarios. Ozone pollution in China will expand from North China to South China and extend into the cold season in a warmer future. The emphasis of this work is to quantify the impacts of future climate change on O3 pollution in Asia, which is of great significance for future O3 pollution mitigation strategies.
Yuanhong Zhao, Marielle Saunois, Philippe Bousquet, Xin Lin, Michaela I. Hegglin, Josep G. Canadell, Robert B. Jackson, and Bo Zheng
Atmos. Chem. Phys., 23, 789–807,Short summary
The large uncertainties in OH simulated by atmospheric chemistry models hinder accurate estimates of CH4 chemical loss through the bottom-up method. This study presents a new approach based on OH precursor observations and a chemical box model to improve the tropospheric OH distributions simulated by atmospheric chemistry models. Through this approach, both the global OH burden and the corresponding methane chemical loss reach consistency with the top-down method based on MCF inversions.
Cynthia H. Whaley, Kathy S. Law, Jens Liengaard Hjorth, Henrik Skov, Stephen R. Arnold, Joakim Langner, Jakob Boyd Pernov, Garance Bergeron, Ilann Bourgeois, Jesper H. Christensen, Rong-You Chien, Makoto Deushi, Xinyi Dong, Peter Effertz, Gregory Faluvegi, Mark Flanner, Joshua S. Fu, Michael Gauss, Greg Huey, Ulas Im, Rigel Kivi, Louis Marelle, Tatsuo Onishi, Naga Oshima, Irina Petropavlovskikh, Jeff Peischl, David A. Plummer, Luca Pozzoli, Jean-Christophe Raut, Tom Ryerson, Ragnhild Skeie, Sverre Solberg, Manu A. Thomas, Chelsea Thompson, Kostas Tsigaridis, Svetlana Tsyro, Steven T. Turnock, Knut von Salzen, and David W. Tarasick
Atmos. Chem. Phys., 23, 637–661,Short summary
This study summarizes recent research on ozone in the Arctic, a sensitive and rapidly warming region. We find that the seasonal cycles of near-surface atmospheric ozone are variable depending on whether they are near the coast, inland, or at high altitude. Several global model simulations were evaluated, and we found that because models lack some of the ozone chemistry that is important for the coastal Arctic locations, they do not accurately simulate ozone there.
Pooja V. Pawar, Sachin D. Ghude, Gaurav Govardhan, Prodip Acharja, Rachana Kulkarni, Rajesh Kumar, Baerbel Sinha, Vinayak Sinha, Chinmay Jena, Preeti Gunwani, Tapan Kumar Adhya, Eiko Nemitz, and Mark A. Sutton
Atmos. Chem. Phys., 23, 41–59,Short summary
In this study, for the first time in South Asia we compare simulated ammonia, ammonium, and total ammonia using the WRF-Chem model and MARGA measurements during winter in the Indo-Gangetic Plain region. Since observations show HCl promotes the fraction of high chlorides in Delhi, we added HCl / Cl emissions to the model. We conducted three sensitivity experiments with changes in HCl emissions, and improvements are reported in accurately simulating ammonia, ammonium, and total ammonia.
James D. East, Barron H. Henderson, Sergey L. Napelenok, Shannon N. Koplitz, Golam Sarwar, Robert Gilliam, Allen Lenzen, Daniel Q. Tong, R. Bradley Pierce, and Fernando Garcia-Menendez
Atmos. Chem. Phys., 22, 15981–16001,Short summary
We present a framework that uses a computer model of air quality, along with air pollution data from satellite instruments, to estimate emissions of nitrogen oxides (NOx) across the Northern Hemisphere. The framework, which advances current methods to infer emissions from satellite observations, provides observationally constrained NOx estimates, including in regions of the world where emissions are highly uncertain, and can improve simulations of air pollutants relevant for health and policy.
Joël Thanwerdas, Marielle Saunois, Isabelle Pison, Didier Hauglustaine, Antoine Berchet, Bianca Baier, Colm Sweeney, and Philippe Bousquet
Atmos. Chem. Phys., 22, 15489–15508,Short summary
Atmospheric methane (CH4) concentrations have been rising since 2007, resulting from an imbalance between CH4 sources and sinks. The CH4 budget is generally estimated through top-down approaches using CH4 and δ13C(CH4) observations as constraints. The oxidation by chlorine (Cl) contributes little to the total oxidation of CH4 but strongly influences δ13C(CH4). Here, we compare multiple recent Cl fields and quantify the influence of Cl concentrations on CH4, δ13C(CH4), and CH4 budget estimates.
Claudia Bernier, Yuxuan Wang, Guillaume Gronoff, Timothy Berkoff, K. Emma Knowland, John T. Sullivan, Ruben Delgado, Vanessa Caicedo, and Brian Carroll
Atmos. Chem. Phys., 22, 15313–15331,Short summary
Coastal regions are susceptible to variable and high ozone which is difficult to simulate. We developed a method to characterize large datasets of multi-dimensional measurements from lidar instruments taken in coastal regions. Using the clustered ozone groups, we evaluated model performance in simulating the coastal ozone variability vertically and diurnally. The approach allowed us to pinpoint areas where the models succeed in simulating coastal ozone and areas where there are still gaps.
Agnan, Y., Le Dantec, T., Moore, C. W., Edwards, G. C., and Obrist D.: New Constraints on Terrestrial Surface–Atmosphere Fluxes of Gaseous Elemental Mercury Using a Global Database, Environ. Sci. Technol., 50, 507–524, 2016.
AMAP: AMAP Assessment 2009: Human health in the Arctic, Arctic Monitoring and Assessment Programme (AMAP), Oslo, Norway, 2009.
AMAP: Updating Historical Global Inventories of Anthropogenic Mercury Emissions to Air, AMAP Technical Report No. 3, Arctic Monitoring and Assessment Programme (AMAP), Oslo, Norway, 2010.
AMAP/UNEP: Technical Background Report for the Global Mercury Assessment 2013, Arctic Monitoring and Assessment Programme, Oslo, Norway/UNEP Chemicals Branch, Geneva, Switzerland, vi + 263 pp., available at: http://www.amap.no/documents/download/1265 (last access: 12 June 2015), 2013a.
AMAP/UNEP: Geospatially distributed mercury emissions dataset 2010v1, http://www.amap.no/mercury-emissions (last access: 1 August 2016), 2013b.
Ambio: Special issue: Swain, E. B., Jakus, P. M., Rice, G., Lupi, F., Maxson, P. A., Pacyna, J. M., Penn, A. F., Spiegel, S. J., and Veiga, M. M.: Socioeconomic consequences of mercury use and pollution, Ambio, 36, 45–61, 2007.
Amos, H. M., Jacob, D. J., Holmes, C. D., Fisher, J. A., Wang, Q., Yantosca, R. M., Corbitt, E. S., Galarneau, E., Rutter, A. P., Gustin, M. S., Steffen, A., Schauer, J. J., Graydon, J. A., Louis, V. L. St., Talbot, R. W., Edgerton, E. S., Zhang, Y., and Sunderland, E. M.: Gas-particle partitioning of atmospheric Hg(II) and its effect on global mercury deposition, Atmos. Chem. Phys., 12, 591–603, https://doi.org/10.5194/acp-12-591-2012, 2012.
Amos, H. M., Jacob, D. J., Streets, D. G., and Sunderland, E. M.: Legacy impacts of all-time anthropogenic emissions on the global mercury cycle, Global Biogeochem. Cy., 27, 410–421, 2013.
Amos, H. M., Jacob, D. J., Kocman, D., Horowitz, H. M., Zhang, Y., Dutkiewicz, S., Horvat, M., Corbitt, E. S., Krabbenhoft, D. P., and Sunderland, E. M.: Global Biogeochemical Implications of Mercury Discharges from Rivers and Sediment Burial, Environ. Sci. Technol., 48, 9514–9522, 2014.
Amos, H. M., Sonke, J. E., Obrist, D., Robins, N., Hagan, N., Horowitz, H. M., Mason, R. P., Witt, M., Hedgecock, I. M., Corbitt, E. S., and Sunderland, E. M.: Observational and Modeling Constraints on Global Anthropogenic Enrichment of Mercury, Environ. Sci. Technol., 49, 4036–4047, 2015.
Ariya, P. A., Khalizov, A., and Gidas, A.: Reactions of Gaseous Mercury with Atomic and Molecular Halogens: Kinetics, Product Studies, and Atmospheric Implications, J. Phys. Chem. A, 106, 7310–7320, 2002.
Ariya, P. A., Amyot, M., Dastoor, A., Deeds, D., Feinberg, A., Kos, G., Poulain, A., Ryjkov, A., Semeniuk, K., Subir, M., and Toyota, K.: Mercury Physicochemical and Biogeochemical Transformation in the Atmosphere and at Atmospheric Interfaces: A Review and Future Directions, Chem. Rev., 15, 3760–3802, https://doi.org/10.1021/cr500667e, 2015.
Baker, K. R. and Bash, J. O.: Regional Scale Photochemical Model Evaluation of Total Mercury Wet Deposition and Speciated Ambient Mercury, Atmos. Environ., 49, 151–162, 2012.
Bullock, O. R., Atkinson, D., Braverman, T., Civerolo, K., Dastoor, A., Davignon, D., Ku, J.-Y., Lohman, K., Myers, T. C., Park, R. J., Seigneur, C., Selin, N. E., Sistla, G., and Vijayaraghavan, K.: The North American Mercury Model Intercomparison Study (NAMMIS): Study description and model-to-model comparisons, J. Geophys. Res., 113, D17310, 2008.
Calvert, J. G. and Lindberg, S. E.: echanisms of mercury removal by O3 and OH in the atmosphere, Atmos. Environ., 39, 3355–3367, https://doi.org/10.1016/j.atmosenv.2005.01.055, 2005.
Chen, L., Wang, H. H., Liu, J. F., Tong, Y. D., Ou, L. B., Zhang, W., Hu, D., Chen, C., and Wang, X. J.: Intercontinental transport and deposition patterns of atmospheric mercury from anthropogenic emissions, Atmos. Chem. Phys., 14, 10163–10176, https://doi.org/10.5194/acp-14-10163-2014, 2014.
Christensen, J. H., Brandt, J., Frohn, L. M., and Skov, H.: Modelling of Mercury in the Arctic with the Danish Eulerian Hemispheric Model, Atmos. Chem. Phys., 4, 2251–2257, https://doi.org/10.5194/acp-4-2251-2004, 2004.
Cohen, M. D., Draxler, R. R., Artz, R. S., Gustin, M., Han, Y.-J., Holsen, T. M., Jaffe, D., Kelley, P., Lei, H., Loughner, C., Luke, W., Lyman, S., Niemi, D., Pacyna, J. M., Pilote, M., Poissant, L., Ratte, D., Ren, X., Steenhouisen, F., Tordon, R., and Wilson, S.: Modeling the global atmospheric transport and deposition of mercury to the Great Lakes, Elementa: Science of the Anthropocene, 4, 000118, https://doi.org/10.12952/journal.elementa.000118, 2016.
Corbitt, E. S., Jacob, D. J., Holmes, C. D., Streets, D. G., and Sunderland, E. M.: Global source-receptor relationships for mercury deposition under present-day and 2050 emissions scenarios, Environ. Sci. Technol., 45, 10477–10484, 2011.
Cremer, D., Kraka, E., and Filatov, M.: Bonding in Mercury Molecules Described by the Normalized Elimination of the Small Component and Coupled Cluster Theory, Chem. Phys. Chem., 9, 2510–2521, https://doi.org/10.1002/cphc.200800510, 2008.
Dastoor, A., Ryzhkov, A., Durnford, D., Lehnherr, I., Steffen, A., and Morrison, H.: Atmospheric mercury in the Canadian Arctic. Part II: Insight from modeling, Sci. Total Environ., 509–510, 16–27, https://doi.org/10.1016/j.scitotenv.2014.10.112, 2015
De Simone, F., Gencarelli, C., Hedgecock, I., and Pirrone, N.: Global atmospheric cycle of mercury: a model study on the impact of oxidation mechanisms, Environ. Sci. Poll. Res., 21, 4110–4123, 2014.
De Simone, F., Cinnirella, S., Gencarelli, C. N., Yang, X., Hedgecock, I. M., Pirrone, N.: Model Study of Global Mercury Deposition from Biomass Burning, Environ. Sci. Technol., 49, 6712–6721, 2015.
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An assessment of current and future emissions, air concentrations and atmospheric deposition of mercury worldwide is presented on the basis of results obtained during the performance of the EU GMOS (Global Mercury Observation System) project. Emission estimates for mercury were prepared with the main goal of applying them in models to assess current (2013) and future (2035) air concentrations and atmospheric deposition of this contaminant.
An assessment of current and future emissions, air concentrations and atmospheric deposition of...