Articles | Volume 21, issue 16
https://doi.org/10.5194/acp-21-12783-2021
© Author(s) 2021. This work is distributed under
the Creative Commons Attribution 4.0 License.
the Creative Commons Attribution 4.0 License.
https://doi.org/10.5194/acp-21-12783-2021
© Author(s) 2021. This work is distributed under
the Creative Commons Attribution 4.0 License.
the Creative Commons Attribution 4.0 License.
Impact of Athabasca oil sands operations on mercury levels in air and deposition
Ashu Dastoor
CORRESPONDING AUTHOR
Air Quality Research Division, Environment and Climate Change Canada,
2121 Trans-Canada Highway, Dorval, Québec, Canada
Andrei Ryjkov
Air Quality Research Division, Environment and Climate Change Canada,
2121 Trans-Canada Highway, Dorval, Québec, Canada
Gregor Kos
Department of Chemistry and Biochemistry, Concordia University, 7141
Sherbrooke Street West, Montreal, Québec, Canada
Junhua Zhang
Air Quality Research Division, Environment and Climate Change Canada,
4905 Dufferin Street, Toronto, Ontario, Canada
Jane Kirk
Aquatic Contaminants Research Division, Environment and Climate Change
Canada, 867 Lakeshore Road, Burlington, Ontario, Canada
Matthew Parsons
Meteorological Service of Canada, Environment and Climate Change
Canada, 9250 49 Street NW, Edmonton, Alberta, Canada
Alexandra Steffen
Air Quality Research Division, Environment and Climate Change Canada,
4905 Dufferin Street, Toronto, Ontario, Canada
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The MOSAIC inorganic aerosol sub-model has been implemented in the GEM-MACH air quality model. MOSAIC includes metal cation reactions and is a non-equilibrium, two-moment scheme that conserves aerosol number. Compared to the current aerosol sub-model, MOSAIC produces a more accurate size distribution and aerosol number concentration. It also improves the simulated nitrate and ammonium distribution. This work serves to expand the capacity of GEM-MACH for chemistry and weather coupling.
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Geosci. Model Dev., 17, 335–346, https://doi.org/10.5194/gmd-17-335-2024, https://doi.org/10.5194/gmd-17-335-2024, 2024
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The interpolation process is the most computationally expensive step of the semi-Lagrangian (SL) approach. In this paper we implement a new interpolation scheme into the semi-Lagrangian approach which has the same computational cost as a third-order polynomial scheme but with the accuracy of a fourth-order interpolation scheme. This improvement is achieved by using two third-order backward and forward polynomial interpolation schemes in two consecutive time steps.
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Atmos. Chem. Phys., 22, 13527–13549, https://doi.org/10.5194/acp-22-13527-2022, https://doi.org/10.5194/acp-22-13527-2022, 2022
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Absorbing particles like black carbon can be coated with other matter. How much radiation these particles absorb depends on the coating thickness. The removal of these particles by clouds and rain depends on the coating composition. These effects are important for both climate and air quality. We implement a more detailed representation of these particles in an air quality model which accounts for both coating thickness and composition. We find a significant effect on particle concentrations.
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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, https://doi.org/10.5194/acp-17-6925-2017, https://doi.org/10.5194/acp-17-6925-2017, 2017
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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.
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, https://doi.org/10.5194/acp-17-5271-2017, https://doi.org/10.5194/acp-17-5271-2017, 2017
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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.
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, https://doi.org/10.5194/acp-16-10735-2016, https://doi.org/10.5194/acp-16-10735-2016, 2016
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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.
K. Toyota, J. C. McConnell, R. M. Staebler, and A. P. Dastoor
Atmos. Chem. Phys., 14, 4101–4133, https://doi.org/10.5194/acp-14-4101-2014, https://doi.org/10.5194/acp-14-4101-2014, 2014
K. Toyota, A. P. Dastoor, and A. Ryzhkov
Atmos. Chem. Phys., 14, 4135–4167, https://doi.org/10.5194/acp-14-4135-2014, https://doi.org/10.5194/acp-14-4135-2014, 2014
G. Kos, A. Ryzhkov, A. Dastoor, J. Narayan, A. Steffen, P. A. Ariya, and L. Zhang
Atmos. Chem. Phys., 13, 4839–4863, https://doi.org/10.5194/acp-13-4839-2013, https://doi.org/10.5194/acp-13-4839-2013, 2013
Kirill Semeniuk, Ashu Dastoor, and Alex Lupu
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This paper introduces the Multi-Compartment Mercury (Hg) Modeling and Analysis Project (MCHgMAP) aimed to inform the effectiveness evaluations of two multilateral environmental agreements: the Minamata Convention on Mercury and Convention on Long-Range Transboundary Air Pollution. The experimental design exploits a variety of models (atmospheric, land, oceanic and multi-media mass balance models) to assess the short- and long-term influences of anthropogenic Hg releases in the environment.
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Geosci. Model Dev., 17, 335–346, https://doi.org/10.5194/gmd-17-335-2024, https://doi.org/10.5194/gmd-17-335-2024, 2024
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Robin Stevens, Andrei Ryjkov, Mahtab Majdzadeh, and Ashu Dastoor
Atmos. Chem. Phys., 22, 13527–13549, https://doi.org/10.5194/acp-22-13527-2022, https://doi.org/10.5194/acp-22-13527-2022, 2022
Short summary
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Absorbing particles like black carbon can be coated with other matter. How much radiation these particles absorb depends on the coating thickness. The removal of these particles by clouds and rain depends on the coating composition. These effects are important for both climate and air quality. We implement a more detailed representation of these particles in an air quality model which accounts for both coating thickness and composition. We find a significant effect on particle concentrations.
Paul A. Makar, Craig Stroud, Ayodeji Akingunola, Junhua Zhang, Shuzhan Ren, Philip Cheung, and Qiong Zheng
Atmos. Chem. Phys., 21, 12291–12316, https://doi.org/10.5194/acp-21-12291-2021, https://doi.org/10.5194/acp-21-12291-2021, 2021
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Vehicle pollutant emissions occur in an environment where upward transport can be enhanced due to the turbulence created by the vehicles as they move through the atmosphere. An approach for including these turbulence effects in regional air pollution forecast models has been derived from theoretical, observation, and higher-resolution modeling. The enhanced mixing, which occurs in the immediate vicinity of roadways, changes pollutant concentrations on the regional to continental scale.
Paul A. Makar, Ayodeji Akingunola, Jack Chen, Balbir Pabla, Wanmin Gong, Craig Stroud, Christopher Sioris, Kerry Anderson, Philip Cheung, Junhua Zhang, and Jason Milbrandt
Atmos. Chem. Phys., 21, 10557–10587, https://doi.org/10.5194/acp-21-10557-2021, https://doi.org/10.5194/acp-21-10557-2021, 2021
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We have examined the effects of airborne particles on absorption and scattering of incoming sunlight by the particles themselves via cloud formation. We used an advanced, combined high-resolution weather forecast and chemical transport computer model, for western North America, and simulations with and without the connections between particles and weather enabled. Feedbacks improved weather and air pollution forecasts and changed cloud behaviour and forest-fire pollutant amount and height.
Katherine Hayden, Shao-Meng Li, Paul Makar, John Liggio, Samar G. Moussa, Ayodeji Akingunola, Robert McLaren, Ralf M. Staebler, Andrea Darlington, Jason O'Brien, Junhua Zhang, Mengistu Wolde, and Leiming Zhang
Atmos. Chem. Phys., 21, 8377–8392, https://doi.org/10.5194/acp-21-8377-2021, https://doi.org/10.5194/acp-21-8377-2021, 2021
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We developed a method using aircraft measurements to determine lifetimes with respect to dry deposition for oxidized sulfur and nitrogen compounds over the boreal forest in Alberta, Canada. Atmospheric lifetimes were significantly shorter than derived from chemical transport models with differences related to modelled dry deposition velocities. The shorter lifetimes suggest models need to reassess dry deposition treatment and predictions of sulfur and nitrogen in the atmosphere and ecosystems.
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, https://doi.org/10.5194/amt-14-3657-2021, https://doi.org/10.5194/amt-14-3657-2021, 2021
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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.
David S. McLagan, Geoff W. Stupple, Andrea Darlington, Katherine Hayden, and Alexandra Steffen
Atmos. Chem. Phys., 21, 5635–5653, https://doi.org/10.5194/acp-21-5635-2021, https://doi.org/10.5194/acp-21-5635-2021, 2021
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An assessment of mercury emissions from a burning boreal forest was made by flying an aircraft through its plume to collect in situ gas and particulate measurements. Direct data show that in-plume gaseous elemental mercury concentrations reach up to 2.4× background for this fire and up to 5.6× when using a correlation with CO data. These unique data are applied to a series of known empirical emissions estimates and used to highlight current uncertainties in the literature.
Cynthia H. Whaley, Elisabeth Galarneau, Paul A. Makar, Michael D. Moran, and Junhua Zhang
Atmos. Chem. Phys., 20, 2911–2925, https://doi.org/10.5194/acp-20-2911-2020, https://doi.org/10.5194/acp-20-2911-2020, 2020
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Benzene and polycyclic aromatic compounds are toxic air pollutants and ubiquitous in the environment. Using a chemical transport model, we have determined the net impact of vehicle emissions on ambient concentrations of these species. Traffic emissions were found to be a significant fraction of ambient pollution in the densely populated modelled region of North America. Our simulations demonstrate the air quality benefits that would result from transitioning to a zero-emission vehicle fleet.
Mark W. Shephard, Enrico Dammers, Karen E. Cady-Pereira, Shailesh K. Kharol, Jesse Thompson, Yonatan Gainariu-Matz, Junhua Zhang, Chris A. McLinden, Andrew Kovachik, Michael Moran, Shabtai Bittman, Christopher E. Sioris, Debora Griffin, Matthew J. Alvarado, Chantelle Lonsdale, Verica Savic-Jovcic, and Qiong Zheng
Atmos. Chem. Phys., 20, 2277–2302, https://doi.org/10.5194/acp-20-2277-2020, https://doi.org/10.5194/acp-20-2277-2020, 2020
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Presented is a description and survey demonstrating the capabilities of the CrIS ammonia product for monitoring, air quality forecast model evaluation, dry deposition estimates, and emission estimates of an agricultural hotspot.
Matthew Russell, Amir Hakami, Paul A. Makar, Ayodeji Akingunola, Junhua Zhang, Michael D. Moran, and Qiong Zheng
Atmos. Chem. Phys., 19, 4393–4417, https://doi.org/10.5194/acp-19-4393-2019, https://doi.org/10.5194/acp-19-4393-2019, 2019
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High-resolution air-quality forecast modeling results are compared for two different grid spacings for the Environment and Climate Change Canada GEM-MACH model. While the higher-resolution simulations have worse formal error scores, we show that the higher-resolution model nevertheless has the ability to better resolve plume maxima and has better performance when the evaluation occurs using new scoring metrics which operate on an equal-representative-area basis.
Wanmin Gong, Stephen R. Beagley, Sophie Cousineau, Mourad Sassi, Rodrigo Munoz-Alpizar, Sylvain Ménard, Jacinthe Racine, Junhua Zhang, Jack Chen, Heather Morrison, Sangeeta Sharma, Lin Huang, Pascal Bellavance, Jim Ly, Paul Izdebski, Lynn Lyons, and Richard Holt
Atmos. Chem. Phys., 18, 16653–16687, https://doi.org/10.5194/acp-18-16653-2018, https://doi.org/10.5194/acp-18-16653-2018, 2018
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The navigability of the Arctic Ocean is increasing with the warming in recent years. Using model simulations at a much finer resolution than previous pan-Arctic studies, the impact of marine shipping emissions on air pollution in the Canadian Arctic is assessed for present (2010) and projected levels in 2030. The study found that shipping emissions have a local-to-regional impact in the Arctic at the current level; the impact will increase significantly in a projected business-as-usual scenario.
Mark Gordon, Paul A. Makar, Ralf M. Staebler, Junhua Zhang, Ayodeji Akingunola, Wanmin Gong, and Shao-Meng Li
Atmos. Chem. Phys., 18, 14695–14714, https://doi.org/10.5194/acp-18-14695-2018, https://doi.org/10.5194/acp-18-14695-2018, 2018
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This work uses aircraft-based measurements of smokestack plumes carried out in northern Alberta in 2013. These measurements are used to test equations used to predict how high in the air smokestack plumes rise. It is important to predict plume rise height accurately as it tells us how far downwind pollutants are carried and what air quality can be expected at the surface. We found that the equations that are typically used significantly underestimate the plume rise at this location.
Craig A. Stroud, Paul A. Makar, Junhua Zhang, Michael D. Moran, Ayodeji Akingunola, Shao-Meng Li, Amy Leithead, Katherine Hayden, and May Siu
Atmos. Chem. Phys., 18, 13531–13545, https://doi.org/10.5194/acp-18-13531-2018, https://doi.org/10.5194/acp-18-13531-2018, 2018
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It is shown that using measurement-derived volatile organic compound (VOC) and organic aerosol (OA) emissions in the GEM-MACH air quality model provides better overall predictions compared to using bottom-up emission inventories. This work was done to better constrain the fugitive organic emissions from the Athabasca oil sands region, which are a challenge to estimate with bottom-up emission approaches. We use observations from the 2013 Joint Oil Sands Monitoring study.
Junhua Zhang, Michael D. Moran, Qiong Zheng, Paul A. Makar, Pegah Baratzadeh, George Marson, Peter Liu, and Shao-Meng Li
Atmos. Chem. Phys., 18, 10459–10481, https://doi.org/10.5194/acp-18-10459-2018, https://doi.org/10.5194/acp-18-10459-2018, 2018
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This paper discusses the development of new synthesized emissions inventories and the generation of air quality model-ready emissions files for the Athabasca Oil Sands Region of Alberta, Canada, using multiple emissions inventories, continuous emissions monitoring data, and inferred emission rates based on aircraft measurements. Novel facility-specific gridded spatial surrogate fields were generated to allocate emissions spatially within each huge mining facility.
Paul A. Makar, Ayodeji Akingunola, Julian Aherne, Amanda S. Cole, Yayne-abeba Aklilu, Junhua Zhang, Isaac Wong, Katherine Hayden, Shao-Meng Li, Jane Kirk, Ken Scott, Michael D. Moran, Alain Robichaud, Hazel Cathcart, Pegah Baratzedah, Balbir Pabla, Philip Cheung, Qiong Zheng, and Dean S. Jeffries
Atmos. Chem. Phys., 18, 9897–9927, https://doi.org/10.5194/acp-18-9897-2018, https://doi.org/10.5194/acp-18-9897-2018, 2018
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Complex computer model output was compared to and fused with observation data, to estimate potential damage due to acidifying precipitation for ecosystems in the Canadian provinces of Alberta and Saskatchewan. Estimated deposition was compared to the maximum no-damage ecosystem capacity for sulfur and/or nitrogen uptake; these critical loads were exceeded, for areas between 10 000 and 330 000 square kilometres, depending on ecosystem type: ecosystem damage will occur at 2013 emission levels.
Cynthia H. Whaley, Elisabeth Galarneau, Paul A. Makar, Ayodeji Akingunola, Wanmin Gong, Sylvie Gravel, Michael D. Moran, Craig Stroud, Junhua Zhang, and Qiong Zheng
Geosci. Model Dev., 11, 2609–2632, https://doi.org/10.5194/gmd-11-2609-2018, https://doi.org/10.5194/gmd-11-2609-2018, 2018
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We present a new, high-resolution, North American model of PAHs and benzene, which are toxic air pollutants that cause a variety of negative health impacts. Our simulation in a densely populated region of Canada and the U.S. shows that the model is improved over a previous model. The new model is particularly refined regarding the gas–particle partitioning of these pollutants, which has impacts on deposition and inhalation. The simulation was sensitive to the selection of vehicle emissions.
Ayodeji Akingunola, Paul A. Makar, Junhua Zhang, Andrea Darlington, Shao-Meng Li, Mark Gordon, Michael D. Moran, and Qiong Zheng
Atmos. Chem. Phys., 18, 8667–8688, https://doi.org/10.5194/acp-18-8667-2018, https://doi.org/10.5194/acp-18-8667-2018, 2018
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We examine the manner in which air-quality models simulate lofting of buoyant plumes of emissions from stacks (plume rise) and the impact of the level of detail in algorithms simulating particles' variation in size (particle size distribution). The most commonly used plume rise algorithm underestimates the height of plumes compared to observations, while a revised algorithm has much better performance. A 12-bin size distribution reduced the forecast 2-bin size distribution bias error by 32 %.
Annemarie Fraser, Ashu Dastoor, and Andrei Ryjkov
Atmos. Chem. Phys., 18, 7263–7286, https://doi.org/10.5194/acp-18-7263-2018, https://doi.org/10.5194/acp-18-7263-2018, 2018
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This paper quantifies the emissions of mercury from biomass burning in Canada. Using an emissions inventory of mercury in the GEM-MACH-Hg model, surface observations of mercury concentration, and a top-down inversion method, we generate optimized emissions of mercury. We find that biomass burning is an important source of mercury emissions and deposition in Canada. Significant uncertainty remains, due to uncertainty in the speciation of emitted mercury.
David S. McLagan, Carl P. J. Mitchell, Alexandra Steffen, Hayley Hung, Cecilia Shin, Geoff W. Stupple, Mark L. Olson, Winston T. Luke, Paul Kelley, Dean Howard, Grant C. Edwards, Peter F. Nelson, Hang Xiao, Guey-Rong Sheu, Annekatrin Dreyer, Haiyong Huang, Batual Abdul Hussain, Ying D. Lei, Ilana Tavshunsky, and Frank Wania
Atmos. Chem. Phys., 18, 5905–5919, https://doi.org/10.5194/acp-18-5905-2018, https://doi.org/10.5194/acp-18-5905-2018, 2018
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A new passive air sampler for gaseous mercury was tested at 20 sites on four continents. These sites have in common that they use the state-of-the-art active air sampling technique for gaseous mercury on a continuous basis and therefore allow for an evaluation and calibration of the passive sampler. The sampler proved to work exceptionally well, with a precision and accuracy on par with the active
instrument and better than what has previously been achieved with passive samplers.
Stephanie C. Pugliese, Jennifer G. Murphy, Felix R. Vogel, Michael D. Moran, Junhua Zhang, Qiong Zheng, Craig A. Stroud, Shuzhan Ren, Douglas Worthy, and Gregoire Broquet
Atmos. Chem. Phys., 18, 3387–3401, https://doi.org/10.5194/acp-18-3387-2018, https://doi.org/10.5194/acp-18-3387-2018, 2018
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We developed the Southern Ontario CO2 Emissions (SOCE) inventory, which identifies the spatial and temporal distribution (2.5 km and hourly, respectively) of CO2 emissions from seven source sectors. When the SOCE inventory was used with a chemistry transport model, we found strong agreement between modelled and measured mixing ratios. We were able to quantify that natural gas combustion contributes > 80 % of CO2 emissions at nighttime while on-road emissions contribute > 70 % during the day.
Cynthia H. Whaley, Paul A. Makar, Mark W. Shephard, Leiming Zhang, Junhua Zhang, Qiong Zheng, Ayodeji Akingunola, Gregory R. Wentworth, Jennifer G. Murphy, Shailesh K. Kharol, and Karen E. Cady-Pereira
Atmos. Chem. Phys., 18, 2011–2034, https://doi.org/10.5194/acp-18-2011-2018, https://doi.org/10.5194/acp-18-2011-2018, 2018
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Using a modified air quality forecasting model, we have found that a significant fraction (> 50 %) of ambient ammonia comes from re-emission from plants and soils in the broader Athabasca Oil Sands region and much of Alberta and Saskatchewan. We also found that about 20 % of ambient ammonia in Alberta and Saskatchewan came from forest fires in the summer of 2013. The addition of these two processes improved modelled ammonia, which was a motivating factor in undertaking this research.
Yuan You, Ralf M. Staebler, Samar G. Moussa, Yushan Su, Tony Munoz, Craig Stroud, Junhua Zhang, and Michael D. Moran
Atmos. Chem. Phys., 17, 14119–14143, https://doi.org/10.5194/acp-17-14119-2017, https://doi.org/10.5194/acp-17-14119-2017, 2017
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A novel approach for traffic emission measurements is shown to have the capacity to provide high-time-resolution accurate concentrations of key air pollutants. A top-down method for quantifying real-world emission rates produced vehicular emission factor estimates for carbon monoxide that agreed well with bottom-up values. Significant ammonia and hydrogen cyanide emissions were observed. The main factors modulating the concentrations were turbulent mixing and traffic density.
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, https://doi.org/10.5194/acp-17-6925-2017, https://doi.org/10.5194/acp-17-6925-2017, 2017
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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.
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, https://doi.org/10.5194/acp-17-5271-2017, https://doi.org/10.5194/acp-17-5271-2017, 2017
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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.
Craig A. Emmerton, Vincent L. St. Louis, Igor Lehnherr, Jennifer A. Graydon, Jane L. Kirk, and Kimberly J. Rondeau
Biogeosciences, 13, 5849–5863, https://doi.org/10.5194/bg-13-5849-2016, https://doi.org/10.5194/bg-13-5849-2016, 2016
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It is unknown if lakes are important contributors to the total transfer of greenhouse gases between high Arctic regions and the atmosphere. We measured the transfer of carbon greenhouse gases between lakes and the atmosphere and compared results with adjacent landscapes. We found lakes were weak emitters of the gases to the atmosphere, compared to contributions of terrestrial ecosystems, and will likely continue to be inconsequential to regional carbon cycling in a warmer future climate.
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, https://doi.org/10.5194/acp-16-10735-2016, https://doi.org/10.5194/acp-16-10735-2016, 2016
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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.
K. Toyota, J. C. McConnell, R. M. Staebler, and A. P. Dastoor
Atmos. Chem. Phys., 14, 4101–4133, https://doi.org/10.5194/acp-14-4101-2014, https://doi.org/10.5194/acp-14-4101-2014, 2014
K. Toyota, A. P. Dastoor, and A. Ryzhkov
Atmos. Chem. Phys., 14, 4135–4167, https://doi.org/10.5194/acp-14-4135-2014, https://doi.org/10.5194/acp-14-4135-2014, 2014
A. Steffen, J. Bottenheim, A. Cole, R. Ebinghaus, G. Lawson, and W. R. Leaitch
Atmos. Chem. Phys., 14, 2219–2231, https://doi.org/10.5194/acp-14-2219-2014, https://doi.org/10.5194/acp-14-2219-2014, 2014
A. Steffen, J. Bottenheim, A. Cole, T. A. Douglas, R. Ebinghaus, U. Friess, S. Netcheva, S. Nghiem, H. Sihler, and R. Staebler
Atmos. Chem. Phys., 13, 7007–7021, https://doi.org/10.5194/acp-13-7007-2013, https://doi.org/10.5194/acp-13-7007-2013, 2013
T. Berg, K. A. Pfaffhuber, A. S. Cole, O. Engelsen, and A. Steffen
Atmos. Chem. Phys., 13, 6575–6586, https://doi.org/10.5194/acp-13-6575-2013, https://doi.org/10.5194/acp-13-6575-2013, 2013
G. Kos, A. Ryzhkov, A. Dastoor, J. Narayan, A. Steffen, P. A. Ariya, and L. Zhang
Atmos. Chem. Phys., 13, 4839–4863, https://doi.org/10.5194/acp-13-4839-2013, https://doi.org/10.5194/acp-13-4839-2013, 2013
A. S. Cole, A. Steffen, K. A. Pfaffhuber, T. Berg, M. Pilote, L. Poissant, R. Tordon, and H. Hung
Atmos. Chem. Phys., 13, 1535–1545, https://doi.org/10.5194/acp-13-1535-2013, https://doi.org/10.5194/acp-13-1535-2013, 2013
Related subject area
Subject: Gases | Research Activity: Atmospheric Modelling and Data Analysis | Altitude Range: Troposphere | Science Focus: Chemistry (chemical composition and reactions)
Assessing the relative impacts of satellite ozone and its precursor observations to improve global tropospheric ozone analysis using multiple chemical reanalysis systems
Evaluating present-day and future impacts of agricultural ammonia emissions on atmospheric chemistry and climate
Air-pollution-satellite-based CO2 emission inversion: system evaluation, sensitivity analysis, and future research direction
Insights into ozone pollution control in urban areas by decoupling meteorological factors based on machine learning
Quantification of regional net CO2 flux errors in the Orbiting Carbon Observatory-2 (OCO-2) v10 model intercomparison project (MIP) ensemble using airborne measurements
Reactive nitrogen in and around the northeastern and mid-Atlantic US: sources, sinks, and connections with ozone
Preindustrial-to-present-day changes in atmospheric carbon monoxide: agreement and gaps between ice archives and global model reconstructions
Investigating processes influencing simulation of local Arctic wintertime anthropogenic pollution in Fairbanks, Alaska, during ALPACA-2022
Urban ozone formation and sensitivities to volatile chemical products, cooking emissions, and NOx upwind of and within two Los Angeles Basin cities
Causes of growing middle-to-upper tropospheric ozone over the northwest Pacific region
Impact of introducing electric vehicles on ground-level O3 and PM2.5 in the Greater Tokyo Area: yearly trends and the importance of changes in the urban heat island effect
A CO2–Δ14CO2 inversion setup for estimating European fossil CO2 emissions
Maximum ozone concentrations in the southwestern US and Texas: implications of the growing predominance of the background contribution
Derivation of atmospheric reaction mechanisms for volatile organic compounds by the SAPRC mechanism generation system (MechGen)
Seasonal, regional, and vertical characteristics of high-carbon-monoxide plumes along with their associated ozone anomalies, as seen by IAGOS between 2002 and 2019
The potential of drone observations to improve air quality predictions by 4D-Var
Process analysis of elevated concentrations of organic acids at Whiteface Mountain, New York
Ozone source attribution in polluted European areas during summer 2017 as simulated with MECO(n)
Opinion: Challenges and needs of tropospheric chemical mechanism development
The atmospheric oxidizing capacity in China – Part 2: Sensitivity to emissions of primary pollutants
Role of chemical production and depositional losses on formaldehyde in the Community Regional Atmospheric Chemistry Multiphase Mechanism (CRACMM)
Review of source analyses of ambient volatile organic compounds considering reactive losses: methods of reducing loss effects, impacts of losses, and sources
Interpreting summertime hourly variation of NO2 columns with implications for geostationary satellite applications
An investigation into atmospheric nitrous acid (HONO) processes in South Korea
Performance evaluation of UKESM1 for surface ozone across the pan-tropics
Constraining light dependency in modeled emissions through comparison to observed biogenic volatile organic compound (BVOC) concentrations in a southeastern US forest
A global re-analysis of regionally resolved emissions and atmospheric mole fractions of SF6 for the period 2005–2021
Monoterpene oxidation pathways initiated by acyl peroxy radical addition
Tropospheric ozone precursors: global and regional distributions, trends, and variability
The contribution of transport emissions to ozone mixing ratios and methane lifetime in 2015 and 2050 in the Shared Socioeconomic Pathways (SSPs)
Local and transboundary contributions to nitrogen loadings across East Asia using CMAQ-ISAM and GEMS-informed emissions inventory during the winter-spring transition
Ether and ester formation from peroxy radical recombination: a qualitative reaction channel analysis
ACEIC: a comprehensive anthropogenic chlorine emission inventory for China
Impact of methane and other precursor emission reductions on surface ozone in Europe: scenario analysis using the European Monitoring and Evaluation Programme (EMEP) Meteorological Synthesizing Centre – West (MSC-W) model
Investigating the response of China’s surface ozone concentration to the future changes of multiple factors
Chemistry-climate feedback of atmospheric methane in a methane emission flux driven chemistry-climate model
Natural emissions of VOC and NOx over Africa constrained by TROPOMI HCHO and NO2 data using the MAGRITTEv1.1 model
Verifying national inventory-based combustion emissions of CO2 across the UK and mainland Europe using satellite observations of atmospheric CO and CO2
Revisiting the high tropospheric ozone over Southern Africa: overestimated biomass burning and underestimated anthropogenic emissions
Enhanced understanding of atmospheric blocking modulation on ozone dynamics within a high-resolution Earth system model
Estimating the variability of NOx emissions from Wuhan with TROPOMI NO2 data during 2018 to 2023
An improved estimate of inorganic iodine emissions from the ocean using a coupled surface microlayer box model
Technical note: A comparative study of chemistry schemes for volcanic sulfur dioxide in Lagrangian transport simulations: a case study of the 2019 Raikoke eruption
Evaluating tropospheric nitrogen dioxide in UKCA using OMI satellite retrievals over South and East Asia
Impact of improved representation of volatile organic compound emissions and production of NOx reservoirs on modeled urban ozone production
The effect of different climate and air quality policies in China on in situ ozone production in Beijing
Enhancing long-term trend simulation of the global tropospheric hydroxyl (TOH) and its drivers from 2005 to 2019: a synergistic integration of model simulations and satellite observations
Intercomparison of GEOS-Chem and CAM-chem tropospheric oxidant chemistry within the Community Earth System Model version 2 (CESM2)
Development of a detailed gaseous oxidation scheme of naphthalene for secondary organic aerosol (SOA) formation and speciation
Anthropogenic emission controls reduce summertime ozone-temperature sensitivity in the United States
Takashi Sekiya, Emanuele Emili, Kazuyuki Miyazaki, Antje Inness, Zhen Qu, R. Bradley Pierce, Dylan Jones, Helen Worden, William Y. Y. Cheng, Vincent Huijnen, and Gerbrand Koren
Atmos. Chem. Phys., 25, 2243–2268, https://doi.org/10.5194/acp-25-2243-2025, https://doi.org/10.5194/acp-25-2243-2025, 2025
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Five global chemical reanalysis datasets were used to assess the relative impacts of assimilating satellite ozone and its precursor measurements on tropospheric ozone analyses for 2010. The multiple reanalysis system comparison allows an evaluation of the dependency of the impacts on different reanalysis systems. The results suggested the importance of satellite ozone and its precursor measurements for improving ozone analysis in the whole troposphere, with varying magnitudes among the systems.
Maureen Beaudor, Didier Hauglustaine, Juliette Lathière, Martin Van Damme, Lieven Clarisse, and Nicolas Vuichard
Atmos. Chem. Phys., 25, 2017–2046, https://doi.org/10.5194/acp-25-2017-2025, https://doi.org/10.5194/acp-25-2017-2025, 2025
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Agriculture is the biggest ammonia (NH3) source, impacting air quality, climate, and ecosystems. Because of food demand, NH3 emissions are projected to rise by 2100. Using a global model, we analyzed the impact of present and future NH3 emissions generated from a land model. Our results show improved ammonia patterns compared to a reference inventory. Future scenarios predict up to 70 % increase in global NH3 burden, with significant changes in radiative forcing that can greatly elevate N2O.
Hui Li, Jiaxin Qiu, and Bo Zheng
Atmos. Chem. Phys., 25, 1949–1963, https://doi.org/10.5194/acp-25-1949-2025, https://doi.org/10.5194/acp-25-1949-2025, 2025
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We conduct a sensitivity analysis with 31 tests on various factors including prior emissions, model resolution, satellite constraint, and other system configurations to assess the vulnerability of emission estimates across temporal, sectoral, and regional dimensions. This reveals the robustness of emissions estimated by this air-pollution-satellite-based CO2 emission inversion system, with relative change between tests and base inversion below 4.0 % for national annual NOx and CO2 emissions.
Yuqing Qiu, Xin Li, Wenxuan Chai, Yi Liu, Mengdi Song, Xudong Tian, Qiaoli Zou, Wenjun Lou, Wangyao Zhang, Juan Li, and Yuanhang Zhang
Atmos. Chem. Phys., 25, 1749–1763, https://doi.org/10.5194/acp-25-1749-2025, https://doi.org/10.5194/acp-25-1749-2025, 2025
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The chemical reactions of ozone (O3) formation are related to meteorology and local emissions. Here, a random forest approach was used to eliminate the effects of meteorological factors (dispersion or transport) on O3 and its precursors. Variations in the sensitivity of O3 formation and the apportionment of emission sources were revealed after meteorological normalization. Our results suggest that meteorological variations should be considered when diagnosing O3 formation.
Jeongmin Yun, Junjie Liu, Brendan Byrne, Brad Weir, Lesley E. Ott, Kathryn McKain, Bianca C. Baier, Luciana V. Gatti, and Sebastien C. Biraud
Atmos. Chem. Phys., 25, 1725–1748, https://doi.org/10.5194/acp-25-1725-2025, https://doi.org/10.5194/acp-25-1725-2025, 2025
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This study quantifies errors in regional net surface–atmosphere CO2 flux estimates from an inverse model ensemble using airborne CO2 measurements. Our results show that flux error estimates based on observations significantly exceed those computed from the ensemble spread of flux estimates in regions with high fossil fuel emissions. This finding suggests the presence of systematic biases in the inversion estimates, associated with errors in the fossil fuel emissions common to all models.
Min Huang, Gregory R. Carmichael, Kevin W. Bowman, Isabelle De Smedt, Andreas Colliander, Michael H. Cosh, Sujay V. Kumar, Alex B. Guenther, Scott J. Janz, Ryan M. Stauffer, Anne M. Thompson, Niko M. Fedkin, Robert J. Swap, John D. Bolten, and Alicia T. Joseph
Atmos. Chem. Phys., 25, 1449–1476, https://doi.org/10.5194/acp-25-1449-2025, https://doi.org/10.5194/acp-25-1449-2025, 2025
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We use model simulations along with multiplatform, multidisciplinary observations and a range of analysis methods to estimate and understand the distributions, temporal changes, and impacts of reactive nitrogen and ozone over the most populous US region that has undergone significant environmental changes. Deposition, biogenic emissions, and extra-regional sources have been playing increasingly important roles in controlling pollutant budgets in this area as local anthropogenic emissions drop.
Xavier Faïn, Sophie Szopa, Vaishali Naïk, Patricia Martinerie, David M. Etheridge, Rachael H. Rhodes, Cathy M. Trudinger, Vasilii V. Petrenko, Kévin Fourteau, and Philip Place
Atmos. Chem. Phys., 25, 1105–1119, https://doi.org/10.5194/acp-25-1105-2025, https://doi.org/10.5194/acp-25-1105-2025, 2025
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Carbon monoxide (CO) plays a crucial role in the atmosphere's oxidizing capacity. In this study, we analyse how historical (1850–2014) [CO] outputs from state-of-the-art global chemistry–climate models over Greenland and Antarctica are able to capture both absolute values and trends recorded in multi-site ice archives. A disparity in [CO] growth rates emerges in the Northern Hemisphere between models and observations from 1920–1975 CE, possibly linked to uncertainties in CO emission factors.
Natalie Brett, Kathy S. Law, Steve R. Arnold, Javier G. Fochesatto, Jean-Christophe Raut, Tatsuo Onishi, Robert Gilliam, Kathleen Fahey, Deanna Huff, George Pouliot, Brice Barret, Elsa Dieudonné, Roman Pohorsky, Julia Schmale, Andrea Baccarini, Slimane Bekki, Gianluca Pappaccogli, Federico Scoto, Stefano Decesari, Antonio Donateo, Meeta Cesler-Maloney, William Simpson, Patrice Medina, Barbara D'Anna, Brice Temime-Roussel, Joel Savarino, Sarah Albertin, Jingqiu Mao, Becky Alexander, Allison Moon, Peter F. DeCarlo, Vanessa Selimovic, Robert Yokelson, and Ellis S. Robinson
Atmos. Chem. Phys., 25, 1063–1104, https://doi.org/10.5194/acp-25-1063-2025, https://doi.org/10.5194/acp-25-1063-2025, 2025
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Processes influencing dispersion of local anthropogenic pollution in Arctic wintertime are investigated with Lagrangian dispersion modelling. Simulated power plant plume rise that considers temperature inversion layers improves results compared to observations (interior Alaska). Modelled surface concentrations are improved by representation of vertical mixing and emission estimates. Large increases in diesel vehicle emissions at temperatures reaching −35°C are required to reproduce observed NOx.
Chelsea E. Stockwell, Matthew M. Coggon, Rebecca H. Schwantes, Colin Harkins, Bert Verreyken, Congmeng Lyu, Qindan Zhu, Lu Xu, Jessica B. Gilman, Aaron Lamplugh, Jeff Peischl, Michael A. Robinson, Patrick R. Veres, Meng Li, Andrew W. Rollins, Kristen Zuraski, Sunil Baidar, Shang Liu, Toshihiro Kuwayama, Steven S. Brown, Brian C. McDonald, and Carsten Warneke
Atmos. Chem. Phys., 25, 1121–1143, https://doi.org/10.5194/acp-25-1121-2025, https://doi.org/10.5194/acp-25-1121-2025, 2025
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In urban areas, emissions from everyday products like paints, cleaners, and personal care products, along with non-traditional sources such as cooking, are increasingly important and impact air quality. This study uses a box model to evaluate how these emissions impact ozone in the Los Angeles Basin and quantifies the impact of gaseous cooking emissions. Accurate representation of these and other anthropogenic sources in inventories is crucial for informing effective air quality policies.
Xiaodan Ma, Jianping Huang, Michaela I. Hegglin, Patrick Jöckel, and Tianliang Zhao
Atmos. Chem. Phys., 25, 943–958, https://doi.org/10.5194/acp-25-943-2025, https://doi.org/10.5194/acp-25-943-2025, 2025
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Our research explored changes in ozone levels in the northwest Pacific region over 30 years, revealing a significant increase in the middle-to-upper troposphere, especially during spring and summer. This rise is influenced by both stratospheric and tropospheric sources, which affect climate and air quality in East Asia. This work underscores the need for continued study to understand underlying mechanisms.
Hiroo Hata, Norifumi Mizushima, and Tomohiko Ihara
Atmos. Chem. Phys., 25, 1037–1061, https://doi.org/10.5194/acp-25-1037-2025, https://doi.org/10.5194/acp-25-1037-2025, 2025
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The introduction of battery electric vehicles (BEVs) is expected to reduce the primary air pollutants from vehicular exhaust and evaporative emissions while reducing the anthropogenic heat produced by vehicles, ultimately mitigating the urban heat island (UHI) effect. This study revealed the impact of introducing BEVs on the decrease in the UHI effect and the impact of BEVs on the formation of tropospheric ozone and fine particulate matter in the Greater Tokyo Area of Japan.
Carlos Gómez-Ortiz, Guillaume Monteil, Sourish Basu, and Marko Scholze
Atmos. Chem. Phys., 25, 397–424, https://doi.org/10.5194/acp-25-397-2025, https://doi.org/10.5194/acp-25-397-2025, 2025
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In this paper, we test new implementations of our inverse modeling tool to estimate the weekly and regional CO2 emissions from fossil fuels in Europe. We use synthetic atmospheric observations of CO2 and radiocarbon (14CO2) to trace emissions to their sources, while separating the natural and fossil CO2. Our tool accurately estimates fossil CO2 emissions in densely monitored regions like western/central Europe. This approach aids in developing strategies for reducing CO2 emissions.
David D. Parrish, Ian C. Faloona, and Richard G. Derwent
Atmos. Chem. Phys., 25, 263–289, https://doi.org/10.5194/acp-25-263-2025, https://doi.org/10.5194/acp-25-263-2025, 2025
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Observation-based estimates of contributions to maximum ozone (O3) concentrations show that background O3 can exceed the air quality standard of 70 ppb in the southwestern US, precluding standard attainment. Over the past 4 decades, US anthropogenic O3 has decreased by a factor of ~ 6.3, while wildfire contributions have increased, so that the background now dominates maximum concentrations, even in Los Angeles, and the occurrence of maximum O3 has shifted from the eastern to the western US.
William P. L. Carter, Jia Jiang, John J. Orlando, and Kelley C. Barsanti
Atmos. Chem. Phys., 25, 199–242, https://doi.org/10.5194/acp-25-199-2025, https://doi.org/10.5194/acp-25-199-2025, 2025
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This paper describes the scientific basis for gas-phase atmospheric chemical mechanisms derived using the SAPRC mechanism generation system, MechGen. It can derive mechanisms for most organic compounds with C, H, O, or N atoms, including initial reactions of organics with OH, O3, NO3, and O3P or by photolysis, as well as the reactions of the various types of intermediates that are formed. The paper includes a description of areas of uncertainty where additional research and updates are needed.
Thibaut Lebourgeois, Bastien Sauvage, Pawel Wolff, Béatrice Josse, Virginie Marécal, Yasmine Bennouna, Romain Blot, Damien Boulanger, Hannah Clark, Jean-Marc Cousin, Philippe Nedelec, and Valérie Thouret
Atmos. Chem. Phys., 24, 13975–14004, https://doi.org/10.5194/acp-24-13975-2024, https://doi.org/10.5194/acp-24-13975-2024, 2024
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Our study examines intense-carbon-monoxide (CO) pollution events measured by commercial aircraft from the In-service Aircraft for a Global Observing System (IAGOS) research infrastructure. We combine these measurements with the SOFT-IO model to trace the origin of the observed CO. A comprehensive analysis of the geographical origin, source type, seasonal variation, and ozone levels of these pollution events is provided.
Hassnae Erraji, Philipp Franke, Astrid Lampert, Tobias Schuldt, Ralf Tillmann, Andreas Wahner, and Anne Caroline Lange
Atmos. Chem. Phys., 24, 13913–13934, https://doi.org/10.5194/acp-24-13913-2024, https://doi.org/10.5194/acp-24-13913-2024, 2024
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Four-dimensional variational data assimilation allows for the simultaneous optimisation of initial values and emission rates by using trace-gas profiles from drone observations in a regional air quality model. Assimilated profiles positively impact the representation of air pollutants in the model by improving their vertical distribution and ground-level concentrations. This case study highlights the potential of drone data to enhance air quality analyses including local emission evaluation.
Christopher Lawrence, Mary Barth, John Orlando, Paul Casson, Richard Brandt, Daniel Kelting, Elizabeth Yerger, and Sara Lance
Atmos. Chem. Phys., 24, 13693–13713, https://doi.org/10.5194/acp-24-13693-2024, https://doi.org/10.5194/acp-24-13693-2024, 2024
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This work uses chemical transport and box modeling to study the gas- and aqueous-phase production of organic acid concentrations measured in cloud water at the summit of Whiteface Mountain on 1 July 2018. Isoprene was the major source of formic, acetic, and oxalic acid. Gas-phase chemistry greatly underestimated formic and acetic acid, indicating missing sources, while cloud chemistry was a key source of oxalic acid. More studies of organic acids are required to better constrain their sources.
Markus Kilian, Volker Grewe, Patrick Jöckel, Astrid Kerkweg, Mariano Mertens, Andreas Zahn, and Helmut Ziereis
Atmos. Chem. Phys., 24, 13503–13523, https://doi.org/10.5194/acp-24-13503-2024, https://doi.org/10.5194/acp-24-13503-2024, 2024
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Anthropogenic emissions are a major source of precursors of tropospheric ozone. As ozone formation is highly non-linear, we apply a global–regional chemistry–climate model with a source attribution method (tagging) to quantify the contribution of anthropogenic emissions to ozone. Our analysis shows that the contribution of European anthropogenic emissions largely increases during large ozone periods, indicating that emissions from these sectors drive ozone values.
Barbara Ervens, Andrew Rickard, Bernard Aumont, William P. L. Carter, Max McGillen, Abdelwahid Mellouki, John Orlando, Bénédicte Picquet-Varrault, Paul Seakins, William R. Stockwell, Luc Vereecken, and Timothy J. Wallington
Atmos. Chem. Phys., 24, 13317–13339, https://doi.org/10.5194/acp-24-13317-2024, https://doi.org/10.5194/acp-24-13317-2024, 2024
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Chemical mechanisms describe the chemical processes in atmospheric models that are used to describe the changes in the atmospheric composition. Therefore, accurate chemical mechanisms are necessary to predict the evolution of air pollution and climate change. The article describes all steps that are needed to build chemical mechanisms and discusses the advances and needs of experimental and theoretical research activities needed to build reliable chemical mechanisms.
Jianing Dai, Guy P. Brasseur, Mihalis Vrekoussis, Maria Kanakidou, Kun Qu, Yijuan Zhang, Hongliang Zhang, and Tao Wang
Atmos. Chem. Phys., 24, 12943–12962, https://doi.org/10.5194/acp-24-12943-2024, https://doi.org/10.5194/acp-24-12943-2024, 2024
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This paper employs a regional chemical transport model to quantify the sensitivity of air pollutants and photochemical parameters to specified emission reductions in China for representative winter and summer conditions. The study provides insights into further air quality control in China with reduced primary emissions.
T. Nash Skipper, Emma L. D'Ambro, Forwood C. Wiser, V. Faye McNeill, Rebecca H. Schwantes, Barron H. Henderson, Ivan R. Piletic, Colleen B. Baublitz, Jesse O. Bash, Andrew R. Whitehill, Lukas C. Valin, Asher P. Mouat, Jennifer Kaiser, Glenn M. Wolfe, Jason M. St. Clair, Thomas F. Hanisco, Alan Fried, Bryan K. Place, and Havala O.T. Pye
Atmos. Chem. Phys., 24, 12903–12924, https://doi.org/10.5194/acp-24-12903-2024, https://doi.org/10.5194/acp-24-12903-2024, 2024
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We develop the Community Regional Atmospheric Chemistry Multiphase Mechanism (CRACMM) version 2 to improve predictions of formaldehyde in ambient air compared to satellite-, aircraft-, and ground-based observations. With the updated chemistry, we estimate the cancer risk from inhalation exposure to ambient formaldehyde across the contiguous USA and predict that 40 % of this risk is controllable through reductions in anthropogenic emissions of nitrogen oxides and reactive organic carbon.
Baoshuang Liu, Yao Gu, Yutong Wu, Qili Dai, Shaojie Song, Yinchang Feng, and Philip K. Hopke
Atmos. Chem. Phys., 24, 12861–12879, https://doi.org/10.5194/acp-24-12861-2024, https://doi.org/10.5194/acp-24-12861-2024, 2024
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Reactive loss of volatile organic compounds (VOCs) is a long-term issue yet to be resolved in VOC source analyses. We assess common methods of, and existing issues in, reducing losses, impacts of losses, and sources in current source analyses. We offer a potential supporting role for solving issues of VOC conversion. Source analyses of consumed VOCs that reacted to produce ozone and secondary organic aerosols can play an important role in the effective control of secondary pollution in air.
Deepangsu Chatterjee, Randall V. Martin, Chi Li, Dandan Zhang, Haihui Zhu, Daven K. Henze, James H. Crawford, Ronald C. Cohen, Lok N. Lamsal, and Alexander M. Cede
Atmos. Chem. Phys., 24, 12687–12706, https://doi.org/10.5194/acp-24-12687-2024, https://doi.org/10.5194/acp-24-12687-2024, 2024
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We investigate the hourly variation of NO2 columns and surface concentrations by applying the GEOS-Chem model to interpret aircraft and ground-based measurements over the US and Pandora sun photometer measurements over the US, Europe, and Asia. Corrections to the Pandora columns and finer model resolution improve the modeled representation of the summertime hourly variation of total NO2 columns to explain the weaker hourly variation in NO2 columns than at the surface.
Kiyeon Kim, Kyung Man Han, Chul Han Song, Hyojun Lee, Ross Beardsley, Jinhyeok Yu, Greg Yarwood, Bonyoung Koo, Jasper Madalipay, Jung-Hun Woo, and Seogju Cho
Atmos. Chem. Phys., 24, 12575–12593, https://doi.org/10.5194/acp-24-12575-2024, https://doi.org/10.5194/acp-24-12575-2024, 2024
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We incorporated each HONO process into the current CMAQ modeling framework to enhance the accuracy of HONO mixing ratio predictions. These results expand our understanding of HONO photochemistry and identify crucial sources of HONO that impact the total HONO budget in Seoul, South Korea. Through this investigation, we contribute to resolving discrepancies in understanding chemical transport models, with implications for better air quality management and environmental protection in the region.
Flossie Brown, Gerd Folberth, Stephen Sitch, Paulo Artaxo, Marijn Bauters, Pascal Boeckx, Alexander W. Cheesman, Matteo Detto, Ninong Komala, Luciana Rizzo, Nestor Rojas, Ines dos Santos Vieira, Steven Turnock, Hans Verbeeck, and Alfonso Zambrano
Atmos. Chem. Phys., 24, 12537–12555, https://doi.org/10.5194/acp-24-12537-2024, https://doi.org/10.5194/acp-24-12537-2024, 2024
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Ozone is a pollutant that is detrimental to human and plant health. Ozone monitoring sites in the tropics are limited, so models are often used to understand ozone exposure. We use measurements from the tropics to evaluate ozone from the UK Earth system model, UKESM1. UKESM1 is able to capture the pattern of ozone in the tropics, except in southeast Asia, although it systematically overestimates it at all sites. This work highlights that UKESM1 can capture seasonal and hourly variability.
Namrata Shanmukh Panji, Deborah F. McGlynn, Laura E. R. Barry, Todd M. Scanlon, Manuel T. Lerdau, Sally E. Pusede, and Gabriel Isaacman-VanWertz
Atmos. Chem. Phys., 24, 12495–12507, https://doi.org/10.5194/acp-24-12495-2024, https://doi.org/10.5194/acp-24-12495-2024, 2024
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Climate change will bring about changes in parameters that are currently used in global-scale models to calculate biogenic emissions. This study seeks to understand the factors driving these models by comparing long-term datasets of biogenic compounds to modeled emissions. We note that the light-dependent fractions currently used in models do not accurately represent regional observations. We provide evidence for the time-dependent variation in this parameter for future modifications to models.
Martin Vojta, Andreas Plach, Saurabh Annadate, Sunyoung Park, Gawon Lee, Pallav Purohit, Florian Lindl, Xin Lan, Jens Mühle, Rona L. Thompson, and Andreas Stohl
Atmos. Chem. Phys., 24, 12465–12493, https://doi.org/10.5194/acp-24-12465-2024, https://doi.org/10.5194/acp-24-12465-2024, 2024
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We constrain the global emissions of the very potent greenhouse gas sulfur hexafluoride (SF6) between 2005 and 2021. We show that SF6 emissions are decreasing in the USA and in the EU, while they are substantially growing in China, leading overall to an increasing global emission trend. The national reports for the USA, EU, and China all underestimated their SF6 emissions. However, stringent mitigation measures can successfully reduce SF6 emissions, as can be seen in the EU emission trend.
Dominika Pasik, Thomas Golin Almeida, Emelda Ahongshangbam, Siddharth Iyer, and Nanna Myllys
EGUsphere, https://doi.org/10.5194/egusphere-2024-3464, https://doi.org/10.5194/egusphere-2024-3464, 2024
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We used quantum chemistry methods to investigate the oxidation mechanisms of acyl peroxy radicals (APRs) with various monoterpenes. Our findings reveal unique oxidation pathways for different monoterpenes, leading to either chain-terminating products or highly reactive intermediates that can contribute to particle formation in the atmosphere. This research highlights APRs as potentially significant but underexplored atmospheric oxidants, which may influence future approaches to modeling climate.
Yasin Elshorbany, Jerald R. Ziemke, Sarah Strode, Hervé Petetin, Kazuyuki Miyazaki, Isabelle De Smedt, Kenneth Pickering, Rodrigo J. Seguel, Helen Worden, Tamara Emmerichs, Domenico Taraborrelli, Maria Cazorla, Suvarna Fadnavis, Rebecca R. Buchholz, Benjamin Gaubert, Néstor Y. Rojas, Thiago Nogueira, Thérèse Salameh, and Min Huang
Atmos. Chem. Phys., 24, 12225–12257, https://doi.org/10.5194/acp-24-12225-2024, https://doi.org/10.5194/acp-24-12225-2024, 2024
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We investigated tropospheric ozone spatial variability and trends from 2005 to 2019 and related those to ozone precursors on global and regional scales. We also investigate the spatiotemporal characteristics of the ozone formation regime in relation to ozone chemical sources and sinks. Our analysis is based on remote sensing products of the tropospheric column of ozone and its precursors, nitrogen dioxide, formaldehyde, and total column CO, as well as ozonesonde data and model simulations.
Mariano Mertens, Sabine Brinkop, Phoebe Graf, Volker Grewe, Johannes Hendricks, Patrick Jöckel, Anna Lanteri, Sigrun Matthes, Vanessa S. Rieger, Mattia Righi, and Robin N. Thor
Atmos. Chem. Phys., 24, 12079–12106, https://doi.org/10.5194/acp-24-12079-2024, https://doi.org/10.5194/acp-24-12079-2024, 2024
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We quantified the contributions of land transport, shipping, and aviation emissions to tropospheric ozone; its radiative forcing; and the reductions of the methane lifetime using chemistry-climate model simulations. The contributions were analysed for the conditions of 2015 and for three projections for the year 2050. The results highlight the challenges of mitigating ozone formed by emissions of the transport sector, caused by the non-linearitiy of the ozone chemistry and the long lifetime.
Jincheol Park, Yunsoo Choi, and Sagun Kayastha
EGUsphere, https://doi.org/10.5194/egusphere-2024-3312, https://doi.org/10.5194/egusphere-2024-3312, 2024
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We investigated NOx emissions’ contributions to nitrogen loadings across five regions of East Asia during the 2022 winter-spring transition through chemical transport modeling informed by satellite data. As seasons progress, local contributions within each region to its NOy budget decreased from 32 %–43 % to 23 %–30 %, while transboundary contributions increased from 16 %–33 % to 27 %–37 %, driven by a shift in synoptic settings that allowed pollutants to spread more broadly across the regions.
Lauri Franzon, Marie Camredon, Richard Valorso, Bernard Aumont, and Theo Kurtén
Atmos. Chem. Phys., 24, 11679–11699, https://doi.org/10.5194/acp-24-11679-2024, https://doi.org/10.5194/acp-24-11679-2024, 2024
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In this article we investigate the formation of large, sticky molecules from various organic compounds entering the atmosphere as primary emissions and the degree to which these processes may contribute to organic aerosol particle mass. More specifically, we qualitatively investigate a recently discovered chemical reaction channel for one of the most important short-lived radical compounds, peroxy radicals, and discover which of these reactions are most atmospherically important.
Siting Li, Yiming Liu, Yuqi Zhu, Yinbao Jin, Yingying Hong, Ao Shen, Yifei Xu, Haofan Wang, Haichao Wang, Xiao Lu, Shaojia Fan, and Qi Fan
Atmos. Chem. Phys., 24, 11521–11544, https://doi.org/10.5194/acp-24-11521-2024, https://doi.org/10.5194/acp-24-11521-2024, 2024
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This study establishes an inventory of anthropogenic chlorine emissions in China in 2019 with expanded species (HCl, Cl-, Cl2, HOCl) and sources (41 specific sources). The inventory is validated by a modeling study against the observations. This study enhances the understanding of anthropogenic chlorine emissions in the atmosphere, identifies key sources, and provides scientific support for pollution control and climate change.
Willem E. van Caspel, Zbigniew Klimont, Chris Heyes, and Hilde Fagerli
Atmos. Chem. Phys., 24, 11545–11563, https://doi.org/10.5194/acp-24-11545-2024, https://doi.org/10.5194/acp-24-11545-2024, 2024
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Methane in the atmosphere contributes to the production of ozone gas – an air pollutant and greenhouse gas. Our results highlight that simultaneous reductions in methane emissions help avoid offsetting the air pollution benefits already achieved by the already-approved precursor emission reductions by 2050 in the European Monitoring and Evaluation Programme region, while also playing an important role in bringing air pollution further down towards World Health Organization guideline limits.
Jinya Yang, Yutong Wang, Lei Zhang, and Yu Zhao
EGUsphere, https://doi.org/10.5194/egusphere-2024-2713, https://doi.org/10.5194/egusphere-2024-2713, 2024
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We develop a modeling framework to predict future ozone concentrations (till 2060s) in China following an IPCC scenario. We further evaluate and separate the contributions of climatic, anthropogenic, and biogenic factors by season and region. We find persistent emission controls will alter the nonlinear response of ozone to its precursors, and dominate the declining ozone level. The outcomes highlight the importance of human actions even with a climate penalty on air quality in the future.
Laura Stecher, Franziska Winterstein, Patrick Jöckel, Michael Ponater, Mariano Mertens, and Martin Dameris
EGUsphere, https://doi.org/10.5194/egusphere-2024-2938, https://doi.org/10.5194/egusphere-2024-2938, 2024
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Methane, the second most important anthropogenic greenhouse gas, is chemically decomposed in the atmosphere. The chemical sink of atmospheric methane is not constant, but depends on the temperature and on the abundance of its reaction partners. In this study, we use a global chemistry-climate model to assess the feedback of atmospheric methane induced by changes of the chemical sink in a warming climate, and its implications for the chemical composition and the surface air temperature change.
Beata Opacka, Trissevgeni Stavrakou, Jean-François Müller, Isabelle De Smedt, Jos van Geffen, Eloise A. Marais, Rebekah P. Horner, Dylan B. Millet, Kelly C. Wells, and Alex B. Guenther
EGUsphere, https://doi.org/10.5194/egusphere-2024-2912, https://doi.org/10.5194/egusphere-2024-2912, 2024
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Vegetation releases biogenic volatile organic compounds, while soils and lightning contribute to the natural emissions of nitrogen oxides into the atmosphere. These gases interact in complex ways. Using satellite data and models, we developed a new method to simultaneously optimise these natural emissions over Africa in 2019. Our approach led to an increase in natural emissions that is supported by independent data showing that current estimates are underestimated.
Tia R. Scarpelli, Paul I. Palmer, Mark Lunt, Ingrid Super, and Arjan Droste
Atmos. Chem. Phys., 24, 10773–10791, https://doi.org/10.5194/acp-24-10773-2024, https://doi.org/10.5194/acp-24-10773-2024, 2024
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Under the Paris Agreement, countries must track their anthropogenic greenhouse gas emissions. This study describes a method to determine self-consistent estimates for combustion emissions and natural fluxes of CO2 from atmospheric data. We report consistent estimates inferred using this approach from satellite data and ground-based data over Europe, suggesting that satellite data can be used to determine national anthropogenic CO2 emissions for countries where ground-based CO2 data are absent.
Yufen Wang, Ke Li, Xi Chen, Zhenjiang Yang, Minglong Tang, Pascoal M. D. Campos, Yang Yang, Xu Yue, and Hong Liao
EGUsphere, https://doi.org/10.5194/egusphere-2024-2576, https://doi.org/10.5194/egusphere-2024-2576, 2024
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The impact of biomass burning and anthropogenic emissions on high tropospheric ozone was not well studied in Southern Africa. We combined the model simulation with recent observations at the surface and from space to quantify tropospheric ozone and its main drivers in Southern Africa. Our work focuses on the impact of emissions from different sources at different spatial scales, contributing to a comprehensive understanding of air pollution drivers and their uncertainties in Southern Africa.
Wenbin Kou, Yang Gao, Dan Tong, Xiaojie Guo, Xiadong An, Wenyu Liu, Mengshi Cui, Xiuwen Guo, Shaoqing Zhang, Huiwang Gao, and Lixin Wu
EGUsphere, https://doi.org/10.5194/egusphere-2024-2500, https://doi.org/10.5194/egusphere-2024-2500, 2024
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Unlike traditional numerical studies, we apply a high-resolution Earth system model, improving simulations of ozone and large-scale circulations such as atmospheric blocking. In addition to local heatwave effects, we quantify the impact of atmospheric blocking on downstream ozone concentrations, which is closely associated with the blocking position. We identify three major pathways of Rossby wave propagation, stressing the critical role of large-scale circulation play in regional air quality.
Qianqian Zhang, K. Folkert Boersma, Chiel van der Laan, Alba Mols, Bin Zhao, Shengyue Li, and Yuepeng Pan
EGUsphere, https://doi.org/10.5194/egusphere-2024-2641, https://doi.org/10.5194/egusphere-2024-2641, 2024
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Accurate NOx emission estimates are required to better understand air pollution. This study investigates and demonstrates the ability of the superposition column model in combination with TROPOMI tropospheric NO2 column data to estimate city-scale NOx emissions and lifetimes and their variabilities. The results of this work nevertheless confirm the strength of the superposition column model in estimating urban NOx emissions with reasonable accuracy.
Ryan J. Pound, Lucy V. Brown, Mat J. Evans, and Lucy J. Carpenter
Atmos. Chem. Phys., 24, 9899–9921, https://doi.org/10.5194/acp-24-9899-2024, https://doi.org/10.5194/acp-24-9899-2024, 2024
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Iodine-mediated loss of ozone to the ocean surface and the subsequent emission of iodine species has a large effect on the troposphere. Here we combine recent experimental insights to develop a box model of the process, which we then parameterize and incorporate into the GEOS-Chem transport model. We find that these new insights have a small impact on the total emission of iodine but significantly change its distribution.
Mingzhao Liu, Lars Hoffmann, Jens-Uwe Grooß, Zhongyin Cai, Sabine Grießbach, and Yi Heng
EGUsphere, https://doi.org/10.5194/egusphere-2024-2596, https://doi.org/10.5194/egusphere-2024-2596, 2024
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We studied the transport and chemical decomposition of volcanic SO2, focusing on the 2019 Raikoke event. By comparing two different chemistry modeling schemes, we found that including complex chemical reactions leads to a more accurate prediction of how long SO2 stays in the atmosphere. This research helps improve our understanding of volcanic pollution and its impact on air quality and climate, providing better tools for scientists to track and predict the movement of these pollutants.
Alok K. Pandey, David S. Stevenson, Alcide Zhao, Richard J. Pope, Ryan Hossaini, Krishan Kumar, and Marytn P. Chipperfield
EGUsphere, https://doi.org/10.5194/egusphere-2024-2686, https://doi.org/10.5194/egusphere-2024-2686, 2024
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Nitrogen dioxide is an air pollutant largely controlled by human activity that affects ozone, methane and aerosols. Satellite instruments can quantify column NO2, and by carefully matching the time and location of measurements, enable evaluation of model simulations. NO2 over SE Asia is assessed, showing that the model captures many features of the measurements, but also important differences that suggest model deficiencies in representing several aspects of the atmospheric chemistry of NO2.
Katherine R. Travis, Benjamin A. Nault, James H. Crawford, Kelvin H. Bates, Donald R. Blake, Ronald C. Cohen, Alan Fried, Samuel R. Hall, L. Gregory Huey, Young Ro Lee, Simone Meinardi, Kyung-Eun Min, Isobel J. Simpson, and Kirk Ullman
Atmos. Chem. Phys., 24, 9555–9572, https://doi.org/10.5194/acp-24-9555-2024, https://doi.org/10.5194/acp-24-9555-2024, 2024
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Human activities result in the emission of volatile organic compounds (VOCs) that contribute to air pollution. Detailed VOC measurements were taken during a field study in South Korea. When compared to VOC inventories, large discrepancies showed underestimates from chemical products, liquefied petroleum gas, and long-range transport. Improved emissions and chemistry of these VOCs better described urban pollution. The new chemical scheme is relevant to urban areas and other VOC sources.
Beth S. Nelson, Zhenze Liu, Freya A. Squires, Marvin Shaw, James R. Hopkins, Jacqueline F. Hamilton, Andrew R. Rickard, Alastair C. Lewis, Zongbo Shi, and James D. Lee
Atmos. Chem. Phys., 24, 9031–9044, https://doi.org/10.5194/acp-24-9031-2024, https://doi.org/10.5194/acp-24-9031-2024, 2024
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The impact of combined air quality and carbon neutrality policies on O3 formation in Beijing was investigated. Emissions inventory data were used to estimate future pollutant mixing ratios relative to ground-level observations. O3 production was found to be most sensitive to changes in alkenes, but large reductions in less reactive compounds led to larger reductions in future O3 production. This study highlights the importance of understanding the emissions of organic pollutants.
Amir H. Souri, Bryan N. Duncan, Sarah A. Strode, Daniel C. Anderson, Michael E. Manyin, Junhua Liu, Luke D. Oman, Zhen Zhang, and Brad Weir
Atmos. Chem. Phys., 24, 8677–8701, https://doi.org/10.5194/acp-24-8677-2024, https://doi.org/10.5194/acp-24-8677-2024, 2024
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We explore a new method of using the wealth of information obtained from satellite observations of Aura OMI NO2, HCHO, and MERRA-2 reanalysis in NASA’s GEOS model equipped with an efficient tropospheric OH (TOH) estimator to enhance the representation of TOH spatial distribution and its long-term trends. This new framework helps us pinpoint regional inaccuracies in TOH and differentiate between established prior knowledge and newly acquired information from satellites on TOH trends.
Haipeng Lin, Louisa K. Emmons, Elizabeth W. Lundgren, Laura Hyesung Yang, Xu Feng, Ruijun Dang, Shixian Zhai, Yunxiao Tang, Makoto M. Kelp, Nadia K. Colombi, Sebastian D. Eastham, Thibaud M. Fritz, and Daniel J. Jacob
Atmos. Chem. Phys., 24, 8607–8624, https://doi.org/10.5194/acp-24-8607-2024, https://doi.org/10.5194/acp-24-8607-2024, 2024
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Tropospheric ozone is a major air pollutant, a greenhouse gas, and a major indicator of model skill. Global atmospheric chemistry models show large differences in simulations of tropospheric ozone, but isolating sources of differences is complicated by different model environments. By implementing the GEOS-Chem model side by side to CAM-chem within a common Earth system model, we identify and evaluate specific differences between the two models and their impacts on key chemical species.
Victor Lannuque and Karine Sartelet
Atmos. Chem. Phys., 24, 8589–8606, https://doi.org/10.5194/acp-24-8589-2024, https://doi.org/10.5194/acp-24-8589-2024, 2024
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Large uncertainties remain in understanding secondary organic aerosol (SOA) formation and speciation from naphthalene oxidation. This study details the development of the first near-explicit chemical scheme for naphthalene oxidation by OH, which includes kinetic and mechanistic data, and is able to reproduce most of the experimentally identified products in both gas and particle phases.
Shuai Li, Xiao Lu, and Haolin Wang
EGUsphere, https://doi.org/10.5194/egusphere-2024-1889, https://doi.org/10.5194/egusphere-2024-1889, 2024
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We report that the summertime ozone-temperature sensitivity decreased by 50 % from 3.0 ppbv/K in 1990 to 1.5 ppb/K in 2021 in the US. GEOS-Chem simulations show that anthropogenic NOx emission reduction is the dominant driver of the ozone-temperature sensitivity decline, through influencing both the temperature-direct and temperature-indirect processes. Reduced ozone-temperature sensitivity has decreased the ozone enhancement from low to high temperatures by an average of 6.8 ppbv across the US.
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Short summary
An assessment of mercury levels in air and deposition in the Athabasca oil sands region (AOSR) in Northern Alberta, Canada, was conducted to investigate the contribution of Hg emitted from oil sands activities to the surrounding landscape using a 3D process-based Hg model in 2012–2015. Oil sands Hg emissions are found to be important sources of Hg contamination to the local landscape in proximity to the processing activities, particularly in wintertime.
An assessment of mercury levels in air and deposition in the Athabasca oil sands region (AOSR)...
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