Articles | Volume 21, issue 7
https://doi.org/10.5194/acp-21-5635-2021
© 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-21-5635-2021
© Author(s) 2021. This work is distributed under
the Creative Commons Attribution 4.0 License.
the Creative Commons Attribution 4.0 License.
Where there is smoke there is mercury: Assessing boreal forest fire mercury emissions using aircraft and highlighting uncertainties associated with upscaling emissions estimates
David S. McLagan
Air Quality Research Division (ARQD), Environment and Climate Change
Canada, 4905 Dufferin St, North York, ON M3H 5T4, Canada
Dept. Environmental Geochemistry, Institute for Geoecology, Technical
University of Braunschweig, Langer Kamp 19c, 38106 Braunschweig, Germany
Geoff W. Stupple
Air Quality Research Division (ARQD), Environment and Climate Change
Canada, 4905 Dufferin St, North York, ON M3H 5T4, Canada
Andrea Darlington
Air Quality Research Division (ARQD), Environment and Climate Change
Canada, 4905 Dufferin St, North York, ON M3H 5T4, Canada
Katherine Hayden
Air Quality Research Division (ARQD), Environment and Climate Change
Canada, 4905 Dufferin St, North York, ON M3H 5T4, Canada
Alexandra Steffen
CORRESPONDING AUTHOR
Air Quality Research Division (ARQD), Environment and Climate Change
Canada, 4905 Dufferin St, North York, ON M3H 5T4, Canada
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David S. McLagan, Carina Esser, Lorenz Schwab, Jan G. Wiederhold, Jan-Helge Richard, and Harald Biester
SOIL, 10, 77–92, https://doi.org/10.5194/soil-10-77-2024, https://doi.org/10.5194/soil-10-77-2024, 2024
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Sorption of mercury in soils, aquifer materials, and sediments is primarily linked to organic matter. Using column experiments, mercury concentration, speciation, and stable isotope analyses, we show that large quantities of mercury in soil water and groundwater can be sorbed to inorganic minerals; sorption to the solid phase favours lighter isotopes. Data provide important insights on the transport and fate of mercury in soil–groundwater systems and particularly in low-organic-matter systems.
David S. McLagan, Harald Biester, Tomas Navrátil, Stephan M. Kraemer, and Lorenz Schwab
Biogeosciences, 19, 4415–4429, https://doi.org/10.5194/bg-19-4415-2022, https://doi.org/10.5194/bg-19-4415-2022, 2022
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Spruce and larch trees are effective archiving species for historical atmospheric mercury using growth rings of bole wood. Mercury stable isotope analysis proved an effective tool to characterise industrial mercury signals and assess mercury uptake pathways (leaf uptake for both wood and bark) and mercury cycling within the trees. These data detail important information for understanding the mercury biogeochemical cycle particularly in forest systems.
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.
David S. McLagan, Carl P. J. Mitchell, Haiyong Huang, Batual Abdul Hussain, Ying Duan Lei, and Frank Wania
Atmos. Meas. Tech., 10, 3651–3660, https://doi.org/10.5194/amt-10-3651-2017, https://doi.org/10.5194/amt-10-3651-2017, 2017
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Laboratory experiments indicate that the sampling rate of a passive air sampler for gaseous mercury is (1) not affected by relative humidity, (2) increases slightly with increasing temperature because of the effect of temperature on molecular diffusivity, (3) increases only slightly with wind speed as long as the wind speed is at least 1 m/s, and (4) is not changed when previously deployed diffusive barriers are used.
David S. McLagan, Maxwell E. E. Mazur, Carl P. J. Mitchell, and Frank Wania
Atmos. Chem. Phys., 16, 3061–3076, https://doi.org/10.5194/acp-16-3061-2016, https://doi.org/10.5194/acp-16-3061-2016, 2016
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For more than 20 years, scientists and engineers have tried to design simple sampling devices that can collect gaseous elemental mercury from the atmosphere without the use of a pump. A thorough review of the sampler designs that have been presented so far suggests that while some may be suitable for measuring higher air concentrations close to sources, none of them have the accuracy and precision required to record the low atmospheric mercury concentrations prevalent in background regions.
David S. McLagan, Carina Esser, Lorenz Schwab, Jan G. Wiederhold, Jan-Helge Richard, and Harald Biester
SOIL, 10, 77–92, https://doi.org/10.5194/soil-10-77-2024, https://doi.org/10.5194/soil-10-77-2024, 2024
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Sorption of mercury in soils, aquifer materials, and sediments is primarily linked to organic matter. Using column experiments, mercury concentration, speciation, and stable isotope analyses, we show that large quantities of mercury in soil water and groundwater can be sorbed to inorganic minerals; sorption to the solid phase favours lighter isotopes. Data provide important insights on the transport and fate of mercury in soil–groundwater systems and particularly in low-organic-matter systems.
David S. McLagan, Harald Biester, Tomas Navrátil, Stephan M. Kraemer, and Lorenz Schwab
Biogeosciences, 19, 4415–4429, https://doi.org/10.5194/bg-19-4415-2022, https://doi.org/10.5194/bg-19-4415-2022, 2022
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Spruce and larch trees are effective archiving species for historical atmospheric mercury using growth rings of bole wood. Mercury stable isotope analysis proved an effective tool to characterise industrial mercury signals and assess mercury uptake pathways (leaf uptake for both wood and bark) and mercury cycling within the trees. These data detail important information for understanding the mercury biogeochemical cycle particularly in forest systems.
Debora Griffin, Chris A. McLinden, Enrico Dammers, Cristen Adams, Chelsea E. Stockwell, Carsten Warneke, Ilann Bourgeois, Jeff Peischl, Thomas B. Ryerson, Kyle J. Zarzana, Jake P. Rowe, Rainer Volkamer, Christoph Knote, Natalie Kille, Theodore K. Koenig, Christopher F. Lee, Drew Rollins, Pamela S. Rickly, Jack Chen, Lukas Fehr, Adam Bourassa, Doug Degenstein, Katherine Hayden, Cristian Mihele, Sumi N. Wren, John Liggio, Ayodeji Akingunola, and Paul Makar
Atmos. Meas. Tech., 14, 7929–7957, https://doi.org/10.5194/amt-14-7929-2021, https://doi.org/10.5194/amt-14-7929-2021, 2021
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Satellite-derived NOx emissions from biomass burning are estimated with TROPOMI observations. Two common emission estimation methods are applied, and sensitivity tests with model output were performed to determine the accuracy of these methods. The effect of smoke aerosols on TROPOMI NO2 columns is estimated and compared to aircraft observations from four different aircraft campaigns measuring biomass burning plumes in 2018 and 2019 in North America.
Sepehr Fathi, Mark Gordon, Paul A. Makar, Ayodeji Akingunola, Andrea Darlington, John Liggio, Katherine Hayden, and Shao-Meng Li
Atmos. Chem. Phys., 21, 15461–15491, https://doi.org/10.5194/acp-21-15461-2021, https://doi.org/10.5194/acp-21-15461-2021, 2021
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We have investigated the accuracy of aircraft-based mass balance methodologies through computer model simulations of the atmosphere and air quality at a regional high-resolution scale. We have defined new quantitative metrics to reduce emission retrieval uncertainty by evaluating top-down mass balance estimates against the known simulated meteorology and input emissions. We also recommend methodologies and flight strategies for improved retrievals in future aircraft-based studies.
Ashu Dastoor, Andrei Ryjkov, Gregor Kos, Junhua Zhang, Jane Kirk, Matthew Parsons, and Alexandra Steffen
Atmos. Chem. Phys., 21, 12783–12807, https://doi.org/10.5194/acp-21-12783-2021, https://doi.org/10.5194/acp-21-12783-2021, 2021
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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.
Konstantin Baibakov, Samuel LeBlanc, Keyvan Ranjbar, Norman T. O'Neill, Mengistu Wolde, Jens Redemann, Kristina Pistone, Shao-Meng Li, John Liggio, Katherine Hayden, Tak W. Chan, Michael J. Wheeler, Leonid Nichman, Connor Flynn, and Roy Johnson
Atmos. Chem. Phys., 21, 10671–10687, https://doi.org/10.5194/acp-21-10671-2021, https://doi.org/10.5194/acp-21-10671-2021, 2021
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We find that the airborne measurements of the vertical extinction due to aerosols (aerosol optical depth, AOD) obtained in the Athabasca Oil Sands Region (AOSR) can significantly exceed ground-based values. This can have an effect on estimating the AOSR radiative impact and is relevant to satellite validation based on ground-based measurements. We also show that the AOD can marginally increase as the plumes are being transported away from the source and the new particles are being formed.
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.
Jenna C. Ditto, Megan He, Tori N. Hass-Mitchell, Samar G. Moussa, Katherine Hayden, Shao-Meng Li, John Liggio, Amy Leithead, Patrick Lee, Michael J. Wheeler, Jeremy J. B. Wentzell, and Drew R. Gentner
Atmos. Chem. Phys., 21, 255–267, https://doi.org/10.5194/acp-21-255-2021, https://doi.org/10.5194/acp-21-255-2021, 2021
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Forest fires are an important source of reactive organic gases and aerosols to the atmosphere. We analyzed organic aerosols collected from an aircraft above a boreal forest fire and reported an increasing contribution from compounds containing oxygen, nitrogen, and sulfur as the plume aged, with sulfide and ring-bound nitrogen functionality. Our results demonstrated chemistry that is important in biomass burning but also in urban/developing regions with high local nitrogen and sulfur emissions.
Travis W. Tokarek, Charles A. Odame-Ankrah, Jennifer A. Huo, Robert McLaren, Alex K. Y. Lee, Max G. Adam, Megan D. Willis, Jonathan P. D. Abbatt, Cristian Mihele, Andrea Darlington, Richard L. Mittermeier, Kevin Strawbridge, Katherine L. Hayden, Jason S. Olfert, Elijah G. Schnitzler, Duncan K. Brownsey, Faisal V. Assad, Gregory R. Wentworth, Alex G. Tevlin, Douglas E. J. Worthy, Shao-Meng Li, John Liggio, Jeffrey R. Brook, and Hans D. Osthoff
Atmos. Chem. Phys., 18, 17819–17841, https://doi.org/10.5194/acp-18-17819-2018, https://doi.org/10.5194/acp-18-17819-2018, 2018
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Measurements of air pollutants at a ground site near Fort McKay in the Athabasca oil sands region in the summer of 2013 are presented. A large number of intermediate-volatility organic compounds (IVOCs) were observed; these molecules were shown previously to generate atmospheric particles downwind of the region. A principal component analysis was performed to identify major pollution source types, including which source(s) is(are) associated with IVOC emissions (e.g., freshly mined bitumen).
Sumi N. Wren, John Liggio, Yuemei Han, Katherine Hayden, Gang Lu, Cris M. Mihele, Richard L. Mittermeier, Craig Stroud, Jeremy J. B. Wentzell, and Jeffrey R. Brook
Atmos. Chem. Phys., 18, 16979–17001, https://doi.org/10.5194/acp-18-16979-2018, https://doi.org/10.5194/acp-18-16979-2018, 2018
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We made measurements from a mobile laboratory across a large urban area and determined fleet-average vehicle emission factors (EFs) for a suite of traffic-related air pollutants. We present the first real-world EFs for isocyanic acid (HNCO) and hydrogen cyanide (HCN) and insight into their on-road variability. We find that vehicles may represent an important source of these air toxics at an urban scale. This work has implications for understanding population exposure to these species.
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.
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.
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 %.
Sabour Baray, Andrea Darlington, Mark Gordon, Katherine L. Hayden, Amy Leithead, Shao-Meng Li, Peter S. K. Liu, Richard L. Mittermeier, Samar G. Moussa, Jason O'Brien, Ralph Staebler, Mengistu Wolde, Doug Worthy, and Robert McLaren
Atmos. Chem. Phys., 18, 7361–7378, https://doi.org/10.5194/acp-18-7361-2018, https://doi.org/10.5194/acp-18-7361-2018, 2018
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Methane emissions from major oil sands facilities in the Athabasca Oil Sands Region (AOSR) of Alberta were measured in the summer of 2013 using two related aircraft mass-balance approaches. Tailings ponds and fugitive emissions of methane from open pit mines were found to be the major sources of methane in the region. Total methane emissions in the AOSR were measured to be ~ 20 tonnes of CH4 per hour, which is 48 % higher than the Canadian Greenhouse Gas Reporting Program Emissions Inventory.
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.
David S. McLagan, Carl P. J. Mitchell, Haiyong Huang, Batual Abdul Hussain, Ying Duan Lei, and Frank Wania
Atmos. Meas. Tech., 10, 3651–3660, https://doi.org/10.5194/amt-10-3651-2017, https://doi.org/10.5194/amt-10-3651-2017, 2017
Short summary
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Laboratory experiments indicate that the sampling rate of a passive air sampler for gaseous mercury is (1) not affected by relative humidity, (2) increases slightly with increasing temperature because of the effect of temperature on molecular diffusivity, (3) increases only slightly with wind speed as long as the wind speed is at least 1 m/s, and (4) is not changed when previously deployed diffusive barriers are used.
John Liggio, Samar G. Moussa, Jeremy Wentzell, Andrea Darlington, Peter Liu, Amy Leithead, Katherine Hayden, Jason O'Brien, Richard L. Mittermeier, Ralf Staebler, Mengistu Wolde, and Shao-Meng Li
Atmos. Chem. Phys., 17, 8411–8427, https://doi.org/10.5194/acp-17-8411-2017, https://doi.org/10.5194/acp-17-8411-2017, 2017
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The emission and formation of gaseous organic acids from the oil sands industry in Canada is explored through aircraft measurements directly over and downwind wind of industrial facilities. Results demonstrated that the formation of organic acids through atmospheric chemical reactions dominated over the direct emissions from mining activities but could not be explicitly modeled. The results highlight the need for improved understanding of photochemical mechanisms leading to these species.
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.
David S. McLagan, Maxwell E. E. Mazur, Carl P. J. Mitchell, and Frank Wania
Atmos. Chem. Phys., 16, 3061–3076, https://doi.org/10.5194/acp-16-3061-2016, https://doi.org/10.5194/acp-16-3061-2016, 2016
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For more than 20 years, scientists and engineers have tried to design simple sampling devices that can collect gaseous elemental mercury from the atmosphere without the use of a pump. A thorough review of the sampler designs that have been presented so far suggests that while some may be suitable for measuring higher air concentrations close to sources, none of them have the accuracy and precision required to record the low atmospheric mercury concentrations prevalent in background regions.
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: Field Measurements | Altitude Range: Troposphere | Science Focus: Chemistry (chemical composition and reactions)
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Sarah Albertin, Joël Savarino, Slimane Bekki, Albane Barbero, Roberto Grilli, Quentin Fournier, Irène Ventrillard, Nicolas Caillon, and Kathy Law
Atmos. Chem. Phys., 24, 1361–1388, https://doi.org/10.5194/acp-24-1361-2024, https://doi.org/10.5194/acp-24-1361-2024, 2024
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This study reports the first simultaneous records of oxygen (Δ17O) and nitrogen (δ15N) isotopes in nitrogen dioxide (NO2) and nitrate (NO3−). These data are combined with atmospheric observations to explore sub-daily N reactive chemistry and quantify N fractionation effects in an Alpine winter city. The results highlight the necessity of using Δ17O and δ15N in both NO2 and NO3− to avoid biased estimations of NOx sources and fates from NO3− isotopic records in urban winter environments.
Shigeyuki Ishidoya, Kazuhiro Tsuboi, Hiroaki Kondo, Kentaro Ishijima, Nobuyuki Aoki, Hidekazu Matsueda, and Kazuyuki Saito
Atmos. Chem. Phys., 24, 1059–1077, https://doi.org/10.5194/acp-24-1059-2024, https://doi.org/10.5194/acp-24-1059-2024, 2024
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A method evaluating techniques for carbon neutrality, such as carbon capture and storage (CCS), is important. This study presents a method to evaluate CO2 emissions from a cement plant based on atmospheric O2 and CO2 measurements. The method will also be useful for evaluating CO2 capture from flue gas at CCS plants, since the plants remove CO2 from the atmosphere without causing any O2 changes, just as cement plants do, differing only in the direction of CO2 exchange with the atmosphere.
Magdalena Pühl, Anke Roiger, Alina Fiehn, Alan M. Gorchov Negron, Eric A. Kort, Stefan Schwietzke, Ignacio Pisso, Amy Foulds, James Lee, James L. France, Anna E. Jones, Dave Lowry, Rebecca E. Fisher, Langwen Huang, Jacob Shaw, Prudence Bateson, Stephen Andrews, Stuart Young, Pamela Dominutti, Tom Lachlan-Cope, Alexandra Weiss, and Grant Allen
Atmos. Chem. Phys., 24, 1005–1024, https://doi.org/10.5194/acp-24-1005-2024, https://doi.org/10.5194/acp-24-1005-2024, 2024
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In April–May 2019 we carried out an airborne field campaign in the southern North Sea with the aim of studying methane emissions of offshore gas installations. We determined methane emissions from elevated methane measured downstream of the sampled installations. We compare our measured methane emissions with estimated methane emissions from national and global annual inventories. As a result, we find inconsistencies of inventories and large discrepancies between measurements and inventories.
Georgios I. Gkatzelis, Matthew M. Coggon, Chelsea E. Stockwell, Rebecca S. Hornbrook, Hannah Allen, Eric C. Apel, Megan M. Bela, Donald R. Blake, Ilann Bourgeois, Steven S. Brown, Pedro Campuzano-Jost, Jason M. St. Clair, James H. Crawford, John D. Crounse, Douglas A. Day, Joshua P. DiGangi, Glenn S. Diskin, Alan Fried, Jessica B. Gilman, Hongyu Guo, Johnathan W. Hair, Hannah S. Halliday, Thomas F. Hanisco, Reem Hannun, Alan Hills, L. Gregory Huey, Jose L. Jimenez, Joseph M. Katich, Aaron Lamplugh, Young Ro Lee, Jin Liao, Jakob Lindaas, Stuart A. McKeen, Tomas Mikoviny, Benjamin A. Nault, J. Andrew Neuman, John B. Nowak, Demetrios Pagonis, Jeff Peischl, Anne E. Perring, Felix Piel, Pamela S. Rickly, Michael A. Robinson, Andrew W. Rollins, Thomas B. Ryerson, Melinda K. Schueneman, Rebecca H. Schwantes, Joshua P. Schwarz, Kanako Sekimoto, Vanessa Selimovic, Taylor Shingler, David J. Tanner, Laura Tomsche, Krystal T. Vasquez, Patrick R. Veres, Rebecca Washenfelder, Petter Weibring, Paul O. Wennberg, Armin Wisthaler, Glenn M. Wolfe, Caroline C. Womack, Lu Xu, Katherine Ball, Robert J. Yokelson, and Carsten Warneke
Atmos. Chem. Phys., 24, 929–956, https://doi.org/10.5194/acp-24-929-2024, https://doi.org/10.5194/acp-24-929-2024, 2024
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This study reports emissions of gases and particles from wildfires. These emissions are related to chemical proxies that can be measured by satellite and incorporated into models to improve predictions of wildfire impacts on air quality and climate.
Jie Wang, Haichao Wang, Yee Jun Tham, Lili Ming, Zelong Zheng, Guizhen Fang, Cuizhi Sun, Zhenhao Ling, Jun Zhao, and Shaojia Fan
Atmos. Chem. Phys., 24, 977–992, https://doi.org/10.5194/acp-24-977-2024, https://doi.org/10.5194/acp-24-977-2024, 2024
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Many works report NO3 chemistry in inland regions while less target marine regions. We measured N2O5 and related species on a typical island and found intensive nighttime chemistry and rapid NO3 loss. NO contributed significantly to NO3 loss despite its sub-ppbv level, suggesting nocturnal NO3 reactions would be largely enhanced once free from NO emissions in the open ocean. This highlights the strong influences of urban outflow on downward marine areas in terms of nighttime chemistry.
Tanja J. Schuck, Johannes Degen, Eric Hintsa, Peter Hoor, Markus Jesswein, Timo Keber, Daniel Kunkel, Fred Moore, Florian Obersteiner, Matt Rigby, Thomas Wagenhäuser, Luke M. Western, Andreas Zahn, and Andreas Engel
Atmos. Chem. Phys., 24, 689–705, https://doi.org/10.5194/acp-24-689-2024, https://doi.org/10.5194/acp-24-689-2024, 2024
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We study the interhemispheric gradient of sulfur hexafluoride (SF6), a strong long-lived greenhouse gas. Its emissions are stronger in the Northern Hemisphere; therefore, mixing ratios in the Southern Hemisphere lag behind. Comparing the observations to a box model, the model predicts air in the Southern Hemisphere to be older. For a better agreement, the emissions used as model input need to be increased (and their spatial pattern changed), and we need to modify north–south transport.
Jérémy Gueffier, François Gheusi, Marie Lothon, Véronique Pont, Alban Philibert, Fabienne Lohou, Solène Derrien, Yannick Bezombes, Gilles Athier, Yves Meyerfeld, Antoine Vial, and Emmanuel Leclerc
Atmos. Chem. Phys., 24, 287–316, https://doi.org/10.5194/acp-24-287-2024, https://doi.org/10.5194/acp-24-287-2024, 2024
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This study investigates the link between weather regime and atmospheric composition at a Pyrenean observatory. Five years of meteorological data were synchronized on a daily basis and then, using a clustering method, separated into six groups of observation days, with most showing marked characteristics of different weather regimes (fair and disturbed weather, winter windstorms, foehn). Statistical differences in gas and particle concentrations appeared between the groups and are discussed.
Nathaniel Brockway, Peter K. Peterson, Katja Bigge, Kristian D. Hajny, Paul B. Shepson, Kerri A. Pratt, Jose D. Fuentes, Tim Starn, Robert Kaeser, Brian H. Stirm, and William R. Simpson
Atmos. Chem. Phys., 24, 23–40, https://doi.org/10.5194/acp-24-23-2024, https://doi.org/10.5194/acp-24-23-2024, 2024
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Bromine monoxide (BrO) strongly affects atmospheric chemistry in the springtime Arctic, yet there are still many uncertainties around its sources and recycling, particularly in the context of a rapidly changing Arctic. In this study, we observed BrO as a function of altitude above the Alaskan Arctic. We found that BrO was often most concentrated near the ground, confirming the ability of snow to produce and recycle reactive bromine, and identified four common vertical distributions of BrO.
Alina Fiehn, Maximilian Eckl, Julian Kostinek, Michał Gałkowski, Christoph Gerbig, Michael Rothe, Thomas Röckmann, Malika Menoud, Hossein Maazallahi, Martina Schmidt, Piotr Korbeń, Jarosław Neçki, Mila Stanisavljević, Justyna Swolkień, Andreas Fix, and Anke Roiger
Atmos. Chem. Phys., 23, 15749–15765, https://doi.org/10.5194/acp-23-15749-2023, https://doi.org/10.5194/acp-23-15749-2023, 2023
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During the CoMet mission in the Upper Silesian Coal Basin (USCB) ground-based and airborne air samples were taken and analyzed for the isotopic composition of CH4 to derive the mean signature of the USCB and source signatures of individual coal mines. Using δ2H signatures, the biogenic emissions from the USCB account for 15 %–50 % of total emissions, which is underestimated in common emission inventories. This demonstrates the importance of δ2H-CH4 observations for methane source apportionment.
Yifei Song, Chaoyang Xue, Yuanyuan Zhang, Pengfei Liu, Fengxia Bao, Xuran Li, and Yujing Mu
Atmos. Chem. Phys., 23, 15733–15747, https://doi.org/10.5194/acp-23-15733-2023, https://doi.org/10.5194/acp-23-15733-2023, 2023
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We present measurements of HONO flux and related parameters over an agricultural field during a whole growing season of summer maize. This dataset allows studies on the characteristics and influencing factors of soil HONO emissions, determination of HONO emission factors, estimation of total HONO emissions at a national scale, and the discussion on future environmental policies in terms of mitigating regional air pollution.
Can Ye, Keding Lu, Xuefei Ma, Wanyi Qiu, Shule Li, Xinping Yang, Chaoyang Xue, Tianyu Zhai, Yuhan Liu, Xuan Li, Yang Li, Haichao Wang, Zhaofeng Tan, Xiaorui Chen, Huabin Dong, Limin Zeng, Min Hu, and Yuanhang Zhang
Atmos. Chem. Phys., 23, 15455–15472, https://doi.org/10.5194/acp-23-15455-2023, https://doi.org/10.5194/acp-23-15455-2023, 2023
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In this study, combining comprehensive field measurements and a box model, we found NO2 conversion on the ground surface was the most important source for HONO production among the proposed heterogeneous and gas-phase HONO sources. In addition, HONO was found to evidently enhance O3 production and aggravate O3 pollution in summer in China. Our study improved our understanding of the relative importance of different HONO sources and the crucial role of HONO in O3 formation in polluted areas.
Yann Cohen, Didier Hauglustaine, Bastien Sauvage, Susanne Rohs, Patrick Konjari, Ulrich Bundke, Andreas Petzold, Valérie Thouret, Andreas Zahn, and Helmut Ziereis
Atmos. Chem. Phys., 23, 14973–15009, https://doi.org/10.5194/acp-23-14973-2023, https://doi.org/10.5194/acp-23-14973-2023, 2023
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The upper troposphere–lower stratosphere (UTLS) is a key region regarding the lower atmospheric composition. This study consists of a comprehensive evaluation of an up-to-date chemistry–climate model in this layer, using regular in situ measurements based on passenger aircraft. For this purpose, a specific software (Interpol-IAGOS) has been updated and made publicly available. The model reproduces the carbon monoxide peaks due to biomass burning over the continental tropics particularly well.
Yifan Jiang, Men Xia, Zhe Wang, Penggang Zheng, Yi Chen, and Tao Wang
Atmos. Chem. Phys., 23, 14813–14828, https://doi.org/10.5194/acp-23-14813-2023, https://doi.org/10.5194/acp-23-14813-2023, 2023
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This study provides the first estimate of high rates of formic acid (HCOOH) production from the photochemical aging of real ambient particles and demonstrates the potential importance of this pathway in the formation of HCOOH under ambient conditions. Incorporating this pathway significantly improved the performance of a widely used chemical model. Our solution irradiation experiments demonstrated the importance of nitrate photolysis in HCOOH production via the production of oxidants.
Xuelian Zhong, Hengqing Shen, Min Zhao, Ji Zhang, Yue Sun, Yuhong Liu, Yingnan Zhang, Ye Shan, Hongyong Li, Jiangshan Mu, Yu Yang, Yanqiu Nie, Jinghao Tang, Can Dong, Xinfeng Wang, Yujiao Zhu, Mingzhi Guo, Wenxing Wang, and Likun Xue
Atmos. Chem. Phys., 23, 14761–14778, https://doi.org/10.5194/acp-23-14761-2023, https://doi.org/10.5194/acp-23-14761-2023, 2023
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Nitrous acid (HONO) is vital for atmospheric oxidation. In research at Mount Lao, China, models revealed a significant unidentified marine HONO source. Overlooking this could skew our understanding of air quality and climate change. This finding emphasizes HONO’s importance in the coastal atmosphere, uncovering previously unnoticed interactions.
Steven Job Thomas, Toni Tykkä, Heidi Hellén, Federico Bianchi, and Arnaud P. Praplan
Atmos. Chem. Phys., 23, 14627–14642, https://doi.org/10.5194/acp-23-14627-2023, https://doi.org/10.5194/acp-23-14627-2023, 2023
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The study employed total ozone reactivity to demonstrate how emissions of Norway spruce readily react with ozone and could be a major ozone sink, particularly under stress. Additionally, this approach provided insight into the limitations of current analytical techniques that measure the compounds present or emitted into the atmosphere. The study shows how the technique used was not enough to measure all compounds emitted, and this could potentially underestimate various atmospheric processes.
Jinsol Kim, John B. Miller, Charles E. Miller, Scott J. Lehman, Sylvia E. Michel, Vineet Yadav, Nick E. Rollins, and William M. Berelson
Atmos. Chem. Phys., 23, 14425–14436, https://doi.org/10.5194/acp-23-14425-2023, https://doi.org/10.5194/acp-23-14425-2023, 2023
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In this study, we present the partitioning of CO2 signals from biogenic, petroleum and natural gas sources by combining CO, 13CO2 and 14CO2 measurements. Using measurements from flask air samples at three sites in the greater Los Angeles region, we find larger and positive contributions of biogenic signals in winter and smaller and negative contributions in summer. The largest contribution of natural gas combustion generally occurs in summer.
Robert Woodward-Massey, Roberto Sommariva, Lisa K. Whalley, Danny R. Cryer, Trevor Ingham, William J. Bloss, Stephen M. Ball, Sam Cox, James D. Lee, Chris P. Reed, Leigh R. Crilley, Louisa J. Kramer, Brian J. Bandy, Grant L. Forster, Claire E. Reeves, Paul S. Monks, and Dwayne E. Heard
Atmos. Chem. Phys., 23, 14393–14424, https://doi.org/10.5194/acp-23-14393-2023, https://doi.org/10.5194/acp-23-14393-2023, 2023
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Measurements of OH, HO2 and RO2 radicals and also OH reactivity were made at a UK coastal site and compared to calculations from a constrained box model utilising the Master Chemical Mechanism. The model agreement displayed a strong dependence on the NO concentration. An experimental budget analysis for OH, HO2, RO2 and total ROx demonstrated significant imbalances between HO2 and RO2 production rates. Ozone production rates were calculated from measured radicals and compared to modelled values.
Leonard Kirago, Örjan Gustafsson, Samuel Mwaniki Gaita, Sophie L. Haslett, Michael J. Gatari, Maria Elena Popa, Thomas Röckmann, Christoph Zellweger, Martin Steinbacher, Jörg Klausen, Christian Félix, David Njiru, and August Andersson
Atmos. Chem. Phys., 23, 14349–14357, https://doi.org/10.5194/acp-23-14349-2023, https://doi.org/10.5194/acp-23-14349-2023, 2023
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This study provides ground-observational evidence that supports earlier suggestions that savanna fires are the main emitters and modulators of carbon monoxide gas in Africa. Using isotope-based techniques, the study has shown that about two-thirds of this gas is emitted from savanna fires, while for urban areas, in this case Nairobi, primary sources approach 100 %. The latter has implications for air quality policy, suggesting primary emissions such as traffic should be targeted.
Ziyan Guo, Keding Lu, Pengxiang Qiu, Mingyi Xu, and Zhaobing Guo
EGUsphere, https://doi.org/10.5194/egusphere-2023-2554, https://doi.org/10.5194/egusphere-2023-2554, 2023
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The formation of secondary sulfate in the atmosphere remains controversial, and it is urgent to seek for a new method to quantify different sulfate formation pathways. Due to their sensitivity for the reaction environment, Isotope fractionation has widely used in trace of atmospheric processes. In this work, the contributions of typical oxidation pathways of sulfate formation are calculated on the basis of laboratory simulation and field observation via sulfur and oxygen isotope fractionation.
Delaney B. Kilgour, Gordon A. Novak, Megan S. Claflin, Brian M. Lerner, and Timothy H. Bertram
EGUsphere, https://doi.org/10.5194/egusphere-2023-2210, https://doi.org/10.5194/egusphere-2023-2210, 2023
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Laboratory experiments with seawater mimics suggest ozone deposition to the surface ocean can be a source of reactive carbon to the marine atmosphere. We conduct both field and laboratory measurements to assess abiotic VOC composition and yields from ozonolysis of real surface seawater. We show that C5–C11 aldehydes contribute to the observed VOC emission flux. We estimate that VOC generated by the ozonolysis of surface seawater is competitive with biological VOC production and emission.
Clara M. Nussbaumer, Bryan K. Place, Qindan Zhu, Eva Y. Pfannerstill, Paul Wooldridge, Benjamin C. Schulze, Caleb Arata, Ryan Ward, Anthony Bucholtz, John H. Seinfeld, Allen H. Goldstein, and Ronald C. Cohen
Atmos. Chem. Phys., 23, 13015–13028, https://doi.org/10.5194/acp-23-13015-2023, https://doi.org/10.5194/acp-23-13015-2023, 2023
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NOx is a precursor to hazardous tropospheric ozone and can be emitted from various anthropogenic sources. It is important to quantify NOx emissions in urban environments to improve the local air quality, which still remains a challenge, as sources are heterogeneous in space and time. In this study, we calculate NOx emissions over Los Angeles, based on aircraft measurements in June 2021, and compare them to a local emission inventory, which we find mostly overpredicts the measured values.
Magdalena Okuljar, Olga Garmash, Miska Olin, Joni Kalliokoski, Hilkka Timonen, Jarkko V. Niemi, Pauli Paasonen, Jenni Kontkanen, Yanjun Zhang, Heidi Hellén, Heino Kuuluvainen, Minna Aurela, Hanna E. Manninen, Mikko Sipilä, Topi Rönkkö, Tuukka Petäjä, Markku Kulmala, Miikka Dal Maso, and Mikael Ehn
Atmos. Chem. Phys., 23, 12965–12983, https://doi.org/10.5194/acp-23-12965-2023, https://doi.org/10.5194/acp-23-12965-2023, 2023
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Highly oxygenated organic molecules (HOMs) form secondary organic aerosol that affects air quality and health. In this study, we demonstrate that in a moderately polluted city with abundant vegetation, the composition of HOMs is largely controlled by the effect of NOx on the biogenic volatile organic compound oxidation. Comparing the results from two nearby stations, we show that HOM composition and formation pathways can change considerably within small distances in urban environments.
Si-Wan Kim, Kyoung-Min Kim, Yujoo Jeong, Seunghwan Seo, Yeonsu Park, and Jeongyeon Kim
Atmos. Chem. Phys., 23, 12867–12886, https://doi.org/10.5194/acp-23-12867-2023, https://doi.org/10.5194/acp-23-12867-2023, 2023
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Surface ozone is a pollutant regulated for public health. This study derived surface ozone trends over South Korea from 2001 to 2021 and highlighted that South Korea has been a nonattainment area since 2010, based on the US EPA standard. However, the occurrences of high ozone condition decreased in spring during the COVID-19 pandemic, partly due to large reductions of ozone precursor concentrations in China and South Korea.
Zeyu Sun, Zheng Zong, Yang Tan, Chongguo Tian, Zeyu Liu, Fan Zhang, Rong Sun, Yingjun Chen, Jun Li, and Gan Zhang
Atmos. Chem. Phys., 23, 12851–12865, https://doi.org/10.5194/acp-23-12851-2023, https://doi.org/10.5194/acp-23-12851-2023, 2023
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This is the first report of ship-emitted nitrogen stable isotope composition (δ15N) of nitrogen oxides (NOx). The results showed that δ15N–NOx from ships was −18.5 ± 10.9 ‰ and increased monotonically with tightening emission regulations. The selective catalytic reduction system was the most vital factor. The temporal variation in δ15N–NOx was evaluated and can be used to select suitable δ15N–NOx for a more accurate assessment of the contribution of ship-emitted exhaust to atmospheric NOx.
Eva Y. Pfannerstill, Caleb Arata, Qindan Zhu, Benjamin C. Schulze, Roy Woods, John H. Seinfeld, Anthony Bucholtz, Ronald C. Cohen, and Allen H. Goldstein
Atmos. Chem. Phys., 23, 12753–12780, https://doi.org/10.5194/acp-23-12753-2023, https://doi.org/10.5194/acp-23-12753-2023, 2023
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The San Joaquin Valley is an agricultural area with poor air quality. Organic gases drive the formation of hazardous air pollutants. Agricultural emissions of these gases are not well understood and have rarely been quantified at landscape scale. By combining aircraft-based emission measurements with land cover information, we found mis- or unrepresented emission sources. Our results help in understanding of pollution sources and in improving predictions of air quality in agricultural regions.
Yao Yan Huang and D. James Donaldson
EGUsphere, https://doi.org/10.5194/egusphere-2023-1751, https://doi.org/10.5194/egusphere-2023-1751, 2023
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Ground-level ozone interacts at the lake-land boundary; this is important to our understanding and modelling of atmospheric chemistry and air pollution in the lower atmosphere. We show that a steep ozone gradient occurs year-round moving inland up to 1 km from the lake and that this gradient is influenced by seasonal factors on the local land environment, where more rural areas are greater affected seasonally.
Youwei Hong, Keran Zhang, Dan Liao, Gaojie Chen, Min Zhao, Yiling Lin, Xiaoting Ji, Ke Xu, Yu Wu, Ruilian Yu, Gongren Hu, Sung-Deuk Choi, Likun Xue, and Jinsheng Chen
Atmos. Chem. Phys., 23, 10795–10807, https://doi.org/10.5194/acp-23-10795-2023, https://doi.org/10.5194/acp-23-10795-2023, 2023
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Particle uptakes of HCHO and the impacts on PM2.5 and O3 production remain highly uncertain. Based on the investigation of co-occurring wintertime O3 and PM2.5 pollution in a coastal city of southeast China, we found enhanced heterogeneous formation of hydroxymethanesulfonate (HMS) and increased ROx concentrations and net O3 production rates. The findings of this study are helpful to better explore the mechanisms of key precursors for co-occurring PM2.5 and O3 pollution.
Foteini Stavropoulou, Katarina Vinković, Bert Kers, Marcel de Vries, Steven van Heuven, Piotr Korbeń, Martina Schmidt, Julia Wietzel, Pawel Jagoda, Jaroslav M. Necki, Jakub Bartyzel, Hossein Maazallahi, Malika Menoud, Carina van der Veen, Sylvia Walter, Béla Tuzson, Jonas Ravelid, Randulph Paulo Morales, Lukas Emmenegger, Dominik Brunner, Michael Steiner, Arjan Hensen, Ilona Velzeboer, Pim van den Bulk, Hugo Denier van der Gon, Antonio Delre, Maklawe Essonanawe Edjabou, Charlotte Scheutz, Marius Corbu, Sebastian Iancu, Denisa Moaca, Alin Scarlat, Alexandru Tudor, Ioana Vizireanu, Andreea Calcan, Magdalena Ardelean, Sorin Ghemulet, Alexandru Pana, Aurel Constantinescu, Lucian Cusa, Alexandru Nica, Calin Baciu, Cristian Pop, Andrei Radovici, Alexandru Mereuta, Horatiu Stefanie, Alexandru Dandocsi, Bas Hermans, Stefan Schwietzke, Daniel Zavala-Araiza, Huilin Chen, and Thomas Röckmann
Atmos. Chem. Phys., 23, 10399–10412, https://doi.org/10.5194/acp-23-10399-2023, https://doi.org/10.5194/acp-23-10399-2023, 2023
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In this study, we quantify CH4 emissions from onshore oil production sites in Romania at source and facility level using a combination of ground- and drone-based measurement techniques. We show that the total CH4 emissions in our studied areas are much higher than the emissions reported to UNFCCC, and up to three-quarters of the detected emissions are related to operational venting. Our results suggest that oil and gas production infrastructure in Romania holds a massive mitigation potential.
Chunxiang Ye, Shuzheng Guo, Weili Lin, Fangjie Tian, Jianshu Wang, Chong Zhang, Suzhen Chi, Yi Chen, Yingjie Zhang, Limin Zeng, Xin Li, Duo Bu, Jiacheng Zhou, and Weixiong Zhao
Atmos. Chem. Phys., 23, 10383–10397, https://doi.org/10.5194/acp-23-10383-2023, https://doi.org/10.5194/acp-23-10383-2023, 2023
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Online volatile organic compound (VOC) measurements by gas chromatography–mass spectrometry, with other O3 precursors, were used to identify key VOC and other key sources in Lhasa. Total VOCs (TVOCs), alkanes, and aromatics are half as abundant as in Beijing. Oxygenated VOCs (OVOCs) consist of 52 % of the TVOCs. Alkenes and OVOCs account for 80 % of the ozone formation potential. Aromatics dominate secondary organic aerosol potential. Positive matrix factorization decomposed residential sources.
Brandon Bottorff, Michelle M. Lew, Youngjun Woo, Pamela Rickly, Matthew D. Rollings, Benjamin Deming, Daniel C. Anderson, Ezra Wood, Hariprasad D. Alwe, Dylan B. Millet, Andrew Weinheimer, Geoff Tyndall, John Ortega, Sebastien Dusanter, Thierry Leonardis, James Flynn, Matt Erickson, Sergio Alvarez, Jean C. Rivera-Rios, Joshua D. Shutter, Frank Keutsch, Detlev Helmig, Wei Wang, Hannah M. Allen, Johnathan H. Slade, Paul B. Shepson, Steven Bertman, and Philip S. Stevens
Atmos. Chem. Phys., 23, 10287–10311, https://doi.org/10.5194/acp-23-10287-2023, https://doi.org/10.5194/acp-23-10287-2023, 2023
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The hydroxyl (OH), hydroperoxy (HO2), and organic peroxy (RO2) radicals play important roles in atmospheric chemistry and have significant air quality implications. Here, we compare measurements of OH, HO2, and total peroxy radicals (XO2) made in a remote forest in Michigan, USA, to predictions from a series of chemical models. Lower measured radical concentrations suggest that the models may be missing an important radical sink and overestimating the rate of ozone production in this forest.
Jenny Oh, Chubashini Shunthirasingham, Ying Duan Lei, Faqiang Zhan, Yuening Li, Abigaëlle Dalpé Castilloux, Amina Ben Chaaben, Zhe Lu, Kelsey Lee, Frank A. P. C. Gobas, Sabine Eckhardt, Nick Alexandrou, Hayley Hung, and Frank Wania
Atmos. Chem. Phys., 23, 10191–10205, https://doi.org/10.5194/acp-23-10191-2023, https://doi.org/10.5194/acp-23-10191-2023, 2023
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An emerging brominated flame retardant (BFR) called TBECH (1,2-dibromo-4-(1,2-dibromoethyl)cyclohexane) has never been produced or imported for use in Canada yet is found to be one of the most abundant gaseous BFRs in the Canadian atmosphere. The recorded spatial and temporal variability of TBECH suggest that the release from imported consumer products containing TBECH is the most likely explanation for its environmental occurrence in Canada.
Olivia E. Clifton, Donna Schwede, Christian Hogrefe, Jesse O. Bash, Sam Bland, Philip Cheung, Mhairi Coyle, Lisa Emberson, Johannes Flemming, Erick Fredj, Stefano Galmarini, Laurens Ganzeveld, Orestis Gazetas, Ignacio Goded, Christopher D. Holmes, László Horváth, Vincent Huijnen, Qian Li, Paul A. Makar, Ivan Mammarella, Giovanni Manca, J. William Munger, Juan L. Pérez-Camanyo, Jonathan Pleim, Limei Ran, Roberto San Jose, Sam J. Silva, Ralf Staebler, Shihan Sun, Amos P. K. Tai, Eran Tas, Timo Vesala, Tamás Weidinger, Zhiyong Wu, and Leiming Zhang
Atmos. Chem. Phys., 23, 9911–9961, https://doi.org/10.5194/acp-23-9911-2023, https://doi.org/10.5194/acp-23-9911-2023, 2023
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A primary sink of air pollutants is dry deposition. Dry deposition estimates differ across the models used to simulate atmospheric chemistry. Here, we introduce an effort to examine dry deposition schemes from atmospheric chemistry models. We provide our approach’s rationale, document the schemes, and describe datasets used to drive and evaluate the schemes. We also launch the analysis of results by evaluating against observations and identifying the processes leading to model–model differences.
Qindan Zhu, Bryan Place, Eva Y. Pfannerstill, Sha Tong, Huanxin Zhang, Jun Wang, Clara M. Nussbaumer, Paul Wooldridge, Benjamin C. Schulze, Caleb Arata, Anthony Bucholtz, John H. Seinfeld, Allen H. Goldstein, and Ronald C. Cohen
Atmos. Chem. Phys., 23, 9669–9683, https://doi.org/10.5194/acp-23-9669-2023, https://doi.org/10.5194/acp-23-9669-2023, 2023
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Nitrogen oxide (NOx) is a hazardous air pollutant, and it is the precursor of short-lived climate forcers like tropospheric ozone and aerosol particles. While NOx emissions from transportation has been strictly regulated, soil NOx emissions are overlooked. We use the airborne flux measurements to observe NOx emissions from highways and urban and cultivated soil land cover types. We show non-negligible soil NOx emissions, which are significantly underestimated in current model simulations.
Money Ossohou, Jonathan Edward Hickman, Lieven Clarisse, Pierre-François Coheur, Martin Van Damme, Marcellin Adon, Véronique Yoboué, Eric Gardrat, Maria Dias Alvès, and Corinne Galy-Lacaux
Atmos. Chem. Phys., 23, 9473–9494, https://doi.org/10.5194/acp-23-9473-2023, https://doi.org/10.5194/acp-23-9473-2023, 2023
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The updated analyses of ground-based concentrations and satellite total vertical columns of atmospheric ammonia help us to better understand 21st century ammonia dynamics in sub-Saharan Africa. We conclude that the drivers of trends are agriculture in the dry savanna of Katibougou, Mali; air temperature and agriculture in the wet savanna of Djougou, Benin, and Lamto, Côte d'Ivoire; and leaf area index, air temperature, residential, and agriculture in forests of Bomassa, Republic of Congo.
Hyeri Park, Jooil Kim, Haklim Choi, Sohyeon Geum, Yeaseul Kim, Rona L. Thompson, Jens Mühle, Peter K. Salameh, Christina M. Harth, Kieran M. Stanley, Simon O'Doherty, Paul J. Fraser, Peter G. Simmonds, Paul B. Krummel, Ray F. Weiss, Ronald G. Prinn, and Sunyoung Park
Atmos. Chem. Phys., 23, 9401–9411, https://doi.org/10.5194/acp-23-9401-2023, https://doi.org/10.5194/acp-23-9401-2023, 2023
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Based on atmospheric HFC-23 observations, the first estimate of post-CDM HFC-23 emissions in eastern Asia for 2008–2019 shows that these emissions contribute significantly to the global emissions rise. The observation-derived emissions were much larger than the bottom-up estimates expected to approach zero after 2015 due to national abatement activities. These discrepancies could be attributed to unsuccessful factory-level HFC-23 abatement and inaccurate quantification of emission reductions.
Philipp Eger, Theresa Mathes, Alex Zavarsky, and Lars Duester
Atmos. Chem. Phys., 23, 8769–8788, https://doi.org/10.5194/acp-23-8769-2023, https://doi.org/10.5194/acp-23-8769-2023, 2023
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We investigated the contribution of inland shipping to air pollution at the river Rhine in Germany. Land-based measurements of gaseous and particulate pollutants were carried out for more than 1 year to provide a realistic estimate for the exposure of people to air pollution close to the riverside. Emissions of nitrogen oxides and particulate matter relative to the amount of fuel used, as well as their dependence on ship size, engine type and operating conditions, were examined.
Imran A. Girach, Narendra Ojha, Prabha R. Nair, Kandula V. Subrahmanyam, Neelakantan Koushik, Mohammed M. Nazeer, Nadimpally Kiran Kumar, Surendran Nair Suresh Babu, Jos Lelieveld, and Andrea Pozzer
EGUsphere, https://doi.org/10.5194/egusphere-2023-1524, https://doi.org/10.5194/egusphere-2023-1524, 2023
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We investigated surface ozone variability at East Antarctica based on the measurements and EMAC global model simulations during austral summer. Nearly half of the surface ozone is found to be of stratospheric origin. The east coast of Antarctica acts as a stronger sink of ozone than surrounding regions. Photochemical loss of ozone is counterbalanced by downward transport of ozone. Study highlights intertwined role of chemistry and dynamics in governing the ozone variations over East Antarctica.
Romain Salignat, Matti Rissanen, Siddharth Iyer, Jean-Luc Baray, Pierre Tulet, Jean-Marc Metzger, Jérôme Brioude, Karine Sellegri, and Clémence Rose
EGUsphere, https://doi.org/10.5194/egusphere-2023-1319, https://doi.org/10.5194/egusphere-2023-1319, 2023
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Using mass spectrometry data collected at the Maïdo observatory (2160 m a.s.l., Reunion island), we provide the first detailed analysis of molecular clusters chemical composition specifically in the marine free troposphere. The abundance of the identified species is related both to in-situ meteorological parameters and air-mass history, which also provide insight into their origin. Our work makes an important contribution to documenting the chemistry and physics of the marine free troposphere.
Hejun Hu, Haichao Wang, Keding Lu, Jie Wang, Zelong Zheng, Xuezhen Xu, Tianyu Zhai, Xiaorui Chen, Xiao Lu, Wenxing Fu, Xin Li, Limin Zeng, Min Hu, Yuanhang Zhang, and Shaojia Fan
Atmos. Chem. Phys., 23, 8211–8223, https://doi.org/10.5194/acp-23-8211-2023, https://doi.org/10.5194/acp-23-8211-2023, 2023
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Nitrate radical chemistry is critical to the degradation of volatile organic compounds (VOCs) and secondary organic aerosol formation. This work investigated the level, seasonal variation, and trend of nitrate radical reactivity towards volatile organic compounds (kNO3) in Beijing. We show the key role of isoprene and styrene in regulating seasonal variation in kNO3 and rebuild a long-term record of kNO3 based on the reported VOC measurements.
Eliane Gomes Alves, Raoni Aquino Santana, Cléo Quaresma Dias-Júnior, Santiago Botía, Tyeen Taylor, Ana Maria Yáñez-Serrano, Jürgen Kesselmeier, Efstratios Bourtsoukidis, Jonathan Williams, Pedro Ivo Lembo Silveira de Assis, Giordane Martins, Rodrigo de Souza, Sérgio Duvoisin Júnior, Alex Guenther, Dasa Gu, Anywhere Tsokankunku, Matthias Sörgel, Bruce Nelson, Davieliton Pinto, Shujiro Komiya, Diogo Martins Rosa, Bettina Weber, Cybelli Barbosa, Michelle Robin, Kenneth J. Feeley, Alvaro Duque, Viviana Londoño Lemos, Maria Paula Contreras, Alvaro Idarraga, Norberto López, Chad Husby, Brett Jestrow, and Iván Mauricio Cely Toro
Atmos. Chem. Phys., 23, 8149–8168, https://doi.org/10.5194/acp-23-8149-2023, https://doi.org/10.5194/acp-23-8149-2023, 2023
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Isoprene is emitted mainly by plants and can influence atmospheric chemistry and air quality. But, there are uncertainties in model emission estimates and follow-up atmospheric processes. In our study, with long-term observational datasets of isoprene and biological and environmental factors from central Amazonia, we show that isoprene emission estimates could be improved when biological processes were mechanistically incorporated into the model.
Thais Luarte, Victoria A. Gómez-Aburto, Ignacio Poblete-Castro, Eduardo Castro-Nallar, Nicolas Huneeus, Marco Molina-Montenegro, Claudia Egas, Germán Azcune, Andrés Pérez-Parada, Rainier Lohmann, Pernilla Bohlin-Nizzetto, Jordi Dachs, Susan Bengtson-Nash, Gustavo Chiang, Karla Pozo, and Cristóbal J. Galbán-Malagón
Atmos. Chem. Phys., 23, 8103–8118, https://doi.org/10.5194/acp-23-8103-2023, https://doi.org/10.5194/acp-23-8103-2023, 2023
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In the last 40 years, different research groups have reported on the atmospheric concentrations of persistent organic pollutants in Antarctica. In the present work, we make a compilation to understand the historical trends and estimate the atmospheric half-life of each compound. Of the compounds studied, HCB was the only one that showed no clear trend, while the rest of the studied compounds showed a significant decrease over time. This is consistent with results for polar and sub-polar zones.
Midhun George, Maria Dolores Andrés Hernández, Vladyslav Nenakhov, Yangzhuoran Liu, John Philip Burrows, Birger Bohn, Eric Förster, Florian Obersteiner, Andreas Zahn, Theresa Harlaß, Helmut Ziereis, Hans Schlager, Benjamin Schreiner, Flora Kluge, Katja Bigge, and Klaus Pfeilsticker
Atmos. Chem. Phys., 23, 7799–7822, https://doi.org/10.5194/acp-23-7799-2023, https://doi.org/10.5194/acp-23-7799-2023, 2023
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The applicability of photostationary steady-state (PSS) assumptions to estimate the amount of the sum of peroxy radicals (RO2*) during the EMeRGe airborne observations from the known radical chemistry and onboard measurements of RO2* precursors, photolysis frequencies, and other trace gases such as NOx and O3 was investigated. The comparison of the calculated RO2* with the actual measurements provides an insight into the main processes controlling their concentration in the air masses measured.
Ross Petersen, Thomas Holst, Meelis Mölder, Natascha Kljun, and Janne Rinne
Atmos. Chem. Phys., 23, 7839–7858, https://doi.org/10.5194/acp-23-7839-2023, https://doi.org/10.5194/acp-23-7839-2023, 2023
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We investigate variability in the vertical distribution of volatile organic compounds (VOCs) in boreal forest, determined through multiyear measurements at several heights in a boreal forest in Sweden. VOC source/sink seasonality in canopy was explored using these vertical profiles and with measurements from a collection of sonic anemometers on the station flux tower. Our results show seasonality in the source/sink distribution for several VOCs, such as monoterpenes and water-soluble compounds.
Wanyun Xu, Yuxuan Bian, Weili Lin, Yingjie Zhang, Yaru Wang, Zhiqiang Ma, Xiaoyi Zhang, Gen Zhang, Chunxiang Ye, and Xiaobin Xu
Atmos. Chem. Phys., 23, 7635–7652, https://doi.org/10.5194/acp-23-7635-2023, https://doi.org/10.5194/acp-23-7635-2023, 2023
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Tropospheric ozone (O3) and peroxyacetyl nitrate (PAN) are both photochemical pollutants harmful to the ecological environment and human health, especially in the Tibetan Plateau (TP). However, the factors determining their variations in the TP have not been comprehensively investigated. Results from field measurements and observation-based models revealed that day-to-day variations in O3 and PAN were in fact controlled by distinct physiochemical processes.
Megan E. McCabe, Ilana B. Pollack, Emily V. Fischer, Kathryn M. Steinmann, and Dana R. Caulton
Atmos. Chem. Phys., 23, 7479–7494, https://doi.org/10.5194/acp-23-7479-2023, https://doi.org/10.5194/acp-23-7479-2023, 2023
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Agriculture emissions, including those from beef and dairy cattle feeding operations, make up a large portion of the United States’ total greenhouse gas emissions, but many of these operations reside in areas where methane from oil and natural gas is prevalent, making it difficult to attribute methane in these areas. This work investigates two approaches to emission attribution for cattle feeding operations and provides guidance for emission attribution in other complicated regions.
Kai Qin, Wei Hu, Qin He, Fan Lu, and Jason Blake Cohen
EGUsphere, https://doi.org/10.5194/egusphere-2023-1210, https://doi.org/10.5194/egusphere-2023-1210, 2023
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Shanxi accounts for 10 % of the world’s coal production. This work computes CH4 emissions and uncertainty on a mine-by-mine basis, including underground, overground, and abandoned. This work uses a flux tower to observe and calculate emissions at one mine over 4 months. The half-hour variability and bias correction are propagated over the emissions dataset. Comparisons show the emissions are higher where mines are located, and regions with significant emissions but no mines are identified.
Haeyoung Lee, Wonick Seo, Shanlan Li, Soojeong Lee, Samuel Takele Kenea, and Sangwon Joo
Atmos. Chem. Phys., 23, 7141–7159, https://doi.org/10.5194/acp-23-7141-2023, https://doi.org/10.5194/acp-23-7141-2023, 2023
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We introduced three Korea Meteorological Administration (KMA) monitoring stations with monitoring systems and measurement uncertainty. We also analyzed the regional characteristics of CH4 at each KMA station. CH4 levels measured at KMA stations are compared to those measured at other Asian stations. From the long-term records of CH4 and δ13CH4 at AMY, we confirmed that the source of CH4xs changed from the past (2006 to 2010) to recent (2016 to 2020) years in East Asia.
Robert G. Ryan, Eloise A. Marais, Eleanor Gershenson-Smith, Robbie Ramsay, Jan-Peter Muller, Jan-Lukas Tirpitz, and Udo Frieß
Atmos. Chem. Phys., 23, 7121–7139, https://doi.org/10.5194/acp-23-7121-2023, https://doi.org/10.5194/acp-23-7121-2023, 2023
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We describe the first data retrieval from a newly installed instrument providing measurements of vertical profiles of air pollution over Central London during heatwaves in summer 2022. We use these observations with surface air quality network measurements to support interpretation that an exponential increase in biogenic emissions of isoprene during heatwaves provides the limiting ingredient for severe ozone pollution, leading to non-compliance with the national ozone air quality standard.
Zhouxing Zou, Qianjie Chen, Men Xia, Qi Yuan, Yi Chen, Yanan Wang, Enyu Xiong, Zhe Wang, and Tao Wang
Atmos. Chem. Phys., 23, 7057–7074, https://doi.org/10.5194/acp-23-7057-2023, https://doi.org/10.5194/acp-23-7057-2023, 2023
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We present OH observation and model simulation results at a coastal site in Hong Kong. The model predicted the OH concentration under high-NOx well but overpredicted it under low-NOx conditions. This implies an insufficient understanding of OH chemistry under low-NOx conditions. We show evidence of missing OH sinks as a possible cause of the overprediction.
Yaqin Gao, Hongli Wang, Lingling Yuan, Shengao Jing, Bin Yuan, Guofeng Shen, Liang Zhu, Abigail Koss, Yingjie Li, Qian Wang, Dan Dan Huang, Shuhui Zhu, Shikang Tao, Shengrong Lou, and Cheng Huang
Atmos. Chem. Phys., 23, 6633–6646, https://doi.org/10.5194/acp-23-6633-2023, https://doi.org/10.5194/acp-23-6633-2023, 2023
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A near-complete speciation of reactive organic gases from residential combustion was developed to get more insights into their atmospheric effects. Oxygenated species, higher hydrocarbons and nitrogen-containing species played larger roles in these emissions compared with common hydrocarbons. Based on the near-complete speciation, these emissions were largely underestimated, leading to more underestimation of their hydroxyl radical reactivity and secondary organic aerosol formation potential.
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Short summary
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.
An assessment of mercury emissions from a burning boreal forest was made by flying an aircraft...
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