Articles | Volume 17, issue 3
Atmos. Chem. Phys., 17, 1689–1698, 2017
https://doi.org/10.5194/acp-17-1689-2017
© Author(s) 2017. This work is distributed under
the Creative Commons Attribution 3.0 License.
the Creative Commons Attribution 3.0 License.
Special issue: Data collection, analysis and application of speciated atmospheric...
Atmos. Chem. Phys., 17, 1689–1698, 2017
https://doi.org/10.5194/acp-17-1689-2017
© Author(s) 2017. This work is distributed under
the Creative Commons Attribution 3.0 License.
the Creative Commons Attribution 3.0 License.
Research article 03 Feb 2017
Research article | 03 Feb 2017
Deciphering potential chemical compounds of gaseous oxidized mercury in Florida, USA
Jiaoyan Huang et al.
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M. S. Gustin, H. M. Amos, J. Huang, M. B. Miller, and K. Heidecorn
Atmos. Chem. Phys., 15, 5697–5713, https://doi.org/10.5194/acp-15-5697-2015, https://doi.org/10.5194/acp-15-5697-2015, 2015
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The Minamata Convention for mercury (Hg) has been signed by many nations and the primary objective is to protect human health and the environment from releases of Hg. A key challenge researchers is developing linkages between Hg in the atmosphere, deposition, and ecosystem contamination. Here we critically review where the science on measuring and modeling atmospheric Hg stands and offer suggestions for future research that will both advance understanding of Hg cycling and serve the convention.
J. Huang, M. B. Miller, E. Edgerton, and M. S. Gustin
Atmos. Chem. Phys. Discuss., https://doi.org/10.5194/acpd-15-12069-2015, https://doi.org/10.5194/acpd-15-12069-2015, 2015
Revised manuscript not accepted
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Gaseous oxidized Hg (GOM) is a major contributor to Hg in wet and dry deposition. Recent work has indicated that the concentrations of GOM as measured are too low by 3-to-12 times; and that compounds vary across space and time. Data collected in Florida indicate five potential GOM compounds, including HgBr2, HgO, Hg(NO3)2, HgSO4, and an unknown compound. Sources include local combustion (cars and power plants), the marine boundary layer, and long range transport from Asia.
Alexandra J. Boris, Satoshi Takahama, Andrew T. Weakley, Bruno M. Debus, Stephanie L. Shaw, Eric S. Edgerton, Taekyu Joo, Nga L. Ng, and Ann M. Dillner
Atmos. Meas. Tech., 14, 4355–4374, https://doi.org/10.5194/amt-14-4355-2021, https://doi.org/10.5194/amt-14-4355-2021, 2021
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Infrared spectrometry can be applied in routine monitoring of atmospheric particles to give comprehensive characterization of the organic material by bond rather than species. Using this technique, the concentrations of particle organic material were found to decrease 2011–2016 in the southeastern US, driven by a decline in highly aged material, concurrent with declining anthropogenic emissions. However, an increase was observed in the fraction of more moderately aged organic matter.
Yiqi Zheng, Joel A. Thornton, Nga Lee Ng, Hansen Cao, Daven K. Henze, Erin E. McDuffie, Weiwei Hu, Jose L. Jimenez, Eloise A. Marais, Eric Edgerton, and Jingqiu Mao
Atmos. Chem. Phys., 20, 13091–13107, https://doi.org/10.5194/acp-20-13091-2020, https://doi.org/10.5194/acp-20-13091-2020, 2020
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This study aims to address a challenge in biosphere–atmosphere interactions: to what extent can biogenic organic aerosol (OA) be modified through human activities? From three surface network observations, we show OA is weakly dependent on sulfate and aerosol acidity in the summer southeast US, on both long-term trends and monthly variability. The results are in strong contrast to a global model, GEOS-Chem, suggesting the need to revisit the representation of aqueous-phase secondary OA formation.
Alexandra J. Boris, Satoshi Takahama, Andrew T. Weakley, Bruno M. Debus, Carley D. Fredrickson, Martin Esparza-Sanchez, Charlotte Burki, Matteo Reggente, Stephanie L. Shaw, Eric S. Edgerton, and Ann M. Dillner
Atmos. Meas. Tech., 12, 5391–5415, https://doi.org/10.5194/amt-12-5391-2019, https://doi.org/10.5194/amt-12-5391-2019, 2019
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Organic species are abundant in atmospheric particle-phase (aerosol) pollution and originate from a variety of biogenic and anthropogenic sources. Infrared spectrometry of filter-based atmospheric particle samples can afford a direct measurement of the particulate organic matter concentration and a characterization of its composition. This work discusses recent method improvements and compositions measured in samples from the SouthEastern Aerosol Research and Characterization (SEARCH) network.
Matthieu B. Miller, Sarrah M. Dunham-Cheatham, Mae Sexauer Gustin, and Grant C. Edwards
Atmos. Meas. Tech., 12, 1207–1217, https://doi.org/10.5194/amt-12-1207-2019, https://doi.org/10.5194/amt-12-1207-2019, 2019
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This study was undertaken to demonstrate that a cation exchange membrane (CEM) material used for sampling reactive mercury (RM) does not possess an inherent tendency to collect gaseous elemental mercury (GEM). Using a custom-built mercury vapor permeation system, we found that the CEM material has a very small GEM uptake of approximately 0.004 %, too small to create a significant artifact. We also found that a representative RM compound was collected by the CEM material with high efficiency.
Shino Toma, Steve Bertman, Christopher Groff, Fulizi Xiong, Paul B. Shepson, Paul Romer, Kaitlin Duffey, Paul Wooldridge, Ronald Cohen, Karsten Baumann, Eric Edgerton, Abigail R. Koss, Joost de Gouw, Allen Goldstein, Weiwei Hu, and Jose L. Jimenez
Atmos. Chem. Phys., 19, 1867–1880, https://doi.org/10.5194/acp-19-1867-2019, https://doi.org/10.5194/acp-19-1867-2019, 2019
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Acyl peroxy nitrates (APN) were measured near the ground in Alabama using GC in summer 2013 to study biosphere–atmosphere interactions. APN were lower than measured in the SE USA over the past 2 decades. Historical data showed APN in 2013 was limited by NOx and production was dominated by biogenic precursors more than in the past. Isoprene-derived MPAN correlated with isoprene hydroxynitrates as NOx-dependent products. MPAN varied with aerosol growth, but not with N-containing particles.
Matthieu B. Miller, Mae S. Gustin, and Grant C. Edwards
Atmos. Meas. Tech. Discuss., https://doi.org/10.5194/amt-2018-360, https://doi.org/10.5194/amt-2018-360, 2018
Revised manuscript not accepted
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In the atmosphere there are 2 gaseous forms of mercury (Hg), elemental (Hgo) and oxidized compounds (GOM). Hgo is oxidized by gases such as ozone and chlorine compounds. GOM is readily deposited to ecosystems and converted to methylmercury (a subtle neurotoxin). Here we explain development of a method for measurement of GOM deposition and emission associated with surfaces, and demonstrate that both occur. This has significant implications, because no one has been able to do this successfully.
Xi Chen, Mingjie Xie, Michael D. Hays, Eric Edgerton, Donna Schwede, and John T. Walker
Atmos. Chem. Phys., 18, 6829–6846, https://doi.org/10.5194/acp-18-6829-2018, https://doi.org/10.5194/acp-18-6829-2018, 2018
Ashley M. Pierce, S. Marcela Loría-Salazar, W. Patrick Arnott, Grant C. Edwards, Matthieu B. Miller, and Mae S. Gustin
Atmos. Meas. Tech., 11, 2225–2237, https://doi.org/10.5194/amt-11-2225-2018, https://doi.org/10.5194/amt-11-2225-2018, 2018
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This paper investigates the possible sources of anomalous particulate matter collected at a high-elevation site during June to November 2014. Particles were collected on a sample filter that were > 2.5 µm in aerodynamic diameter, on a system that theoretically should not collect particulate matter that large. These samples indicated that either the observed particles had unique dimensions and behavior or that there was an issue with the particulate monitor inlet setup.
Paul S. Romer, Kaitlin C. Duffey, Paul J. Wooldridge, Eric Edgerton, Karsten Baumann, Philip A. Feiner, David O. Miller, William H. Brune, Abigail R. Koss, Joost A. de Gouw, Pawel K. Misztal, Allen H. Goldstein, and Ronald C. Cohen
Atmos. Chem. Phys., 18, 2601–2614, https://doi.org/10.5194/acp-18-2601-2018, https://doi.org/10.5194/acp-18-2601-2018, 2018
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Observations of increased ozone on hotter days are widely reported, but the mechanisms driving this relationship remain uncertain. We use measurements from the rural southeastern United States to study how temperature affects ozone production. We find that changing NOx emissions, most likely from soil microbes, can be a major driver of increased ozone with temperature in the continental background. These findings suggest that ozone will increase with temperature under a wide range of conditions.
Leiming Zhang, Seth Lyman, Huiting Mao, Che-Jen Lin, David A. Gay, Shuxiao Wang, Mae Sexauer Gustin, Xinbin Feng, and Frank Wania
Atmos. Chem. Phys., 17, 9133–9144, https://doi.org/10.5194/acp-17-9133-2017, https://doi.org/10.5194/acp-17-9133-2017, 2017
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Future research needs are proposed for improving the understanding of atmospheric mercury cycling. These include refinement of mercury emission estimations, quantification of dry deposition and air–surface exchange, improvement of the treatment of chemical mechanisms in chemical transport models, increase in the accuracy of oxidized mercury measurements, better interpretation of atmospheric mercury chemistry data, and harmonization of network operation.
J. Kaiser, K. M. Skog, K. Baumann, S. B. Bertman, S. B. Brown, W. H. Brune, J. D. Crounse, J. A. de Gouw, E. S. Edgerton, P. A. Feiner, A. H. Goldstein, A. Koss, P. K. Misztal, T. B. Nguyen, K. F. Olson, J. M. St. Clair, A. P. Teng, S. Toma, P. O. Wennberg, R. J. Wild, L. Zhang, and F. N. Keutsch
Atmos. Chem. Phys., 16, 9349–9359, https://doi.org/10.5194/acp-16-9349-2016, https://doi.org/10.5194/acp-16-9349-2016, 2016
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OH reactivity can be used to assess the amount of reactive carbon in an air mass. “Missing” reactivity is commonly found in forested environments and is attributed to either direct emissions of unmeasured volatile organic compounds or to unmeasured/underpredicted oxidation products. Using a box model and measurements from the 2013 SOAS campaign, we find only small discrepancies in measured and calculated reactivity. Our results suggest the discrepancies stem from unmeasured direct emissions.
Luping Su, Edward G. Patton, Jordi Vilà-Guerau de Arellano, Alex B. Guenther, Lisa Kaser, Bin Yuan, Fulizi Xiong, Paul B. Shepson, Li Zhang, David O. Miller, William H. Brune, Karsten Baumann, Eric Edgerton, Andrew Weinheimer, Pawel K. Misztal, Jeong-Hoo Park, Allen H. Goldstein, Kate M. Skog, Frank N. Keutsch, and John E. Mak
Atmos. Chem. Phys., 16, 7725–7741, https://doi.org/10.5194/acp-16-7725-2016, https://doi.org/10.5194/acp-16-7725-2016, 2016
Sri Hapsari Budisulistiorini, Karsten Baumann, Eric S. Edgerton, Solomon T. Bairai, Stephen Mueller, Stephanie L. Shaw, Eladio M. Knipping, Avram Gold, and Jason D. Surratt
Atmos. Chem. Phys., 16, 5171–5189, https://doi.org/10.5194/acp-16-5171-2016, https://doi.org/10.5194/acp-16-5171-2016, 2016
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A year-long near-real-time characterization of non-refractory submicron aerosol (NR-PM1) was conducted at an urban (Atlanta, Georgia, in 2012) and rural (Look Rock, Tennessee, in 2013) site in the southeastern US using the Aerodyne Aerosol Chemical Speciation Monitor, collocated with established air-monitoring network measurements, to identify sources of organic aerosol (OA). Further, high-volume filter samples were collected for measurements of OA tracers by offline mass spectrometry tools.
Weruka Rattanavaraha, Kevin Chu, Sri Hapsari Budisulistiorini, Matthieu Riva, Ying-Hsuan Lin, Eric S. Edgerton, Karsten Baumann, Stephanie L. Shaw, Hongyu Guo, Laura King, Rodney J. Weber, Miranda E. Neff, Elizabeth A. Stone, John H. Offenberg, Zhenfa Zhang, Avram Gold, and Jason D. Surratt
Atmos. Chem. Phys., 16, 4897–4914, https://doi.org/10.5194/acp-16-4897-2016, https://doi.org/10.5194/acp-16-4897-2016, 2016
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The mechanisms by which specific anthropogenic pollutants enhance isoprene SOA in ambient PM2.5 remain unclear. As one aspect of an investigation to examine how anthropogenic pollutants influence isoprene-derived SOA formation, high-volume PM2.5 filter samples were collected from Birmingham, AL, during the 2013 Southern Oxidant and Aerosol Study (SOAS). Isoprene SOA tracers were measured from these samples and compared to gas and aerosol data collected from the SEARCH network.
Sean Coburn, Barbara Dix, Eric Edgerton, Christopher D. Holmes, Douglas Kinnison, Qing Liang, Arnout ter Schure, Siyuan Wang, and Rainer Volkamer
Atmos. Chem. Phys., 16, 3743–3760, https://doi.org/10.5194/acp-16-3743-2016, https://doi.org/10.5194/acp-16-3743-2016, 2016
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Here we present a day of case study measurements of the vertical distribution of bromine monoxide over the coastal region of the Gulf of Mexico. These measurements are used to assess the contribution of bromine radicals to the oxidation of elemental mercury in the troposphere. We find that the measured levels of bromine in the troposphere are sufficient to quickly oxidize mercury, which has significant implications for our understanding of atmospheric mercury processes.
C. L. Blanchard, G. M. Hidy, S. Shaw, K. Baumann, and E. S. Edgerton
Atmos. Chem. Phys., 16, 215–238, https://doi.org/10.5194/acp-16-215-2016, https://doi.org/10.5194/acp-16-215-2016, 2016
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Fifteen years of gas and particle measurements at eight monitoring sites comprising the Southeastern Aerosol Research and Characterization (SEARCH) network offer insights into the sources of organic aerosol in the southeastern United States. Between 1999 and 2013, mean organic aerosol concentrations declined due to decreasing particle emissions from motor vehicles and to less secondary organic aerosol with declining emissions of sulfur dioxide, nitrogen oxides, and volatile organic compounds.
B. R. Ayres, H. M. Allen, D. C. Draper, S. S. Brown, R. J. Wild, J. L. Jimenez, D. A. Day, P. Campuzano-Jost, W. Hu, J. de Gouw, A. Koss, R. C. Cohen, K. C. Duffey, P. Romer, K. Baumann, E. Edgerton, S. Takahama, J. A. Thornton, B. H. Lee, F. D. Lopez-Hilfiker, C. Mohr, P. O. Wennberg, T. B. Nguyen, A. Teng, A. H. Goldstein, K. Olson, and J. L. Fry
Atmos. Chem. Phys., 15, 13377–13392, https://doi.org/10.5194/acp-15-13377-2015, https://doi.org/10.5194/acp-15-13377-2015, 2015
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This paper reports atmospheric gas- and aerosol-phase field measurements from the southeastern United States in summer 2013 to demonstrate that the oxidation of biogenic volatile organic compounds by nitrate radical produces a substantial amount of secondary organic aerosol in this region. This process, driven largely by monoterpenes, results in a comparable aerosol nitrate production rate to inorganic nitrate formation by heterogeneous uptake of HNO3 onto dust particles.
F. Xiong, K. M. McAvey, K. A. Pratt, C. J. Groff, M. A. Hostetler, M. A. Lipton, T. K. Starn, J. V. Seeley, S. B. Bertman, A. P. Teng, J. D. Crounse, T. B. Nguyen, P. O. Wennberg, P. K. Misztal, A. H. Goldstein, A. B. Guenther, A. R. Koss, K. F. Olson, J. A. de Gouw, K. Baumann, E. S. Edgerton, P. A. Feiner, L. Zhang, D. O. Miller, W. H. Brune, and P. B. Shepson
Atmos. Chem. Phys., 15, 11257–11272, https://doi.org/10.5194/acp-15-11257-2015, https://doi.org/10.5194/acp-15-11257-2015, 2015
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Hydroxynitrates from isoprene oxidation were quantified both in the laboratory and through field studies. The yield of hydroxynitrates 9(+4/-3)% derived from chamber experiments was applied in a zero-dimensional model to simulate the production and loss of isoprene hydroxynitrates in an ambient environment during the 2013 Southern Oxidant and Aerosol Study (SOAS). NOx was determined to be the limiting factor for the formation of isoprene hydroxynitrates during SOAS.
H. M. Allen, D. C. Draper, B. R. Ayres, A. Ault, A. Bondy, S. Takahama, R. L. Modini, K. Baumann, E. Edgerton, C. Knote, A. Laskin, B. Wang, and J. L. Fry
Atmos. Chem. Phys., 15, 10669–10685, https://doi.org/10.5194/acp-15-10669-2015, https://doi.org/10.5194/acp-15-10669-2015, 2015
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We report ion chromatographic measurements of gas- and aerosol-phase inorganic species at the SOAS 2013 field study. Our particular focus is on inorganic nitrate aerosol formation via HNO3 uptake onto coarse-mode dust and sea salt particles, which we find to be the dominant source of episodic inorganic nitrate at this site, due to the high acidity of the particles preventing formation of NH4NO3. We calculate a production rate of inorganic nitrate aerosol.
M. S. Gustin, H. M. Amos, J. Huang, M. B. Miller, and K. Heidecorn
Atmos. Chem. Phys., 15, 5697–5713, https://doi.org/10.5194/acp-15-5697-2015, https://doi.org/10.5194/acp-15-5697-2015, 2015
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The Minamata Convention for mercury (Hg) has been signed by many nations and the primary objective is to protect human health and the environment from releases of Hg. A key challenge researchers is developing linkages between Hg in the atmosphere, deposition, and ecosystem contamination. Here we critically review where the science on measuring and modeling atmospheric Hg stands and offer suggestions for future research that will both advance understanding of Hg cycling and serve the convention.
J. Huang, M. B. Miller, E. Edgerton, and M. S. Gustin
Atmos. Chem. Phys. Discuss., https://doi.org/10.5194/acpd-15-12069-2015, https://doi.org/10.5194/acpd-15-12069-2015, 2015
Revised manuscript not accepted
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Gaseous oxidized Hg (GOM) is a major contributor to Hg in wet and dry deposition. Recent work has indicated that the concentrations of GOM as measured are too low by 3-to-12 times; and that compounds vary across space and time. Data collected in Florida indicate five potential GOM compounds, including HgBr2, HgO, Hg(NO3)2, HgSO4, and an unknown compound. Sources include local combustion (cars and power plants), the marine boundary layer, and long range transport from Asia.
P. Weiss-Penzias, H. M. Amos, N. E. Selin, M. S. Gustin, D. A. Jaffe, D. Obrist, G.-R. Sheu, and A. Giang
Atmos. Chem. Phys., 15, 1161–1173, https://doi.org/10.5194/acp-15-1161-2015, https://doi.org/10.5194/acp-15-1161-2015, 2015
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Speciated atmospheric Hg measurements from five high-elevation sites were compared with a global mercury model. The comparison confirmed that reactive mercury is formed in dry free tropospheric air from the oxidation of elemental Hg, more so in the summer than in other seasons. Simulations run with OH-O3 oxidation instead of the Br oxidation mechanism compared more closely with observations at desert sites, suggesting future simulations should include multiple reaction mechanisms simultaneously.
T. Fang, V. Verma, H. Guo, L. E. King, E. S. Edgerton, and R. J. Weber
Atmos. Meas. Tech., 8, 471–482, https://doi.org/10.5194/amt-8-471-2015, https://doi.org/10.5194/amt-8-471-2015, 2015
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This work summarizes a newly developed semi-automated system for quantifying the oxidative potential of aerosol aqueous extracts using the dithiothreitol (DTT) assay. 500 sample analyses indicate that DTT activity in the southeast US is likely not dominated by a unique local source, and sources change with season. The unique large data set generated with the technique described in this paper allows new studies on DTT sources and investigating linkages between reactive oxygen species and health.
V. Verma, T. Fang, H. Guo, L. King, J. T. Bates, R. E. Peltier, E. Edgerton, A. G. Russell, and R. J. Weber
Atmos. Chem. Phys., 14, 12915–12930, https://doi.org/10.5194/acp-14-12915-2014, https://doi.org/10.5194/acp-14-12915-2014, 2014
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The major emission sources of the reactive oxygen species (ROS) associated with ambient particulate matter in the southeastern United States were identified. The study shows biomass burning and secondary aerosol formation as the major sources contributing to the ROS-generating capability of ambient particles. The ubiquitous nature of these two sources suggests widespread population exposures to the toxic aerosol components.
Y. You, V. P. Kanawade, J. A. de Gouw, A. B. Guenther, S. Madronich, M. R. Sierra-Hernández, M. Lawler, J. N. Smith, S. Takahama, G. Ruggeri, A. Koss, K. Olson, K. Baumann, R. J. Weber, A. Nenes, H. Guo, E. S. Edgerton, L. Porcelli, W. H. Brune, A. H. Goldstein, and S.-H. Lee
Atmos. Chem. Phys., 14, 12181–12194, https://doi.org/10.5194/acp-14-12181-2014, https://doi.org/10.5194/acp-14-12181-2014, 2014
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Amiens play important roles in atmospheric secondary aerosol formation and human health, but the fast response measurements of amines are lacking. Here we show measurements in a southeastern US forest and a moderately polluted midwestern site. Our results show that gas to particle conversion is an important process that controls ambient amine concentrations and that biomass burning is an important source of amines.
G. M. Hidy, C. L. Blanchard, K. Baumann, E. Edgerton, S. Tanenbaum, S. Shaw, E. Knipping, I. Tombach, J. Jansen, and J. Walters
Atmos. Chem. Phys., 14, 11893–11914, https://doi.org/10.5194/acp-14-11893-2014, https://doi.org/10.5194/acp-14-11893-2014, 2014
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This paper reviews aerometric measurements from Centreville, Alabama. The measurements show annual trends with air pollution emissions from 1999 to 2013. They provide a context for observations from 1 June to 15 July 2013 supporting the Southern Oxidant and Aerosol Study. An important goal of this experiment was to advance knowledge of aerosols produced in the atmosphere from precursors. The observations were in moist and warm conditions with the lowest gas and particle concentrations recorded.
S. H. Budisulistiorini, M. R. Canagaratna, P. L. Croteau, K. Baumann, E. S. Edgerton, M. S. Kollman, N. L. Ng, V. Verma, S. L. Shaw, E. M. Knipping, D. R. Worsnop, J. T. Jayne, R.J. Weber, and J. D. Surratt
Atmos. Meas. Tech., 7, 1929–1941, https://doi.org/10.5194/amt-7-1929-2014, https://doi.org/10.5194/amt-7-1929-2014, 2014
J. Liu, M. Bergin, H. Guo, L. King, N. Kotra, E. Edgerton, and R. J. Weber
Atmos. Chem. Phys., 13, 12389–12404, https://doi.org/10.5194/acp-13-12389-2013, https://doi.org/10.5194/acp-13-12389-2013, 2013
Y.-H. Lin, E. M. Knipping, E. S. Edgerton, S. L. Shaw, and J. D. Surratt
Atmos. Chem. Phys., 13, 8457–8470, https://doi.org/10.5194/acp-13-8457-2013, https://doi.org/10.5194/acp-13-8457-2013, 2013
Related subject area
Subject: Gases | Research Activity: Field Measurements | Altitude Range: Troposphere | Science Focus: Chemistry (chemical composition and reactions)
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A measurement and model study on ozone characteristics in marine air at a remote island station and its interaction with urban ozone air quality in Shanghai, China
David D. Parrish, Richard G. Derwent, Steven T. Turnock, Fiona M. O'Connor, Johannes Staehelin, Susanne E. Bauer, Makoto Deushi, Naga Oshima, Kostas Tsigaridis, Tongwen Wu, and Jie Zhang
Atmos. Chem. Phys., 21, 9669–9679, https://doi.org/10.5194/acp-21-9669-2021, https://doi.org/10.5194/acp-21-9669-2021, 2021
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The few ozone measurements made before the 1980s indicate that industrial development increased ozone concentrations by a factor of ~ 2 at northern midlatitudes, which are now larger than at southern midlatitudes. This difference was much smaller, and likely reversed, in the pre-industrial atmosphere. Earth system models find similar increases, but not higher pre-industrial ozone in the south. This disagreement may indicate that modeled natural ozone sources and/or deposition loss are inadequate.
Wei Huang, Haiyan Li, Nina Sarnela, Liine Heikkinen, Yee Jun Tham, Jyri Mikkilä, Steven J. Thomas, Neil M. Donahue, Markku Kulmala, and Federico Bianchi
Atmos. Chem. Phys., 21, 8961–8977, https://doi.org/10.5194/acp-21-8961-2021, https://doi.org/10.5194/acp-21-8961-2021, 2021
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We show full characterization of gaseous organic compounds in a boreal forest. Molecular composition and volatility of gaseous organic compounds with different oxidation extents (from volatile organic compounds to highly oxygenated organic molecules) were investigated and discussed. We provide a more comprehensive understanding of atmospheric organic compounds in this boreal forest and new insights into interpreting ambient measurements or testing and improving parameterizations in models.
Elizabeth B. Wiggins, Arlyn Andrews, Colm Sweeney, John B. Miller, Charles E. Miller, Sander Veraverbeke, Roisin Commane, Steven Wofsy, John M. Henderson, and James T. Randerson
Atmos. Chem. Phys., 21, 8557–8574, https://doi.org/10.5194/acp-21-8557-2021, https://doi.org/10.5194/acp-21-8557-2021, 2021
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We analyzed high-resolution trace gas measurements collected from a tower in Alaska during a very active fire season to improve our understanding of trace gas emissions from boreal forest fires. Our results suggest previous studies may have underestimated emissions from smoldering combustion in boreal forest fires.
Chenshuo Ye, Bin Yuan, Yi Lin, Zelong Wang, Weiwei Hu, Tiange Li, Wei Chen, Caihong Wu, Chaomin Wang, Shan Huang, Jipeng Qi, Baolin Wang, Chen Wang, Wei Song, Xinming Wang, E Zheng, Jordan E. Krechmer, Penglin Ye, Zhanyi Zhang, Xuemei Wang, Douglas R. Worsnop, and Min Shao
Atmos. Chem. Phys., 21, 8455–8478, https://doi.org/10.5194/acp-21-8455-2021, https://doi.org/10.5194/acp-21-8455-2021, 2021
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We performed measurements of gaseous and particulate organic compounds using a state-of-the-art online mass spectrometer in urban air. Using the dataset, we provide a holistic chemical characterization of oxygenated organic compounds in the polluted urban atmosphere, which can serve as a reference for the future field measurements of organic compounds in cities.
Astrid Müller, Hiroshi Tanimoto, Takafumi Sugita, Toshinobu Machida, Shin-ichiro Nakaoka, Prabir K. Patra, Joshua Laughner, and David Crisp
Atmos. Chem. Phys., 21, 8255–8271, https://doi.org/10.5194/acp-21-8255-2021, https://doi.org/10.5194/acp-21-8255-2021, 2021
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Over oceans, high uncertainties in satellite CO2 retrievals exist due to limited reference data. We combine commercial ship and aircraft observations and, with the aid of model calculations, obtain column-averaged mixing ratios of CO2 (XCO2) data over the Pacific Ocean. This new dataset has great potential as a robust reference for XCO2 measured from space and can help to better understand changes in the carbon cycle in response to climate change using satellite observations.
Ivan Tadic, Clara M. Nussbaumer, Birger Bohn, Hartwig Harder, Daniel Marno, Monica Martinez, Florian Obersteiner, Uwe Parchatka, Andrea Pozzer, Roland Rohloff, Martin Zöger, Jos Lelieveld, and Horst Fischer
Atmos. Chem. Phys., 21, 8195–8211, https://doi.org/10.5194/acp-21-8195-2021, https://doi.org/10.5194/acp-21-8195-2021, 2021
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Although mechanisms of tropospheric ozone (O3) formation are well understood, studies reporting on ozone formation derived from field measurements are challenging and remain sparse in number. We use airborne measurements to quantify nitric oxide (NO) and O3 distributions in the upper troposphere over the Atlantic Ocean and western Africa and compare our measurements to model simulations. Our results show that NO and ozone formation are greatest over the tropical areas of western Africa.
Heidi Hellén, Arnaud P. Praplan, Toni Tykkä, Aku Helin, Simon Schallhart, Piia P. Schiestl-Aalto, Jaana Bäck, and Hannele Hakola
Atmos. Chem. Phys., 21, 8045–8066, https://doi.org/10.5194/acp-21-8045-2021, https://doi.org/10.5194/acp-21-8045-2021, 2021
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Even though terpene emissions of boreal needle trees have been studied quite intensively, there is less knowledge of the emissions of broadleaved deciduous trees and emissions of larger terpenes and oxygenated volatile organic compounds. Here we studied downy birch (Betula pubescens) emissions, and especially sesquiterpene and oxygenated sesquiterpene emissions were found to be high. These emissions may have significant effects on secondary organic aerosol formation in boreal areas.
Kai Song, Song Guo, Haichao Wang, Ying Yu, Hui Wang, Rongzhi Tang, Shiyong Xia, Yuanzheng Gong, Zichao Wan, Daqi Lv, Rui Tan, Wenfei Zhu, Ruizhe Shen, Xin Li, Xuena Yu, Shiyi Chen, Liming Zeng, and Xiaofeng Huang
Atmos. Chem. Phys., 21, 7917–7932, https://doi.org/10.5194/acp-21-7917-2021, https://doi.org/10.5194/acp-21-7917-2021, 2021
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Nitrated phenols (NPs) are crucial components of brown carbon. To comprehend the constitutes and sources of NPs in winter of Beijing, their concentrations were measured by a CI-LToF-MS. The secondary formation process was simulated by a box model. NPs were mainly influenced by primary emissions and regional transport. Primary emitted phenol rather than benzene oxidation was crucial in the heavy pollution episode in Beijing. This provides more insight into pollution control strategies of NPs.
Clara M. Nussbaumer, Ivan Tadic, Dirk Dienhart, Nijing Wang, Achim Edtbauer, Lisa Ernle, Jonathan Williams, Florian Obersteiner, Isidoro Gutiérrez-Álvarez, Hartwig Harder, Jos Lelieveld, and Horst Fischer
Atmos. Chem. Phys., 21, 7933–7945, https://doi.org/10.5194/acp-21-7933-2021, https://doi.org/10.5194/acp-21-7933-2021, 2021
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Lightning over continental and coastal areas is frequent and accompanied by deep convection, while lightning over marine areas and particularly in tropical cyclones is rare. This research presents in situ observations of the tropical storm Florence 2018 near Cabo Verde. We show the absence of lightning in the tropical storm despite the occurrence of deep convective processes by atmospheric trace gas measurements of O3, NO, CO, H2O2, DMS and CH2I.
Nils Friedrich, Philipp Eger, Justin Shenolikar, Nicolas Sobanski, Jan Schuladen, Dirk Dienhart, Bettina Hottmann, Ivan Tadic, Horst Fischer, Monica Martinez, Roland Rohloff, Sebastian Tauer, Hartwig Harder, Eva Y. Pfannerstill, Nijing Wang, Jonathan Williams, James Brooks, Frank Drewnick, Hang Su, Guo Li, Yafang Cheng, Jos Lelieveld, and John N. Crowley
Atmos. Chem. Phys., 21, 7473–7498, https://doi.org/10.5194/acp-21-7473-2021, https://doi.org/10.5194/acp-21-7473-2021, 2021
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This paper uses NOx and NOz measurements from the 2017 AQABA ship campaign in the Mediterranean Sea and around the Arabian Peninsula to examine the influence e.g. of emissions from shipping and oil and gas production. Night-time losses of NOx dominated in the Arabian Gulf and in the Red Sea, whereas daytime losses were more important in the Mediterranean Sea. Nitric acid and organic nitrates were the most prevalent components of NOz.
Max Thomas, Johannes C. Laube, Jan Kaiser, Samuel Allin, Patricia Martinerie, Robert Mulvaney, Anna Ridley, Thomas Röckmann, William T. Sturges, and Emmanuel Witrant
Atmos. Chem. Phys., 21, 6857–6873, https://doi.org/10.5194/acp-21-6857-2021, https://doi.org/10.5194/acp-21-6857-2021, 2021
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CFC gases are destroying the Earth's life-protecting ozone layer. We improve understanding of CFC destruction by measuring the isotopic fingerprint of the carbon in the three most abundant CFCs. These are the first such measurements in the main region where CFCs are destroyed – the stratosphere. We reconstruct the atmospheric isotope histories of these CFCs back to the 1950s by measuring air extracted from deep snow and using a model. The model and the measurements are generally consistent.
Xuewu Fu, Chen Liu, Hui Zhang, Yue Xu, Hui Zhang, Jun Li, Xiaopu Lyu, Gan Zhang, Hai Guo, Xun Wang, Leiming Zhang, and Xinbin Feng
Atmos. Chem. Phys., 21, 6721–6734, https://doi.org/10.5194/acp-21-6721-2021, https://doi.org/10.5194/acp-21-6721-2021, 2021
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TGM concentrations and isotopic compositions in 10 Chinese cities showed strong seasonality with higher TGM concentrations and Δ199Hg and lower δ202Hg in summer. We found the seasonal variations in TGM concentrations and isotopic compositions were highly related to regional surface Hg(0) emissions, suggesting land surface Hg(0) emissions are an important source of atmospheric TGM that contribute dominantly to the seasonal variations in TGM concentrations and isotopic compositions.
Claire E. Reeves, Graham P. Mills, Lisa K. Whalley, W. Joe F. Acton, William J. Bloss, Leigh R. Crilley, Sue Grimmond, Dwayne E. Heard, C. Nicholas Hewitt, James R. Hopkins, Simone Kotthaus, Louisa J. Kramer, Roderic L. Jones, James D. Lee, Yanhui Liu, Bin Ouyang, Eloise Slater, Freya Squires, Xinming Wang, Robert Woodward-Massey, and Chunxiang Ye
Atmos. Chem. Phys., 21, 6315–6330, https://doi.org/10.5194/acp-21-6315-2021, https://doi.org/10.5194/acp-21-6315-2021, 2021
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The impact of isoprene on atmospheric chemistry is dependent on how its oxidation products interact with other pollutants, specifically nitrogen oxides. Such interactions can lead to isoprene nitrates. We made measurements of the concentrations of individual isoprene nitrate isomers in Beijing and used a model to test current understanding of their chemistry. We highlight areas of uncertainty in understanding, in particular the chemistry following oxidation of isoprene by the nitrate radical.
Dianne Sanchez, Roger Seco, Dasa Gu, Alex Guenther, John Mak, Youngjae Lee, Danbi Kim, Joonyoung Ahn, Don Blake, Scott Herndon, Daun Jeong, John T. Sullivan, Thomas Mcgee, Rokjin Park, and Saewung Kim
Atmos. Chem. Phys., 21, 6331–6345, https://doi.org/10.5194/acp-21-6331-2021, https://doi.org/10.5194/acp-21-6331-2021, 2021
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We present observations of total reactive gases in a suburban forest observatory in the Seoul metropolitan area. The quantitative comparison with speciated trace gas observations illustrated significant underestimation in atmospheric reactivity from the speciated trace gas observational dataset. We present scientific discussion about potential causes.
Eva Y. Pfannerstill, Nina G. Reijrink, Achim Edtbauer, Akima Ringsdorf, Nora Zannoni, Alessandro Araújo, Florian Ditas, Bruna A. Holanda, Marta O. Sá, Anywhere Tsokankunku, David Walter, Stefan Wolff, Jošt V. Lavrič, Christopher Pöhlker, Matthias Sörgel, and Jonathan Williams
Atmos. Chem. Phys., 21, 6231–6256, https://doi.org/10.5194/acp-21-6231-2021, https://doi.org/10.5194/acp-21-6231-2021, 2021
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Tropical forests are globally significant for atmospheric chemistry. However, the mixture of reactive organic gases emitted by these ecosystems is poorly understood. By comprehensive observations at an Amazon forest site, we show that oxygenated species were previously underestimated in their contribution to the tropical-forest reactant mix. Our results show rain and temperature effects and have implications for models and the understanding of ozone and particle formation above tropical forests.
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.
Yishuo Guo, Chao Yan, Chang Li, Wei Ma, Zemin Feng, Ying Zhou, Zhuohui Lin, Lubna Dada, Dominik Stolzenburg, Rujing Yin, Jenni Kontkanen, Kaspar R. Daellenbach, Juha Kangasluoma, Lei Yao, Biwu Chu, Yonghong Wang, Runlong Cai, Federico Bianchi, Yongchun Liu, and Markku Kulmala
Atmos. Chem. Phys., 21, 5499–5511, https://doi.org/10.5194/acp-21-5499-2021, https://doi.org/10.5194/acp-21-5499-2021, 2021
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Fog, cloud and haze are very common natural phenomena. Sulfuric acid (SA) is one of the key compounds forming those suspended particles, technically called aerosols, through gas-to-particle conversion. Therefore, the concentration level, source and sink of SA is very important. Our results show that ozonolysis of alkenes plays a major role in nighttime SA formation under unpolluted conditions in urban Beijing, and nighttime cluster mode particles are probably driven by SA in urban environments.
Mengdi Song, Xin Li, Suding Yang, Xuena Yu, Songxiu Zhou, Yiming Yang, Shiyi Chen, Huabin Dong, Keren Liao, Qi Chen, Keding Lu, Ningning Zhang, Junji Cao, Limin Zeng, and Yuanhang Zhang
Atmos. Chem. Phys., 21, 4939–4958, https://doi.org/10.5194/acp-21-4939-2021, https://doi.org/10.5194/acp-21-4939-2021, 2021
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Due to their lower diffusion capacities and higher conversion capacities, urban areas in Xi’an experienced severe ozone pollution in the summer. In this study, a campaign of comprehensive field observations and VOC grid sampling was conducted in Xi’an from 20 June to 20 July 2019. We found that Xi'an has a strong local emission source of VOCs, and vehicle exhaust was the primary VOC source. In addition, alkenes, aromatics, and oxygenated VOCs played a dominant role in secondary transformations.
Nur H. Orak, Matthew Reeder, and Natalie J. Pekney
Atmos. Chem. Phys., 21, 4729–4739, https://doi.org/10.5194/acp-21-4729-2021, https://doi.org/10.5194/acp-21-4729-2021, 2021
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In this paper, we investigate the effect of unconventional natural gas development activities on local air quality. This is the first study, to our knowledge, to collect high-time-resolution ambient concentrations of compounds emitted from well pad activity on Marcellus Shale during various phases of operation such that the relative air quality effect of each phase of development can be investigated.
Hua Fang, Xiaoqing Huang, Yanli Zhang, Chenglei Pei, Zuzhao Huang, Yujun Wang, Yanning Chen, Jianhong Yan, Jianqiang Zeng, Shaoxuan Xiao, Shilu Luo, Sheng Li, Jun Wang, Ming Zhu, Xuewei Fu, Zhenfeng Wu, Runqi Zhang, Wei Song, Guohua Zhang, Weiwei Hu, Mingjin Tang, Xiang Ding, Xinhui Bi, and Xinming Wang
Atmos. Chem. Phys. Discuss., https://doi.org/10.5194/acp-2021-189, https://doi.org/10.5194/acp-2021-189, 2021
Revised manuscript accepted for ACP
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A tunnel test was initiated to measure the vehicular IVOCs emissions under real-world driving conditions. Higher SOA formations estimated from vehicular IVOCs than that from traditional VOCs emphasized the greater importance of IVOCs in modulating urban SOA. The results also revealed that non-road diesel-fueled engines greatly contributed to IVOCs in China.
Di Liu, Wanqi Sun, Ning Zeng, Pengfei Han, Bo Yao, Zhiqiang Liu, Pucai Wang, Ke Zheng, Han Mei, and Qixiang Cai
Atmos. Chem. Phys., 21, 4599–4614, https://doi.org/10.5194/acp-21-4599-2021, https://doi.org/10.5194/acp-21-4599-2021, 2021
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It is difficult to directly observe the COVID-19 signals in CO2 due to the strong weather induced variations. Here, we determined the on-road CO2 concentration declines in Beijing using mobile observatory data before (BC), during (DC) and after COVID-19 (AC). We chose trips with the most similar weather and calculated the enhancement, the difference between on-road and the city “background”. We showed a clear on-road CO2 decrease in DC, which is consistent with the emissions reductions in DC.
Clémence Rose, Matti P. Rissanen, Siddharth Iyer, Jonathan Duplissy, Chao Yan, John B. Nowak, Aurélie Colomb, Régis Dupuy, Xu-Cheng He, Janne Lampilahti, Yee Jun Tham, Daniela Wimmer, Jean-Marc Metzger, Pierre Tulet, Jérôme Brioude, Céline Planche, Markku Kulmala, and Karine Sellegri
Atmos. Chem. Phys., 21, 4541–4560, https://doi.org/10.5194/acp-21-4541-2021, https://doi.org/10.5194/acp-21-4541-2021, 2021
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Sulfuric acid (H2SO4) is commonly accepted as a key precursor for atmospheric new particle formation. However, direct measurements of [H2SO4] remain challenging, motivating the development of proxies. Using data collected in two different volcanic plumes, we show, under these specific conditions, the good performance of a proxy from the literature and also highlight the benefit of the newly developed proxies for the prediction of the highest [H2SO4] values.
Ziru Lan, Weili Lin, Weiwei Pu, and Zhiqiang Ma
Atmos. Chem. Phys., 21, 4561–4573, https://doi.org/10.5194/acp-21-4561-2021, https://doi.org/10.5194/acp-21-4561-2021, 2021
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Haze related to particulate matter has become a big problem in eastern China, and ammonia (NH3) plays an important role in secondary particulate matter formation. In this work, variations in the NH3 mixing ratio showed that the contributions of NH3 sources and sinks in urban and suburban areas were quite different, although the areas were under the influence of similar weather systems. This study furthers the understanding of the behavior of NH3 in a megacity environment.
Haiyan Li, Manjula R. Canagaratna, Matthieu Riva, Pekka Rantala, Yanjun Zhang, Steven Thomas, Liine Heikkinen, Pierre-Marie Flaud, Eric Villenave, Emilie Perraudin, Douglas Worsnop, Markku Kulmala, Mikael Ehn, and Federico Bianchi
Atmos. Chem. Phys., 21, 4123–4147, https://doi.org/10.5194/acp-21-4123-2021, https://doi.org/10.5194/acp-21-4123-2021, 2021
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For the first time, we performed binPMF analysis on the complex mass spectra acquired with the Vocus PTR-TOF in two European pine forests and identified various primary emission sources and secondary oxidation processes of atmospheric organic vapors, i.e., terpenes and their oxidation products, with varying oxidation degrees. Further insights were gained regarding monoterpene and sesquiterpene reactions based on the interpretation results.
Shona E. Wilde, Pamela A. Dominutti, Grant Allen, Stephen J. Andrews, Prudence Bateson, Stephane J.-B. Bauguitte, Ralph R. Burton, Ioana Colfescu, James France, James R. Hopkins, Langwen Huang, Anna E. Jones, Tom Lachlan-Cope, James D. Lee, Alastair C. Lewis, Stephen D. Mobbs, Alexandra Weiss, Stuart Young, and Ruth M. Purvis
Atmos. Chem. Phys., 21, 3741–3762, https://doi.org/10.5194/acp-21-3741-2021, https://doi.org/10.5194/acp-21-3741-2021, 2021
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We use airborne measurements to evaluate the speciation of volatile organic compound (VOC) emissions from offshore oil and gas (O&G) installations in the North Sea. The composition of emissions varied across regions associated with either gas, condensate or oil extraction, demonstrating that VOC emissions are not uniform across the whole O&G sector. We compare our results to VOC source profiles in the UK emissions inventory, showing these emissions are not currently fully characterized.
Yenny Gonzalez, Róisín Commane, Ethan Manninen, Bruce C. Daube, Luke Schiferl, J. Barry McManus, Kathryn McKain, Eric J. Hintsa, James W. Elkins, Stephen A. Montzka, Colm Sweeney, Fred Moore, Jose L. Jimenez, Pedro Campuzano Jost, Thomas B. Ryerson, Ilann Bourgeois, Jeff Peischl, Chelsea R. Thompson, Eric Ray, Paul O. Wennberg, John Crounse, Michelle Kim, Hannah M. Allen, Paul Newman, Britton B. Stephens, Eric C. Apel, Rebecca S. Hornbrook, Benjamin A. Nault, Eric Morgan, and Steven C. Wofsy
Atmos. Chem. Phys. Discuss., https://doi.org/10.5194/acp-2021-167, https://doi.org/10.5194/acp-2021-167, 2021
Revised manuscript accepted for ACP
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Vertical profiles of N2O and a variety of chemical species and aerosols were collected over the oceans from nearly Pole to Pole during the NASA Atmospheric Tomography mission. We observed that tropospheric N2O variability is strongly driven by the influence of stratospheric air depleted in N2O, especially at middle and high latitudes. We also traced the origins of biomass burning and industrial emissions and investigate their impact on the variability of tropospheric N2O.
Julian Rüdiger, Alexandra Gutmann, Nicole Bobrowski, Marcello Liotta, J. Maarten de Moor, Rolf Sander, Florian Dinger, Jan-Lukas Tirpitz, Martha Ibarra, Armando Saballos, María Martínez, Elvis Mendoza, Arnoldo Ferrufino, John Stix, Juan Valdés, Jonathan M. Castro, and Thorsten Hoffmann
Atmos. Chem. Phys., 21, 3371–3393, https://doi.org/10.5194/acp-21-3371-2021, https://doi.org/10.5194/acp-21-3371-2021, 2021
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We present an innovative approach to study halogen chemistry in the plume of Masaya volcano in Nicaragua. An unique data set was collected using multiple techniques, including drones. These data enabled us to determine the fraction of activation of the respective halogens at various plume ages, where in-mixing of ambient air causes chemical reactions. An atmospheric chemistry box model was employed to further examine the field results and help our understanding of volcanic plume chemistry.
Christian Lamprecht, Martin Graus, Marcus Striednig, Michael Stichaner, and Thomas Karl
Atmos. Chem. Phys., 21, 3091–3102, https://doi.org/10.5194/acp-21-3091-2021, https://doi.org/10.5194/acp-21-3091-2021, 2021
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The first European SARS-CoV-2 (severe acute respiratory syndrome coronavirus 2) wave and associated lockdown provided a unique sensitivity experiment to study air pollution. We find significantly different emission trajectories between classical air pollution and climate gases (e.g., carbon dioxide). The analysis suggests that European policies, shifting residential, public, and commercial energy demand towards cleaner combustion, have helped to improve air quality more than expected.
Daniel P. Phillips, Frances E. Hopkins, Thomas G. Bell, Peter S. Liss, Philip D. Nightingale, Claire E. Reeves, Charel Wohl, and Mingxi Yang
Atmos. Chem. Phys. Discuss., https://doi.org/10.5194/acp-2021-108, https://doi.org/10.5194/acp-2021-108, 2021
Revised manuscript accepted for ACP
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We present the first measurements of the rate of transfer (flux) of three gases between the atmosphere and the ocean, using a direct flux measurement technique, at a coastal site. We show greater atmospheric loss of acetone and acetaldehyde into the ocean than estimated by global models for the open-water; importantly, the acetaldehyde transfer direction is opposite to the model estimates. Measured dimethylsulphide fluxes agreed with a recent model. Isoprene fluxes were too weak to be measured.
Jakob B. Pernov, Rossana Bossi, Thibaut Lebourgeois, Jacob K. Nøjgaard, Rupert Holzinger, Jens L. Hjorth, and Henrik Skov
Atmos. Chem. Phys., 21, 2895–2916, https://doi.org/10.5194/acp-21-2895-2021, https://doi.org/10.5194/acp-21-2895-2021, 2021
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Volatile organic compounds (VOCs) are an important constituent in the Arctic atmosphere due to their effect on aerosol and ozone formation. However, an understanding of their sources is lacking. This research presents a multiseason high-time-resolution dataset of VOCs in the Arctic and details their temporal characteristics and source apportionment. Four sources were identified: biomass burning, marine cryosphere, background, and Arctic haze.
Lisa K. Whalley, Eloise J. Slater, Robert Woodward-Massey, Chunxiang Ye, James D. Lee, Freya Squires, James R. Hopkins, Rachel E. Dunmore, Marvin Shaw, Jacqueline F. Hamilton, Alastair C. Lewis, Archit Mehra, Stephen D. Worrall, Asan Bacak, Thomas J. Bannan, Hugh Coe, Carl J. Percival, Bin Ouyang, Roderic L. Jones, Leigh R. Crilley, Louisa J. Kramer, William J. Bloss, Tuan Vu, Simone Kotthaus, Sue Grimmond, Yele Sun, Weiqi Xu, Siyao Yue, Lujie Ren, W. Joe F. Acton, C. Nicholas Hewitt, Xinming Wang, Pingqing Fu, and Dwayne E. Heard
Atmos. Chem. Phys., 21, 2125–2147, https://doi.org/10.5194/acp-21-2125-2021, https://doi.org/10.5194/acp-21-2125-2021, 2021
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To understand how emission controls will impact ozone, an understanding of the sources and sinks of OH and the chemical cycling between peroxy radicals is needed. This paper presents measurements of OH, HO2 and total RO2 taken in central Beijing. The radical observations are compared to a detailed chemistry model, which shows that under low NO conditions, there is a missing OH source. Under high NOx conditions, the model under-predicts RO2 and impacts our ability to model ozone.
Daniel Say, Alistair J. Manning, Luke M. Western, Dickon Young, Adam Wisher, Matthew Rigby, Stefan Reimann, Martin K. Vollmer, Michela Maione, Jgor Arduini, Paul B. Krummel, Jens Mühle, Christina M. Harth, Brendan Evans, Ray F. Weiss, Ronald G. Prinn, and Simon O'Doherty
Atmos. Chem. Phys., 21, 2149–2164, https://doi.org/10.5194/acp-21-2149-2021, https://doi.org/10.5194/acp-21-2149-2021, 2021
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Perfluorocarbons (PFCs) are potent greenhouse gases with exceedingly long lifetimes. We used atmospheric measurements from a global monitoring network to track the accumulation of these gases in the atmosphere. In the case of the two most abundant PFCs, recent measurements indicate that global emissions are increasing. In Europe, we used a model to estimate regional PFC emissions. Our results show that there was no significant decline in northwest European PFC emissions between 2010 and 2019.
Laura Röhler, Pernilla Bohlin-Nizzetto, Pawel Rostkowski, Roland Kallenborn, and Martin Schlabach
Atmos. Chem. Phys., 21, 1697–1716, https://doi.org/10.5194/acp-21-1697-2021, https://doi.org/10.5194/acp-21-1697-2021, 2021
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A novel non-destructive, sulfuric-acid-free clean-up method for high-volume air samples was developed and evaluated with organic chemicals covering a wide range of polarities (logP 2–11). This method, providing quantitative results of comparable quality to traditional methods, was combined with newly developed data treatment strategies for simultaneous suspect and non-target screening. The application to air samples from southern Norway revealed 90 new potential chemicals of emerging concern.
Mike J. Newland, Daniel J. Bryant, Rachel E. Dunmore, Thomas J. Bannan, W. Joe F. Acton, Ben Langford, James R. Hopkins, Freya A. Squires, William Dixon, William S. Drysdale, Peter D. Ivatt, Mathew J. Evans, Peter M. Edwards, Lisa K. Whalley, Dwayne E. Heard, Eloise J. Slater, Robert Woodward-Massey, Chunxiang Ye, Archit Mehra, Stephen D. Worrall, Asan Bacak, Hugh Coe, Carl J. Percival, C. Nicholas Hewitt, James D. Lee, Tianqu Cui, Jason D. Surratt, Xinming Wang, Alastair C. Lewis, Andrew R. Rickard, and Jacqueline F. Hamilton
Atmos. Chem. Phys., 21, 1613–1625, https://doi.org/10.5194/acp-21-1613-2021, https://doi.org/10.5194/acp-21-1613-2021, 2021
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We report the formation of secondary pollutants in the urban megacity of Beijing that are typically associated with remote regions such as rainforests. This is caused by extremely low levels of nitric oxide (NO), typically expected to be high in urban areas, observed in the afternoon. This work has significant implications for how we understand atmospheric chemistry in the urban environment and thus for how to implement effective policies to improve urban air quality.
Cécile Debevec, Stéphane Sauvage, Valérie Gros, Thérèse Salameh, Jean Sciare, François Dulac, and Nadine Locoge
Atmos. Chem. Phys., 21, 1449–1484, https://doi.org/10.5194/acp-21-1449-2021, https://doi.org/10.5194/acp-21-1449-2021, 2021
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This study provides a better characterization of the seasonal variations in VOC sources impacting the western Mediterranean region, based on a comprehensive chemical composition measured over 25 months at a representative receptor site (Ersa) and by determining factors controlling their temporal variations. Some insights into dominant drivers for VOC concentration variations in Europe are also provided, built on comparisons of Ersa observations with the concomitant ones of 17 European sites.
Christian Mark Garcia Salvador, Rongzhi Tang, Michael Priestley, Linjie Li, Epameinondas Tsiligiannis, Michael Le Breton, Wenfei Zhu, Limin Zeng, Hui Wang, Ying Yu, Min Hu, Song Guo, and Mattias Hallquist
Atmos. Chem. Phys., 21, 1389–1406, https://doi.org/10.5194/acp-21-1389-2021, https://doi.org/10.5194/acp-21-1389-2021, 2021
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High-frequency online measurement of gas- and particle-phase nitro-aromatic compounds (NACs) at a rural site in China, heavily influenced by biomass burning events, enabled the analysis of the production pathway of NACs, including an explanation of strong persistence in the daytime. The contribution of secondary processes was significant, even during the dominant wintertime influence of primary emissions, suggesting the important role of regional secondary chemistry, i.e. photochemical smog.
Shigeyuki Ishidoya, Satoshi Sugawara, Yasunori Tohjima, Daisuke Goto, Kentaro Ishijima, Yosuke Niwa, Nobuyuki Aoki, and Shohei Murayama
Atmos. Chem. Phys., 21, 1357–1373, https://doi.org/10.5194/acp-21-1357-2021, https://doi.org/10.5194/acp-21-1357-2021, 2021
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The surface Ar / N2 ratio showed not only secular increasing trends, but also interannual variations in phase with the global ocean heat content (OHC). Sensitivity test by using a two-dimensional model indicated that the secular trend in the Ar / N2 ratio is modified by the gravitational separation in the stratosphere. The analytical results imply that the surface Ar/N2 ratio is an important tracer for detecting spatiotemporally integrated changes in OHC and stratospheric circulation.
Y. Sim Tang, Chris R. Flechard, Ulrich Dämmgen, Sonja Vidic, Vesna Djuricic, Marta Mitosinkova, Hilde T. Uggerud, Maria J. Sanz, Ivan Simmons, Ulrike Dragosits, Eiko Nemitz, Marsailidh Twigg, Netty van Dijk, Yannick Fauvel, Francisco Sanz, Martin Ferm, Cinzia Perrino, Maria Catrambone, David Leaver, Christine F. Braban, J. Neil Cape, Mathew R. Heal, and Mark A. Sutton
Atmos. Chem. Phys., 21, 875–914, https://doi.org/10.5194/acp-21-875-2021, https://doi.org/10.5194/acp-21-875-2021, 2021
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The DELTA® approach provided speciated, monthly data on reactive gases (NH3, HNO3, SO2, HCl) and aerosols (NH4+, NO3−, SO42−, Cl−, Na+) across Europe (2006–2010). Differences in spatial and temporal concentrations and patterns between geographic regions and four ecosystem types were captured. NH3 and NH4NO3 were dominant components, highlighting their growing relative importance in ecosystem impacts (acidification, eutrophication) and human health effects (NH3 as a precursor to PM2.5) in Europe.
Shuo Liu, Shuangxi Fang, Peng Liu, Miao Liang, Minrui Guo, and Zhaozhong Feng
Atmos. Chem. Phys., 21, 393–413, https://doi.org/10.5194/acp-21-393-2021, https://doi.org/10.5194/acp-21-393-2021, 2021
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We analyzed 26-year CH4 measurements at Mount Waliguan in the Tibetan Plateau, China. The CH4 increased ~ 133 parts per billion (ppb) with a rate of 5.1 ± 0.1 ppb yr-1 from 1994 to 2019. Major source regions were identified in northeast and southwest. The influence of human activities is more and more serious, and northern India has possibly become a stronger contributor than city regions were in the past. It has become urgent to control CH4 emissions in the Tibetan Plateau.
Jun Zhou, Zhangwei Wang, Xiaoshan Zhang, Charles T. Driscoll, and Che-Jen Lin
Atmos. Chem. Phys., 20, 16117–16133, https://doi.org/10.5194/acp-20-16117-2020, https://doi.org/10.5194/acp-20-16117-2020, 2020
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Mercury (Hg) emissions from natural resources have a large uncertainty, which is mainly derived from the forest. A long-term and multiplot (10) study of soil–air fluxes at subtropical and temperate forests was conducted. Forest soils are an important atmospheric Hg source, especially for subtropical forests. The compensation points imply that the atmospheric Hg concentration plays a critical role in inhibiting Hg emissions from the forest floor. Climate change can enhance soil Hg emissions.
Yijing Chen, Qianli Ma, Weili Lin, Xiaobin Xu, Jie Yao, and Wei Gao
Atmos. Chem. Phys., 20, 15969–15982, https://doi.org/10.5194/acp-20-15969-2020, https://doi.org/10.5194/acp-20-15969-2020, 2020
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CO is one of the major air pollutants. Our study showed that the long-term CO levels at a background station in one of the most developed areas of China decreased significantly and verified that this downward trend was attributed to the decrease in anthropogenic emissions, which indicated that the adopted pollution control policies were effective. Also, this decrease has an implication for the atmospheric chemistry considering the negative correlation between CO levels and OH radical's lifetime.
James D. Lee, Will S. Drysdale, Doug P. Finch, Shona E. Wilde, and Paul I. Palmer
Atmos. Chem. Phys., 20, 15743–15759, https://doi.org/10.5194/acp-20-15743-2020, https://doi.org/10.5194/acp-20-15743-2020, 2020
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Efforts to prevent the COVID-19 virus spreading across the globe have included travel restrictions and the closure of workplaces, leading to a significant drop in emissions of primary air pollutants. This provides for a unique opportunity to examine how air pollutant concentrations respond to an abrupt and prolonged reduction. We examine how NO2 and O3 have been affected at several urban measurement sites in the UK. We look at the change in NO2 compared to previous years and the effect on O3.
Patrick A. Barker, Grant Allen, Martin Gallagher, Joseph R. Pitt, Rebecca E. Fisher, Thomas Bannan, Euan G. Nisbet, Stéphane J.-B. Bauguitte, Dominika Pasternak, Samuel Cliff, Marina B. Schimpf, Archit Mehra, Keith N. Bower, James D. Lee, Hugh Coe, and Carl J. Percival
Atmos. Chem. Phys., 20, 15443–15459, https://doi.org/10.5194/acp-20-15443-2020, https://doi.org/10.5194/acp-20-15443-2020, 2020
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Africa is estimated to account for approximately 52 % of global biomass burning (BB) carbon emissions. Despite this, there has been little previous in situ study of African BB emissions. This work presents BB emission factors for various atmospheric trace gases sampled from an aircraft in two distinct areas of Africa (Senegal and Uganda). Intracontinental variability in biomass burning methane emission is identified, which is attributed to difference in the specific fuel mixtures burnt.
W. Joe F. Acton, Zhonghui Huang, Brian Davison, Will S. Drysdale, Pingqing Fu, Michael Hollaway, Ben Langford, James Lee, Yanhui Liu, Stefan Metzger, Neil Mullinger, Eiko Nemitz, Claire E. Reeves, Freya A. Squires, Adam R. Vaughan, Xinming Wang, Zhaoyi Wang, Oliver Wild, Qiang Zhang, Yanli Zhang, and C. Nicholas Hewitt
Atmos. Chem. Phys., 20, 15101–15125, https://doi.org/10.5194/acp-20-15101-2020, https://doi.org/10.5194/acp-20-15101-2020, 2020
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Air quality in Beijing is of concern to both policy makers and the general public. In order to address concerns about air quality it is vital that the sources of atmospheric pollutants are understood. This work presents the first top-down measurement of volatile organic compound (VOC) emissions in Beijing. These measurements are used to evaluate the emissions inventory and assess the impact of VOC emission from the city centre on atmospheric chemistry.
Eloise J. Slater, Lisa K. Whalley, Robert Woodward-Massey, Chunxiang Ye, James D. Lee, Freya Squires, James R. Hopkins, Rachel E. Dunmore, Marvin Shaw, Jacqueline F. Hamilton, Alastair C. Lewis, Leigh R. Crilley, Louisa Kramer, William Bloss, Tuan Vu, Yele Sun, Weiqi Xu, Siyao Yue, Lujie Ren, W. Joe F. Acton, C. Nicholas Hewitt, Xinming Wang, Pingqing Fu, and Dwayne E. Heard
Atmos. Chem. Phys., 20, 14847–14871, https://doi.org/10.5194/acp-20-14847-2020, https://doi.org/10.5194/acp-20-14847-2020, 2020
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The paper details atmospheric chemistry in a megacity (Beijing), focussing on radicals which mediate the formation of secondary pollutants such as ozone and particles. Highly polluted conditions were experienced, including the highest ever levels of nitric oxide (NO), with simultaneous radical measurements. Radical concentrations were large during "haze" events, demonstrating active photochemistry. Modelling showed that our understanding of the chemistry at high NOx levels is incomplete.
Caihong Wu, Chaomin Wang, Sihang Wang, Wenjie Wang, Bin Yuan, Jipeng Qi, Baolin Wang, Hongli Wang, Chen Wang, Wei Song, Xinming Wang, Weiwei Hu, Shengrong Lou, Chenshuo Ye, Yuwen Peng, Zelong Wang, Yibo Huangfu, Yan Xie, Manni Zhu, Junyu Zheng, Xuemei Wang, Bin Jiang, Zhanyi Zhang, and Min Shao
Atmos. Chem. Phys., 20, 14769–14785, https://doi.org/10.5194/acp-20-14769-2020, https://doi.org/10.5194/acp-20-14769-2020, 2020
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Based on measurements from an online mass spectrometer, we quantify volatile organic compound (VOC) concentrations from numerous ions of the mass spectrometer, using information from laboratory-obtained calibration results. We find that most VOC concentrations are from oxygenated VOCs (OVOCs). We further show that these OVOCs also contribute significantly to OH reactivity. Our results suggest the important role of OVOCs in VOC emissions and chemistry in urban air.
Bert Verreyken, Crist Amelynck, Jérôme Brioude, Jean-François Müller, Niels Schoon, Nicolas Kumps, Aurélie Colomb, Jean-Marc Metzger, Christopher F. Lee, Theodore K. Koenig, Rainer Volkamer, and Trissevgeni Stavrakou
Atmos. Chem. Phys., 20, 14821–14845, https://doi.org/10.5194/acp-20-14821-2020, https://doi.org/10.5194/acp-20-14821-2020, 2020
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Biomass burning (BB) plumes arriving at the Maïdo observatory located in the south-west Indian Ocean during August 2018 and August 2019 are studied using trace gas measurements, Lagrangian transport models and the CAMS near-real-time atmospheric composition service. We investigate (i) secondary production of volatile organic compounds during transport, (ii) efficacy of the CAMS model to reproduce the chemical makeup of BB plumes and (iii) the impact of BB on the remote marine boundary layer.
Geoffrey C. Toon, Jean-Francois L. Blavier, Keeyoon Sung, and Katelyn Yu
Atmos. Chem. Phys. Discuss., https://doi.org/10.5194/acp-2020-1135, https://doi.org/10.5194/acp-2020-1135, 2020
Revised manuscript accepted for ACP
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We report measurements of atmospheric propane (C3H8) from analysis of ground-based, infra-red solar absorption spectra measured from various sites. These measurements suggest that exploitation of natural gas fields is a major and growing source of propane in the USA. Also, there seem to be propane sources in large cities such as Los Angeles, possibly related to use of liquified petroleum gas (LPG).
Sarah E. Benish, Hao He, Xinrong Ren, Sandra J. Roberts, Ross J. Salawitch, Zhanqing Li, Fei Wang, Yuying Wang, Fang Zhang, Min Shao, Sihua Lu, and Russell R. Dickerson
Atmos. Chem. Phys., 20, 14523–14545, https://doi.org/10.5194/acp-20-14523-2020, https://doi.org/10.5194/acp-20-14523-2020, 2020
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Airborne observations of ozone and related pollutants show smog was pervasive in spring 2016 over Hebei Province, China. We find high amounts of ozone precursors throughout and even above the PBL, continuing to generate ozone at high rates to be potentially transported downwind. Concentrations even in the rural areas of this highly industrialized province promote widespread ozone production, and we show that to improve air quality over Hebei both NOx and VOCs should be targeted.
Yixuan Gu, Fengxia Yan, Jianming Xu, Yuanhao Qu, Wei Gao, Fangfang He, and Hong Liao
Atmos. Chem. Phys., 20, 14361–14375, https://doi.org/10.5194/acp-20-14361-2020, https://doi.org/10.5194/acp-20-14361-2020, 2020
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High levels and statistically insignificant changes of ozone are detected at a remote monitoring site on Sheshan Island in Shanghai, China, from 2012 to 2017; 6-year observations suggest regional transport exerted minimum influence on the offshore oceanic air in September and October. Both city plumes and oceanic air inflows could contribute to ozone enhancements in Shanghai, and the latter are found to lead to 20–30 % increases in urban ozone concentrations based on WRF-Chem simulations.
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Short summary
The highest mercury (Hg) wet deposition in USA occurs along the Gulf of Mexico. Gaseous oxidized Hg (GOM) is a major contributor due to high water solubility and reactivity. Concentration and dry deposition of GOM were determined for OLF, Florida. Results indicated at least 5 GOM compounds in this area including HgBr2, HgO, and Hg–nitrogen and –sulfur forms. GOM chemistry indicates reactions with local mobile source pollutants and long-range transport from outside of the USA.
The highest mercury (Hg) wet deposition in USA occurs along the Gulf of Mexico. Gaseous oxidized...
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