Articles | Volume 22, issue 12
https://doi.org/10.5194/acp-22-8343-2022
© Author(s) 2022. 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-22-8343-2022
© Author(s) 2022. This work is distributed under
the Creative Commons Attribution 4.0 License.
the Creative Commons Attribution 4.0 License.
A new assessment of global and regional budgets, fluxes, and lifetimes of atmospheric reactive N and S gases and aerosols
School of Chemistry, University of Edinburgh, Joseph Black Building,
David Brewster Road, Edinburgh EH9 3FJ, UK
UK Centre for Ecology & Hydrology, Bush Estate, Penicuik,
Midlothian EH26 0QB, UK
Massimo Vieno
UK Centre for Ecology & Hydrology, Bush Estate, Penicuik,
Midlothian EH26 0QB, UK
David S. Stevenson
School of GeoSciences, University of Edinburgh, Crew Building,
Alexander Crum Brown Road, Edinburgh EH9 3FF, UK
Peter Wind
The Norwegian Meteorological Institute, Henrik Mohns Plass 1, 0313
Oslo, Norway
School of Chemistry, University of Edinburgh, Joseph Black Building,
David Brewster Road, Edinburgh EH9 3FJ, UK
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Atmospheric volatile organic compounds (VOCs) constitute many species, acting as precursors to ozone and aerosol. Given the uncertainties in VOC emissions, lack of evaluation studies, and recent changes in emissions, this work adapts the EMEP MSC-W to evaluate emission inventories in Europe. We focus on the varying agreement between modelled and measured VOCs across different species and underscore potential inaccuracies in total and sector-specific emission estimates.
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Radiation coming from the sun is essential to atmospheric chemistry, driving the breakup, or photodissociation, of atmospheric molecules. This in turn affects the chemical composition and reactivity of the atmosphere. The representation of photodissociation effects is therefore essential in atmospheric chemistry modeling. One such model is the EMEP MSC-W model, for which a new way of calculating the photodissociation rates is tested and evaluated in this paper.
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The sensitivity of fine particles and reactive N and S species to reductions in precursor emissions is investigated using the EMEP MSC-W (European Monitoring and Evaluation Programme Meteorological Synthesizing Centre – West) atmospheric chemistry transport model. This study reveals that the individual emissions reduction has multiple and geographically varying co-benefits and small disbenefits on different species, demonstrating the importance of prioritizing regional emissions controls.
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This study reports the first evaluation of the global EMEP MSC-W ACTM driven by WRF meteorology, with a focus on surface concentrations and wet deposition of reactive N and S species. The model–measurement comparison is conducted both spatially and temporally, covering 10 monitoring networks worldwide. The statistics from the comprehensive evaluations presented in this study support the application of this model framework for global analysis of the budgets and fluxes of reactive N and SIA.
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This paper presents a numerical method to assess the origin of air pollution. Combined with a numerical air pollution transport and chemistry model, it can follow the contributions from a large number of emission sources. The result is a series of maps that give the relative contributions from, for example, all European countries at any point on the map.
Xu-Cheng He, Nathan Luke Abraham, Han Ding, Maria R. Russo, Daniel P. Grosvenor, Yao Ge, Xuemei Wang, Anthony C. Jones, Pedro Campuzano-Jost, Benjamin Nault, Agnieszka Kupc, Donald Blake, Jose L. Jimenez, Christina J. Williamson, Kenneth S. Carslaw, James Weber, Alexander T. Archibald, and Hamish Gordon
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Aerosols affect clouds and climate. However, current climate models still struggle to simulate them accurately. We used aircraft data from a global mission to evaluate how well the UK Earth System Model represents aerosols and their precursors. Our results show that the model misses key formation processes in clean ocean regions, suggesting that future improvements should focus on better representing how aerosols form naturally in the atmosphere.
Jize Jiang, David S. Stevenson, Aimable Uwizeye, Giuseppe Tempio, Alessandra Falcucci, Flavia Casu, and Mark A. Sutton
Geosci. Model Dev., 18, 5051–5099, https://doi.org/10.5194/gmd-18-5051-2025, https://doi.org/10.5194/gmd-18-5051-2025, 2025
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A special model called AMmonia–CLIMate (AMCLIM) has been developed to understand and calculate NH3 emissions from livestock farming. It is estimated that about 30 % of excreted N from livestock is lost due to NH3 emissions from housing, manure management and land application of manure. High NH3 volatilization often occurs in hot regions, while poor management practices also result in significant N losses through NH3 emissions.
Alexander K. Tardito Chaudhri and David S. Stevenson
Atmos. Chem. Phys., 25, 7369–7385, https://doi.org/10.5194/acp-25-7369-2025, https://doi.org/10.5194/acp-25-7369-2025, 2025
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There remains a large uncertainty in the global warming potential of atmospheric hydrogen due to poor constraints on its soil deposition and, therefore, its lifetime. A new analysis of the latitudinal variation in the observed seasonality of hydrogen is used to constrain its surface fluxes. This is complemented with a simple latitude–height model where surface fluxes are adjusted from a prototype deposition scheme.
Alok K. Pandey, David S. Stevenson, Alcide Zhao, Richard J. Pope, Ryan Hossaini, Krishan Kumar, and Martyn P. Chipperfield
Atmos. Chem. Phys., 25, 4785–4802, https://doi.org/10.5194/acp-25-4785-2025, https://doi.org/10.5194/acp-25-4785-2025, 2025
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Nitrogen dioxide is an air pollutant largely controlled by human activity that affects ozone, methane, and aerosols. Satellite instruments can quantify column NO2 and, by carefully matching the time and location of measurements, enable evaluation of model simulations. NO2 over south and east Asia is assessed, showing that the model captures not only many features of the measurements, but also important differences that suggest model deficiencies in representing several aspects of the atmospheric chemistry of NO2.
Jize Jiang, David S. Stevenson, and Mark A. Sutton
Geosci. Model Dev., 17, 8181–8222, https://doi.org/10.5194/gmd-17-8181-2024, https://doi.org/10.5194/gmd-17-8181-2024, 2024
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A special model called AMmonia–CLIMate (AMCLIM) has been developed to understand and calculate NH3 emissions from fertilizer use and also taking into account how the environment influences these NH3 emissions. It is estimated that about 17 % of applied N in fertilizers was lost due to NH3 emissions. Hot and dry conditions and regions with high-pH soils can expect higher NH3 emissions.
Yao Ge, Sverre Solberg, Mathew R. Heal, Stefan Reimann, Willem van Caspel, Bryan Hellack, Thérèse Salameh, and David Simpson
Atmos. Chem. Phys., 24, 7699–7729, https://doi.org/10.5194/acp-24-7699-2024, https://doi.org/10.5194/acp-24-7699-2024, 2024
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Atmospheric volatile organic compounds (VOCs) constitute many species, acting as precursors to ozone and aerosol. Given the uncertainties in VOC emissions, lack of evaluation studies, and recent changes in emissions, this work adapts the EMEP MSC-W to evaluate emission inventories in Europe. We focus on the varying agreement between modelled and measured VOCs across different species and underscore potential inaccuracies in total and sector-specific emission estimates.
Lily Gouldsbrough, Ryan Hossaini, Emma Eastoe, Paul J. Young, and Massimo Vieno
Atmos. Chem. Phys., 24, 3163–3196, https://doi.org/10.5194/acp-24-3163-2024, https://doi.org/10.5194/acp-24-3163-2024, 2024
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High-resolution spatial fields of surface ozone are used to understand spikes in ozone concentration and predict their impact on public health. Such fields are routinely output from complex mathematical models for atmospheric conditions. These outputs are on a coarse spatial resolution and the highest concentrations tend to be biased. Using a novel data-driven machine learning methodology, we show how such output can be corrected to produce fields with both lower bias and higher resolution.
Prerita Agarwal, David S. Stevenson, and Mathew R. Heal
Atmos. Chem. Phys., 24, 2239–2266, https://doi.org/10.5194/acp-24-2239-2024, https://doi.org/10.5194/acp-24-2239-2024, 2024
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Air pollution levels across northern India are amongst some of the worst in the world, with episodic and hazardous haze events. Here, the ability of the WRF-Chem model to predict air quality over northern India is assessed against several datasets. Whilst surface wind speed and particle pollution peaks are over- and underestimated, respectively, meteorology and aerosol trends are adequately captured, and we conclude it is suitable for investigating severe particle pollution events.
Willem E. van Caspel, David Simpson, Jan Eiof Jonson, Anna M. K. Benedictow, Yao Ge, Alcide di Sarra, Giandomenico Pace, Massimo Vieno, Hannah L. Walker, and Mathew R. Heal
Geosci. Model Dev., 16, 7433–7459, https://doi.org/10.5194/gmd-16-7433-2023, https://doi.org/10.5194/gmd-16-7433-2023, 2023
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Radiation coming from the sun is essential to atmospheric chemistry, driving the breakup, or photodissociation, of atmospheric molecules. This in turn affects the chemical composition and reactivity of the atmosphere. The representation of photodissociation effects is therefore essential in atmospheric chemistry modeling. One such model is the EMEP MSC-W model, for which a new way of calculating the photodissociation rates is tested and evaluated in this paper.
Gemma Purser, Mathew R. Heal, Edward J. Carnell, Stephen Bathgate, Julia Drewer, James I. L. Morison, and Massimo Vieno
Atmos. Chem. Phys., 23, 13713–13733, https://doi.org/10.5194/acp-23-13713-2023, https://doi.org/10.5194/acp-23-13713-2023, 2023
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Forest expansion is a ″net-zero“ pathway, but change in land cover alters air quality in many ways. This study combines tree planting suitability data with UK measured emissions of biogenic volatile organic compounds to simulate spatial and temporal changes in atmospheric composition for planting scenarios of four species. Decreases in fine particulate matter are relatively larger than increases in ozone, which may indicate a net benefit of tree planting on human health aspects of air quality.
Yao Ge, Massimo Vieno, David S. Stevenson, Peter Wind, and Mathew R. Heal
Atmos. Chem. Phys., 23, 6083–6112, https://doi.org/10.5194/acp-23-6083-2023, https://doi.org/10.5194/acp-23-6083-2023, 2023
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The sensitivity of fine particles and reactive N and S species to reductions in precursor emissions is investigated using the EMEP MSC-W (European Monitoring and Evaluation Programme Meteorological Synthesizing Centre – West) atmospheric chemistry transport model. This study reveals that the individual emissions reduction has multiple and geographically varying co-benefits and small disbenefits on different species, demonstrating the importance of prioritizing regional emissions controls.
David S. Stevenson, Richard G. Derwent, Oliver Wild, and William J. Collins
Atmos. Chem. Phys., 22, 14243–14252, https://doi.org/10.5194/acp-22-14243-2022, https://doi.org/10.5194/acp-22-14243-2022, 2022
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Atmospheric methane’s growth rate rose by 50 % in 2020 relative to 2019. Lower nitrogen oxide (NOx) emissions tend to increase methane’s atmospheric residence time; lower carbon monoxide (CO) and non-methane volatile organic compound (NMVOC) emissions decrease its lifetime. Combining model sensitivities with emission changes, we find that COVID-19 lockdown emission reductions can explain over half the observed increases in methane in 2020.
Svetlana Tsyro, Wenche Aas, Augustin Colette, Camilla Andersson, Bertrand Bessagnet, Giancarlo Ciarelli, Florian Couvidat, Kees Cuvelier, Astrid Manders, Kathleen Mar, Mihaela Mircea, Noelia Otero, Maria-Teresa Pay, Valentin Raffort, Yelva Roustan, Mark R. Theobald, Marta G. Vivanco, Hilde Fagerli, Peter Wind, Gino Briganti, Andrea Cappelletti, Massimo D'Isidoro, and Mario Adani
Atmos. Chem. Phys., 22, 7207–7257, https://doi.org/10.5194/acp-22-7207-2022, https://doi.org/10.5194/acp-22-7207-2022, 2022
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Particulate matter (PM) air pollution causes adverse health effects. In Europe, the emissions caused by anthropogenic activities have been reduced in the last decades. To assess the efficiency of emission reductions in improving air quality, we have studied the evolution of PM pollution in Europe. Simulations with six air quality models and observational data indicate a decrease in PM concentrations by 10 % to 30 % across Europe from 2000 to 2010, which is mainly a result of emission reductions.
Fanlei Meng, Yibo Zhang, Jiahui Kang, Mathew R. Heal, Stefan Reis, Mengru Wang, Lei Liu, Kai Wang, Shaocai Yu, Pengfei Li, Jing Wei, Yong Hou, Ying Zhang, Xuejun Liu, Zhenling Cui, Wen Xu, and Fusuo Zhang
Atmos. Chem. Phys., 22, 6291–6308, https://doi.org/10.5194/acp-22-6291-2022, https://doi.org/10.5194/acp-22-6291-2022, 2022
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PM2.5 pollution is a pressing environmental issue threatening human health and food security globally. We combined a meta-analysis of nationwide measurements and air quality modeling to identify efficiency gains by striking a balance between controlling NH3 and acid gas emissions. Persistent secondary inorganic aerosol pollution in China is limited by acid gas emissions, while an additional control on NH3 emissions would become more important as reductions in SO2 and NOx emissions progress.
Yao Ge, Mathew R. Heal, David S. Stevenson, Peter Wind, and Massimo Vieno
Geosci. Model Dev., 14, 7021–7046, https://doi.org/10.5194/gmd-14-7021-2021, https://doi.org/10.5194/gmd-14-7021-2021, 2021
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This study reports the first evaluation of the global EMEP MSC-W ACTM driven by WRF meteorology, with a focus on surface concentrations and wet deposition of reactive N and S species. The model–measurement comparison is conducted both spatially and temporally, covering 10 monitoring networks worldwide. The statistics from the comprehensive evaluations presented in this study support the application of this model framework for global analysis of the budgets and fluxes of reactive N and SIA.
Ernesto Reyes-Villegas, Upasana Panda, Eoghan Darbyshire, James M. Cash, Rutambhara Joshi, Ben Langford, Chiara F. Di Marco, Neil J. Mullinger, Mohammed S. Alam, Leigh R. Crilley, Daniel J. Rooney, W. Joe F. Acton, Will Drysdale, Eiko Nemitz, Michael Flynn, Aristeidis Voliotis, Gordon McFiggans, Hugh Coe, James Lee, C. Nicholas Hewitt, Mathew R. Heal, Sachin S. Gunthe, Tuhin K. Mandal, Bhola R. Gurjar, Shivani, Ranu Gadi, Siddhartha Singh, Vijay Soni, and James D. Allan
Atmos. Chem. Phys., 21, 11655–11667, https://doi.org/10.5194/acp-21-11655-2021, https://doi.org/10.5194/acp-21-11655-2021, 2021
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This paper shows the first multisite online measurements of PM1 in Delhi, India, with measurements over different seasons in Old Delhi and New Delhi in 2018. Organic aerosol (OA) source apportionment was performed using positive matrix factorisation (PMF). Traffic was the main primary aerosol source for both OAs and black carbon, seen with PMF and Aethalometer model analysis, indicating that control of primary traffic exhaust emissions would make a significant reduction to Delhi air pollution.
James M. Cash, Ben Langford, Chiara Di Marco, Neil J. Mullinger, James Allan, Ernesto Reyes-Villegas, Ruthambara Joshi, Mathew R. Heal, W. Joe F. Acton, C. Nicholas Hewitt, Pawel K. Misztal, Will Drysdale, Tuhin K. Mandal, Shivani, Ranu Gadi, Bhola Ram Gurjar, and Eiko Nemitz
Atmos. Chem. Phys., 21, 10133–10158, https://doi.org/10.5194/acp-21-10133-2021, https://doi.org/10.5194/acp-21-10133-2021, 2021
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We present the first real-time composition of submicron particulate matter (PM1) in Old Delhi using high-resolution aerosol mass spectrometry. Seasonal analysis shows peak concentrations occur during the post-monsoon, and novel-tracers reveal the largest sources are a combination of local open and regional crop residue burning. Strong links between increased chloride aerosol concentrations and burning sources of PM1 suggest burning sources are responsible for the post-monsoon chloride peak.
Robbie Ramsay, Chiara F. Di Marco, Mathew R. Heal, Matthias Sörgel, Paulo Artaxo, Meinrat O. Andreae, and Eiko Nemitz
Biogeosciences, 18, 2809–2825, https://doi.org/10.5194/bg-18-2809-2021, https://doi.org/10.5194/bg-18-2809-2021, 2021
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The exchange of the gas ammonia between the atmosphere and the surface is an important biogeochemical process, but little is known of this exchange for certain ecosystems, such as the Amazon rainforest. This study took measurements of ammonia exchange over an Amazon rainforest site and subsequently modelled the observed deposition and emission patterns. We observed emissions of ammonia from the rainforest, which can be simulated accurately by using a canopy resistance modelling approach.
Gemma Purser, Julia Drewer, Mathew R. Heal, Robert A. S. Sircus, Lara K. Dunn, and James I. L. Morison
Biogeosciences, 18, 2487–2510, https://doi.org/10.5194/bg-18-2487-2021, https://doi.org/10.5194/bg-18-2487-2021, 2021
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Short-rotation forest plantations could help reduce greenhouse gases but can emit biogenic volatile organic compounds. Emissions were measured at a plantation trial in Scotland. Standardised emissions of isoprene from foliage were higher from hybrid aspen than from Sitka spruce and low from Italian alder. Emissions of total monoterpene were lower. The forest floor was only a small source. Model estimates suggest an SRF expansion of 0.7 Mha could increase total UK emissions between < 1 %–35 %.
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.
Jize Jiang, David S. Stevenson, Aimable Uwizeye, Giuseppe Tempio, and Mark A. Sutton
Biogeosciences, 18, 135–158, https://doi.org/10.5194/bg-18-135-2021, https://doi.org/10.5194/bg-18-135-2021, 2021
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Ammonia is a key water and air pollutant and impacts human health and climate change. Ammonia emissions mainly originate from agriculture. We find that chicken agriculture contributes to large ammonia emissions, especially in hot and wet regions. These emissions can be greatly affected by the local environment, i.e. temperature and humidity, and also by human management. We develop a model that suggests ammonia emissions from chicken farming are likely to increase under a warming climate.
Robbie Ramsay, Chiara F. Di Marco, Matthias Sörgel, Mathew R. Heal, Samara Carbone, Paulo Artaxo, Alessandro C. de Araùjo, Marta Sá, Christopher Pöhlker, Jost Lavric, Meinrat O. Andreae, and Eiko Nemitz
Atmos. Chem. Phys., 20, 15551–15584, https://doi.org/10.5194/acp-20-15551-2020, https://doi.org/10.5194/acp-20-15551-2020, 2020
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The Amazon rainforest is a unique
laboratoryto study the processes which govern the exchange of gases and aerosols to and from the atmosphere. This study investigated these processes by measuring the atmospheric concentrations of trace gases and particles at the Amazon Tall Tower Observatory. We found that the long-range transport of pollutants can affect the atmospheric composition above the Amazon rainforest and that the gases ammonia and nitrous acid can be emitted from the rainforest.
Bruce Rolstad Denby, Michael Gauss, Peter Wind, Qing Mu, Eivind Grøtting Wærsted, Hilde Fagerli, Alvaro Valdebenito, and Heiko Klein
Geosci. Model Dev., 13, 6303–6323, https://doi.org/10.5194/gmd-13-6303-2020, https://doi.org/10.5194/gmd-13-6303-2020, 2020
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Air pollution is both a local and a global problem. Since measurements cannot be made everywhere, mathematical models are used to calculate air quality over cities or countries. Modelling over countries limits the level of detail of the models. For countries, the level of detail is only a few kilometres, so air quality at kerb sides is not properly represented. The uEMEP model is used together with the regional air quality model EMEP MSC-W to model details down to kerb side for all of Norway.
David S. Stevenson, Alcide Zhao, Vaishali Naik, Fiona M. O'Connor, Simone Tilmes, Guang Zeng, Lee T. Murray, William J. Collins, Paul T. Griffiths, Sungbo Shim, Larry W. Horowitz, Lori T. Sentman, and Louisa Emmons
Atmos. Chem. Phys., 20, 12905–12920, https://doi.org/10.5194/acp-20-12905-2020, https://doi.org/10.5194/acp-20-12905-2020, 2020
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We present historical trends in atmospheric oxidizing capacity (OC) since 1850 from the latest generation of global climate models and compare these with estimates from measurements. OC controls levels of many key reactive gases, including methane (CH4). We find small model trends up to 1980, then increases of about 9 % up to 2014, disagreeing with (uncertain) measurement-based trends. Major drivers of OC trends are emissions of CH4, NOx, and CO; these will be important for future CH4 trends.
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Short summary
Reactive N and S gases and aerosols are critical determinants of air quality. We report a comprehensive analysis of the concentrations, wet and dry deposition, fluxes, and lifetimes of these species globally as well as for 10 world regions. We used the EMEP MSC-W model coupled with WRF meteorology and 2015 global emissions. Our work demonstrates the substantial regional variation in these quantities and the need for modelling to simulate atmospheric responses to precursor emissions.
Reactive N and S gases and aerosols are critical determinants of air quality. We report a...
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