Articles | Volume 21, issue 19
https://doi.org/10.5194/acp-21-15283-2021
© 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-21-15283-2021
© Author(s) 2021. This work is distributed under
the Creative Commons Attribution 4.0 License.
the Creative Commons Attribution 4.0 License.
Research article
| 
14 Oct 2021
Research article |
| 14 Oct 2021
| 14 Oct 2021
Spatially and temporally resolved measurements of NOx fluxes by airborne eddy covariance over Greater London
Wolfson Atmospheric Chemistry Laboratories, Department of Chemistry, University of York, York, YO10 5DD, UK
James D. Lee
Wolfson Atmospheric Chemistry Laboratories, Department of Chemistry, University of York, York, YO10 5DD, UK
National Centre for Atmospheric Science, University of York, York,
YO10 5DD, UK
Stefan Metzger
Battelle, National Ecological Observatory Network, 1685 38th Street, Boulder, CO 80301, USA
Department of Atmospheric and Oceanic Sciences, University of
Wisconsin-Madison, 1225 West Dayton Street, Madison, WI 53706, USA
David Durden
Battelle, National Ecological Observatory Network, 1685 38th Street, Boulder, CO 80301, USA
Alastair C. Lewis
Wolfson Atmospheric Chemistry Laboratories, Department of Chemistry, University of York, York, YO10 5DD, UK
National Centre for Atmospheric Science, University of York, York,
YO10 5DD, UK
Marvin D. Shaw
Wolfson Atmospheric Chemistry Laboratories, Department of Chemistry, University of York, York, YO10 5DD, UK
National Centre for Atmospheric Science, University of York, York,
YO10 5DD, UK
Will S. Drysdale
Wolfson Atmospheric Chemistry Laboratories, Department of Chemistry, University of York, York, YO10 5DD, UK
National Centre for Atmospheric Science, University of York, York,
YO10 5DD, UK
Ruth M. Purvis
Wolfson Atmospheric Chemistry Laboratories, Department of Chemistry, University of York, York, YO10 5DD, UK
National Centre for Atmospheric Science, University of York, York,
YO10 5DD, UK
Brian Davison
Lancaster Environment Centre, Lancaster University, Lancaster, UK
C. Nicholas Hewitt
Lancaster Environment Centre, Lancaster University, Lancaster, UK
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Matthew J. Rowlinson, Mat J. Evans, Lucy J. Carpenter, Katie A. Read, Shalini Punjabi, Adedayo Adedeji, Luke Fakes, Ally Lewis, Ben Richmond, Neil Passant, Tim Murrells, Barron Henderson, Kelvin H. Bates, and Detlev Helmig
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Jianghao Li, Alastair C. Lewis, Jim R. Hopkins, Stephen J. Andrews, Tim Murrells, Neil Passant, Ben Richmond, Siqi Hou, William J. Bloss, Roy M. Harrison, and Zongbo Shi
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Changxing Lan, Matthias Mauder, Stavros Stagakis, Benjamin Loubet, Claudio D'Onofrio, Stefan Metzger, David Durden, and Pedro-Henrique Herig-Coimbra
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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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Xuewei Hou, Oliver Wild, Bin Zhu, and James Lee
Atmos. Chem. Phys., 23, 15395–15411, https://doi.org/10.5194/acp-23-15395-2023, https://doi.org/10.5194/acp-23-15395-2023, 2023
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In response to the climate crisis, many countries have committed to net zero in a certain future year. The impacts of net-zero scenarios on tropospheric O3 are less well studied and remain unclear. In this study, we quantified the changes of tropospheric O3 budgets, spatiotemporal distributions of future surface O3 in east Asia and regional O3 source contributions for 2060 under a net-zero scenario using the NCAR Community Earth System Model (CESM) and online O3-tagging methods.
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.
Danica L. Lombardozzi, William R. Wieder, Negin Sobhani, Gordon B. Bonan, David Durden, Dawn Lenz, Michael SanClements, Samantha Weintraub-Leff, Edward Ayres, Christopher R. Florian, Kyla Dahlin, Sanjiv Kumar, Abigail L. S. Swann, Claire M. Zarakas, Charles Vardeman, and Valerio Pascucci
Geosci. Model Dev., 16, 5979–6000, https://doi.org/10.5194/gmd-16-5979-2023, https://doi.org/10.5194/gmd-16-5979-2023, 2023
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We present a novel cyberinfrastructure system that uses National Ecological Observatory Network measurements to run Community Terrestrial System Model point simulations in a containerized system. The simple interface and tutorials expand access to data and models used in Earth system research by removing technical barriers and facilitating research, educational opportunities, and community engagement. The NCAR–NEON system enables convergence of climate and ecological sciences.
Adedayo R. Adedeji, Stephen J. Andrews, Matthew J. Rowlinson, Mathew J. Evans, Alastair C. Lewis, Shigeru Hashimoto, Hitoshi Mukai, Hiroshi Tanimoto, Yasunori Tohjima, and Takuya Saito
Atmos. Chem. Phys., 23, 9229–9244, https://doi.org/10.5194/acp-23-9229-2023, https://doi.org/10.5194/acp-23-9229-2023, 2023
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We use the GEOS-Chem model to interpret observations of CO, C2H6, C3H8, NOx, NOy and O3 made from Hateruma Island in 2018. The model captures many synoptic-scale events and the seasonality of most pollutants at the site but underestimates C2H6 and C3H8 during the winter. These underestimates are unlikely to be reconciled by increases in biomass burning emissions but could be reconciled by increasing the Asian anthropogenic source of C2H6 and C3H8 by factors of around 2 and 3, respectively.
Joanna E. Dyson, Lisa K. Whalley, Eloise J. Slater, Robert Woodward-Massey, Chunxiang Ye, James D. Lee, Freya Squires, James R. Hopkins, Rachel E. Dunmore, Marvin Shaw, Jacqueline F. Hamilton, Alastair C. Lewis, Stephen D. Worrall, Asan Bacak, Archit Mehra, Thomas J. Bannan, Hugh Coe, Carl J. Percival, Bin Ouyang, C. Nicholas Hewitt, Roderic L. Jones, Leigh R. Crilley, Louisa J. Kramer, W. Joe F. Acton, William J. Bloss, Supattarachai Saksakulkrai, Jingsha Xu, Zongbo Shi, Roy M. Harrison, Simone Kotthaus, Sue Grimmond, Yele Sun, Weiqi Xu, Siyao Yue, Lianfang Wei, Pingqing Fu, Xinming Wang, Stephen R. Arnold, and Dwayne E. Heard
Atmos. Chem. Phys., 23, 5679–5697, https://doi.org/10.5194/acp-23-5679-2023, https://doi.org/10.5194/acp-23-5679-2023, 2023
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The hydroxyl (OH) and closely coupled hydroperoxyl (HO2) radicals are vital for their role in the removal of atmospheric pollutants. In less polluted regions, atmospheric models over-predict HO2 concentrations. In this modelling study, the impact of heterogeneous uptake of HO2 onto aerosol surfaces on radical concentrations and the ozone production regime in Beijing in the summertime is investigated, and the implications for emissions policies across China are considered.
Samuel J. Cliff, Will Drysdale, James D. Lee, Carole Helfter, Eiko Nemitz, Stefan Metzger, and Janet F. Barlow
Atmos. Chem. Phys., 23, 2315–2330, https://doi.org/10.5194/acp-23-2315-2023, https://doi.org/10.5194/acp-23-2315-2023, 2023
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Emissions of nitrogen oxides (NOx) to the atmosphere are an ongoing air quality issue. This study directly measures emissions of NOx and carbon dioxide from a tall tower in central London during the coronavirus pandemic. It was found that transport NOx emissions had reduced by >73 % since 2017 as a result of air quality policy and reduced congestion during coronavirus restrictions. During this period, central London was thought to be dominated by point-source heat and power generation emissions.
Jacob T. Shaw, Amy Foulds, Shona Wilde, Patrick Barker, Freya A. Squires, James Lee, Ruth Purvis, Ralph Burton, Ioana Colfescu, Stephen Mobbs, Samuel Cliff, Stéphane J.-B. Bauguitte, Stuart Young, Stefan Schwietzke, and Grant Allen
Atmos. Chem. Phys., 23, 1491–1509, https://doi.org/10.5194/acp-23-1491-2023, https://doi.org/10.5194/acp-23-1491-2023, 2023
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Flaring is used by the oil and gas sector to dispose of unwanted natural gas or for safety. However, few studies have assessed the efficiency with which the gas is combusted. We sampled flaring emissions from offshore facilities in the North Sea. Average measured flaring efficiencies were ~ 98 % but with a skewed distribution, including many flares of lower efficiency. NOx and ethane emissions were also measured. Inefficient flaring practices could be a target for mitigating carbon emissions.
Daniel J. Bryant, Beth S. Nelson, Stefan J. Swift, Sri Hapsari Budisulistiorini, Will S. Drysdale, Adam R. Vaughan, Mike J. Newland, James R. Hopkins, James M. Cash, Ben Langford, Eiko Nemitz, W. Joe F. Acton, C. Nicholas Hewitt, Tuhin Mandal, Bhola R. Gurjar, Shivani, Ranu Gadi, James D. Lee, Andrew R. Rickard, and Jacqueline F. Hamilton
Atmos. Chem. Phys., 23, 61–83, https://doi.org/10.5194/acp-23-61-2023, https://doi.org/10.5194/acp-23-61-2023, 2023
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This paper investigates the sources of isoprene and monoterpene compounds and their particulate-phase oxidation products in Delhi, India. This was done to improve our understanding of the sources, concentrations, and fate of volatile emissions in megacities. By studying the chemical composition of offline filter samples, we report that a significant share of the oxidised organic aerosol in Delhi is from isoprene and monoterpenes. This has implications for human health and policy development.
Simone T. Andersen, Beth S. Nelson, Katie A. Read, Shalini Punjabi, Luis Neves, Matthew J. Rowlinson, James Hopkins, Tomás Sherwen, Lisa K. Whalley, James D. Lee, and Lucy J. Carpenter
Atmos. Chem. Phys., 22, 15747–15765, https://doi.org/10.5194/acp-22-15747-2022, https://doi.org/10.5194/acp-22-15747-2022, 2022
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The cycling of NO and NO2 is important to understand to be able to predict O3 concentrations in the atmosphere. We have used long-term measurements from the Cape Verde Atmospheric Observatory together with model outputs to investigate the cycling of nitrogen oxide (NO) and nitrogen dioxide (NO2) in very clean marine air. This study shows that we understand the processes occurring in very clean air, but with small amounts of pollution in the air, known chemistry cannot explain what is observed.
Alfred W. Mayhew, Ben H. Lee, Joel A. Thornton, Thomas J. Bannan, James Brean, James R. Hopkins, James D. Lee, Beth S. Nelson, Carl Percival, Andrew R. Rickard, Marvin D. Shaw, Peter M. Edwards, and Jaqueline F. Hamilton
Atmos. Chem. Phys., 22, 14783–14798, https://doi.org/10.5194/acp-22-14783-2022, https://doi.org/10.5194/acp-22-14783-2022, 2022
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Isoprene nitrates are chemical species commonly found in the atmosphere that are important for their impacts on air quality and climate. This paper compares 3 different representations of the chemistry of isoprene nitrates in computational models highlighting cases where the choice of chemistry included has significant impacts on the concentration and composition of the modelled nitrates. Calibration of mass spectrometers is also shown to be an important factor when analysing isoprene nitrates.
Will S. Drysdale, Adam R. Vaughan, Freya A. Squires, Sam J. Cliff, Stefan Metzger, David Durden, Natchaya Pingintha-Durden, Carole Helfter, Eiko Nemitz, C. Sue B. Grimmond, Janet Barlow, Sean Beevers, Gregor Stewart, David Dajnak, Ruth M. Purvis, and James D. Lee
Atmos. Chem. Phys., 22, 9413–9433, https://doi.org/10.5194/acp-22-9413-2022, https://doi.org/10.5194/acp-22-9413-2022, 2022
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Measurements of NOx emissions are important for a good understanding of air quality. While there are many direct measurements of NOx concentration, there are very few measurements of its emission. Measurements of emissions provide constraints on emissions inventories and air quality models. This article presents measurements of NOx emission from the BT Tower in central London in 2017 and compares them with inventories, finding that they underestimate by a factor of ∼1.48.
Marios Panagi, Roberto Sommariva, Zoë L. Fleming, Paul S. Monks, Gongda Lu, Eloise A. Marais, James R. Hopkins, Alastair C. Lewis, Qiang Zhang, James D. Lee, Freya A. Squires, Lisa K. Whalley, Eloise J. Slater, Dwayne E. Heard, Robert Woodward-Massey, Chunxiang Ye, and Joshua D. Vande Hey
Atmos. Chem. Phys. Discuss., https://doi.org/10.5194/acp-2022-379, https://doi.org/10.5194/acp-2022-379, 2022
Revised manuscript not accepted
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A dispersion model and a box model were combined to investigate the evolution of VOCs in Beijing once they are emitted from anthropogenic sources. It was determined that during the winter time the VOC concentrations in Beijing are driven predominantly by sources within Beijing and by a combination of transport and chemistry during the summer. Furthermore, the results in the paper highlight the need for a season specific policy.
Hannah Walker, Daniel Stone, Trevor Ingham, Sina Hackenberg, Danny Cryer, Shalini Punjabi, Katie Read, James Lee, Lisa Whalley, Dominick V. Spracklen, Lucy J. Carpenter, Steve R. Arnold, and Dwayne E. Heard
Atmos. Chem. Phys., 22, 5535–5557, https://doi.org/10.5194/acp-22-5535-2022, https://doi.org/10.5194/acp-22-5535-2022, 2022
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Glyoxal is a ubiquitous reactive organic compound in the atmosphere, which may form organic aerosol and impact the atmosphere's oxidising capacity. There are limited measurements of glyoxal's abundance in the remote marine atmosphere. We made new measurements of glyoxal using a highly sensitive technique over two 4-week periods in the tropical Atlantic atmosphere. We show that daytime measurements are mostly consistent with our chemical understanding but a potential missing source at night.
Robert Woodward-Massey, Roberto Sommariva, Lisa K. Whalley, Danny R. Cryer, Trevor Ingham, William J1 Bloss, 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. Discuss., https://doi.org/10.5194/acp-2022-207, https://doi.org/10.5194/acp-2022-207, 2022
Preprint withdrawn
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We measured radicals (OH, HO2, RO2) and OH reactivity at a UK coastal site and compared our observations to the predictions of an MCMv3.3.1 box model. We find variable agreement between measured and modelled radical concentrations and OH reactivity, where the levels of agreement for individual species display strong dependences on NO concentrations. The most substantial disagreement is found for RO2 at high NO (> 1 ppbv), when RO2 levels are underpredicted by a factor of ~10–30.
Amy Foulds, Grant Allen, Jacob T. Shaw, Prudence Bateson, Patrick A. Barker, Langwen Huang, Joseph R. Pitt, James D. Lee, Shona E. Wilde, Pamela Dominutti, Ruth M. Purvis, David Lowry, James L. France, Rebecca E. Fisher, Alina Fiehn, Magdalena Pühl, Stéphane J. B. Bauguitte, Stephen A. Conley, Mackenzie L. Smith, Tom Lachlan-Cope, Ignacio Pisso, and Stefan Schwietzke
Atmos. Chem. Phys., 22, 4303–4322, https://doi.org/10.5194/acp-22-4303-2022, https://doi.org/10.5194/acp-22-4303-2022, 2022
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We measured CH4 emissions from 21 offshore oil and gas facilities in the Norwegian Sea in 2019. Measurements compared well with operator-reported emissions but were greatly underestimated when compared with a 2016 global fossil fuel inventory. This study demonstrates the need for up-to-date and accurate inventories for use in research and policy and the important benefits of best-practice reporting methods by operators. Airborne measurements are an effective tool to validate such inventories.
Leigh R. Crilley, Louisa J. Kramer, Francis D. Pope, Chris Reed, James D. Lee, Lucy J. Carpenter, Lloyd D. J. Hollis, Stephen M. Ball, and William J. Bloss
Atmos. Chem. Phys., 21, 18213–18225, https://doi.org/10.5194/acp-21-18213-2021, https://doi.org/10.5194/acp-21-18213-2021, 2021
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Nitrous acid (HONO) is a key source of atmospheric oxidants. We evaluate if the ocean surface is a source of HONO for the marine boundary layer, using measurements from two contrasting coastal locations. We observed no evidence for a night-time ocean surface source, in contrast to previous work. This points to significant geographical variation in the predominant HONO formation mechanisms in marine environments, reflecting possible variability in the sea-surface microlayer composition.
Stefan Metzger, David Durden, Sreenath Paleri, Matthias Sühring, Brian J. Butterworth, Christopher Florian, Matthias Mauder, David M. Plummer, Luise Wanner, Ke Xu, and Ankur R. Desai
Atmos. Meas. Tech., 14, 6929–6954, https://doi.org/10.5194/amt-14-6929-2021, https://doi.org/10.5194/amt-14-6929-2021, 2021
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The key points are the following. (i) Integrative observing system design can multiply the information gain of surface–atmosphere field measurements. (ii) Catalyzing numerical simulations and first-principles machine learning open up observing system simulation experiments to novel applications. (iii) Use cases include natural climate solutions, emission inventory validation, urban air quality, and industry leak detection.
Rebecca L. Wagner, Naomi J. Farren, Jack Davison, Stuart Young, James R. Hopkins, Alastair C. Lewis, David C. Carslaw, and Marvin D. Shaw
Atmos. Meas. Tech., 14, 6083–6100, https://doi.org/10.5194/amt-14-6083-2021, https://doi.org/10.5194/amt-14-6083-2021, 2021
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We describe the use of a selected-ion flow-tube mass spectrometer (SIFT-MS) in a mobile laboratory to provide on-road, high spatial and temporal measurements of CO2, CH4, multiple volatile organic compounds (VOCs) and other trace gases. Results are presented that highlight the potential of this platform for developing characterisation methods of different emissions sources in complex urban areas.
Beth S. Nelson, Gareth J. Stewart, Will S. Drysdale, Mike J. Newland, Adam R. Vaughan, Rachel E. Dunmore, Pete M. Edwards, Alastair C. Lewis, Jacqueline F. Hamilton, W. Joe Acton, C. Nicholas Hewitt, Leigh R. Crilley, Mohammed S. Alam, Ülkü A. Şahin, David C. S. Beddows, William J. Bloss, Eloise Slater, Lisa K. Whalley, Dwayne E. Heard, James M. Cash, Ben Langford, Eiko Nemitz, Roberto Sommariva, Sam Cox, Shivani, Ranu Gadi, Bhola R. Gurjar, James R. Hopkins, Andrew R. Rickard, and James D. Lee
Atmos. Chem. Phys., 21, 13609–13630, https://doi.org/10.5194/acp-21-13609-2021, https://doi.org/10.5194/acp-21-13609-2021, 2021
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Ozone production at an urban site in Delhi is sensitive to volatile organic compound (VOC) concentrations, particularly those of the aromatic, monoterpene, and alkene VOC classes. The change in ozone production by varying atmospheric pollutants according to their sources, as defined in an emissions inventory, is investigated. The study suggests that reducing road transport emissions alone does not reduce reactive VOCs in the atmosphere enough to perturb an increase in ozone production.
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.
Gongda Lu, Eloise A. Marais, Tuan V. Vu, Jingsha Xu, Zongbo Shi, James D. Lee, Qiang Zhang, Lu Shen, Gan Luo, and Fangqun Yu
Atmos. Chem. Phys. Discuss., https://doi.org/10.5194/acp-2021-428, https://doi.org/10.5194/acp-2021-428, 2021
Revised manuscript not accepted
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Emission controls were imposed in Beijing-Tianjin-Hebei in northern China in autumn-winter 2017. We find that regional PM2.5 targets (15 % decrease relative to previous year) were exceeded. Our analysis shows that decline in precursor emissions only leads to less than half (43 %) the improved air quality. Most of the change (57 %) is due to interannual variability in meteorology. Stricter emission controls may be necessary in years with unfavourable meteorology.
Esther Borrás, Luis A. Tortajada-Genaro, Milagro Ródenas, Teresa Vera, Thomas Speak, Paul Seakins, Marvin D. Shaw, Alastair C. Lewis, and Amalia Muñoz
Atmos. Meas. Tech., 14, 4989–4999, https://doi.org/10.5194/amt-14-4989-2021, https://doi.org/10.5194/amt-14-4989-2021, 2021
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This work presents promising results in the characterization of specific atmospheric pollutants (oxygenated VOCs) present at very low but highly relevant concentrations.
We carried out this research at EUPHORE facilities within the framework of the EUROCHAMP project. A new analytical method, with high robustness and precision, also clean in the use of solvents, low cost, and easily adaptable for use in mobile laboratories for air quality monitoring, is presented.
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.
Huihui Wu, Jonathan W. Taylor, Justin M. Langridge, Chenjie Yu, James D. Allan, Kate Szpek, Michael I. Cotterell, Paul I. Williams, Michael Flynn, Patrick Barker, Cathryn Fox, Grant Allen, James Lee, and Hugh Coe
Atmos. Chem. Phys., 21, 9417–9440, https://doi.org/10.5194/acp-21-9417-2021, https://doi.org/10.5194/acp-21-9417-2021, 2021
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Seasonal biomass burning over West Africa is a globally significant source of carbonaceous particles in the atmosphere, which have important climate impacts but are poorly constrained. We conducted in situ airborne measurements to investigate the evolution of smoke aerosol properties in this region. We observed absorption enhancement for both black carbon and brown carbon after emission, which provides new field results and constraints on aerosol parameterizations for future climate models.
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.
Simone T. Andersen, Lucy J. Carpenter, Beth S. Nelson, Luis Neves, Katie A. Read, Chris Reed, Martyn Ward, Matthew J. Rowlinson, and James D. Lee
Atmos. Meas. Tech., 14, 3071–3085, https://doi.org/10.5194/amt-14-3071-2021, https://doi.org/10.5194/amt-14-3071-2021, 2021
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NOx has been measured in remote marine air via chemiluminescence detection using two different methods for NO2 to NO photolytic conversion: (a) internal diodes and a reaction chamber made of Teflon-like barium-doped material, which causes a NO2 artefact, and (b) external diodes and a quartz photolysis cell. Once corrections are made for the artefact of (a), the two converters are shown to give comparable NO2 mixing ratios, giving confidence in the quantitative measurement of NOx at low levels.
Steven J. Campbell, Kate Wolfer, Battist Utinger, Joe Westwood, Zhi-Hui Zhang, Nicolas Bukowiecki, Sarah S. Steimer, Tuan V. Vu, Jingsha Xu, Nicholas Straw, Steven Thomson, Atallah Elzein, Yele Sun, Di Liu, Linjie Li, Pingqing Fu, Alastair C. Lewis, Roy M. Harrison, William J. Bloss, Miranda Loh, Mark R. Miller, Zongbo Shi, and Markus Kalberer
Atmos. Chem. Phys., 21, 5549–5573, https://doi.org/10.5194/acp-21-5549-2021, https://doi.org/10.5194/acp-21-5549-2021, 2021
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In this study, we quantify PM2.5 oxidative potential (OP), a metric widely suggested as a potential measure of particle toxicity, in Beijing in summer and winter using four acellular assays. We correlate PM2.5 OP with a comprehensive range of atmospheric and particle composition measurements, demonstrating inter-assay differences and seasonal variation of PM2.5 OP. Using multivariate statistical analysis, we highlight specific particle chemical components and sources that influence OP.
Stuart K. Grange, James D. Lee, Will S. Drysdale, Alastair C. Lewis, Christoph Hueglin, Lukas Emmenegger, and David C. Carslaw
Atmos. Chem. Phys., 21, 4169–4185, https://doi.org/10.5194/acp-21-4169-2021, https://doi.org/10.5194/acp-21-4169-2021, 2021
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The changes in mobility across Europe due to the COVID-19 lockdowns had consequences for air quality. We compare what was experienced to estimates of "what would have been" without the lockdowns. Nitrogen dioxide (NO2), an important vehicle-sourced pollutant, decreased by a third. However, ozone (O3) increased in response to lower NO2. Because NO2 is decreasing over time, increases in O3 can be expected in European urban areas and will require management to avoid future negative outcomes.
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.
Gareth J. Stewart, Beth S. Nelson, W. Joe F. Acton, Adam R. Vaughan, Naomi J. Farren, James R. Hopkins, Martyn W. Ward, Stefan J. Swift, Rahul Arya, Arnab Mondal, Ritu Jangirh, Sakshi Ahlawat, Lokesh Yadav, Sudhir K. Sharma, Siti S. M. Yunus, C. Nicholas Hewitt, Eiko Nemitz, Neil Mullinger, Ranu Gadi, Lokesh K. Sahu, Nidhi Tripathi, Andrew R. Rickard, James D. Lee, Tuhin K. Mandal, and Jacqueline F. Hamilton
Atmos. Chem. Phys., 21, 2407–2426, https://doi.org/10.5194/acp-21-2407-2021, https://doi.org/10.5194/acp-21-2407-2021, 2021
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Biomass burning releases many lower-molecular-weight organic species which are difficult to analyse but important for the formation of organic aerosol. This study examined a new high-resolution technique to better characterise these difficult-to-analyse organic components. Some burning sources analysed in this study, such as cow dung cake and municipal solid waste, released extremely complex mixtures containing many thousands of different lower-volatility organic compounds.
Gareth J. Stewart, W. Joe F. Acton, Beth S. Nelson, Adam R. Vaughan, James R. Hopkins, Rahul Arya, Arnab Mondal, Ritu Jangirh, Sakshi Ahlawat, Lokesh Yadav, Sudhir K. Sharma, Rachel E. Dunmore, Siti S. M. Yunus, C. Nicholas Hewitt, Eiko Nemitz, Neil Mullinger, Ranu Gadi, Lokesh K. Sahu, Nidhi Tripathi, Andrew R. Rickard, James D. Lee, Tuhin K. Mandal, and Jacqueline F. Hamilton
Atmos. Chem. Phys., 21, 2383–2406, https://doi.org/10.5194/acp-21-2383-2021, https://doi.org/10.5194/acp-21-2383-2021, 2021
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Biomass burning is a major source of trace gases to the troposphere; however, the composition and quantity of emissions vary greatly between different fuel types. This work provided near-total quantitation of non-methane volatile organic compounds from combustion of biofuels from India. Emissions from cow dung cake combustion were significantly larger than conventional fuelwood combustion, potentially indicating that this source has a disproportionately large impact on regional air quality.
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.
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.
Rutambhara Joshi, Dantong Liu, Eiko Nemitz, Ben Langford, Neil Mullinger, Freya Squires, James Lee, Yunfei Wu, Xiaole Pan, Pingqing Fu, Simone Kotthaus, Sue Grimmond, Qiang Zhang, Ruili Wu, Oliver Wild, Michael Flynn, Hugh Coe, and James Allan
Atmos. Chem. Phys., 21, 147–162, https://doi.org/10.5194/acp-21-147-2021, https://doi.org/10.5194/acp-21-147-2021, 2021
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Black carbon (BC) is a component of particulate matter which has significant effects on climate and human health. Sources of BC include biomass burning, transport, industry and domestic cooking and heating. In this study, we measured BC emissions in Beijing, finding a dominance of traffic emissions over all other sources. The quantitative method presented here has benefits for revising widely used emissions inventories and for understanding BC sources with impacts on air quality and climate.
James L. France, Prudence Bateson, Pamela Dominutti, Grant Allen, Stephen Andrews, Stephane Bauguitte, Max Coleman, Tom Lachlan-Cope, Rebecca E. Fisher, Langwen Huang, Anna E. Jones, James Lee, David Lowry, Joseph Pitt, Ruth Purvis, John Pyle, Jacob Shaw, Nicola Warwick, Alexandra Weiss, Shona Wilde, Jonathan Witherstone, and Stuart Young
Atmos. Meas. Tech., 14, 71–88, https://doi.org/10.5194/amt-14-71-2021, https://doi.org/10.5194/amt-14-71-2021, 2021
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Measuring emission rates of methane from installations is tricky, and it is even more so when those installations are located offshore. Here, we show the aircraft set-up and demonstrate an effective methodology for surveying emissions from UK and Dutch offshore oil and gas installations. We present example data collected from two campaigns to demonstrate the challenges and solutions encountered during these surveys.
David C. Loades, Mingxi Yang, Thomas G. Bell, Adam R. Vaughan, Ryan J. Pound, Stefan Metzger, James D. Lee, and Lucy J. Carpenter
Atmos. Meas. Tech., 13, 6915–6931, https://doi.org/10.5194/amt-13-6915-2020, https://doi.org/10.5194/amt-13-6915-2020, 2020
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The loss of ozone to the sea surface was measured from the south coast of the UK and was found to be more rapid than previous observations over the open ocean. This is likely a consequence of different chemistry and biology in coastal environments. Strong winds appeared to speed up the loss of ozone. A better understanding of what influences ozone loss over the sea will lead to better model estimates of total ozone in the troposphere.
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.
Atallah Elzein, Gareth J. Stewart, Stefan J. Swift, Beth S. Nelson, Leigh R. Crilley, Mohammed S. Alam, Ernesto Reyes-Villegas, Ranu Gadi, Roy M. Harrison, Jacqueline F. Hamilton, and Alastair C. Lewis
Atmos. Chem. Phys., 20, 14303–14319, https://doi.org/10.5194/acp-20-14303-2020, https://doi.org/10.5194/acp-20-14303-2020, 2020
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We collected high-frequency air particle samples (PM2.5) in Beijing (China) and Delhi (India) and measured the concentration of PAHs in daytime and night-time. PAHs were higher in Delhi than in Beijing, and the five-ring PAHs contribute the most to the total PAH concentration. We compared the emission sources and identified the major sectors that could be subject to mitigation measures. The adverse health effects from inhalation exposure to PAHs in Delhi are 2.2 times higher than in Beijing.
Mohammed S. Alam, Leigh R. Crilley, James D. Lee, Louisa J. Kramer, Christian Pfrang, Mónica Vázquez-Moreno, Milagros Ródenas, Amalia Muñoz, and William J. Bloss
Atmos. Meas. Tech., 13, 5977–5991, https://doi.org/10.5194/amt-13-5977-2020, https://doi.org/10.5194/amt-13-5977-2020, 2020
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We report on the interference arising in measurements of nitrogen oxides (NOx) from the presence of a range of alkenes in sampled air when using the most widespread air quality monitoring technique for chemiluminescence detection. Interferences of up to 11 % are reported, depending upon the alkene present and conditions used. Such interferences may be of substantial importance for the interpretation of ambient NOx data, particularly for high volatile organic compound and low NOx environments.
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Short summary
Validating emissions estimates of atmospheric pollutants is a vital pathway towards reducing urban concentrations of air pollution and ensuring effective legislative controls are implemented. The work presented here highlights a strategy capable of quantifying and spatially disaggregating NOx emissions over challenging urban terrain. This work shows great scope as a tool for emission inventory validation and independent generation of high-resolution surface emissions on a city-wide scale.
Validating emissions estimates of atmospheric pollutants is a vital pathway towards reducing...
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