Articles | Volume 14, issue 10
https://doi.org/10.5194/amt-14-6905-2021
© 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/amt-14-6905-2021
© Author(s) 2021. This work is distributed under
the Creative Commons Attribution 4.0 License.
the Creative Commons Attribution 4.0 License.
On the use of reference mass spectra for reducing uncertainty in source apportionment of solid-fuel burning in ambient organic aerosol
Chunshui Lin
School of Physics, Ryan Institute's Centre for Climate and Air Pollution Studies, National University of Ireland Galway, University Road, Galway, H91 CF50, Ireland
State Key Laboratory of Loess and Quaternary Geology and Key Laboratory of Aerosol Chemistry and Physics, Chinese Academy of Sciences, Xi'an 710061, China
Center for Excellence in Quaternary Science and Global Change, Institute of Earth Environment, Chinese Academy of Sciences, Xi'an 710061, China
Darius Ceburnis
School of Physics, Ryan Institute's Centre for Climate and Air Pollution Studies, National University of Ireland Galway, University Road, Galway, H91 CF50, Ireland
Anna Trubetskaya
Department of Chemical Engineering, Aalto University, 02150 Espoo, Finland
School of Physics, Ryan Institute's Centre for Climate and Air Pollution Studies, National University of Ireland Galway, University Road, Galway, H91 CF50, Ireland
William Smith
School of Electrical, Electronic and Mechanical Engineering, University College Dublin, Dublin, D04V1W8, Ireland
Stig Hellebust
School of Chemistry and Environmental Research Institute, University College Cork, Cork, T23XE10, Ireland
John Wenger
School of Chemistry and Environmental Research Institute, University College Cork, Cork, T23XE10, Ireland
Colin O'Dowd
CORRESPONDING AUTHOR
School of Physics, Ryan Institute's Centre for Climate and Air Pollution Studies, National University of Ireland Galway, University Road, Galway, H91 CF50, Ireland
Jurgita Ovadnevaite
CORRESPONDING AUTHOR
School of Physics, Ryan Institute's Centre for Climate and Air Pollution Studies, National University of Ireland Galway, University Road, Galway, H91 CF50, Ireland
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This study presents the first source apportionment of organic aerosol at Mace Head via high-resolution mass spectrometry. Introducing transfer entropy as a novel method reveals that aged organic aerosol originates from both open-ocean ozonolysis and local peat-burning oxidation. Methanesulfonic acid and organic sea spray both mirror phytoplankton activity, with the former closely tied to coccolithophore blooms and the latter linked to diatoms, chlorophytes, and cyanobacteria.
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Atmos. Chem. Phys., 25, 3753–3764, https://doi.org/10.5194/acp-25-3753-2025, https://doi.org/10.5194/acp-25-3753-2025, 2025
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Our field campaigns observed a strong diel pattern of chloroacetic acid as well as a strong correlation between its level and that of reactive chlorine species at a coastal site. Using quantum chemical calculations and box model simulation with an updated Master Chemical Mechanism, we found that the formation pathway of chloroacetic acid involved multiphase processes. Our study enhances understanding of atmospheric organic chlorine chemistry and emphasizes the importance of multiphase reactions.
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Atmos. Chem. Phys., 24, 10815–10831, https://doi.org/10.5194/acp-24-10815-2024, https://doi.org/10.5194/acp-24-10815-2024, 2024
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The chemical composition and sources of submicron aerosol in the Dublin Port area were investigated over a month-long campaign. Two distinct types of ship emissions were identified and characterised: sulfate-rich plumes from the use of heavy fuel oil with scrubbers and organic-rich plumes from the use of low-sulfur fuels. The latter were more frequent, emitting double the particle number and having a typical V / Ni ratio for ship emission.
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The chemical composition of atmospheric particles has shown significant changes in recent years. We investigated the potential effects of changes in inorganics on aerosol water uptake and, thus, secondary organic aerosol formation in wintertime haze based on the size-resolved measurements of non-refractory fine particulate matter (NR-PM2.5) in Xi’an, northwestern China. We highlight the key role of aerosol water as a medium to link inorganics and organics in their multiphase processes.
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Secondary organic aerosol (SOA) can be produced by various pathways, but its formation mechanisms are unclear. Observations were conducted in the North China Plain during a highly oxidizing atmosphere in summer. We found that fast photochemistry dominated SOA formation during daytime. Two types of aqueous-phase chemistry (nocturnal and daytime processing) take place at high relative humidity. The potential transformation from primary organic aerosol (POA) to SOA was also an important pathway.
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This preprint is open for discussion and under review for Atmospheric Chemistry and Physics (ACP).
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Since China's 2013 Clean Air Act cut PM2.5 by over half, winter haze in the North China Plain persists due to secondary organic aerosols now dominating primary pollutants, requiring urgent regional cooperation to address model-underestimated chemical transformations and cross-border pollution.
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Baihua Chen, Lu Lei, Emmanuel Chevassus, Wei Xu, Ling Zhen, Haobin Zhong, Lin Wang, Chunshui Lin, Ru-Jin Huang, Darius Ceburnis, Colin O'Dowd, and Jurgita Ovadnevaite
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This study uses machine learning to separate marine primary (POA) and secondary organic aerosols (SOA) from a decade of high-resolution data. POA averages 51 % of marine organic aerosols annually, peaking at 63 % in summer. A support vector regression model, validated via fuzzy clustering and Monte Carlo simulations, identifies POA’s seasonal patterns linked to biological activity. We found diverse impacts of marine POA and SOA on the aerosol hygroscopicity and mixing state.
Emmanuel Chevassus, Kirsten N. Fossum, Darius Ceburnis, Lu Lei, Chunshui Lin, Wei Xu, Colin O'Dowd, and Jurgita Ovadnevaite
Atmos. Chem. Phys., 25, 4107–4129, https://doi.org/10.5194/acp-25-4107-2025, https://doi.org/10.5194/acp-25-4107-2025, 2025
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This study presents the first source apportionment of organic aerosol at Mace Head via high-resolution mass spectrometry. Introducing transfer entropy as a novel method reveals that aged organic aerosol originates from both open-ocean ozonolysis and local peat-burning oxidation. Methanesulfonic acid and organic sea spray both mirror phytoplankton activity, with the former closely tied to coccolithophore blooms and the latter linked to diatoms, chlorophytes, and cyanobacteria.
Mingxue Li, Men Xia, Chunshui Lin, Yifan Jiang, Weihang Sun, Yurun Wang, Yingnan Zhang, Maoxia He, and Tao Wang
Atmos. Chem. Phys., 25, 3753–3764, https://doi.org/10.5194/acp-25-3753-2025, https://doi.org/10.5194/acp-25-3753-2025, 2025
Short summary
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Our field campaigns observed a strong diel pattern of chloroacetic acid as well as a strong correlation between its level and that of reactive chlorine species at a coastal site. Using quantum chemical calculations and box model simulation with an updated Master Chemical Mechanism, we found that the formation pathway of chloroacetic acid involved multiphase processes. Our study enhances understanding of atmospheric organic chlorine chemistry and emphasizes the importance of multiphase reactions.
Kirsten N. Fossum, Chunshui Lin, Niall O'Sullivan, Lu Lei, Stig Hellebust, Darius Ceburnis, Aqeel Afzal, Anja Tremper, David Green, Srishti Jain, Steigvilė Byčenkienė, Colin O'Dowd, John Wenger, and Jurgita Ovadnevaite
Atmos. Chem. Phys., 24, 10815–10831, https://doi.org/10.5194/acp-24-10815-2024, https://doi.org/10.5194/acp-24-10815-2024, 2024
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The chemical composition and sources of submicron aerosol in the Dublin Port area were investigated over a month-long campaign. Two distinct types of ship emissions were identified and characterised: sulfate-rich plumes from the use of heavy fuel oil with scrubbers and organic-rich plumes from the use of low-sulfur fuels. The latter were more frequent, emitting double the particle number and having a typical V / Ni ratio for ship emission.
Rósín Byrne, John C. Wenger, and Stig Hellebust
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Karam Mansour, Stefano Decesari, Darius Ceburnis, Jurgita Ovadnevaite, Lynn M. Russell, Marco Paglione, Laurent Poulain, Shan Huang, Colin O'Dowd, and Matteo Rinaldi
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We propose and evaluate machine learning predictive algorithms to model freshly formed biogenic methanesulfonic acid and sulfate concentrations. The long-term constructed dataset covers the North Atlantic at an unprecedented resolution. The improved parameterization of biogenic sulfur aerosols at regional scales is essential for determining their radiative forcing, which could help further understand marine-aerosol–cloud interactions and reduce uncertainties in climate models
Hayley Furnell, John Wenger, Astrid Wingler, Kieran N. Kilcawley, David T. Mannion, Iwona Skibinska, and Julien Kammer
EGUsphere, https://doi.org/10.5194/egusphere-2024-154, https://doi.org/10.5194/egusphere-2024-154, 2024
Preprint archived
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The BVOCs emitted by Sitka spruce (picea sitchensis), the most commonly planted tree species in Ireland and the UK were characterised, their temperature and PPFD dependences determined and standardised emission fluxes calculated. The majority of the 74 detected BVOCs were oxygenated, with piperitone, isoprene and monoterpenes dominating. At standardised conditions piperitone is the main emission. However, at the current climate conditions in Ireland and UK, the emission of isoprene dominates.
Yuquan Gong, Ru-Jin Huang, Lu Yang, Ting Wang, Wei Yuan, Wei Xu, Wenjuan Cao, Yang Wang, and Yongjie Li
Atmos. Chem. Phys., 23, 15197–15207, https://doi.org/10.5194/acp-23-15197-2023, https://doi.org/10.5194/acp-23-15197-2023, 2023
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We measured the number size distribution of 2.5–300 nm particles and cloud condensation nuclei (CCN) number concentrations at King Sejong Station on the Antarctic Peninsula continuously from 1 January to 31 December 2018. During the pristine and clean periods, 97 new particle formation (NPF) events were detected. For 83 of these, CCN concentrations increased by 2 %–268 % (median 44 %) following 1 to 36 h (median 8 h) after NPF events.
Yifang Gu, Ru-Jin Huang, Jing Duan, Wei Xu, Chunshui Lin, Haobin Zhong, Ying Wang, Haiyan Ni, Quan Liu, Ruiguang Xu, Litao Wang, and Yong Jie Li
Atmos. Chem. Phys., 23, 5419–5433, https://doi.org/10.5194/acp-23-5419-2023, https://doi.org/10.5194/acp-23-5419-2023, 2023
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Secondary organic aerosol (SOA) can be produced by various pathways, but its formation mechanisms are unclear. Observations were conducted in the North China Plain during a highly oxidizing atmosphere in summer. We found that fast photochemistry dominated SOA formation during daytime. Two types of aqueous-phase chemistry (nocturnal and daytime processing) take place at high relative humidity. The potential transformation from primary organic aerosol (POA) to SOA was also an important pathway.
Chunshui Lin, Ru-Jin Huang, Haobin Zhong, Jing Duan, Zixi Wang, Wei Huang, and Wei Xu
Atmos. Chem. Phys., 23, 3595–3607, https://doi.org/10.5194/acp-23-3595-2023, https://doi.org/10.5194/acp-23-3595-2023, 2023
Short summary
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The complex interaction between O3 and PM2.5, coupled with the topology of the Fenwei Plain and the evolution of the boundary layer height, highlights the challenges in further reducing particulate pollution in winter despite years of efforts to reduce emissions. Through scenario analysis in a chemical box model constrained by observation, we show the co-benefits of reducing NOx and VOCs simultaneously in reducing ozone and SOA.
Ville Leinonen, Harri Kokkola, Taina Yli-Juuti, Tero Mielonen, Thomas Kühn, Tuomo Nieminen, Simo Heikkinen, Tuuli Miinalainen, Tommi Bergman, Ken Carslaw, Stefano Decesari, Markus Fiebig, Tareq Hussein, Niku Kivekäs, Radovan Krejci, Markku Kulmala, Ari Leskinen, Andreas Massling, Nikos Mihalopoulos, Jane P. Mulcahy, Steffen M. Noe, Twan van Noije, Fiona M. O'Connor, Colin O'Dowd, Dirk Olivie, Jakob B. Pernov, Tuukka Petäjä, Øyvind Seland, Michael Schulz, Catherine E. Scott, Henrik Skov, Erik Swietlicki, Thomas Tuch, Alfred Wiedensohler, Annele Virtanen, and Santtu Mikkonen
Atmos. Chem. Phys., 22, 12873–12905, https://doi.org/10.5194/acp-22-12873-2022, https://doi.org/10.5194/acp-22-12873-2022, 2022
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We provide the first extensive comparison of detailed aerosol size distribution trends between in situ observations from Europe and five different earth system models. We investigated aerosol modes (nucleation, Aitken, and accumulation) separately and were able to show the differences between measured and modeled trends and especially their seasonal patterns. The differences in model results are likely due to complex effects of several processes instead of certain specific model features.
Meng Wang, Yusen Duan, Wei Xu, Qiyuan Wang, Zhuozhi Zhang, Qi Yuan, Xinwei Li, Shuwen Han, Haijie Tong, Juntao Huo, Jia Chen, Shan Gao, Zhongbiao Wu, Long Cui, Yu Huang, Guangli Xiu, Junji Cao, Qingyan Fu, and Shun-cheng Lee
Atmos. Chem. Phys., 22, 12789–12802, https://doi.org/10.5194/acp-22-12789-2022, https://doi.org/10.5194/acp-22-12789-2022, 2022
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In this study, we report the long-term measurement of organic carbon (OC) and elementary carbon (EC) in PM2.5 with hourly time resolution conducted at a regional site in Shanghai from 2016 to 2020. The results from this study provide critical information about the long-term trend of carbonaceous aerosol, in particular secondary OC, in one of the largest megacities in the world and are helpful for developing pollution control measures from a long-term planning perspective.
Marta Via, Gang Chen, Francesco Canonaco, Kaspar R. Daellenbach, Benjamin Chazeau, Hasna Chebaicheb, Jianhui Jiang, Hannes Keernik, Chunshui Lin, Nicolas Marchand, Cristina Marin, Colin O'Dowd, Jurgita Ovadnevaite, Jean-Eudes Petit, Michael Pikridas, Véronique Riffault, Jean Sciare, Jay G. Slowik, Leïla Simon, Jeni Vasilescu, Yunjiang Zhang, Olivier Favez, André S. H. Prévôt, Andrés Alastuey, and María Cruz Minguillón
Atmos. Meas. Tech., 15, 5479–5495, https://doi.org/10.5194/amt-15-5479-2022, https://doi.org/10.5194/amt-15-5479-2022, 2022
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This work presents the differences resulting from two techniques (rolling and seasonal) of the positive matrix factorisation model that can be run for organic aerosol source apportionment. The current state of the art suggests that the rolling technique is more accurate, but no proof of its effectiveness has been provided yet. This paper tackles this issue in the context of a synthetic dataset and a multi-site real-world comparison.
Jing Duan, Ru-Jin Huang, Yifang Gu, Chunshui Lin, Haobin Zhong, Wei Xu, Quan Liu, Yan You, Jurgita Ovadnevaite, Darius Ceburnis, Thorsten Hoffmann, and Colin O'Dowd
Atmos. Chem. Phys., 22, 10139–10153, https://doi.org/10.5194/acp-22-10139-2022, https://doi.org/10.5194/acp-22-10139-2022, 2022
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Biomass-burning-influenced oxygenated organic aerosol (OOA-BB), formed from the photochemical oxidation and aging of biomass burning OA (BBOA), was resolved in urban Xi’an. The aqueous-phase processed oxygenated OA (aq-OOA) concentration was more dependent on secondary inorganic aerosol (SIA) content and aerosol liquid water content (ALWC). The increased aq-OOA contribution during SIA-enhanced periods likely reflects OA evolution due to the addition of alcohol or peroxide groups
Haobin Zhong, Ru-Jin Huang, Chunshui Lin, Wei Xu, Jing Duan, Yifang Gu, Wei Huang, Haiyan Ni, Chongshu Zhu, Yan You, Yunfei Wu, Renjian Zhang, Jurgita Ovadnevaite, Darius Ceburnis, and Colin D. O'Dowd
Atmos. Chem. Phys., 22, 9513–9524, https://doi.org/10.5194/acp-22-9513-2022, https://doi.org/10.5194/acp-22-9513-2022, 2022
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To investigate the physico-chemical properties of aerosol transported from major pollution regions in China, observations were conducted ~200 m above the ground at the junction location of the two key pollution areas. We found that the formation efficiency, oxidation state and production rate of secondary aerosol were different in the transport sectors from different pollution regions, and they were largely enhanced by the regional long-distance transport.
Youwei Hong, Xinbei Xu, Dan Liao, Taotao Liu, Xiaoting Ji, Ke Xu, Chunyang Liao, Ting Wang, Chunshui Lin, and Jinsheng Chen
Atmos. Chem. Phys., 22, 7827–7841, https://doi.org/10.5194/acp-22-7827-2022, https://doi.org/10.5194/acp-22-7827-2022, 2022
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Secondary organic aerosol (SOA) simulation remains uncertain, due to the unknown SOA formation mechanisms. Aerosol samples with a 4 h time resolution were collected, along with online measurements of aerosol chemical compositions and meteorological parameters. We found that anthropogenic emissions, atmospheric oxidation capacity and halogen chemistry have significant effects on the formation of biogenic SOA (BSOA). The findings of this study are helpful to better explore the missed SOA sources.
Gloria Titos, María A. Burgos, Paul Zieger, Lucas Alados-Arboledas, Urs Baltensperger, Anne Jefferson, James Sherman, Ernest Weingartner, Bas Henzing, Krista Luoma, Colin O'Dowd, Alfred Wiedensohler, and Elisabeth Andrews
Atmos. Chem. Phys., 21, 13031–13050, https://doi.org/10.5194/acp-21-13031-2021, https://doi.org/10.5194/acp-21-13031-2021, 2021
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This paper investigates the impact of water uptake on aerosol optical properties, in particular the aerosol light-scattering coefficient. Although in situ measurements are performed at low relative humidity (typically at
RH < 40 %), to address the climatic impact of aerosol particles it is necessary to take into account the effect that water uptake may have on the aerosol optical properties.
Wei Xu, Kirsten N. Fossum, Jurgita Ovadnevaite, Chunshui Lin, Ru-Jin Huang, Colin O'Dowd, and Darius Ceburnis
Atmos. Chem. Phys., 21, 8655–8675, https://doi.org/10.5194/acp-21-8655-2021, https://doi.org/10.5194/acp-21-8655-2021, 2021
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Cloud condensation nuclei (CCN) are an important topic in atmospheric studies, especially for evaluating the climate impact of aerosol. Here in this study, CCN closure is studied by using chemical composition based on an aerosol mass spectrometer (AMS) and hygroscopicity growth measurements based on a humidified tandem differential mobility analyzer (HTDMA) at the Mace Head atmospheric research station.
Wei Yuan, Ru-Jin Huang, Lu Yang, Ting Wang, Jing Duan, Jie Guo, Haiyan Ni, Yang Chen, Qi Chen, Yongjie Li, Ulrike Dusek, Colin O'Dowd, and Thorsten Hoffmann
Atmos. Chem. Phys., 21, 3685–3697, https://doi.org/10.5194/acp-21-3685-2021, https://doi.org/10.5194/acp-21-3685-2021, 2021
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We characterized the seasonal variations in nitrated aromatic compounds (NACs) in composition, sources, and their light absorption contribution to brown carbon (BrC) aerosol in Xi'an, Northwest China. Our results show that secondary formation and vehicular emission were dominant sources in summer (~80 %), and biomass burning and coal combustion were major sources in winter (~75 %), and they indicate that the composition and sources of NACs have a profound impact on the light absorption of BrC
Chunshui Lin, Darius Ceburnis, Wei Xu, Eimear Heffernan, Stig Hellebust, John Gallagher, Ru-Jin Huang, Colin O'Dowd, and Jurgita Ovadnevaite
Atmos. Chem. Phys., 20, 10513–10529, https://doi.org/10.5194/acp-20-10513-2020, https://doi.org/10.5194/acp-20-10513-2020, 2020
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Chemical composition and sources of submicron aerosols (PM1) were simultaneously investigated at a kerbside site in the Dublin city center and at a residential site in suburban Dublin (~5 km apart) during both a nonheating and a heating period in 2018. This study highlights the temporal and spatial variability of sources within the Dublin city center and the need for additional aerosol characterization studies to improve targeted mitigation solutions for a greater impact on urban air quality.
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Short summary
Source apportionment of solid-fuel-burning emissions can be complicated by the use of different fuels, stoves, and burning conditions. Here, the organic aerosol mass spectra produced from burning a range of solid fuels in several stoves were compared. This study accounts for the source variability and provides better constraints on the primary factor contributions to the ambient organic aerosol estimations, holding significant implications for public health and policymakers.
Source apportionment of solid-fuel-burning emissions can be complicated by the use of different...