Articles | Volume 16, issue 10
https://doi.org/10.5194/amt-16-2641-2023
© Author(s) 2023. 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-16-2641-2023
© Author(s) 2023. This work is distributed under
the Creative Commons Attribution 4.0 License.
the Creative Commons Attribution 4.0 License.
Research article
| 
30 May 2023
Research article |
| 30 May 2023
| 30 May 2023
An automated online field instrument to quantify the oxidative potential of aerosol particles via ascorbic acid oxidation
Battist Utinger
Department of Environmental Sciences, University of Basel, 4056 Basel, Switzerland
Steven John Campbell
Department of Environmental Sciences, University of Basel, 4056 Basel, Switzerland
Department of Atmospheric and Oceanic Sciences, University of
California at Los Angeles, Los Angeles, CA 90095-1565, USA
Nicolas Bukowiecki
Department of Environmental Sciences, University of Basel, 4056 Basel, Switzerland
Alexandre Barth
Department of Environmental Sciences, University of Basel, 4056 Basel, Switzerland
Benjamin Gfeller
Department of Environmental Sciences, University of Basel, 4056 Basel, Switzerland
Ray Freshwater
Department of Chemistry, Centre for Atmospheric Science, University of Cambridge, Cambridge, CB2 1EW, UK
Hans-Rudolf Rüegg
Department of Environmental Sciences, University of Basel, 4056 Basel, Switzerland
Markus Kalberer
CORRESPONDING AUTHOR
Department of Environmental Sciences, University of Basel, 4056 Basel, Switzerland
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Cited articles
Alpert, P. A., Dou, J., Corral Arroyo, P., Schneider, F., Xto, J., Luo, B.,
Peter, T., Huthwelker, T., Borca, C. N., Henzler, K. D., Schaefer, T.,
Herrmann, H., Raabe, J., Watts, B., Krieger, U. K., and Ammann, M.:
Photolytic radical persistence due to anoxia in viscous aerosol particles,
Nat. Commun., 12, 1–8, https://doi.org/10.1038/s41467-021-21913-x, 2021.
Bates, J. T., Fang, T., Verma, V., Zeng, L., Weber, R. J., Tolbert, P. E.,
Abrams, J. Y., Sarnat, S. E., Klein, M., Mulholland, J. A., and Russell, A.
G.: Review of Acellular Assays of Ambient Particulate Matter Oxidative
Potential: Methods and Relationships with Composition, Sources, and Health
Effects, Environ. Sci. Technol., 53, 4003–4019,
https://doi.org/10.1021/acs.est.8b03430, 2019.
Baulig, A., Garlatti, M., Bonvallot, V., Marchand, A., Barouki, R., Marano,
F., and Baeza-Squiban, A.: Involvement of reactive oxygen species in the
metabolic pathways triggered by diesel exhaust particles in human airway
epithelial cells, Am. J. Physiol.-Lung C., 285, L671–L679, https://doi.org/10.1152/ajplung.00419.2002, 2003.
Birdwell, J. E. and Engel, A. S.: Characterization of dissolved organic
matter in cave and spring waters using UV-Vis absorbance and fluorescence
spectroscopy, Org. Geochem., 41, 270–280,
https://doi.org/10.1016/J.ORGGEOCHEM.2009.11.002, 2010.
Brunekreef, B. and Holgate, S. T.: Air pollution and health, Lancet
(London, England), 360, 1233–1242, https://doi.org/10.1016/S0140-6736(02)11274-8, 2002.
Calas, A., Uzu, G., Martins, J. M. F., Voisin, D., Spadini, L., Lacroix, T.,
and Jaffrezo, J. L.: The importance of simulated lung fluid (SLF)
extractions for a more relevant evaluation of the oxidative potential of
particulate matter, Scientific Reports, 7, 1–12, https://doi.org/10.1038/s41598-017-11979-3, 2017.
Calvo, A. I., Alves, C., Castro, A., Pont, V., Vicente, A. M., and Fraile,
R.: Research on aerosol sources and chemical composition: Past, current and
emerging issues, Atmos. Res., 120–121, 1–28,
https://doi.org/10.1016/J.ATMOSRES.2012.09.021, 2013.
Campbell, S. J., Utinger, B., Lienhard, D. M., Paulson, S. E., Shen, J.,
Griffiths, P. T., Stell, A. C., and Kalberer, M.: Development of a
physiologically relevant online chemical assay to quantify aerosol oxidative
potential, Anal. Chem., 91, 13088–13095, https://doi.org/10.1021/acs.analchem.9b03282, 2019a.
Campbell, S. J., Stevanovic, S., Miljevic, B., Bottle, S. E., Ristovski, Z.,
and Kalberer, M.: Quantification of Particle-Bound Organic Radicals in
Secondary Organic Aerosol, Environ. Sci. Technol., 53, 6729–6737,
https://doi.org/10.1021/acs.est.9b00825, 2019b.
Campbell, S. J., Wolfer, K., Utinger, B., Westwood, J., Zhang, Z.-H., Bukowiecki, N., Steimer, S. S., Vu, T. V., Xu, J., Straw, N., Thomson, S., Elzein, A., Sun, Y., Liu, D., Li, L., Fu, P., Lewis, A. C., Harrison, R. M., Bloss, W. J., Loh, M., Miller, M. R., Shi, Z., and Kalberer, M.: Atmospheric conditions and composition that influence PM2.5 oxidative potential in Beijing, China, Atmos. Chem. Phys., 21, 5549–5573, https://doi.org/10.5194/acp-21-5549-2021, 2021.
Chen, G., Canonaco, F., Tobler, A., Aas, W., Alastuey, A., Allan, J.,
Atabakhsh, S., Aurela, M., Baltensperger, U., Bougiatioti, A., De Brito, J.
F., Ceburnis, D., Chazeau, B., Chebaicheb, H., Daellenbach, K. R., Ehn, M.,
El Haddad, I., Eleftheriadis, K., Favez, O., Flentje, H., Font, A., Fossum,
K., Freney, E., Gini, M., Green, D. C., Heikkinen, L., Herrmann, H.,
Kalogridis, A.-C., Keernik, H., Lhotka, R., Lin, C., Lunder, C., Maasikmets,
M., Manousakas, M. I., Marchand, N., Marin, C., Marmureanu, L.,
Mihalopoulos, N., Močnik, G., Nęcki, J., O'Dowd, C., Ovadnevaite,
J., Peter, T., Petit, J.-E., Pikridas, M., Matthew Platt, S., Pokorná,
P., Poulain, L., Priestman, M., Riffault, V., Rinaldi, M.,
Różański, K., Schwarz, J., Sciare, J., Simon, L., Skiba, A.,
Slowik, J. G., Sosedova, Y., Stavroulas, I., Styszko, K., Teinemaa, E.,
Timonen, H., Tremper, A., Vasilescu, J., Via, M., Vodička, P.,
Wiedensohler, A., Zografou, O., Cruz Minguillón, M., and Prévôt,
A. S. H.: European aerosol phenomenology – 8: Harmonised source
apportionment of organic aerosol using 22 Year-long ACSM/AMS datasets,
Environ. Int., 166, 107325, https://doi.org/10.1016/j.envint.2022.107325, 2022.
Chowdhury, P. H., He, Q., Lasitza Male, T., Brune, W. H., Rudich, Y., and
Pardo, M.: Exposure of Lung Epithelial Cells to Photochemically Aged
Secondary Organic Aerosol Shows Increased Toxic Effects, Environ. Sci.
Tech. Let., 5, 424–430, https://doi.org/10.1021/acs.estlett.8b00256, 2018.
Donaldson, K., Stone, V., Seaton, A., and MacNee, W.: Ambient particle
inhalation and the cardiovascular system: Potential mechanisms, Environ.
Health Persp., 109, 523–527, https://doi.org/10.1289/ehp.01109s4523, 2001.
Fang, T., Verma, V., Guo, H., King, L. E., Edgerton, E. S., and Weber, R. J.: A semi-automated system for quantifying the oxidative potential of ambient particles in aqueous extracts using the dithiothreitol (DTT) assay: results from the Southeastern Center for Air Pollution and Epidemiology (SCAPE), Atmos. Meas. Tech., 8, 471–482, https://doi.org/10.5194/amt-8-471-2015, 2015.
Ferreira, C. M. H., Pinto, I. S. S., Soares, E. V., and Soares, H. M. V. M.:
(Un)suitability of the use of pH buffers in biological, biochemical and
environmental studies and their interaction with metal ions – a review, RSC
Adv., 5, 30989–31003, https://doi.org/10.1039/c4ra15453c, 2015.
Fuller, S. J., Wragg, F. P. H., Nutter, J., and Kalberer, M.: Comparison of
on-line and off-line methods to quantify reactive oxygen species (ROS) in
atmospheric aerosols, Atmos. Environ., 92, 97–103,
https://doi.org/10.1016/j.atmosenv.2014.04.006, 2014.
Gao, D., Fang, T., Verma, V., Zeng, L., and Weber, R. J.: A method for measuring total aerosol oxidative potential (OP) with the dithiothreitol (DTT) assay and comparisons between an urban and roadside site of water-soluble and total OP, Atmos. Meas. Tech., 10, 2821–2835, https://doi.org/10.5194/amt-10-2821-2017, 2017.
GBD 2013 Risk Factors Collaborators: Global, regional, and national
comparative risk assessment of 79 behavioural, environmental and
occupational, and metabolic risks or clusters of risks in 188 countries,
1990–2013: A systematic analysis for the Global Burden of Disease Study
2013, Lancet, 386, 2287–2323, https://doi.org/10.1016/S0140-6736(15)00128-2, 2015.
Godri, K. J., Duggan, S. T., Fuller, G. W., Baker, T., Green, D., Kelly, F.
J., and Mudway, I. S.: Particulate matter oxidative potential from waste
transfer station activity, Environ. Health Persp., 118, 493–498,
https://doi.org/10.1289/ehp.0901303, 2010.
Godri, K. J., Harrison, R. M., Evans, T., Baker, T., Dunster, C., Mudway, I.
S., and Kelly, F. J.: Increased oxidative burden associated with traffic
component of ambient particulate matter at roadside and Urban background
schools sites in London, PLoS One, 6, e21961, https://doi.org/10.1371/journal.pone.0021961, 2011.
Hama, S. M. L., Cordell, R. L., Staelens, J., Mooibroek, D., and Monks, P.
S.: Chemical composition and source identification of PM10 in five North
Western European cities, Atmos. Res., 214, 135–149,
https://doi.org/10.1016/J.ATMOSRES.2018.07.014, 2018.
Hart, J. E., Liao, X., Hong, B., Puett, R. C., Yanosky, J. D., Suh, H.,
Kioumourtzoglou, M. A., Spiegelman, D., and Laden, F.: The association of
long-term exposure to PM2.5 on all-cause mortality in the Nurses' Health
Study and the impact of measurement-error correction, Environmental Health, 14, 38, https://doi.org/10.1186/s12940-015-0027-6, 2015.
Huang, S., Gan, W., Yan, M., Zhang, X., Zhong, Y., and Yang, X.: Differential
UV–vis absorbance can characterize the reaction of organic matter with
ClO2, Water Res., 139, 442–449, https://doi.org/10.1016/J.WATRES.2018.04.006, 2018.
Huelin, F. E.: Investigations on the stability and determination of
dehydroascorbic acid, Aust. J. Biol. Sci., 2, 346–354,
https://doi.org/10.1071/BI9490346, 1949.
Isaacs, N. S. and Van Eldik, R.: A mechanistic study of the reduction of
quinones by ascorbic acid, J. Chem. Soc. Perk. T. 2, 8, 1465–1467,
https://doi.org/10.1039/a701072i, 1997.
Kamphus, M., Ettner-Mahl, M., Klimach, T., Drewnick, F., Keller, L., Cziczo, D. J., Mertes, S., Borrmann, S., and Curtius, J.: Chemical composition of ambient aerosol, ice residues and cloud droplet residues in mixed-phase clouds: single particle analysis during the Cloud and Aerosol Characterization Experiment (CLACE 6), Atmos. Chem. Phys., 10, 8077–8095, https://doi.org/10.5194/acp-10-8077-2010, 2010.
Keller, A., Kalbermatter, D. M., Wolfer, K., Specht, P., Steigmeier, P.,
Resch, J., Kalberer, M., Hammer, T., and Vasilatou, K.: The organic coating
unit, an all-in-one system for reproducible generation of secondary organic
matter aerosol, Aerosol Sci. Technol., 56, 947–958,
https://doi.org/10.1080/02786826.2022.2110448, 2022.
Koike, E. and Kobayashi, T.: Chemical and biological oxidative effects of
carbon black nanoparticles, Chemosphere, 65, 946–951,
https://doi.org/10.1016/j.chemosphere.2006.03.078, 2006.
Kostenidou, E., Pandis, S. N., Pathak, R. K., Pandis, S. N., Kostenidou, E.,
and Pandis, S. N.: An Algorithm for the Calculation of Secondary Organic
Aerosol Density Combining AMS and SMPS Data, Aerosol Sci. Tech., 41, 1002–1010, https://doi.org/10.1080/02786820701666270, 2007.
Künzi, L., Mertes, P., Schneider, S., Jeannet, N., Menzi, C., Dommen, J., Baltensperger, U., Prévôt, A. S. H., Salathe, M., Kalberer, M., and Geiser, M.: Responses of lung cells to realistic exposure of primary and aged carbonaceous aerosols, Atmos. Environ., 68, 143–150, https://doi.org/10.1016/j.atmosenv.2012.11.055, 2013.
Laden, F., Schwartz, J., Speizer, F. E., and Dockery, D. W.: Reduction in
fine particulate air pollution and mortality: Extended follow-up of the
Harvard Six Cities Study, Am. J. Resp. Crit. Care, 173, 667–672,
https://doi.org/10.1164/rccm.200503-443OC, 2006.
Lehman, S. E., Morris, A. S., Mueller, P. S., Salem, A. K., Grassian, V. H.,
and Larsen, S. C.: Silica nanoparticle-generated ROS as a predictor of
cellular toxicity: Mechanistic insights and safety by design, Environ. Sci.-Nano, 3, 56–66, https://doi.org/10.1039/c5en00179j, 2016.
Lepeule, J., Laden, F., Dockery, D., and Schwartz, J.: Chronic exposure to
fine particles and mortality: An extended follow-up of the Harvard six
cities study from 1974 to 2009, Environ. Health Persp., 120, 965–970,
https://doi.org/10.1289/ehp.1104660, 2012.
Li, N., Hao, M., Phalen, R. F., Hinds, W. C., and Nel, A. E.: Particulate air
pollutants and asthma: A paradigm for the role of oxidative stress in
PM-induced adverse health effects, Clin. Immunol., 109, 250–265,
https://doi.org/10.1016/j.clim.2003.08.006, 2003.
Lufthygiene Amt beider Basel: Luftqualität Nordwestschweiz,
https://luftqualitaet.ch/messdaten/datenarchiv/abfrage, last access: 7 January 2023.
McWhinney, R. D., Zhou, S., and Abbatt, J. P. D.: Naphthalene SOA: redox activity and naphthoquinone gas–particle partitioning, Atmos. Chem. Phys., 13, 9731–9744, https://doi.org/10.5194/acp-13-9731-2013, 2013.
Oberdörster, G., Oberdörster, E., and Oberdörster, J.:
Nanotoxicology: An emerging discipline evolving from studies of ultrafine
particles, Environ. Health Persp., 113, 823–839, https://doi.org/10.1289/ehp.7339, 2005.
Offer, S., Hartner, E., Di Bucchianico, S., Bisig, C., Bauer, S., Pantzke,
J., Zimmermann, E. J., Cao, X., Binder, S., Kuhn, E., Huber, A., Jeong, S.,
Käfer, U., Martens, P., Mesceriakovas, A., Bendl, J., Brejcha, R.,
Buchholz, A., Gat, D., Hohaus, T., Rastak, N., Jakobi, G., Kalberer, M.,
Kanashova, T., Hu, Y., Ogris, C., Marsico, A., Theis, F., Pardo, M.,
Gröger, T., Oeder, S., Orasche, J., Paul, A., Ziehm, T., Zhang, Z.-H.
H., Adam, T., Sippula, O., Sklorz, M., Schnelle-Kreis, J., Czech, H.,
Kiendler-Scharr, A., Rudich, Y., and Zimmermann, R.: Effect of Atmospheric
Aging on Soot Particle Toxicity in Lung Cell Models at the Air-Liquid
Interface: Differential Toxicological Impacts of Biogenic and Anthropogenic
Secondary Organic Aerosols (SOAs), Environ. Health Persp., 130, 1–19,
https://doi.org/10.1289/EHP9413, 2022.
Pietrogrande, M. C., Bertoli, I., Manarini, F., and Russo, M.: Ascorbate
assay as a measure of oxidative potential for ambient particles: Evidence
for the importance of cell-free surrogate lung fluid composition, Atmos.
Environ., 211, 103–112, https://doi.org/10.1016/j.atmosenv.2019.05.012, 2019.
Pietrogrande, M. C., Romanato, L., and Russo, M.: Synergistic and
Antagonistic Effects of Aerosol Components on Its Oxidative Potential as
Predictor of Particle Toxicity, Toxics, 10, 196, https://doi.org/10.3390/TOXICS10040196, 2022.
Prahalad, A. K., Inmon, J., Dailey, L. A., Madden, M. C., Ghio, A. J., and
Gallagher, J. E.: Air pollution particles mediated oxidative DNA base damage
in a cell free system and in human airway epithelial cells in relation to
particulate metal content and bioreactivity, Chem. Res. Toxicol., 14,
879–887, https://doi.org/10.1021/tx010022e, 2001.
Roginsky, V. A., Barsukova, T. K., and Stegmann, H. B.: Kinetics of redox
interaction between substituted quinones and ascorbate under aerobic
conditions, Chem.-Biol. Interact., 121, 177–197, https://doi.org/10.1016/S0009-2797(99)00099-X, 1999.
Salana, S., Wang, Y., Puthussery, J. V., and Verma, V.: A semi-automated instrument for cellular oxidative potential evaluation (SCOPE) of water-soluble extracts of ambient particulate matter, Atmos. Meas. Tech., 14, 7579–7593, https://doi.org/10.5194/amt-14-7579-2021, 2021.
Shen, J., Griffiths, P. T., Campbell, S. J., Utinger, B., Kalberer, M., and
Paulson, S. E.: Ascorbate oxidation by iron, copper and reactive oxygen
species: review, model development, and derivation of key rate constants,
Sci. Rep.-UK, 11, 1–14, https://doi.org/10.1038/s41598-021-86477-8, 2021.
Shi, Z., Vu, T., Kotthaus, S., Harrison, R. M., Grimmond, S., Yue, S., Zhu, T., Lee, J., Han, Y., Demuzere, M., Dunmore, R. E., Ren, L., Liu, D., Wang, Y., Wild, O., Allan, J., Acton, W. J., Barlow, J., Barratt, B., Beddows, D., Bloss, W. J., Calzolai, G., Carruthers, D., Carslaw, D. C., Chan, Q., Chatzidiakou, L., Chen, Y., Crilley, L., Coe, H., Dai, T., Doherty, R., Duan, F., Fu, P., Ge, B., Ge, M., Guan, D., Hamilton, J. F., He, K., Heal, M., Heard, D., Hewitt, C. N., Hollaway, M., Hu, M., Ji, D., Jiang, X., Jones, R., Kalberer, M., Kelly, F. J., Kramer, L., Langford, B., Lin, C., Lewis, A. C., Li, J., Li, W., Liu, H., Liu, J., Loh, M., Lu, K., Lucarelli, F., Mann, G., McFiggans, G., Miller, M. R., Mills, G., Monk, P., Nemitz, E., O'Connor, F., Ouyang, B., Palmer, P. I., Percival, C., Popoola, O., Reeves, C., Rickard, A. R., Shao, L., Shi, G., Spracklen, D., Stevenson, D., Sun, Y., Sun, Z., Tao, S., Tong, S., Wang, Q., Wang, W., Wang, X., Wang, X., Wang, Z., Wei, L., Whalley, L., Wu, X., Wu, Z., Xie, P., Yang, F., Zhang, Q., Zhang, Y., Zhang, Y., and Zheng, M.: Introduction to the special issue “In-depth study of air pollution sources and processes within Beijing and its surrounding region (APHH-Beijing)”, Atmos. Chem. Phys., 19, 7519–7546, https://doi.org/10.5194/acp-19-7519-2019, 2019.
Steenhof, M., Gosens, I., Strak, M., Godri, K. J., Hoek, G., Cassee, F. R.,
Mudway, I. S., Kelly, F. J., Harrison, R. M., Lebret, E., Brunekreef, B.,
Janssen, N. A. H., and Pieters, R. H. H.: In vitro toxicity of particulate matter (PM) collected at different sites in the Netherlands is associated with PM composition, size fraction and oxidative potential - the RAPTES project, Part. Fibre Toxicol., 8, 26, https://doi.org/10.1186/1743-8977-8-26, 2011.
Steimer, S. S., Delvaux, A., Campbell, S. J., Gallimore, P. J., Grice, P., Howe, D. J., Pitton, D., Claeys, M., Hoffmann, T., and Kalberer, M.: Synthesis and characterisation of peroxypinic acids as proxies for highly oxygenated molecules (HOMs) in secondary organic aerosol, Atmos. Chem. Phys., 18, 10973–10983, https://doi.org/10.5194/acp-18-10973-2018, 2018.
Timonen, H., Aurela, M., Carbone, S., Saarnio, K., Frey, A., Saarikoski, S.,
Teinilä, K., Kulmala, M., and Hillamo, R.: Seasonal and diurnal changes
in inorganic ions, carbonaceous matter and mass in ambient aerosol particles
in an urban, background area, Boreal Environ. Res., 19, 71–86, https://helda.helsinki.fi/handle/10138/160095 (last access: 27 December 2022), 2014.
Tuet, W. Y., Chen, Y., Fok, S., Gao, D., Weber, R. J., Champion, J. A., and
Ng, N. L.: Chemical and cellular oxidant production induced by naphthalene
secondary organic aerosol (SOA): Effect of redox-active metals and
photochemical aging, Sci. Rep.-UK, 7, 1–10, https://doi.org/10.1038/s41598-017-15071-8, 2017.
Venkatachari, P., Hopke, P. K., Grover, B. D., and Eatough, D. J.:
Measurement of particle-bound reactive oxygen species in rubidoux aerosols,
J. Atmos. Chem., 50, 49–58, https://doi.org/10.1007/s10874-005-1662-z, 2005.
Wang, S., Zhao, Y., Chan, A. W. H., Yao, M., Chen, Z., and Abbatt, J. P. D.:
Organic Peroxides in Aerosol: Key Reactive Intermediates for Multiphase
Processes in the Atmosphere, Chem. Rev., 123, 1635–1679, https://doi.org/10.1021/acs.chemrev.2c00430, 2023.
Wang, Y., Hopke, P. K., Sun, L., Chalupa, D. C., and Utell, M. J.: Laboratory
and Field Testing of an Automated Atmospheric Particle-Bound Reactive Oxygen
Species Sampling-Analysis System, Journal of Toxicology, 2011, 419476,
https://doi.org/10.1155/2011/419476, 2011.
Weber, R. J., Orsini, D., Daun, Y., Lee, Y. N., Klotz, P. J., and Brechtel,
F.: A Particle-into-Liquid Collector for Rapid Measurement of Aerosol Bulk
Chemical Composition, Aerosol Sci. Tech., 35, 718–727, https://doi.org/10.1080/02786820152546761, 2010.
World Health Organisation: Ambient Air Pollution: A Global Assessment of
Exposure and Burden of Disease, World Health Organization,
https://www.who.int/publications/i/item/9789241511353
(last access: 8 February 2021), 2016.
Wragg, F. P. H., Fuller, S. J., Freshwater, R., Green, D. C., Kelly, F. J., and Kalberer, M.: An automated online instrument to quantify aerosol-bound reactive oxygen species (ROS) for ambient measurement and health-relevant aerosol studies, Atmos. Meas. Tech., 9, 4891–4900, https://doi.org/10.5194/amt-9-4891-2016, 2016.
Yang, A., Janssen, N. A. H., Brunekreef, B., Cassee, F. R., Hoek, G., and
Gehring, U.: Children's respiratory health and oxidative potential of PM2.5: the PIAMA birth cohort study, Occup. Environ. Med., 73, 154–160,
https://doi.org/10.1136/oemed-2015-103175, 2016.
Zhang, Z.-H., Hartner, E., Utinger, B., Gfeller, B., Paul, A., Sklorz, M., Czech, H., Yang, B. X., Su, X. Y., Jakobi, G., Orasche, J., Schnelle-Kreis, J., Jeong, S., Gröger, T., Pardo, M., Hohaus, T., Adam, T., Kiendler-Scharr, A., Rudich, Y., Zimmermann, R., and Kalberer, M.: Are reactive oxygen species (ROS) a suitable metric to predict toxicity of carbonaceous aerosol particles?, Atmos. Chem. Phys., 22, 1793–1809, https://doi.org/10.5194/acp-22-1793-2022, 2021.
Zhao, R., Kenseth, C. M., Huang, Y., Dalleska, N. F., Kuang, X. M., Chen,
J., Paulson, S. E., and Seinfeld, J. H.: Rapid Aqueous-Phase Hydrolysis of
Ester Hydroperoxides Arising from Criegee Intermediates and Organic Acids,
J. Phys. Chem. A, 122, 5190–5201, https://doi.org/10.1021/acs.jpca.8b02195, 2018.
Short summary
Exposure to atmospheric aerosols can lead to adverse health effect, but particle components responsible for this are unknown. Redox-active compounds, some with very short lifetimes, are considered to be a toxic class of compounds in particles. We developed the first online field instrument to quantify short-lived and stable redox-active compounds with a physiological assay based on ascorbic acid and a high time resolution and detection limits to allow measurements at unpolluted locations.
Exposure to atmospheric aerosols can lead to adverse health effect, but particle components...
