Articles | Volume 22, issue 2
https://doi.org/10.5194/acp-22-917-2022
© 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-22-917-2022
© Author(s) 2022. This work is distributed under
the Creative Commons Attribution 4.0 License.
the Creative Commons Attribution 4.0 License.
Research article
| 
19 Jan 2022
Research article |
| 19 Jan 2022
| 19 Jan 2022
Secondary organic aerosol formation from the oxidation of decamethylcyclopentasiloxane at atmospherically relevant OH concentrations
Sophia M. Charan
Division of Chemistry and Chemical Engineering, California Institute of Technology, Pasadena, California 91125, USA
Yuanlong Huang
Division of Geological and Planetary Sciences, California Institute of Technology, Pasadena, California 91125, USA
Reina S. Buenconsejo
Division of Chemistry and Chemical Engineering, California Institute of Technology, Pasadena, California 91125, USA
Qi Li
Department of Chemical and Environmental Engineering, University of California – Riverside, Riverside, California 92521, USA
David R. Cocker III
Department of Chemical and Environmental Engineering, University of California – Riverside, Riverside, California 92521, USA
Division of Chemistry and Chemical Engineering, California Institute of Technology, Pasadena, California 91125, USA
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EGUsphere, https://doi.org/10.5194/egusphere-2025-5323, https://doi.org/10.5194/egusphere-2025-5323, 2025
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This study reveals a novel Ultraviolet A-driven, metal-free mechanism for aqueous-phase tetravalent sulfur (S(IV)) oxidation that leads to organosulfates formation, addressing a critical knowledge gap in atmospheric sulfur and organic aerosol chemistry and highlighting a previously overlooked photochemical pathway with broad environmental implications.
Yuchen Wang, Xiang Zhang, Yuanlong Huang, Yutong Liang, and Nga L. Ng
Atmos. Chem. Phys., 25, 5215–5231, https://doi.org/10.5194/acp-25-5215-2025, https://doi.org/10.5194/acp-25-5215-2025, 2025
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This work provides the first fundamental laboratory data to evaluate SOA (secondary organic aerosol) production from styrene and NO3 chemistry. Additionally, the formation mechanisms of aromatic organic nitrates (ONs) are reported, highlighting that previously identified nitroaromatics in ambient field campaigns can be aromatic ONs. Finally, the hydrolysis lifetimes observed for ONs generated from styrene and NO3 oxidation can serve as experimentally constrained parameters for modeling hydrolysis of aromatic ONs in general.
Reina S. Buenconsejo, Sophia M. Charan, John H. Seinfeld, and Paul O. Wennberg
Atmos. Chem. Phys., 25, 1883–1897, https://doi.org/10.5194/acp-25-1883-2025, https://doi.org/10.5194/acp-25-1883-2025, 2025
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We look at the atmospheric chemistry of a volatile chemical product (VCP), benzyl alcohol. Benzyl alcohol and other VCPs may play a significant role in the formation of urban smog. By better understanding the chemistry of VCPs like benzyl alcohol, we may better understand observed data and how VCPs affect air quality. We identify products formed from benzyl alcohol chemistry and use this chemistry to understand how benzyl alcohol forms a key component of smog, secondary organic aerosol.
Tianle Pan, Andrew T. Lambe, Weiwei Hu, Yicong He, Minghao Hu, Huaishan Zhou, Xinming Wang, Qingqing Hu, Hui Chen, Yue Zhao, Yuanlong Huang, Doug R. Worsnop, Zhe Peng, Melissa A. Morris, Douglas A. Day, Pedro Campuzano-Jost, Jose-Luis Jimenez, and Shantanu H. Jathar
Atmos. Meas. Tech., 17, 4915–4939, https://doi.org/10.5194/amt-17-4915-2024, https://doi.org/10.5194/amt-17-4915-2024, 2024
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This study systematically characterizes the temperature enhancement in the lamp-enclosed oxidation flow reactor (OFR). The enhancement varied multiple dimensional factors, emphasizing the complexity of temperature inside of OFR. The effects of temperature on the flow field and gas- or particle-phase reaction inside OFR were also evaluated with experiments and model simulations. Finally, multiple mitigation strategies were demonstrated to minimize this temperature increase.
Ningjin Xu, Chen Le, David R. Cocker, Kunpeng Chen, Ying-Hsuan Lin, and Don R. Collins
Atmos. Meas. Tech., 17, 4227–4243, https://doi.org/10.5194/amt-17-4227-2024, https://doi.org/10.5194/amt-17-4227-2024, 2024
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A flow-through reactor was developed that exposes known mixtures of gases or ambient air to very high concentrations of the oxidants that are responsible for much of the chemistry that takes place in the atmosphere. Like other reactors of its type, it is primarily used to study the formation of particulate matter from the oxidation of common gases. Unlike other reactors of its type, it can simulate the chemical reactions that occur in liquid water that is present in particles or cloud droplets.
Qindan Zhu, Rebecca H. Schwantes, Matthew Coggon, Colin Harkins, Jordan Schnell, Jian He, Havala O. T. Pye, Meng Li, Barry Baker, Zachary Moon, Ravan Ahmadov, Eva Y. Pfannerstill, Bryan Place, Paul Wooldridge, Benjamin C. Schulze, Caleb Arata, Anthony Bucholtz, John H. Seinfeld, Carsten Warneke, Chelsea E. Stockwell, Lu Xu, Kristen Zuraski, Michael A. Robinson, J. Andrew Neuman, Patrick R. Veres, Jeff Peischl, Steven S. Brown, Allen H. Goldstein, Ronald C. Cohen, and Brian C. McDonald
Atmos. Chem. Phys., 24, 5265–5286, https://doi.org/10.5194/acp-24-5265-2024, https://doi.org/10.5194/acp-24-5265-2024, 2024
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Volatile organic compounds (VOCs) fuel the production of air pollutants like ozone and particulate matter. The representation of VOC chemistry remains challenging due to its complexity in speciation and reactions. Here, we develop a chemical mechanism, RACM2B-VCP, that better represents VOC chemistry in urban areas such as Los Angeles. We also discuss the contribution of VOCs emitted from volatile chemical products and other anthropogenic sources to total VOC reactivity and O3.
Elyse A. Pennington, Yuan Wang, Benjamin C. Schulze, Karl M. Seltzer, Jiani Yang, Bin Zhao, Zhe Jiang, Hongru Shi, Melissa Venecek, Daniel Chau, Benjamin N. Murphy, Christopher M. Kenseth, Ryan X. Ward, Havala O. T. Pye, and John H. Seinfeld
Atmos. Chem. Phys., 24, 2345–2363, https://doi.org/10.5194/acp-24-2345-2024, https://doi.org/10.5194/acp-24-2345-2024, 2024
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To assess the air quality in Los Angeles (LA), we improved the CMAQ model by using dynamic traffic emissions and new secondary organic aerosol schemes to represent volatile chemical products. Source apportionment demonstrates that the urban areas of the LA Basin and vicinity are NOx-saturated, with the largest sensitivity of O3 to changes in volatile organic compounds in the urban core. The improvement and remaining issues shed light on the future direction of the model development.
Clara M. Nussbaumer, Bryan K. Place, Qindan Zhu, Eva Y. Pfannerstill, Paul Wooldridge, Benjamin C. Schulze, Caleb Arata, Ryan Ward, Anthony Bucholtz, John H. Seinfeld, Allen H. Goldstein, and Ronald C. Cohen
Atmos. Chem. Phys., 23, 13015–13028, https://doi.org/10.5194/acp-23-13015-2023, https://doi.org/10.5194/acp-23-13015-2023, 2023
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NOx is a precursor to hazardous tropospheric ozone and can be emitted from various anthropogenic sources. It is important to quantify NOx emissions in urban environments to improve the local air quality, which still remains a challenge, as sources are heterogeneous in space and time. In this study, we calculate NOx emissions over Los Angeles, based on aircraft measurements in June 2021, and compare them to a local emission inventory, which we find mostly overpredicts the measured values.
Eva Y. Pfannerstill, Caleb Arata, Qindan Zhu, Benjamin C. Schulze, Roy Woods, John H. Seinfeld, Anthony Bucholtz, Ronald C. Cohen, and Allen H. Goldstein
Atmos. Chem. Phys., 23, 12753–12780, https://doi.org/10.5194/acp-23-12753-2023, https://doi.org/10.5194/acp-23-12753-2023, 2023
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The San Joaquin Valley is an agricultural area with poor air quality. Organic gases drive the formation of hazardous air pollutants. Agricultural emissions of these gases are not well understood and have rarely been quantified at landscape scale. By combining aircraft-based emission measurements with land cover information, we found mis- or unrepresented emission sources. Our results help in understanding of pollution sources and in improving predictions of air quality in agricultural regions.
Qindan Zhu, Bryan Place, Eva Y. Pfannerstill, Sha Tong, Huanxin Zhang, Jun Wang, Clara M. Nussbaumer, Paul Wooldridge, Benjamin C. Schulze, Caleb Arata, Anthony Bucholtz, John H. Seinfeld, Allen H. Goldstein, and Ronald C. Cohen
Atmos. Chem. Phys., 23, 9669–9683, https://doi.org/10.5194/acp-23-9669-2023, https://doi.org/10.5194/acp-23-9669-2023, 2023
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Nitrogen oxide (NOx) is a hazardous air pollutant, and it is the precursor of short-lived climate forcers like tropospheric ozone and aerosol particles. While NOx emissions from transportation has been strictly regulated, soil NOx emissions are overlooked. We use the airborne flux measurements to observe NOx emissions from highways and urban and cultivated soil land cover types. We show non-negligible soil NOx emissions, which are significantly underestimated in current model simulations.
Yuchen Wang, Xvli Guo, Yajie Huo, Mengying Li, Yuqing Pan, Shaocai Yu, Alexander Baklanov, Daniel Rosenfeld, John H. Seinfeld, and Pengfei Li
Atmos. Chem. Phys., 23, 5233–5249, https://doi.org/10.5194/acp-23-5233-2023, https://doi.org/10.5194/acp-23-5233-2023, 2023
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Substantial advances have been made in recent years toward detecting and quantifying methane super-emitters from space. However, such advances have rarely been expanded to measure the global methane pledge because large-scale swaths and high-resolution sampling have not been coordinated. Here we present a versatile spaceborne architecture that can juggle planet-scale and plant-level methane retrievals, challenge official emission reports, and remain relevant for stereoscopic measurements.
Mengying Li, Shaocai Yu, Xue Chen, Zhen Li, Yibo Zhang, Zhe Song, Weiping Liu, Pengfei Li, Xiaoye Zhang, Meigen Zhang, Yele Sun, Zirui Liu, Caiping Sun, Jingkun Jiang, Shuxiao Wang, Benjamin N. Murphy, Kiran Alapaty, Rohit Mathur, Daniel Rosenfeld, and John H. Seinfeld
Atmos. Chem. Phys., 22, 11845–11866, https://doi.org/10.5194/acp-22-11845-2022, https://doi.org/10.5194/acp-22-11845-2022, 2022
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This study constructed an emission inventory of condensable particulate matter (CPM) in China with a focus on organic aerosols (OAs), based on collected CPM emission information. The results show that OA emissions are enhanced twofold for the years 2014 and 2017 after the inclusion of CPM in the new inventory. Sensitivity cases demonstrated the significant contributions of CPM emissions from stationary combustion and mobile sources to primary, secondary, and total OA concentrations.
Shenglun Wu, Hyung Joo Lee, Andrea Anderson, Shang Liu, Toshihiro Kuwayama, John H. Seinfeld, and Michael J. Kleeman
Atmos. Chem. Phys., 22, 4929–4949, https://doi.org/10.5194/acp-22-4929-2022, https://doi.org/10.5194/acp-22-4929-2022, 2022
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An ozone control experiment usually conducted in the laboratory was installed in a trailer and moved to the outdoor environment to directly confirm that we are controlling the right sources in order to lower ambient ozone concentrations. Adding small amounts of precursor oxides of nitrogen and volatile organic compounds to ambient air showed that the highest ozone concentrations are best controlled by reducing concentrations of oxides of nitrogen. The results confirm satellite measurements.
Qi Li, Jia Jiang, Isaac K. Afreh, Kelley C. Barsanti, and David R. Cocker III
Atmos. Chem. Phys., 22, 3131–3147, https://doi.org/10.5194/acp-22-3131-2022, https://doi.org/10.5194/acp-22-3131-2022, 2022
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Chamber-derived secondary organic aerosol (SOA) yields from camphene are reported for the first time. The role of peroxy radicals (RO2) was investigated using chemically detailed box models. We observed higher SOA yields (up to 64 %) in the experiments with added NOx than without due to the formation of highly oxygenated organic molecules (HOMs) when
NOx is present. This work can improve the representation of camphene in air quality models and provide insights into other monoterpene studies.
Elyse A. Pennington, Karl M. Seltzer, Benjamin N. Murphy, Momei Qin, John H. Seinfeld, and Havala O. T. Pye
Atmos. Chem. Phys., 21, 18247–18261, https://doi.org/10.5194/acp-21-18247-2021, https://doi.org/10.5194/acp-21-18247-2021, 2021
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Volatile chemical products (VCPs) are commonly used consumer and industrial items that contribute to the formation of atmospheric aerosol. We implemented the emissions and chemistry of VCPs in a regional-scale model and compared predictions with measurements made in Los Angeles. Our results reduced model bias and suggest that VCPs may contribute up to half of anthropogenic secondary organic aerosol in Los Angeles and are an important source of human-influenced particular matter in urban areas.
Linhui Jiang, Yan Xia, Lu Wang, Xue Chen, Jianjie Ye, Tangyan Hou, Liqiang Wang, Yibo Zhang, Mengying Li, Zhen Li, Zhe Song, Yaping Jiang, Weiping Liu, Pengfei Li, Daniel Rosenfeld, John H. Seinfeld, and Shaocai Yu
Atmos. Chem. Phys., 21, 16985–17002, https://doi.org/10.5194/acp-21-16985-2021, https://doi.org/10.5194/acp-21-16985-2021, 2021
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This paper establishes a bottom-up approach to reveal a unique pattern of urban on-road vehicle emissions at a spatial resolution 1–3 orders of magnitude higher than current inventories. The results show that the hourly average on-road vehicle emissions of CO, NOx, HC, and PM2.5 are 74 kg, 40 kg, 8 kg, and 2 kg, respectively. Integrating our traffic-monitoring-based approach with urban measurements, we could address major data gaps between urban air pollutant emissions and concentrations.
Weimeng Kong, Stavros Amanatidis, Huajun Mai, Changhyuk Kim, Benjamin C. Schulze, Yuanlong Huang, Gregory S. Lewis, Susanne V. Hering, John H. Seinfeld, and Richard C. Flagan
Atmos. Meas. Tech., 14, 5429–5445, https://doi.org/10.5194/amt-14-5429-2021, https://doi.org/10.5194/amt-14-5429-2021, 2021
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We present the design, modeling, and experimental characterization of the nano-scanning electrical mobility spectrometer (nSEMS), a recently developed instrument that probes particle physical properties in the 1.5–25 nm range. The nSEMS has proven to be extremely powerful in examining atmospheric nucleation and the subsequent growth of nanoparticles in the CERN CLOUD experiment, which provides a valuable asset to study atmospheric nanoparticles and to evaluate their impact on climate.
Stavros Amanatidis, Yuanlong Huang, Buddhi Pushpawela, Benjamin C. Schulze, Christopher M. Kenseth, Ryan X. Ward, John H. Seinfeld, Susanne V. Hering, and Richard C. Flagan
Atmos. Meas. Tech., 14, 4507–4516, https://doi.org/10.5194/amt-14-4507-2021, https://doi.org/10.5194/amt-14-4507-2021, 2021
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We assess the performance of a highly portable mobility analyzer, the Spider DMA, in measuring ambient aerosol particle size distributions, with specific attention to its moderate sizing resolution (R=3). Long-term field testing showed excellent correlation with a conventional mobility analyzer (R=10) over the 17–500 nm range, suggesting that moderate resolution may be sufficient to obtain key properties of ambient size distributions, enabling smaller instruments and better counting statistics.
Dana L. McGuffin, Yuanlong Huang, Richard C. Flagan, Tuukka Petäjä, B. Erik Ydstie, and Peter J. Adams
Geosci. Model Dev., 14, 1821–1839, https://doi.org/10.5194/gmd-14-1821-2021, https://doi.org/10.5194/gmd-14-1821-2021, 2021
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Atmospheric particle formation, emissions, and growth process rates are significant sources of uncertainty in predicting climate change. We aim to reduce that uncertainty by using measurements from several ground-based sites across Europe. We developed an estimation technique to adapt the governing process rates so model–measurement bias decays. The estimation framework developed has potential to improve model predictions while providing insight into the underlying atmospheric particle physics.
Cited articles
Ahrens, L., Harner, T., and Shoeib, M.:
Temporal Variations of Cyclic and Linear Volatile Methylsiloxanes in the Atmosphere Using Passive Samplers and High-Volume Air Samplers,
Environ. Sci. Technol.,
48, 9374–9381, https://doi.org/10.1021/es502081j, 2014. a
Atkinson, R.:
Kinetics of the Gas-Phase Reactions of a Series of Organosilicon Compounds with OH and NO3 Radicals and O3 at 297 ± 2 K,
Environ. Sci. Technol.,
25, 863–866, https://doi.org/10.1021/es00017a005, 1991. a, b
Balducci, C., Perilli, M., Romagnoli, P., and Cecinato, A.:
New Developments on Emerging Organic Pollutants in the Atmosphere,
Environ. Sci. Pollut. R.,
19, 1875–1884, https://doi.org/10.1007/s11356-012-0815-2, 2012. a
Bruns, E. A., El Haddad, I., Keller, A., Klein, F., Kumar, N. K., Pieber, S. M., Corbin, J. C., Slowik, J. G., Brune, W. H., Baltensperger, U., and Prévôt, A. S. H.: Inter-comparison of laboratory smog chamber and flow reactor systems on organic aerosol yield and composition, Atmos. Meas. Tech., 8, 2315–2332, https://doi.org/10.5194/amt-8-2315-2015, 2015. a
Burkholder, J. B., Abbatt, J. P., Barnes, I., Roberts, J. M., Melamed, M. L., Ammann, M., Bertram, A. K., Cappa, C. D., Carlton, A. M. G., Carpenter, L. J., Crowley, J. N., Dubowski, Y., George, C., Heard, D. E., Herrmann, H., Keutsch, F. N., Kroll, J. H., McNeill, V. F., Ng, N. L., Nizkorodov, S. A., Orlando, J. J., Percival, C. J., Picquet-Varrault, B., Rudich, Y., Seakins, P. W., Surratt, J. D., Tanimoto, H., Thornton, J. A., Zhu, T., Tyndall, G. S., Wahner, A., Weschler, C. J., Wilson, K. R., and Ziemann, P. J.:
The Essential Role for Laboratory Studies in Atmospheric Chemistry,
Environ. Sci. Technol.,
51, 2519–2528, https://doi.org/10.1021/acs.est.6b04947, 2017. a
Buser, A. M., Kierkegaard, A., Bogdal, C., MacLeod, M., Scheringer, M., and Hungerbühler, K.:
Concentrations in Ambient Air and Emissions of Cyclic Volatile Methylsiloxanes in Zurich, Switzerland,
Environ. Sci. Technol.,
47, 7045–7051, https://doi.org/10.1021/es3046586, 2013. a
Buser, A. M., Bogdal, C., MacLeod, M., and Scheringer, M.:
Emissions of Decamethylcyclopentasiloxane from Chicago,
Chemosphere,
107, 473–475, https://doi.org/10.1016/j.chemosphere.2013.12.034, 2014. a
Bzdek, B. R., Horan, A. J., Pennington, M. R., Janechek, N. J., Baek, J., Stanier, C. O., and Johnston, M. V.:
Silicon is a Frequent Component of Atmospheric Nanoparticles,
Environ. Sci. Technol.,
48, 11137–11145, https://doi.org/10.1021/es5026933, 2014. a
Carter, L., Perry, J., Kayatin, M. J., Wilson, M., Gentry, G. J., Bowman, E., Monje, O., Rector, T., and Steele, J.:
Process Development for Removal of Siloxanes from ISS Atmosphere,
in: 45th International Conference on Environmental Systems (12–16 July 2015), 74, Bellevue, Washington,
available at: http://hdl.handle.net/2346/64361 (last access: 20 October 2020), 2015. a
Chandramouli, B. and Kamens, R. M.:
The photochemical formation and gas–particle partitioning of oxidation products of decamethyl cyclopentasiloxane and decamethyl tetrasiloxane in the atmosphere,
Atmos. Environ.,
35, 87–95, https://doi.org/10.1016/S1352-2310(00)00289-2, 2001. a
Charan, S. M.: Experiment Set: D5 Chamber Experiments, Index of Chamber Atmospheric Research in the United States (ICARUS) [data set], available at: https://icarus.ucdavis.edu/experimentset/220, last access: 29 September 2021. a
Charan, S. M. and Huang, Y.: Experiment Set: D5 CPOT Experiments, Index of Chamber Atmospheric Research in the United States (ICARUS) [data set], https://icarus.ucdavis.edu/experimentset/221, last access: 29 September 2021. a
Charan, S. M., Kong, W., Flagan, R. C., and Seinfeld, J. H.:
Effect of Particle Charge on Aerosol Dynamics in Teflon Environmental Chambers,
Aerosol Sci. Technol.,
52, 854–871, https://doi.org/10.1080/02786826.2018.1474167, 2018. a
Charan, S. M., Buenconsejo, R. S., and Seinfeld, J. H.: Secondary organic aerosol yields from the oxidation of benzyl alcohol, Atmos. Chem. Phys., 20, 13167–13190, https://doi.org/10.5194/acp-20-13167-2020, 2020. a, b, c
Coggon, M. M., McDonald, B. C., Vlasenko, A., Veres, P. R., Bernard, F., Koss, A. R., Yuan, B., Gilman, J. B., Peischl, J., Aikin, K. C., Durant, J., Warneke, C., Li, S. M., and De Gouw, J. A.:
Diurnal Variability and Emission Pattern of Decamethylcyclopentasiloxane (D5) from the Application of Personal Care Products in Two North American Cities,
Environ. Sci. Technol.,
52, 5610–5618, https://doi.org/10.1021/acs.est.8b00506, 2018. a
Finewax, Z., Pagonis, D., Claflin, M. S., Handschy, A. V., Brown, W. L., Jenks, O., Nault, B. A., Day, D. A., Lerner, B. M., Jimenez, J. L., Ziemann, P. J., and de Gouw, J. A.:
Quantification and Source Characterization of Volatile Organic Compounds from Exercising and Application of Chlorine-Based Cleaning Products in a University Athletic Center,
Indoor Air,
31, 1–17, https://doi.org/10.1111/ina.12781, 2020. a
Fu, Z., Xie, H. B., Elm, J., Guo, X., Fu, Z., Fu, Z., and Chen, J.:
Formation of Low-Volatile Products and Unexpected High Formaldehyde Yield from the Atmospheric Oxidation of Methylsiloxanes,
Environ. Sci. Technol.,
54, 7136–7145, https://doi.org/10.1021/acs.est.0c01090, 2020. a
Gkatzelis, G. I., Coggon, M. M., McDonald, B. C., Peischl, J., Aikin, K. C., Gilman, J. B., Trainer, M., and Warneke, C.:
Identifying Volatile Chemical Product Tracer Compounds in U. S. Cities,
Environ. Sci. Technol.,
55, 188–199, https://doi.org/10.1021/acs.est.0c05467, 2021. a, b
Hall, W. A., Pennington, M. R., and Johnston, M. V.:
Molecular Transformations Accompanying the Aging of Laboratory Secondary Organic Aerosol,
Environ. Sci. Technol.,
47, 2230–2237, https://doi.org/10.1021/es303891q, 2013. a
Hobson, J. F., Atkinson, R., and L, C. W. P.:
Chapter 6: Volatile Methylsiloxanes,
in: The Handbook of Environmental Chemistry Vol. 3 Part H: Organosilicon Materials,
edited by: Chandra, G., 9, pp. 137–180, Springer, Berlin, https://doi.org/10.1007/978-3-540-68331-5, 1997. a
Huang, Y. and Seinfeld, J. H.:
A Note on Flow Behavior in Axially-Dispersed Plug Flow Reactors with Step Input of Tracer,
Atmos. Environ. X,
1, 1–6, https://doi.org/10.1016/j.aeaoa.2019.100006, 2019. a
Huang, Y., Coggon, M. M., Zhao, R., Lignell, H., Bauer, M. U., Flagan, R. C., and Seinfeld, J. H.: The Caltech Photooxidation Flow Tube reactor: design, fluid dynamics and characterization, Atmos. Meas. Tech., 10, 839–867, https://doi.org/10.5194/amt-10-839-2017, 2017. a, b, c
Hughes, L., Mackay, D., Powell, D. E., and Kim, J.:
An Updated State of the Science EQC Model for Evaluating Chemical Fate in the Environment: Application to D5 (Decamethylcyclopentasiloxane),
Chemosphere,
87, 118–124, https://doi.org/10.1016/j.chemosphere.2011.11.072, 2012. a
Janechek, N. J., Hansen, K. M., and Stanier, C. O.: Comprehensive atmospheric modeling of reactive cyclic siloxanes and their oxidation products, Atmos. Chem. Phys., 17, 8357–8370, https://doi.org/10.5194/acp-17-8357-2017, 2017. a, b
Janechek, N. J., Marek, R. F., Bryngelson, N., Singh, A., Bullard, R. L., Brune, W. H., and Stanier, C. O.: Physical properties of secondary photochemical aerosol from OH oxidation of a cyclic siloxane, Atmos. Chem. Phys., 19, 1649–1664, https://doi.org/10.5194/acp-19-1649-2019, 2019. a, b, c, d, e, f, g, h, i, j, k, l
Kim, J. and Xu, S.:
Quantitative Structure-Reactivity Relationships of Hydroxyl Radical Rate Constants for Linear and Cyclic Volatile Methylsiloxanes,
Environ. Toxicol. Chem.,
36, 3240–3245, https://doi.org/10.1002/etc.3914, 2017. a
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. Technol.,
41, 1002–1010, https://doi.org/10.1080/02786820701666270, 2007. a
Krechmer, J. E., Day, D. A., and Jimenez, J. L.:
Always Lost but Never Forgotten: Gas-Phase Wall Losses Are Important in All Teflon Environmental Chambers,
Environ. Sci. Technol.,
54, 12890–12897, https://doi.org/10.1021/acs.est.0c03381, 2020. a
Kroll, J. H. and Seinfeld, J. H.:
Chemistry of Secondary Organic Aerosol: Formation and Evolution of Low-Volatility Organics in the Atmosphere,
Atmos. Environ.,
42, 3593–3624, https://doi.org/10.1016/j.atmosenv.2008.01.003, 2008. a
Lambe, A. T., Chhabra, P. S., Onasch, T. B., Brune, W. H., Hunter, J. F., Kroll, J. H., Cummings, M. J., Brogan, J. F., Parmar, Y., Worsnop, D. R., Kolb, C. E., and Davidovits, P.: Effect of oxidant concentration, exposure time, and seed particles on secondary organic aerosol chemical composition and yield, Atmos. Chem. Phys., 15, 3063–3075, https://doi.org/10.5194/acp-15-3063-2015, 2015. a
Latimer, H. K., Kamens, R. M., and Chandra, G.:
The atmospheric partitioning of decamethylcyclopentasiloxane(D5) and 1-hydroxynonamethylcyclopentasiloxane(D4TOH) on different types of atmospheric particles,
Chemosphere,
36, 2401–2414, https://doi.org/10.1016/S0045-6535(97)10209-0, 1998. a
Li, R., Palm, B. B., Ortega, A. M., Hlywiak, J., Hu, W., Peng, Z., Day, D. A., Knote, C., Brune, W. H., Gouw, J. A. D., and Jimenez, J. L.:
Modeling the Radical Chemistry in an Oxidation Flow Reactor: Radical Formation and Recycling, Sensitivities, and the OH Exposure Estimation Equation,
J. Phys. Chem. A,
119, 4418–4432, https://doi.org/10.1021/jp509534k, 2015. a
Liu, C.-L., Smith, J. D., Che, D. L., Ahmed, M., Leone, S. R., and Wilson, K. R.:
The direct observation of secondary radical chain chemistry in the heterogeneous reaction of chlorine atoms with submicron squalane droplets,
Phys. Chem. Chem. Phys.,
13, 8993–9008, https://doi.org/10.1039/c1cp20236g, 2011. a
Mackay, D., Cowan-Ellsberry, C. E., Powell, D. E., Woodburn, K. B., Xu, S., Kozerski, G. E., and Kim, J.:
Decamethylcyclopentasiloxane (D5) Environmental Sources, Fate, Transport, and Routes of Exposure,
Environ. Toxicol. Chem.,
34, 2689–2702, https://doi.org/10.1002/etc.2941, 2015. a
Mai, H., Kong, W., Seinfeld, J. H., and Flagan, R. C.:
Scanning DMA Data Analysis II. Integrated DMA-CPC Instrument Response and Data Inversion,
Aerosol Sci. Technol.,
6826, 1–35, https://doi.org/10.1080/02786826.2018.1528006, 2018. a
Malloy, Q. G. J., Nakao, S., Qi, L., Austin, R., Stothers, C., Hagino, H., and Cocker III, D. R.:
Real-Time Aerosol Density Determination Utilizing a Modified Scanning Mobility Particle Sizer–Aerosol Particle Mass Analyzer System,
Aerosol Sci. Technol.,
43, 673–678, https://doi.org/10.1080/02786820902832960, 2009. a
McDonald, B. C., de Gouw, J. A., Gilman, J. B., Jathar, S. H., Akherati, A., Cappa, C. D., Jimenez, J. L., Lee-Taylor, J., Hayes, P. L., McKeen, S. A., Cui, Y. Y., Kim, S.-W., Gentner, D. R., Isaacman-VanWertz, G., Goldstein, A. H., Harley, R. A., Frost, G. J., Roberts, J. M., Ryerson, T. B., and Trainer, M.:
Volatile Chemical Products Emerging as Largest Petrochemical Source of Urban Organic Emissions,
Science,
359, 760–764, https://doi.org/10.1126/science.aaq0524, 2018. a, b, c
McLachlan, M. S., Kierkegaard, A., Hansen, K. M., Van Egmond, R., Christensen, J. H., and Skjøth, C. A.:
Concentrations and Fate of Decamethylcyclopentasiloxane (D5) in the Atmosphere,
Environ. Sci. Technol.,
44, 5365–5370, https://doi.org/10.1021/es100411w, 2010. a
McNeill, V. F., Yatavelli, R. L. N., Thornton, J. A., Stipe, C. B., and Landgrebe, O.: Heterogeneous OH oxidation of palmitic acid in single component and internally mixed aerosol particles: vaporization and the role of particle phase, Atmos. Chem. Phys., 8, 5465–5476, https://doi.org/10.5194/acp-8-5465-2008, 2008. a
Odum, J. R., Hoffman, T., Bowman, F., Collins, D., Flagan, R. C., and Seinfeld, J. H.:
Gas particle partitioning and secondary organic aerosol yields,
Environ. Sci. Technol.,
30, 2580–2585, https://doi.org/10.1021/es950943+, 1996.
a, b
Pennington, M. R., Klems, J. P., Bzdek, B. R., and Johnston, M. V.:
Nanoparticle Chemical Composition and Diurnal Dependence at the CalNex Los Angeles Ground Site,
J. Geophys. Res.-Atmos.,
117, 1–9, https://doi.org/10.1029/2011JD017061, 2012. a
Renbaum, L. H. and Smith, G. D.: Artifacts in measuring aerosol uptake kinetics: the roles of time, concentration and adsorption, Atmos. Chem. Phys., 11, 6881–6893, https://doi.org/10.5194/acp-11-6881-2011, 2011. a, b
Safron, A., Strandell, M., Kierkegaard, A., and Macleod, M.:
Rate Constants and Activation Energies for Gas-Phase Reactions of Three Cyclic Volatile Methyl Siloxanes with the Hydroxyl Radical,
Int. J. Chem. Kinet.,
47, 420–428, https://doi.org/10.1002/kin.20919, 2015. a, b, c
Schwantes, R. H., Charan, S. M., Bates, K. H., Huang, Y., Nguyen, T. B., Mai, H., Kong, W., Flagan, R. C., and Seinfeld, J. H.: Low-volatility compounds contribute significantly to isoprene secondary organic aerosol (SOA) under high-NOx conditions, Atmos. Chem. Phys., 19, 7255–7278, https://doi.org/10.5194/acp-19-7255-2019, 2019. a
Tang, X., Misztal, P. K., Nazaroff, W. W., and Goldstein, A. H.:
Siloxanes are the Most Abundant Volatile Organic Compound Emitted from Engineering Students in a Classroom,
Environ. Sci. Technol.
Let., 2, 303–307, https://doi.org/10.1021/acs.estlett.5b00256, 2015. a
Trump, E. R., Epstein, S. A., Riipinen, I., and Donahue, N. M.:
Wall Effects in Smog Chamber Experiments: A Model Study,
Aerosol Sci. Technol.,
50, 1180–1200, https://doi.org/10.1080/02786826.2016.1232858, 2016. a
Weschler, C. J.:
Polydimethylsiloxanes Associated with Indoor and Outdoor Airborne Particles,
Sci. Total Environ.,
73, 53–63, https://doi.org/10.1016/0048-9697(88)90186-6, 1988. a
Xiao, R., Zammit, I., Wei, Z., Hu, W. P., MacLeod, M., and Spinney, R.:
Kinetics and Mechanism of the Oxidation of Cyclic Methylsiloxanes by Hydroxyl Radical in the Gas Phase: An Experimental and Theoretical Study,
Environ. Sci. Technol.,
49, 13322–13330, https://doi.org/10.1021/acs.est.5b03744, 2015. a, b
Xu, N. and Collins, D. R.: Design and characterization of a new oxidation flow reactor for laboratory and long-term ambient studies, Atmos. Meas. Tech., 14, 2891–2906, https://doi.org/10.5194/amt-14-2891-2021, 2021. a
Xu, S., Warner, N., Bohlin-Nizzetto, P., Durham, J., and McNett, D.:
Long-Range Transport Potential and Atmospheric Persistence of Cyclic Volatile Methylsiloxanes Based on Global Measurements,
Chemosphere,
228, 460–468, https://doi.org/10.1016/j.chemosphere.2019.04.130, 2019. a
Short summary
In this study, we investigate the secondary organic aerosol formation potential of decamethylcyclopentasiloxane (D5), which is used as a tracer for volatile chemical products and measured in high concentrations both outdoors and indoors. By performing experiments in different types of reactors, we find that D5’s aerosol formation is highly dependent on OH, and, at low OH concentrations or exposures, D5 forms little aerosol. We also reconcile results from other studies.
In this study, we investigate the secondary organic aerosol formation potential of...
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