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Stratospheric Gas-Phase Production Alone Cannot Explain Observations of Atmospheric Perchlorate on Earth
dc.contributor.authorChan, Yuk-Chun
dc.contributor.authorJaeglé, Lyatt
dc.contributor.authorCampuzano-Jost, Pedro
dc.contributor.authorCatling, David C.
dc.contributor.authorCole-Dai, Jihong
dc.contributor.authorFurdui, Vasile I.
dc.contributor.authorJackson, W. Andrew
dc.contributor.authorJimenez, Jose L.
dc.contributor.authorKim, Dongwook
dc.contributor.authorWedum, Alanna E.
dc.contributor.authorAlexander, Becky
dc.date.accessioned2023-06-01T20:48:02Z
dc.date.available2024-06-01 16:48:00en
dc.date.available2023-06-01T20:48:02Z
dc.date.issued2023-05-16
dc.identifier.citationChan, Yuk-Chun ; Jaeglé, Lyatt ; Campuzano-Jost, Pedro ; Catling, David C.; Cole-Dai, Jihong ; Furdui, Vasile I.; Jackson, W. Andrew; Jimenez, Jose L.; Kim, Dongwook; Wedum, Alanna E.; Alexander, Becky (2023). "Stratospheric Gas- Phase Production Alone Cannot Explain Observations of Atmospheric Perchlorate on Earth." Geophysical Research Letters 50(9): n/a-n/a.
dc.identifier.issn0094-8276
dc.identifier.issn1944-8007
dc.identifier.urihttps://hdl.handle.net/2027.42/176814
dc.description.abstractPerchlorate has been observed in many environments on Earth and Mars but its sources remain poorly quantified. In this study, we use a global three-dimensional chemical transport model to simulate perchlorate’s gas-phase photochemical production, atmospheric transport, and deposition on Earth’s surface. Model predictions are compared to newly compiled observations of atmospheric concentrations, deposition flux, and oxygen isotopic composition of perchlorate. We find that the modeled gas-phase production of perchlorate is consistent with reported stratospheric observations. Nevertheless, we show that this mechanism alone cannot explain the high levels of perchlorate observed at many near-surface sites (aerosol concentrations >0.1 ng m−3 and deposition fluxes >10 g km−2 yr−1) or the low 17O-excess observed in perchlorate sampled from pristine environments (<+18.4‰). We discuss four hypotheses to explain the model-observation discrepancies and recommend laboratory and field observations to address key uncertainties in atmospheric sources of perchlorate.Plain Language SummaryPerchlorate (ClO4−) pollution is an environmental issue because excessive exposure can affect the thyroid and disrupt hormonal balance, especially for infants. Perchlorate on Earth has both human and natural sources. Industrial perchlorate is used for explosives and rocket fuels. Perchlorate also occurs naturally and accumulates in many deserts on Earth and in the soil of Mars. Atmospheric chemistry has long been considered a source of natural perchlorate, but its contribution remains uncertain. In this study, we use a 3-D atmospheric model to estimate how much of the perchlorate occurrence on Earth can be explained by known and plausible reactions between gases containing chlorine and oxygen. We find that these reactions can explain the abundance of stratospheric perchlorate. However, they cannot explain many tropospheric observations of perchlorate, especially those in Antarctica and urban areas. Our analysis of oxygen isotopic anomalies also suggests that stratospheric chemistry alone cannot account for all the natural perchlorate found in deserts. We discuss four possible explanations for the differences between observations and model predictions. We recommend some future research that can reduce the uncertainties in the sources of atmospheric perchlorate and improve our understanding of the occurrence of natural perchlorate in planetary atmospheres.Key PointsWe conduct the first global simulation of atmospheric perchlorate using a three-dimensional chemical transport modelGas-phase production of perchlorate in the stratosphere and its subsequent transport cannot explain observations at many surface sitesAnalysis of modeled and observed 17O excess suggests that non-stratospheric sources are important for the occurrence of natural perchlorate
dc.publisherWiley Periodicals, Inc.
dc.publisherRakuno Gakuen University
dc.subject.otheroxygen isotopes
dc.subject.otherperchlorate
dc.subject.otherGEOS-Chem
dc.subject.otherglobal modeling
dc.subject.otherphotochemistry
dc.subject.other17O excess
dc.titleStratospheric Gas-Phase Production Alone Cannot Explain Observations of Atmospheric Perchlorate on Earth
dc.typeArticle
dc.rights.robotsIndexNoFollow
dc.subject.hlbsecondlevelGeological Sciences
dc.subject.hlbtoplevelScience
dc.description.peerreviewedPeer Reviewed
dc.description.bitstreamurlhttp://deepblue.lib.umich.edu/bitstream/2027.42/176814/1/grl65724.pdf
dc.description.bitstreamurlhttp://deepblue.lib.umich.edu/bitstream/2027.42/176814/2/2023GL102745-sup-0001-Supporting_Information_SI-S01.pdf
dc.description.bitstreamurlhttp://deepblue.lib.umich.edu/bitstream/2027.42/176814/3/grl65724_am.pdf
dc.identifier.doi10.1029/2023GL102745
dc.identifier.sourceGeophysical Research Letters
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dc.owningcollnameInterdisciplinary and Peer-Reviewed


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