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Unraveling Urban NOx Emission Sources in Polluted Arctic Wintertime Using NO2 Nitrogen Isotopes.

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Title: Unraveling Urban NOx Emission Sources in Polluted Arctic Wintertime Using NO2 Nitrogen Isotopes.
Authors: Albertin, Sarah1,2,3 (AUTHOR) sarah.albertin@noaa.gov, Bekki, Slimane2 (AUTHOR), Savarino, Joël1 (AUTHOR), Brett, Natalie2,4 (AUTHOR), Law, Kathy S.2 (AUTHOR), Cesler‐Maloney, Meeta5 (AUTHOR), Flynn, James H.6 (AUTHOR), Guo, Fangzhou6,7 (AUTHOR), Barret, Brice8 (AUTHOR), Caillon, Nicolas1 (AUTHOR), D'Anna, Barbara9 (AUTHOR), Dieudonné, Elsa10 (AUTHOR), Lamothe, Alexis1 (AUTHOR), Richard, Soline1 (AUTHOR), Temime‐Roussel, Brice9 (AUTHOR), Alexander, Becky11 (AUTHOR), Arnold, Steve R.4 (AUTHOR), Decesari, Stefano12 (AUTHOR), Fochesatto, Gilberto J.13 (AUTHOR), Mao, Jingqiu5 (AUTHOR)
Source: Journal of Geophysical Research. Atmospheres. 10/28/2024, Vol. 129 Issue 20, p1-12. 12p.
Subject Terms: *Atmospheric nitrogen dioxide, Nitrogen isotopes, Reactive nitrogen species, Isotopic fractionation, Analytical chemistry
Abstract: Nitrogen (N) isotopic fractionation during nitrogen oxides (NOx) cycling and conversion into atmospheric nitrate alters the original N isotopic composition (δ15N) of NOx emissions. Limited quantification of these isotopic effects in urban settings hampers the δ15N‐based identification and apportionment of NOx sources. δ15N of nitrogen dioxide (NO2) measured during winter in downtown Fairbanks, Alaska, displayed a large temporal variability, from −10.2 to 24.1‰. δ15N(NO2) records are found to be driven by equilibrium isotopic fractionation, at a rate in very close agreement with theoretical predictions. This result confirms that N isotopic partitioning between NO and NO2 can be accurately predicted over a wide range of conditions. This represents an important step for inferring NOx emission sources from isotopic composition measurement of reactive nitrogen species. After correcting our δ15N(NO2) measurements for N fractionation effects, a δ15N‐based source apportionment analysis identifies vehicle and space heating oil emissions as the dominant sources of breathing‐level NOx at this urban site. Despite their large NOx emissions, coal‐fired power plants with elevated chimney stacks (>26 m) appear to make a small contribution to surface NOx levels in downtown Fairbanks (likely less than 18% on average). The combined uncertainties of the δ15N of NOx from heating oil combustion and of the influence of low temperatures on the δ15N of NOx emitted by vehicle exhaust prevent a more detailed partitioning of surface NOx sources in Fairbanks. Plain Language Summary: Nitrogen (N) stable isotopes measured in atmospheric reactive N (Nr) species can help trace emission sources of nitrogen oxides (NOx). However, large uncertainties subsist regarding the factors controlling the variability of N isotopes in Nr species, preventing a precise isotope‐based emission source apportionment. This study presents a comprehensive analysis of the enrichment of 15N–14N (δ15N) in atmospheric nitrogen dioxide (NO2) collected during the Alaskan Layered Pollution And Chemical Analysis (ALPACA) 2022 international winter campaign in Fairbanks, Alaska. Building on in situ meteorological and trace gas, the isotopic fractionation effect driving the significant δ15N variability of NO2 observed in downtown Fairbanks is quantified with great precision. The δ15N records corrected for equilibrium fractionation effects are discussed in light of a local NOx emission inventory. In particular, the influence of emissions from coal‐fired power plants with high stack heights on surface air pollution is addressed. Key Points: A temporal variability in NO2 nitrogen isotopes is measured during winter in downtown Fairbanks, AlaskaIsotope exchange fractionation drives NO2 nitrogen isotope distribution, at a rate in excellent agreement with theoretical predictionsA15N‐based source apportionment indicates vehicle and oil space heating emissions are the main sources of NOx in downtown Fairbanks [ABSTRACT FROM AUTHOR]
Copyright of Journal of Geophysical Research. Atmospheres is the property of Wiley-Blackwell and its content may not be copied or emailed to multiple sites without the copyright holder's express written permission. Additionally, content may not be used with any artificial intelligence tools or machine learning technologies. However, users may print, download, or email articles for individual use. This abstract may be abridged. No warranty is given about the accuracy of the copy. Users should refer to the original published version of the material for the full abstract. (Copyright applies to all Abstracts.)
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  Data: Unraveling Urban NO<subscript>x</subscript> Emission Sources in Polluted Arctic Wintertime Using NO<subscript>2</subscript> Nitrogen Isotopes.
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  Data: <searchLink fieldCode="AR" term="%22Albertin%2C+Sarah%22">Albertin, Sarah</searchLink><relatesTo>1,2,3</relatesTo> (AUTHOR)<i> sarah.albertin@noaa.gov</i><br /><searchLink fieldCode="AR" term="%22Bekki%2C+Slimane%22">Bekki, Slimane</searchLink><relatesTo>2</relatesTo> (AUTHOR)<br /><searchLink fieldCode="AR" term="%22Savarino%2C+Joël%22">Savarino, Joël</searchLink><relatesTo>1</relatesTo> (AUTHOR)<br /><searchLink fieldCode="AR" term="%22Brett%2C+Natalie%22">Brett, Natalie</searchLink><relatesTo>2,4</relatesTo> (AUTHOR)<br /><searchLink fieldCode="AR" term="%22Law%2C+Kathy+S%2E%22">Law, Kathy S.</searchLink><relatesTo>2</relatesTo> (AUTHOR)<br /><searchLink fieldCode="AR" term="%22Cesler‐Maloney%2C+Meeta%22">Cesler‐Maloney, Meeta</searchLink><relatesTo>5</relatesTo> (AUTHOR)<br /><searchLink fieldCode="AR" term="%22Flynn%2C+James+H%2E%22">Flynn, James H.</searchLink><relatesTo>6</relatesTo> (AUTHOR)<br /><searchLink fieldCode="AR" term="%22Guo%2C+Fangzhou%22">Guo, Fangzhou</searchLink><relatesTo>6,7</relatesTo> (AUTHOR)<br /><searchLink fieldCode="AR" term="%22Barret%2C+Brice%22">Barret, Brice</searchLink><relatesTo>8</relatesTo> (AUTHOR)<br /><searchLink fieldCode="AR" term="%22Caillon%2C+Nicolas%22">Caillon, Nicolas</searchLink><relatesTo>1</relatesTo> (AUTHOR)<br /><searchLink fieldCode="AR" term="%22D'Anna%2C+Barbara%22">D'Anna, Barbara</searchLink><relatesTo>9</relatesTo> (AUTHOR)<br /><searchLink fieldCode="AR" term="%22Dieudonné%2C+Elsa%22">Dieudonné, Elsa</searchLink><relatesTo>10</relatesTo> (AUTHOR)<br /><searchLink fieldCode="AR" term="%22Lamothe%2C+Alexis%22">Lamothe, Alexis</searchLink><relatesTo>1</relatesTo> (AUTHOR)<br /><searchLink fieldCode="AR" term="%22Richard%2C+Soline%22">Richard, Soline</searchLink><relatesTo>1</relatesTo> (AUTHOR)<br /><searchLink fieldCode="AR" term="%22Temime‐Roussel%2C+Brice%22">Temime‐Roussel, Brice</searchLink><relatesTo>9</relatesTo> (AUTHOR)<br /><searchLink fieldCode="AR" term="%22Alexander%2C+Becky%22">Alexander, Becky</searchLink><relatesTo>11</relatesTo> (AUTHOR)<br /><searchLink fieldCode="AR" term="%22Arnold%2C+Steve+R%2E%22">Arnold, Steve R.</searchLink><relatesTo>4</relatesTo> (AUTHOR)<br /><searchLink fieldCode="AR" term="%22Decesari%2C+Stefano%22">Decesari, Stefano</searchLink><relatesTo>12</relatesTo> (AUTHOR)<br /><searchLink fieldCode="AR" term="%22Fochesatto%2C+Gilberto+J%2E%22">Fochesatto, Gilberto J.</searchLink><relatesTo>13</relatesTo> (AUTHOR)<br /><searchLink fieldCode="AR" term="%22Mao%2C+Jingqiu%22">Mao, Jingqiu</searchLink><relatesTo>5</relatesTo> (AUTHOR)
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  Data: <searchLink fieldCode="JN" term="%22Journal+of+Geophysical+Research%2E+Atmospheres%22">Journal of Geophysical Research. Atmospheres</searchLink>. 10/28/2024, Vol. 129 Issue 20, p1-12. 12p.
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  Data: *<searchLink fieldCode="DE" term="%22Atmospheric+nitrogen+dioxide%22">Atmospheric nitrogen dioxide</searchLink><br /><searchLink fieldCode="DE" term="%22Nitrogen+isotopes%22">Nitrogen isotopes</searchLink><br /><searchLink fieldCode="DE" term="%22Reactive+nitrogen+species%22">Reactive nitrogen species</searchLink><br /><searchLink fieldCode="DE" term="%22Isotopic+fractionation%22">Isotopic fractionation</searchLink><br /><searchLink fieldCode="DE" term="%22Analytical+chemistry%22">Analytical chemistry</searchLink>
– Name: Abstract
  Label: Abstract
  Group: Ab
  Data: Nitrogen (N) isotopic fractionation during nitrogen oxides (NOx) cycling and conversion into atmospheric nitrate alters the original N isotopic composition (δ15N) of NOx emissions. Limited quantification of these isotopic effects in urban settings hampers the δ15N‐based identification and apportionment of NOx sources. δ15N of nitrogen dioxide (NO2) measured during winter in downtown Fairbanks, Alaska, displayed a large temporal variability, from −10.2 to 24.1‰. δ15N(NO2) records are found to be driven by equilibrium isotopic fractionation, at a rate in very close agreement with theoretical predictions. This result confirms that N isotopic partitioning between NO and NO2 can be accurately predicted over a wide range of conditions. This represents an important step for inferring NOx emission sources from isotopic composition measurement of reactive nitrogen species. After correcting our δ15N(NO2) measurements for N fractionation effects, a δ15N‐based source apportionment analysis identifies vehicle and space heating oil emissions as the dominant sources of breathing‐level NOx at this urban site. Despite their large NOx emissions, coal‐fired power plants with elevated chimney stacks (>26 m) appear to make a small contribution to surface NOx levels in downtown Fairbanks (likely less than 18% on average). The combined uncertainties of the δ15N of NOx from heating oil combustion and of the influence of low temperatures on the δ15N of NOx emitted by vehicle exhaust prevent a more detailed partitioning of surface NOx sources in Fairbanks. Plain Language Summary: Nitrogen (N) stable isotopes measured in atmospheric reactive N (Nr) species can help trace emission sources of nitrogen oxides (NOx). However, large uncertainties subsist regarding the factors controlling the variability of N isotopes in Nr species, preventing a precise isotope‐based emission source apportionment. This study presents a comprehensive analysis of the enrichment of 15N–14N (δ15N) in atmospheric nitrogen dioxide (NO2) collected during the Alaskan Layered Pollution And Chemical Analysis (ALPACA) 2022 international winter campaign in Fairbanks, Alaska. Building on in situ meteorological and trace gas, the isotopic fractionation effect driving the significant δ15N variability of NO2 observed in downtown Fairbanks is quantified with great precision. The δ15N records corrected for equilibrium fractionation effects are discussed in light of a local NOx emission inventory. In particular, the influence of emissions from coal‐fired power plants with high stack heights on surface air pollution is addressed. Key Points: A temporal variability in NO2 nitrogen isotopes is measured during winter in downtown Fairbanks, AlaskaIsotope exchange fractionation drives NO2 nitrogen isotope distribution, at a rate in excellent agreement with theoretical predictionsA15N‐based source apportionment indicates vehicle and oil space heating emissions are the main sources of NOx in downtown Fairbanks [ABSTRACT FROM AUTHOR]
– Name: AbstractSuppliedCopyright
  Label:
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  Data: <i>Copyright of Journal of Geophysical Research. Atmospheres is the property of Wiley-Blackwell and its content may not be copied or emailed to multiple sites without the copyright holder's express written permission. Additionally, content may not be used with any artificial intelligence tools or machine learning technologies. However, users may print, download, or email articles for individual use. This abstract may be abridged. No warranty is given about the accuracy of the copy. Users should refer to the original published version of the material for the full abstract.</i> (Copyright applies to all Abstracts.)
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