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Isotope Fractionation of Nitrate During Volatilization in Snow: A Field Investigation in Antarctica
Several postdepositional processes impact snow nitrate; however, only the isotopic effects of nitrate photolysis have been quantified. Here we discuss results from experiments in field Antarctic snow investigating isotopic fractionation of nitrate due to volatilization. At −35 °C, concentration and...
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| Published in: | Geophysical research letters 2019-03, Vol.46 (6), p.3287-3297 |
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| creator | Shi, Guitao Chai, Jiajue Zhu, Zhuoyi Hu, Zhengyi Chen, Zhenlou Yu, Jinhai Ma, Tianming Ma, Hongmei An, Chunlei Jiang, Su Tang, Xueyuan Hastings, Meredith G. |
| description | Several postdepositional processes impact snow nitrate; however, only the isotopic effects of nitrate photolysis have been quantified. Here we discuss results from experiments in field Antarctic snow investigating isotopic fractionation of nitrate due to volatilization. At −35 °C, concentration and isotopic composition of nitrate remained constant during the 16‐day experiment. At −24 °C, 7.5% of nitrate was lost, synchronous with 1.5‰ decrease in δ18O and a constant δ15N. At −4 °C, 38% of nitrate was lost, and δ15N and δ18O decreased by 3.1 and 1.8‰, respectively. Results at −4 °C yield calculated fractionation constants close to theoretical estimates including equilibrium isotopic exchange between nitric acid and nitrate and the desorption of nitric acid from water in quasi‐liquid layers. This suggests that isotopic fractionation associated with nitrate volatilization across most of Antarctica, especially at sites with temperatures |
| doi_str_mv | 10.1029/2019GL081968 |
| format | article |
| fullrecord | <record><control><sourceid>proquest_cross</sourceid><recordid>TN_cdi_proquest_journals_2207457804</recordid><sourceformat>XML</sourceformat><sourcesystem>PC</sourcesystem><sourcerecordid>2207457804</sourcerecordid><originalsourceid>FETCH-LOGICAL-c3727-b9a0f084cf59af421c772d6f953f7cf4667803a8d25c5d428d5c34cfa8d591273</originalsourceid><addsrcrecordid>eNp9kE1LAzEQhoMoWKs3f0DAq6uTr03iraithUXBr-sSs5uSsm5qdmupv96UFfHkZWaY95l3hkHolMAFAaovKRA9K0ARnas9NCKa80wByH00AtCppjI_REddtwQABoyMkJ13oQ-rGk-jsb0PrdkFHBy-9300fY1v1tG3C_wamiQ1_msAfIuf2rC5whM89XVT4Xn7WXe9X_zKk7Y3MVlac4wOnGm6-uQnj9HL9Pb5-i4rHmbz60mRWSapzN60AQeKWye0cZwSKyWtcqcFc9I6nudSATOqosKKilNVCcsSnTpCEyrZGJ0NvqsYPtbpmnIZ1rFNK0tKQXKR5nmizgfKxtB1sXblKvp3E7clgXL3xvLvGxNOB3zjm3r7L1vOHguhci3ZN5rEc2A</addsrcrecordid><sourcetype>Aggregation Database</sourcetype><iscdi>true</iscdi><recordtype>article</recordtype><pqid>2207457804</pqid></control><display><type>article</type><title>Isotope Fractionation of Nitrate During Volatilization in Snow: A Field Investigation in Antarctica</title><source>Wiley-Blackwell AGU Digital Archive</source><creator>Shi, Guitao ; Chai, Jiajue ; Zhu, Zhuoyi ; Hu, Zhengyi ; Chen, Zhenlou ; Yu, Jinhai ; Ma, Tianming ; Ma, Hongmei ; An, Chunlei ; Jiang, Su ; Tang, Xueyuan ; Hastings, Meredith G.</creator><creatorcontrib>Shi, Guitao ; Chai, Jiajue ; Zhu, Zhuoyi ; Hu, Zhengyi ; Chen, Zhenlou ; Yu, Jinhai ; Ma, Tianming ; Ma, Hongmei ; An, Chunlei ; Jiang, Su ; Tang, Xueyuan ; Hastings, Meredith G.</creatorcontrib><description>Several postdepositional processes impact snow nitrate; however, only the isotopic effects of nitrate photolysis have been quantified. Here we discuss results from experiments in field Antarctic snow investigating isotopic fractionation of nitrate due to volatilization. At −35 °C, concentration and isotopic composition of nitrate remained constant during the 16‐day experiment. At −24 °C, 7.5% of nitrate was lost, synchronous with 1.5‰ decrease in δ18O and a constant δ15N. At −4 °C, 38% of nitrate was lost, and δ15N and δ18O decreased by 3.1 and 1.8‰, respectively. Results at −4 °C yield calculated fractionation constants close to theoretical estimates including equilibrium isotopic exchange between nitric acid and nitrate and the desorption of nitric acid from water in quasi‐liquid layers. This suggests that isotopic fractionation associated with nitrate volatilization across most of Antarctica, especially at sites with temperatures <−24 °C, should be minor, but the isotopic effects at warmer sites should be considered in interpreting archived nitrate records.
Plain Language Summary
In polar regions, there is great interest in using nitrate archived in snow/ice to reconstruct aspects of atmospheric composition and the influence of natural versus man‐made emissions. However, nitrate can be lost from the snowpack, such that the archived signals do not directly reflect atmospheric loading. Stable isotopes of nitrate in snow/ice allow for tracking and understanding the origins of nitrate and how it might have changed after deposition. While the isotopic fractionation associated with photolytic loss of nitrate has been directly quantified, that of volatilization remains poorly understood. Thus, we completed field experiments in Antarctica to investigate the isotopic effects of nitrate volatilization from snow. Results show that nitrate volatilization loss is significant at −4 °C, resulting in an important change (depletion of heavy isotopes) in both nitrogen and oxygen in remaining snow nitrate. This can be largely explained by a combination of equilibrium isotopic exchange between nitric acid and nitrate and the desorption of nitric acid from water in ice surface layers. At lower temperatures (<−24 °C), nitrate loss is rather minor, and the isotopic fractionation is found to be negligible. The findings suggest that the isotopic effects of NO3− volatilization in snow are closely related to temperature.
Key Points
Field experiments in Antarctica (over 16 days) were used to quantify the isotopic effects of NO3− volatilization from snow
Volatilization at −4 °C depletes heavy isotopes of NO3− in remaining snow versus relatively constant isotopic ratios observed at −35 °C
Volatilization can decrease δ15N in remaining snow NO3− in warm regions by several per mil, contrary to isotopic effects of photolysis</description><identifier>ISSN: 0094-8276</identifier><identifier>EISSN: 1944-8007</identifier><identifier>DOI: 10.1029/2019GL081968</identifier><language>eng</language><publisher>Washington: John Wiley & Sons, Inc</publisher><subject>Acids ; Antarctic snow ; Atmospheric chemistry ; Atmospheric composition ; Constants ; coupled cluster method ; Depletion ; Desorption ; Exchanging ; Field investigations ; Field tests ; Fractionation ; Ice ; Investigations ; Isotope composition ; Isotope fractionation ; Isotopes ; Low temperature ; nitrate ; Nitrates ; Nitric acid ; Nitric acids ; Oxygen ; Photolysis ; Polar environments ; Polar regions ; Snow ; Snowpack ; stable isotope ; Stable isotopes ; Surface boundary layer ; Surface layers ; Volatilization</subject><ispartof>Geophysical research letters, 2019-03, Vol.46 (6), p.3287-3297</ispartof><rights>2019. American Geophysical Union. All Rights Reserved.</rights><lds50>peer_reviewed</lds50><woscitedreferencessubscribed>false</woscitedreferencessubscribed><citedby>FETCH-LOGICAL-c3727-b9a0f084cf59af421c772d6f953f7cf4667803a8d25c5d428d5c34cfa8d591273</citedby><cites>FETCH-LOGICAL-c3727-b9a0f084cf59af421c772d6f953f7cf4667803a8d25c5d428d5c34cfa8d591273</cites><orcidid>0000-0003-4945-9405 ; 0000-0003-1702-6322 ; 0000-0001-6716-6783 ; 0000-0002-8579-2400 ; 0000-0001-6712-7979 ; 0000-0002-0276-2418</orcidid></display><links><openurl>$$Topenurl_article</openurl><openurlfulltext>$$Topenurlfull_article</openurlfulltext><thumbnail>$$Tsyndetics_thumb_exl</thumbnail><linktopdf>$$Uhttps://onlinelibrary.wiley.com/doi/pdf/10.1029%2F2019GL081968$$EPDF$$P50$$Gwiley$$H</linktopdf><linktohtml>$$Uhttps://onlinelibrary.wiley.com/doi/full/10.1029%2F2019GL081968$$EHTML$$P50$$Gwiley$$H</linktohtml><link.rule.ids>314,776,780,11493,27901,27902,46443,46867</link.rule.ids></links><search><creatorcontrib>Shi, Guitao</creatorcontrib><creatorcontrib>Chai, Jiajue</creatorcontrib><creatorcontrib>Zhu, Zhuoyi</creatorcontrib><creatorcontrib>Hu, Zhengyi</creatorcontrib><creatorcontrib>Chen, Zhenlou</creatorcontrib><creatorcontrib>Yu, Jinhai</creatorcontrib><creatorcontrib>Ma, Tianming</creatorcontrib><creatorcontrib>Ma, Hongmei</creatorcontrib><creatorcontrib>An, Chunlei</creatorcontrib><creatorcontrib>Jiang, Su</creatorcontrib><creatorcontrib>Tang, Xueyuan</creatorcontrib><creatorcontrib>Hastings, Meredith G.</creatorcontrib><title>Isotope Fractionation of Nitrate During Volatilization in Snow: A Field Investigation in Antarctica</title><title>Geophysical research letters</title><description>Several postdepositional processes impact snow nitrate; however, only the isotopic effects of nitrate photolysis have been quantified. Here we discuss results from experiments in field Antarctic snow investigating isotopic fractionation of nitrate due to volatilization. At −35 °C, concentration and isotopic composition of nitrate remained constant during the 16‐day experiment. At −24 °C, 7.5% of nitrate was lost, synchronous with 1.5‰ decrease in δ18O and a constant δ15N. At −4 °C, 38% of nitrate was lost, and δ15N and δ18O decreased by 3.1 and 1.8‰, respectively. Results at −4 °C yield calculated fractionation constants close to theoretical estimates including equilibrium isotopic exchange between nitric acid and nitrate and the desorption of nitric acid from water in quasi‐liquid layers. This suggests that isotopic fractionation associated with nitrate volatilization across most of Antarctica, especially at sites with temperatures <−24 °C, should be minor, but the isotopic effects at warmer sites should be considered in interpreting archived nitrate records.
Plain Language Summary
In polar regions, there is great interest in using nitrate archived in snow/ice to reconstruct aspects of atmospheric composition and the influence of natural versus man‐made emissions. However, nitrate can be lost from the snowpack, such that the archived signals do not directly reflect atmospheric loading. Stable isotopes of nitrate in snow/ice allow for tracking and understanding the origins of nitrate and how it might have changed after deposition. While the isotopic fractionation associated with photolytic loss of nitrate has been directly quantified, that of volatilization remains poorly understood. Thus, we completed field experiments in Antarctica to investigate the isotopic effects of nitrate volatilization from snow. Results show that nitrate volatilization loss is significant at −4 °C, resulting in an important change (depletion of heavy isotopes) in both nitrogen and oxygen in remaining snow nitrate. This can be largely explained by a combination of equilibrium isotopic exchange between nitric acid and nitrate and the desorption of nitric acid from water in ice surface layers. At lower temperatures (<−24 °C), nitrate loss is rather minor, and the isotopic fractionation is found to be negligible. The findings suggest that the isotopic effects of NO3− volatilization in snow are closely related to temperature.
Key Points
Field experiments in Antarctica (over 16 days) were used to quantify the isotopic effects of NO3− volatilization from snow
Volatilization at −4 °C depletes heavy isotopes of NO3− in remaining snow versus relatively constant isotopic ratios observed at −35 °C
Volatilization can decrease δ15N in remaining snow NO3− in warm regions by several per mil, contrary to isotopic effects of photolysis</description><subject>Acids</subject><subject>Antarctic snow</subject><subject>Atmospheric chemistry</subject><subject>Atmospheric composition</subject><subject>Constants</subject><subject>coupled cluster method</subject><subject>Depletion</subject><subject>Desorption</subject><subject>Exchanging</subject><subject>Field investigations</subject><subject>Field tests</subject><subject>Fractionation</subject><subject>Ice</subject><subject>Investigations</subject><subject>Isotope composition</subject><subject>Isotope fractionation</subject><subject>Isotopes</subject><subject>Low temperature</subject><subject>nitrate</subject><subject>Nitrates</subject><subject>Nitric acid</subject><subject>Nitric acids</subject><subject>Oxygen</subject><subject>Photolysis</subject><subject>Polar environments</subject><subject>Polar regions</subject><subject>Snow</subject><subject>Snowpack</subject><subject>stable isotope</subject><subject>Stable isotopes</subject><subject>Surface boundary layer</subject><subject>Surface layers</subject><subject>Volatilization</subject><issn>0094-8276</issn><issn>1944-8007</issn><fulltext>true</fulltext><rsrctype>article</rsrctype><creationdate>2019</creationdate><recordtype>article</recordtype><recordid>eNp9kE1LAzEQhoMoWKs3f0DAq6uTr03iraithUXBr-sSs5uSsm5qdmupv96UFfHkZWaY95l3hkHolMAFAaovKRA9K0ARnas9NCKa80wByH00AtCppjI_REddtwQABoyMkJ13oQ-rGk-jsb0PrdkFHBy-9300fY1v1tG3C_wamiQ1_msAfIuf2rC5whM89XVT4Xn7WXe9X_zKk7Y3MVlac4wOnGm6-uQnj9HL9Pb5-i4rHmbz60mRWSapzN60AQeKWye0cZwSKyWtcqcFc9I6nudSATOqosKKilNVCcsSnTpCEyrZGJ0NvqsYPtbpmnIZ1rFNK0tKQXKR5nmizgfKxtB1sXblKvp3E7clgXL3xvLvGxNOB3zjm3r7L1vOHguhci3ZN5rEc2A</recordid><startdate>20190328</startdate><enddate>20190328</enddate><creator>Shi, Guitao</creator><creator>Chai, Jiajue</creator><creator>Zhu, Zhuoyi</creator><creator>Hu, Zhengyi</creator><creator>Chen, Zhenlou</creator><creator>Yu, Jinhai</creator><creator>Ma, Tianming</creator><creator>Ma, Hongmei</creator><creator>An, Chunlei</creator><creator>Jiang, Su</creator><creator>Tang, Xueyuan</creator><creator>Hastings, Meredith G.</creator><general>John Wiley & Sons, Inc</general><scope>AAYXX</scope><scope>CITATION</scope><scope>7TG</scope><scope>7TN</scope><scope>8FD</scope><scope>F1W</scope><scope>FR3</scope><scope>H8D</scope><scope>H96</scope><scope>KL.</scope><scope>KR7</scope><scope>L.G</scope><scope>L7M</scope><orcidid>https://orcid.org/0000-0003-4945-9405</orcidid><orcidid>https://orcid.org/0000-0003-1702-6322</orcidid><orcidid>https://orcid.org/0000-0001-6716-6783</orcidid><orcidid>https://orcid.org/0000-0002-8579-2400</orcidid><orcidid>https://orcid.org/0000-0001-6712-7979</orcidid><orcidid>https://orcid.org/0000-0002-0276-2418</orcidid></search><sort><creationdate>20190328</creationdate><title>Isotope Fractionation of Nitrate During Volatilization in Snow: A Field Investigation in Antarctica</title><author>Shi, Guitao ; Chai, Jiajue ; Zhu, Zhuoyi ; Hu, Zhengyi ; Chen, Zhenlou ; Yu, Jinhai ; Ma, Tianming ; Ma, Hongmei ; An, Chunlei ; Jiang, Su ; Tang, Xueyuan ; Hastings, Meredith G.</author></sort><facets><frbrtype>5</frbrtype><frbrgroupid>cdi_FETCH-LOGICAL-c3727-b9a0f084cf59af421c772d6f953f7cf4667803a8d25c5d428d5c34cfa8d591273</frbrgroupid><rsrctype>articles</rsrctype><prefilter>articles</prefilter><language>eng</language><creationdate>2019</creationdate><topic>Acids</topic><topic>Antarctic snow</topic><topic>Atmospheric chemistry</topic><topic>Atmospheric composition</topic><topic>Constants</topic><topic>coupled cluster method</topic><topic>Depletion</topic><topic>Desorption</topic><topic>Exchanging</topic><topic>Field investigations</topic><topic>Field tests</topic><topic>Fractionation</topic><topic>Ice</topic><topic>Investigations</topic><topic>Isotope composition</topic><topic>Isotope fractionation</topic><topic>Isotopes</topic><topic>Low temperature</topic><topic>nitrate</topic><topic>Nitrates</topic><topic>Nitric acid</topic><topic>Nitric acids</topic><topic>Oxygen</topic><topic>Photolysis</topic><topic>Polar environments</topic><topic>Polar regions</topic><topic>Snow</topic><topic>Snowpack</topic><topic>stable isotope</topic><topic>Stable isotopes</topic><topic>Surface boundary layer</topic><topic>Surface layers</topic><topic>Volatilization</topic><toplevel>peer_reviewed</toplevel><toplevel>online_resources</toplevel><creatorcontrib>Shi, Guitao</creatorcontrib><creatorcontrib>Chai, Jiajue</creatorcontrib><creatorcontrib>Zhu, Zhuoyi</creatorcontrib><creatorcontrib>Hu, Zhengyi</creatorcontrib><creatorcontrib>Chen, Zhenlou</creatorcontrib><creatorcontrib>Yu, Jinhai</creatorcontrib><creatorcontrib>Ma, Tianming</creatorcontrib><creatorcontrib>Ma, Hongmei</creatorcontrib><creatorcontrib>An, Chunlei</creatorcontrib><creatorcontrib>Jiang, Su</creatorcontrib><creatorcontrib>Tang, Xueyuan</creatorcontrib><creatorcontrib>Hastings, Meredith G.</creatorcontrib><collection>CrossRef</collection><collection>Meteorological & Geoastrophysical Abstracts</collection><collection>Oceanic Abstracts</collection><collection>Technology Research Database</collection><collection>ASFA: Aquatic Sciences and Fisheries Abstracts</collection><collection>Engineering Research Database</collection><collection>Aerospace Database</collection><collection>Aquatic Science & Fisheries Abstracts (ASFA) 2: Ocean Technology, Policy & Non-Living Resources</collection><collection>Meteorological & Geoastrophysical Abstracts - Academic</collection><collection>Civil Engineering Abstracts</collection><collection>Aquatic Science & Fisheries Abstracts (ASFA) Professional</collection><collection>Advanced Technologies Database with Aerospace</collection><jtitle>Geophysical research letters</jtitle></facets><delivery><delcategory>Remote Search Resource</delcategory><fulltext>fulltext</fulltext></delivery><addata><au>Shi, Guitao</au><au>Chai, Jiajue</au><au>Zhu, Zhuoyi</au><au>Hu, Zhengyi</au><au>Chen, Zhenlou</au><au>Yu, Jinhai</au><au>Ma, Tianming</au><au>Ma, Hongmei</au><au>An, Chunlei</au><au>Jiang, Su</au><au>Tang, Xueyuan</au><au>Hastings, Meredith G.</au><format>journal</format><genre>article</genre><ristype>JOUR</ristype><atitle>Isotope Fractionation of Nitrate During Volatilization in Snow: A Field Investigation in Antarctica</atitle><jtitle>Geophysical research letters</jtitle><date>2019-03-28</date><risdate>2019</risdate><volume>46</volume><issue>6</issue><spage>3287</spage><epage>3297</epage><pages>3287-3297</pages><issn>0094-8276</issn><eissn>1944-8007</eissn><abstract>Several postdepositional processes impact snow nitrate; however, only the isotopic effects of nitrate photolysis have been quantified. Here we discuss results from experiments in field Antarctic snow investigating isotopic fractionation of nitrate due to volatilization. At −35 °C, concentration and isotopic composition of nitrate remained constant during the 16‐day experiment. At −24 °C, 7.5% of nitrate was lost, synchronous with 1.5‰ decrease in δ18O and a constant δ15N. At −4 °C, 38% of nitrate was lost, and δ15N and δ18O decreased by 3.1 and 1.8‰, respectively. Results at −4 °C yield calculated fractionation constants close to theoretical estimates including equilibrium isotopic exchange between nitric acid and nitrate and the desorption of nitric acid from water in quasi‐liquid layers. This suggests that isotopic fractionation associated with nitrate volatilization across most of Antarctica, especially at sites with temperatures <−24 °C, should be minor, but the isotopic effects at warmer sites should be considered in interpreting archived nitrate records.
Plain Language Summary
In polar regions, there is great interest in using nitrate archived in snow/ice to reconstruct aspects of atmospheric composition and the influence of natural versus man‐made emissions. However, nitrate can be lost from the snowpack, such that the archived signals do not directly reflect atmospheric loading. Stable isotopes of nitrate in snow/ice allow for tracking and understanding the origins of nitrate and how it might have changed after deposition. While the isotopic fractionation associated with photolytic loss of nitrate has been directly quantified, that of volatilization remains poorly understood. Thus, we completed field experiments in Antarctica to investigate the isotopic effects of nitrate volatilization from snow. Results show that nitrate volatilization loss is significant at −4 °C, resulting in an important change (depletion of heavy isotopes) in both nitrogen and oxygen in remaining snow nitrate. This can be largely explained by a combination of equilibrium isotopic exchange between nitric acid and nitrate and the desorption of nitric acid from water in ice surface layers. At lower temperatures (<−24 °C), nitrate loss is rather minor, and the isotopic fractionation is found to be negligible. The findings suggest that the isotopic effects of NO3− volatilization in snow are closely related to temperature.
Key Points
Field experiments in Antarctica (over 16 days) were used to quantify the isotopic effects of NO3− volatilization from snow
Volatilization at −4 °C depletes heavy isotopes of NO3− in remaining snow versus relatively constant isotopic ratios observed at −35 °C
Volatilization can decrease δ15N in remaining snow NO3− in warm regions by several per mil, contrary to isotopic effects of photolysis</abstract><cop>Washington</cop><pub>John Wiley & Sons, Inc</pub><doi>10.1029/2019GL081968</doi><tpages>11</tpages><orcidid>https://orcid.org/0000-0003-4945-9405</orcidid><orcidid>https://orcid.org/0000-0003-1702-6322</orcidid><orcidid>https://orcid.org/0000-0001-6716-6783</orcidid><orcidid>https://orcid.org/0000-0002-8579-2400</orcidid><orcidid>https://orcid.org/0000-0001-6712-7979</orcidid><orcidid>https://orcid.org/0000-0002-0276-2418</orcidid></addata></record> |
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| ispartof | Geophysical research letters, 2019-03, Vol.46 (6), p.3287-3297 |
| issn | 0094-8276 1944-8007 |
| language | eng |
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| source | Wiley-Blackwell AGU Digital Archive |
| subjects | Acids Antarctic snow Atmospheric chemistry Atmospheric composition Constants coupled cluster method Depletion Desorption Exchanging Field investigations Field tests Fractionation Ice Investigations Isotope composition Isotope fractionation Isotopes Low temperature nitrate Nitrates Nitric acid Nitric acids Oxygen Photolysis Polar environments Polar regions Snow Snowpack stable isotope Stable isotopes Surface boundary layer Surface layers Volatilization |
| title | Isotope Fractionation of Nitrate During Volatilization in Snow: A Field Investigation in Antarctica |
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