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Investigation of post-depositional processing of nitrate in East Antarctic snow: isotopic constraints on photolytic loss, re-oxidation, and source inputs
Shi, G.1,2,3; Buffen, A. M.2,3; Hastings, M. G.2,3; Li, C.4; Ma, H.1; Li, Y.1; Sun, B.1; An, C.1; Jiang, S.1
刊名ATMOSPHERIC CHEMISTRY AND PHYSICS
2015
卷号15期号:16页码:9435-9453
ISSN号1680-7316
DOI10.5194/acp-15-9435-2015
通讯作者Hastings, M. G.(meredith_hastings@brown.edu)
英文摘要Snowpits along a traverse from coastal East Antarctica to the summit of the ice sheet (Dome Argus) are used to investigate the post-depositional processing of nitrate (NO3-) in snow. Seven snowpits from sites with accumulation rates between 24 and 172 kg m(-2) a(-1) were sampled to depths of 150 to 300 cm. At sites from the continental interior (low accumulation, < 55 kg m(-2) a(-1)), nitrate mass fraction is generally > 200 ng g(-1) in surface snow and decreases quickly with depth to < 50 ng g(-1). Considerably increasing values of delta N-15 of nitrate are also observed (16-461% vs. air N-2), particularly in the top 20 cm, which is consistent with predicted fractionation constants for the photolysis of nitrate. The delta O-18 of nitrate (17-84% vs. VSMOW (Vienna Standard Mean Ocean Water)), on the other hand, decreases with increasing delta N-15, suggestive of secondary formation of nitrate in situ (following photolysis) with a low delta O-18 source. Previous studies have suggested that delta N-15 and delta O-18 of nitrate at deeper snow depths should be predictable based upon an exponential change derived near the surface. At deeper depths sampled in this study, however, the relationship between nitrate mass fraction and delta O-18 changes, with increasing delta O-18 of nitrate observed between 100 and 200 cm. Predicting the impact of post-depositional loss, and therefore changes in the isotopes with depth, is highly sensitive to the depth interval over which an exponential change is assumed. In the snowpits collected closer to the coast (accu-mulation > 91 kg m(-2) a(-1)), there are no obvious trends detected with depth and instead seasonality in nitrate mass fraction and isotopic composition is found. In comparison to the interior sites, the coastal pits are lower in delta N-15 (-15-71 parts per thousand vs. air N-2) and higher in delta O-18 of nitrate (53-111 parts per thousand vs. VSMOW). The relationships found amongst mass fraction, delta N-15, delta O-18 and Delta O-17 (Delta O-17 = delta O-17-0.52 x delta O-18) of nitrate cannot be explained by local post-depositional processes alone, and are instead interpreted in the context of a primary atmospheric signal. Consistent with other Antarctic observational and modeling studies, the isotopic results are suggestive of an important influence of stratospheric ozone chemistry on nitrate formation during the cold season and a mix of tropospheric sources and chemistry during the warm season. Overall, the findings in this study speak to the sensitivity of nitrate isotopic composition to post-depositional processing and highlight the strength of combined use of the nitrogen and oxygen isotopes for a mechanistic understanding of this processing.
收录类别SCI
WOS关键词DEEP ICE CORE ; ATMOSPHERIC NITRATE ; NITROGEN-DIOXIDE ; COASTAL ANTARCTICA ; DENITRIFIER METHOD ; ZHONGSHAN STATION ; QUANTUM YIELDS ; NOX EMISSIONS ; GLOBAL-MODEL ; SURFACE SNOW
WOS研究方向Meteorology & Atmospheric Sciences
WOS类目Meteorology & Atmospheric Sciences
语种英语
出版者COPERNICUS GESELLSCHAFT MBH
WOS记录号WOS:000360646500021
内容类型期刊论文
URI标识http://www.corc.org.cn/handle/1471x/2557028
专题寒区旱区环境与工程研究所
通讯作者Hastings, M. G.
作者单位1.Polar Res Inst China, Key Lab Polar Sci State Ocean Adm, Shanghai 200062, Peoples R China
2.Brown Univ, Dept Earth Environm & Planetary Sci, Providence, RI 02912 USA
3.Brown Univ, Inst Brown Environm & Soc, Providence, RI 02912 USA
4.Chinese Acad Sci, Cold & Arid Reg Environm & Engn Res Inst, State Key Lab Cryospher Sci, Lanzhou 730000, Peoples R China
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GB/T 7714
Shi, G.,Buffen, A. M.,Hastings, M. G.,et al. Investigation of post-depositional processing of nitrate in East Antarctic snow: isotopic constraints on photolytic loss, re-oxidation, and source inputs[J]. ATMOSPHERIC CHEMISTRY AND PHYSICS,2015,15(16):9435-9453.
APA Shi, G..,Buffen, A. M..,Hastings, M. G..,Li, C..,Ma, H..,...&Jiang, S..(2015).Investigation of post-depositional processing of nitrate in East Antarctic snow: isotopic constraints on photolytic loss, re-oxidation, and source inputs.ATMOSPHERIC CHEMISTRY AND PHYSICS,15(16),9435-9453.
MLA Shi, G.,et al."Investigation of post-depositional processing of nitrate in East Antarctic snow: isotopic constraints on photolytic loss, re-oxidation, and source inputs".ATMOSPHERIC CHEMISTRY AND PHYSICS 15.16(2015):9435-9453.
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