Isotopic constraints on sources, production, and phase partitioning for nitrate in the atmosphere and snowfall in coastal East Antarctica

Isotopic constraints on sources, production, and phase partitioning for nitrate in the atmosphere and snowfall in coastal East Antarctica
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东南极洲沿海大气和降雪中硝酸盐来源、生产和相分配的同位素限制

DOI:
10.1016/j.epsl.2021.117300
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发表时间:
2022-01
影响因子:
5.3
通讯作者:
Meredith G. Hastings
Meredith G. Hastings
中科院分区:
地球科学1区
文献类型:
--
作者:
Guitao Shi;Chuanjin Li;Yilan Li;Zhenlou Chen;Minghu Ding;Hongmei Ma;Su Jiang;Chunlei An;Jingxue Guo;Bo Sun;Meredith G. Hastings

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利用南极东部沿海地区近两年来采集的大气样品和降雪资料,根据NO3-(δ 15 N,δ 18 O,Δ 17 O)同位素组成,研究了大气NO3-的来源、产生及其与降雪NO3-的关系。降雪和大气中NO 3−的浓度和同位素组成显示出相似的季节性趋势。在夏季,大气中的NO3-与积雪中NO3-光解产生的NOx排放密切相关。在冬季,降雪和大气中NO3 −的δ 15 N和δ 18 O(或Δ 17 O)之间的线性关系表明平流层输入和对流层源之间的混合对NO3 −起作用,平流层输入占大气NO3 −预算的55±21%。线性关系表明,平流层源NO3-的δ 15 N、δ 18 O和Δ 17 O的下限分别接近1.18 ‰、1.120 ‰和1.45 ‰。浓度与冬季NO3 −的同位素组成相关性很好,表明对流层源的贡献较小。NO 3−的δ 18 O和Δ 17 O之间的显著线性相关性表明O3和H2 O/OH的氧化过程混合,这可能会影响NOx循环和NO 3−的产生。在9月的O3耗竭事件中,观测到大气NO3 −的Δ 17 O值较低,表明NO3 −的氧同位素可能比BrO浓度对地表O3的变化更敏感。降雪中NO3 −的氧同位素组成与大气中的氧同位素组成全年接近,这表明降雪NO3 −可以传递大气中NOx氧化化学的信息。冬季降雪的δ 15 N值与大气中的δ 15 N值接近,而夏季降雪的δ 15 N值比大气中的δ 15 N值高出约20‰,这可能与大气NO3-气溶胶分配的季节变化有关。这表明,雪中δ 15 N的解释需要考虑来源和化学的季节变化。
Atmospheric samples and snowfall collected in coastal East Antarctica over two years are used to investigate the sources, production of atmospheric nitrate (NO 3−) and its link with snowfall NO 3− based upon the isotopic composition of NO 3−(δ 15 N, δ 18 O, and Δ 17 O). Snowfall and the atmosphere show similar seasonal trends in concentrations and isotopic composition of NO 3−. In summer, atmospheric NO 3− is closely associated with snowpack emissions of NO x from photolysis of snow NO 3−. In winter, linear relationships between δ 15 N and δ 18 O (or Δ 17 O) of NO 3− in both snowfall and the atmosphere indicate mixing between stratospheric inputs and tropospheric sources contributing to NO 3−, with stratospheric inputs contributing 55±21% of the atmospheric NO 3− budget. The linear relationships suggest that the lower limits of δ 15 N, δ 18 O, and Δ 17 O of stratospheric-sourced NO 3− are close to∼ 18,∼ 120, and∼ 45‰, respectively. Concentration correlates well with the isotopic composition of NO 3− in winter, indicating less variable contribution of tropospheric sources. A significant linear correlation between δ 18 O and Δ 17 O of NO 3− suggests a mix of oxidation processes by O 3 and H 2 O/OH which can influence NO x cycling and the production of NO 3−. Lower values of Δ 17 O of atmospheric NO 3− were observed during O 3 depletion events in September, suggesting that oxygen isotopes of NO 3− could be more sensitive to the changes in surface O 3 compared to BrO concentrations. Oxygen isotopic composition of NO 3− in snowfall is close to that of the atmosphere throughout the year, suggesting that snowfall NO 3− can relay information on oxidative chemistry of NO x in the atmosphere. Snowfall δ 15 N is close in value to that in the atmosphere during winter, but∼ 20‰ higher than that in the atmosphere during summer, possibly associated with seasonal changes in the gas-aerosol partitioning of atmospheric NO 3−. This suggests that the interpretation of δ 15 N in snow needs to consider seasonal changes in sources and chemistry.
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发表时间: 2017-07
影响因子: 5.1
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