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地球科学进展  2019, Vol. 34 Issue (9): 922-935    DOI: 10.11867/j.issn.1001-8166.2019.09.0922
综述与评述     
大气氧化态活性氮循环与稳定同位素过程:问题与展望
周涛1,2(),蒋壮1,2,耿雷1,2()
1. 冰芯和大气化学稳定同位素实验室 地球和空间科学学院 中国科学技术大学,安徽 合肥 230026
2. 极地环境与全球变化安徽省重点实验室, 安徽 合肥 230026
Atmospheric Reactive Nitrogen Cycle and Stable Nitrogen Isotope Processes: Progresses and Perspectives
Tao Zhou1,2(),Zhuang Jiang1,2,Lei Geng1,2()
1. Stable Isotope Laboratory of Ice Core and Atmospheric Chemistry,School of Earth and Spaces Sciences,University of Science and Technology of China,Hefei 230026,China
2. Anhui Key Laboratory of Polar Environment and Global Change, Hefei 230026,China
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摘要:

大气中氧化态活性氮主要包括氮氧化物(NO X =NO+NO2)和硝酸等。NO X 的循环过程会影响臭氧和羟基自由基的浓度,进而影响大气氧化能力。NO X 的氧化终端产物硝酸是颗粒污染物的重要组成部分,其干湿沉降过程会对生态系统产生影响。氮稳定同位素(δ 15N)在大气活性氮循环,示踪区域和全球活性氮排放、传输和沉降等研究方面都展现出了一定的潜力。回顾目前用δ 15N研究NO X 排放和大气活性氮循环的现状,从NO X 的产生机制和收集分析方法等方面讨论NO X δ 15N数据的不确定性及原因,分析NO X 和硝酸在大气转化和传输过程中氮同位素的分馏效应和影响等,最后讨论用δ 15N示踪NO X 排放的可能性和问题。虽然目前用δ 15N量化示踪排放源还存在比较大的不确定性,但是δ 15N可以有效地示踪大气活性氮循环和转化过程。在此基础上,有望利用大气化学传输模型,结合同位素观测数据和分馏机制,对区域和全球大气活性氮循环过程中的同位素效应进行综合评估,提高用δ 15N研究大气氧化态活性氮来源以及循环的准确性和可靠性。

关键词: 氮氧化物排放大气硝酸活性氮循环氮同位素    
Abstract:

Oxidized reactive nitrogen in the atmosphere mainly consists of nitrogen oxides (NO X =NO+NO2, NO3) and nitric acid. The atmospheric cycling of NO X influences the formation of ozone and hydroxyl radicals that are important for atmospheric oxidation capacity. Nitric acid, the final product of NO X oxidation, not only is an important component of particulate pollutants, but also has a direct impact on the ecosystem through dry and wet deposition.

The stable nitrogen isotope (δ15N) shows the potential to study reactive nitrogen cycle, and to trace the emission, transport and deposition of reactive nitrogen from local to global scales. Here, we reviewed previous studies using δ15N to investigate NO X emission and atmospheric reactive nitrogen cycle, and discuss the uncertainties of δ15N signatures of different NO X sources from two aspects: NO X generation mechanism and NO X collection methods. We also discussed the nitrogen isotope fractionation and the consequences during the conversions of NO y molecules. We ended up with discussions on the possibility of using δ15N to trace NO X emissions. Although there are still large uncertainties in quantifying and tracing NO X emissions using nitrogen stable isotopes, such isotope tool is efficient enough to trace reactive nitrogen cycles in the atmosphere. On the basis of this, we proposed that we can combine atmospheric chemistry transmission models with isotope tracers to improve our understanding of regional and global atmospheric reactive nitrogen cycle regarding the fluxes of different emission sources, their atmospheric transformation, etc.

Key words: NO X emission    Atmospheric nitric acid    Reactive nitrogen cycle    Nitrogen stable isotopes.
收稿日期: 2019-06-23 出版日期: 2019-11-15
ZTFLH:  P402  
基金资助: 国家自然科学基金优秀青年科学基金项目“冰芯同位素地球化学”(41822605);国家自然科学基金面上项目“青藏高原冰雪硝酸盐同位素组成;大气臭氧波动的关系研究”(41871051)
通讯作者: 耿雷     E-mail: zhoutao7@mail.ustc.edu.cn;genglei@ ustc.edu.cn;genglei@ustc.edu.cn
作者简介: 周涛(1996-),女,安徽肥西人,博士研究生,主要从事大气氧化态氮循环及其氮氧同位素研究. E-mail:zhoutao7@mail.ustc.edu.cn
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周涛, 蒋壮, 耿雷. 大气氧化态活性氮循环与稳定同位素过程:问题与展望[J]. 地球科学进展, 2019, 34(9): 922-935.

Tao Zhou, Zhuang Jiang, Lei Geng. Atmospheric Reactive Nitrogen Cycle and Stable Nitrogen Isotope Processes: Progresses and Perspectives. Advances in Earth Science, 2019, 34(9): 922-935.

链接本文:

http://www.adearth.ac.cn/CN/10.11867/j.issn.1001-8166.2019.09.0922        http://www.adearth.ac.cn/CN/Y2019/V34/I9/922

图1  不同源排放的NO X 的 δ 15N值
方法名称 收集装置 NO-NO2转化 吸收溶液 收集对象 收集效率
Heaton method[38] 样气被收集到聚乙烯容器后加入NO2吸收溶液 NaOH/H2O2溶液 NO X /
Freyer method[37] 样气通过NO-NO2转化装置后被NO2吸收溶液收集 固态氧化剂CrO3 三乙醇胺溶液 NO2和NO X /
Ammann method[33] 样气依次通过4根管状溶蚀器,分别收集HNO3,HONO,NO2和NO,第四根管子前放置氧化剂 固态氧化剂CrO3/H3PO4 管状溶蚀器附有KOH/愈创木酚的甲醇溶液涂层 NO2和NO /
Li and Wang method[28] 样气通过NO-NO2转化装置后被溶蚀器收集 固态氧化剂CrO3/H3PO4 管状溶蚀器附有KOH/愈创木酚的甲醇溶液涂层 NO /
Modified US EPA method[36,41,42] 样气通过有NO2收集溶液的真空纯净瓶收集 环境中O2 H2SO4/H2O2 NO X >97.5%
被动采样法(Passive samplers[34,35] 基于分子扩散原理,用采样滤膜收集 三乙醇胺滤膜 NO2 /
Figber method[45,65] 样气通过NO X 气体洗涤瓶 KMnO4/NaOH溶液 NO X 100%
动力学通量箱—三乙醇胺法(DFC-TEA method[44] 样气通过NO-NO2转化装置后被NO2吸收溶液收集 过量O3 20%三乙醇胺溶液 NO >98%
Walters method[62] 样气分别通过两根NO2溶蚀器(第一根收集、第二根检测是否收集完全) 管状溶蚀器附有KOH/愈创木酚的甲醇溶液涂层 NO2 /
表1   NO X 收集方法的总结
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