大气硝酸盐中氮氧稳定同位素研究进展

doi:10.11867/j.issn.1001-8166.2019.02.0124

地球科学进展 ›› 2019, Vol. 34 ›› Issue (2): 124 -139. doi: 10.11867/j.issn.1001-8166.2019.02.0124

大气硝酸盐中氮氧稳定同位素研究进展

秦瑞(

),史贵涛 ^*(

),陈振楼

1. 华东师范大学地理科学学院，地理信息科学教育部重点实验室，上海 200241

收稿日期:2018-08-23 修回日期:2018-12-20 出版日期:2019-02-10
通讯作者: 史贵涛 E-mail:843128305@qq.com;gtshi@geo.ecnu.edu.cn
基金资助:
国家自然科学基金项目“东南极冰盖中山站至昆仑站断面雪层中NO $3 -$ 的沉积后机制研究：δ15N、δ18O和Δ17O证据”(编号：41576190)资助.

Review of the Study on the Stable Isotopes of Nitrogen and Oxygen in Atmospheric Nitrate

Rui Qin( ),Guitao Shi ^*( ),Zhenlou Chen

1. Key Laboratory of Geographic Information Science Ministry of Education, School of Geographic Sciences, East China Normal University, Shanghai 200241, China

Received:2018-08-23 Revised:2018-12-20 Online:2019-02-10 Published:2019-03-26
Contact: Guitao Shi E-mail:843128305@qq.com;gtshi@geo.ecnu.edu.cn
About author:Qin Rui(1991-), female, Lankao City, Henan Province, Master student. Research areas include stable isotope in environment. E-mail:843128305@qq.com|Shi Guitao (1982-), male, Zaozhuang City, Shandong Province, Professor. Research areas include polar environment. E-mail： gtshi@geo.ecnu.edu.cn
Supported by:
Project supported by the National Natural Science Foundation of China “Investigating mechanisms of post-depositional processing of nitrate in the snowpack on the traverse from coastal Zhongshan station to inland Kunlun station, East Antarctica: Evidence of δ15N, δ18O and Δ17O”(No. 41576190);Project supported by the National Natural Science Foundation of China “Investigating mechanisms of post-depositional processing of nitrate in the snowpack on the traverse from coastal Zhongshan station to inland Kunlun station, East Antarctica: Evidence of δ15N, δ18O and Δ17O” (No. 41576190).

全文 ( 20 ) 下载PDF ( 1317 )

受人类活动和工农业快速发展的影响，大气硝酸盐(NO $3 -$ )污染越来越严重且已成为世界范围内的环境问题之一。探究大气NO $3 -$ 的稳定同位素组成(δ¹⁵N，δ¹⁸O和Δ¹⁷O)，可以为深入理解大气氮循环、有效控制大气NO $3 -$ 污染提供有力依据。综述了目前大气NO $3 -$ 不同来源NOx的δ¹⁵N值、NO $3 -$ 的δ¹⁵N季节变化特征及主要影响因素，总结了大气中不同氧化剂的δ¹⁸O值和Δ¹⁷O值，归纳了全球范围内部分大气NO $3 -$ 中δ¹⁸O值和Δ¹⁷O值的时空分布特征及可能影响因素，回顾了NO $3 -$ 同位素分析测试技术的主要进展，在前期工作基础上提出未来大气NO $3 -$ 稳定同位素研究应更多关注NO $3 -$ 的氧化生成机制(不同类型氧化剂同位素组成时空差异)、不同NOx来源的δ¹⁵N组成、借助化学模型开展大气NO $3 -$ 循环过程等方面的研究。

关键词: 大气, 硝酸盐, 稳定同位素

Due to the emissions from intensive human activities and rapid development of industry and agriculture, atmospheric nitrate (NO $3 -$ ) contamination is becoming more serious and now is a worldwide environmental problem. The isotopic compositions of NO $3 -$ (δ¹⁵N, δ¹⁸O and Δ¹⁷O) can deliver more information than the concentration alone, i.e., the nitrogen and oxygen isotopes can suggest the sources of NO $3 -$ and oxidation capability of the atmosphere, providing a powerful tool for investigating atmospheric nitrogen cycling and atmospheric NO $3 -$ pollution control. The δ¹⁵N of different sourced NO $3 -$ in the atmosphere, as well as the seasonal variation of δ¹⁵N (NO $3 -$ ) and the associated mechanisms were reviewed. In addition, the oxygen isotopes of various oxidants and NO $3 -$ (δ¹⁸O and Δ¹⁷O) in the atmosphere were summarized, and the global distribution patterns of the oxygen isotopes of NO $3 -$ were discussed. Lastly, the available analysis techniques of isotopic compositions of NO $3 -$ were reviewed. Based on the research progress of NO $3 -$ isotopes in the atmosphere, it was suggested that further investigations should focus on measuring the isotopic compositions of oxidants and NOx from different sources, characterizing the production mechanisms of NO $3 -$ , as well as investigating chemical recycling between NOx and NO $3 -$ with the aid of atmospheric chemical models.

Key words: Atmosphere, Nitrate, Stable isotopes.

中图分类号:

P593
X51

表1 不同来源 NOx的 δ¹⁵N值

Table 1 The δ ¹⁵N values of NOx from different sources

来源	收集对象	δ¹⁵N/ $‰$	采集原理和处理方法	参考文献
车辆	HNO₃	5.7 ± 2.8	硝酸被动采样法—三乙醇胺吸收液法	[ 19 ]
	NO₂	10.0~17.0	Ogawa被动采样法—三乙醇胺吸收液法	[ 19 ]
		1.0±3.5	Ogawa被动采样法—三乙醇胺吸收液法	[ 20 ]
		5.7±2.8	CrO₃/H₃PO₄吸收氧化NO为NO₂，甲醇溶液吸收	[ 21 ]
	NOx	-9.0~-2.0	气体洗涤器采集NOx，KMnO₄/NaOH将其氧化为NO $3 -$	[ 22 ]
	NOx	-13.0~2.0	样气加入NaOH/H₂O₂后，静止震荡，甲醇溶液吸收	[ 23 ]
土壤释放	NO₂	-30.8~-26.5	Ogawa被动采样法—三乙醇胺吸收液法	[ 24 ]
	NO₂	-35.5,-29.1	CrO₃/H₃PO₄吸收氧化NO为NO₂，甲醇溶液吸收	[ 25 ]
	NO	-59.8~-23.4	NO-NO₂转化法吸收NO，过量O₃将其氧化为NO₂，20 $%$ 三乙醇胺吸收液吸收（动力通量箱法）	[ 26 ]
多种生物质燃烧	NOx	-7.0~12.0	气体洗涤器采集NOx，KMnO₄/NaOH将其氧化为NO $3 -$	[ 27 ]
单一生物质燃烧	总氮	10.6~25.7	—	[ 28 ]
肥料	NO $3 -$	-5.0~5.0	去离子水浸取水溶性NO $3 -$ ，然后将其转化为KNO₃	[ 29 ]
闪电	NOx	-0.5~1.4	—	[ 30 ]
化石燃料燃烧	NOx	6.0~13.0	样气中加入NaOH/H₂O₂后，静止震荡，甲醇溶液吸收	[ 22 ]

表1 不同来源 NOx的 δ¹⁵N值

Table 1 The δ ¹⁵N values of NOx from different sources

来源	收集对象	δ¹⁵N/ $‰$	采集原理和处理方法	参考文献
车辆	HNO₃	5.7 ± 2.8	硝酸被动采样法—三乙醇胺吸收液法	[ 19 ]
	NO₂	10.0~17.0	Ogawa被动采样法—三乙醇胺吸收液法	[ 19 ]
		1.0±3.5	Ogawa被动采样法—三乙醇胺吸收液法	[ 20 ]
		5.7±2.8	CrO₃/H₃PO₄吸收氧化NO为NO₂，甲醇溶液吸收	[ 21 ]
	NOx	-9.0~-2.0	气体洗涤器采集NOx，KMnO₄/NaOH将其氧化为NO $3 -$	[ 22 ]
	NOx	-13.0~2.0	样气加入NaOH/H₂O₂后，静止震荡，甲醇溶液吸收	[ 23 ]
土壤释放	NO₂	-30.8~-26.5	Ogawa被动采样法—三乙醇胺吸收液法	[ 24 ]
	NO₂	-35.5,-29.1	CrO₃/H₃PO₄吸收氧化NO为NO₂，甲醇溶液吸收	[ 25 ]
	NO	-59.8~-23.4	NO-NO₂转化法吸收NO，过量O₃将其氧化为NO₂，20 $%$ 三乙醇胺吸收液吸收（动力通量箱法）	[ 26 ]
多种生物质燃烧	NOx	-7.0~12.0	气体洗涤器采集NOx，KMnO₄/NaOH将其氧化为NO $3 -$	[ 27 ]
单一生物质燃烧	总氮	10.6~25.7	—	[ 28 ]
肥料	NO $3 -$	-5.0~5.0	去离子水浸取水溶性NO $3 -$ ，然后将其转化为KNO₃	[ 29 ]
闪电	NOx	-0.5~1.4	—	[ 30 ]
化石燃料燃烧	NOx	6.0~13.0	样气中加入NaOH/H₂O₂后，静止震荡，甲醇溶液吸收	[ 22 ]

表2 不同氧化剂的 δ¹⁸O值和 Δ¹⁷O值

Table 2 The δ ¹⁸O and Δ ¹⁷O values of different oxidants

氧化剂种类	δ¹⁸O/ $‰$	Δ¹⁷O/ $‰$	研究方法与原理	研究区域或方式	参考文献
O₃	—	24.9	利用NO $2 -$ 涂层，O₃+NO $2 -$ →O₂+ NO $3 -$	DomeC	[ 67 ]
	95.2	34.3	数据插值模拟	实验室模拟	[ 14 ]
	115.0	23.0, 26.0	利用NO $2 -$ 涂层，O₃+NO $2 -$ →O₂+ NO $3 -$	50°S~50°N	[ 68 , 69 ]
	75.0~85.0	32.0~37.0	利用NO $2 -$ 涂层，O₃+NO $2 -$ →O₂+ NO $3 -$	美国加利福尼亚	[ 70 ]
	—	38.0	光化学平衡模型模拟	中纬度对流层	[ 66 ]
	109.0	26.0	低温试验法，T=-218 $℃$ ,O₃+Xe→O₂+O	美国对流层	[ 71 ]
	117.0	25.0	低温试验法，T=-218 $℃$ ,O₃+Xe→O₂+O	德国海德堡市	[ 72 ]
	90.0	32.0	放电O₃→O₂+O，质谱仪分析	实验室实验	[ 73 ]
O₂	23.2	-0.4	盒子模型预测	实验室模型预测	[ 74 ]
	23.4	-0.5	基于GC色谱柱提取纯化空气中O₂后， MAT253分析	全球尺度	[ 74 ]
	23.9	-0.5	CoF₃+H₂O→O₂，多接口质谱分析	实验室校正实验	[ 75 ]
	23.9	-0.5	CoF₃+H₂O→O₂，多接口质谱分析	实验室实验	[ 76 ]
	23.5	-0.3	O₂+BrF₅→O₂+其他，MAT251分析	实验室实验	[ 77 ]
	23.8	—	CO₂ ? H₂O (H₂+O₂)，质谱仪分析	—	[ 78 ]
	23.5	—	O₂→CO₂ ? H₂O，质谱仪分析	—	[ 79 ]
OH	-40.0~-60.2 (凝聚相)	0.0	模拟假设δ¹⁸O (OH)=δ¹⁸O (H₂O)	南极高原	[ 50 ]
	-69.1~-81.3 (气相)	0.0	模拟假设δ¹⁸O (OH)=δ¹⁸O (H₂O)(v)	南极高原	[ 50 ]
	<-50.0	0.0	模拟假设δ¹⁸O (OH)=δ¹⁸O (H₂O)	北极对流层	[ 80 ]
RO₂	—	0.0	—	美国普罗维登斯	[ 45 ]
RO₂	—	0.0	—	北半球地方	[ 81 ]
BrO	—	30.0～42.0	Br+O₃→BrO+O₂，理论计算	北极加拿大阿勒特	[ 16 ]
BrO	—	44.0	边界层大气，蒙特卡洛算法	北极阿勒特北部海岸	[ 82 ]

表2 不同氧化剂的 δ¹⁸O值和 Δ¹⁷O值

Table 2 The δ ¹⁸O and Δ ¹⁷O values of different oxidants

氧化剂种类	δ¹⁸O/ $‰$	Δ¹⁷O/ $‰$	研究方法与原理	研究区域或方式	参考文献
O₃	—	24.9	利用NO $2 -$ 涂层，O₃+NO $2 -$ →O₂+ NO $3 -$	DomeC	[ 67 ]
	95.2	34.3	数据插值模拟	实验室模拟	[ 14 ]
	115.0	23.0, 26.0	利用NO $2 -$ 涂层，O₃+NO $2 -$ →O₂+ NO $3 -$	50°S~50°N	[ 68 , 69 ]
	75.0~85.0	32.0~37.0	利用NO $2 -$ 涂层，O₃+NO $2 -$ →O₂+ NO $3 -$	美国加利福尼亚	[ 70 ]
	—	38.0	光化学平衡模型模拟	中纬度对流层	[ 66 ]
	109.0	26.0	低温试验法，T=-218 $℃$ ,O₃+Xe→O₂+O	美国对流层	[ 71 ]
	117.0	25.0	低温试验法，T=-218 $℃$ ,O₃+Xe→O₂+O	德国海德堡市	[ 72 ]
	90.0	32.0	放电O₃→O₂+O，质谱仪分析	实验室实验	[ 73 ]
O₂	23.2	-0.4	盒子模型预测	实验室模型预测	[ 74 ]
	23.4	-0.5	基于GC色谱柱提取纯化空气中O₂后， MAT253分析	全球尺度	[ 74 ]
	23.9	-0.5	CoF₃+H₂O→O₂，多接口质谱分析	实验室校正实验	[ 75 ]
	23.9	-0.5	CoF₃+H₂O→O₂，多接口质谱分析	实验室实验	[ 76 ]
	23.5	-0.3	O₂+BrF₅→O₂+其他，MAT251分析	实验室实验	[ 77 ]
	23.8	—	CO₂ ? H₂O (H₂+O₂)，质谱仪分析	—	[ 78 ]
	23.5	—	O₂→CO₂ ? H₂O，质谱仪分析	—	[ 79 ]
OH	-40.0~-60.2 (凝聚相)	0.0	模拟假设δ¹⁸O (OH)=δ¹⁸O (H₂O)	南极高原	[ 50 ]
	-69.1~-81.3 (气相)	0.0	模拟假设δ¹⁸O (OH)=δ¹⁸O (H₂O)(v)	南极高原	[ 50 ]
	<-50.0	0.0	模拟假设δ¹⁸O (OH)=δ¹⁸O (H₂O)	北极对流层	[ 80 ]
RO₂	—	0.0	—	美国普罗维登斯	[ 45 ]
RO₂	—	0.0	—	北半球地方	[ 81 ]
BrO	—	30.0～42.0	Br+O₃→BrO+O₂，理论计算	北极加拿大阿勒特	[ 16 ]
BrO	—	44.0	边界层大气，蒙特卡洛算法	北极阿勒特北部海岸	[ 82 ]

图1 大气中δ¹⁸O-NO $3 -$ 纬度梯度分布情况^{[

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Fig.1 The distributions of δ¹⁸O-NO $3 -$ of the atmosphere in different latitudes ^{[

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图1 大气中δ¹⁸O-NO $3 -$ 纬度梯度分布情况^{[

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Fig.1 The distributions of δ¹⁸O-NO $3 -$ of the atmosphere in different latitudes ^{[

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图2 大气中Δ¹⁷O-NO $3 -$ 纬度梯度分布情况^{[

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Fig.2 The distributions of Δ¹⁷O-NO $3 -$ of the atmosphere in different latitudes ^{[

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图2 大气中Δ¹⁷O-NO $3 -$ 纬度梯度分布情况^{[

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