大气气溶胶硝酸盐氧同位素异常值测定方法

引用本文: 俞浩然, 曹芳, 张雯淇, 赵祝钰, 章炎麟. 大气气溶胶硝酸盐氧同位素异常值测定方法[J]. 分析化学, 2021, 49(2): 253-262. doi: 10.19756/j.issn.0253-3820.201479 shu

Citation: YU Hao-Ran, CAO Fang, ZHANG Wen-Qi, ZHAO Zhu-Yu, ZHANG Yan-Lin. Determination of ¹⁷O Anomaly in Atmospheric Aerosol Nitrate[J]. Chinese Journal of Analytical Chemistry, 2021, 49(2): 253-262. doi: 10.19756/j.issn.0253-3820.201479 shu

大气气溶胶硝酸盐氧同位素异常值测定方法

南京信息工程大学气候与环境变化国际合作联合实验室大气环境中心, 气象灾害预报预警与评估协同创新中心/气象灾害教育部重点实验室, 南京 210044

通讯作者: 章炎麟,E-mail:dryanlinzhang@outlook.com

基金项目:
国家自然科学基金项目（No.41977305）、国家重点研发计划项目（2017YFC0212704）、江苏省自然科学基金项目（No.BK20180040）和江苏省双创团队项目资助。

摘要: 改造了稳定同位素比质谱仪的外设设备，优化了细菌反硝化方法，并对金管高温热分解温度进行了讨论，建立了一种高灵敏度、高精度的适用于大气气溶胶硝酸盐氧同位素异常值（Δ¹⁷O-NO₃^-）快速测定的方法。本方法前处理步骤耗时约4 h，测定时间仅需15 min，所需样品含氮量检出限0.4 μg N（Δ¹⁷O测定精确度达到0.6‰），在0.8 μg N水平具有更好的测定精度（Δ¹⁷O测定精确度可达到0.19‰）。利用反硝化细菌（ATCC13985）将样品中的硝酸盐转化为N₂O，再利用自动进样器以及预浓缩装置将细菌反硝化，产生的N₂O气体通入纯金反应管热分解为N₂和O₂，继而进入MAT253稳定同位素比质谱仪测定其δ¹⁵N、δ¹⁷O、δ¹⁸O，并计算Δ¹⁷O。根据Δ¹⁷O国际标准样品建立Δ¹⁷O标准曲线，可换算出样品中硝酸盐的Δ¹⁷O，使用相同步骤可获得样品中硝酸盐的δ¹⁵N。使用0.8 μg含氮量IAEA-NO-3标准样品进行方法验证，Δ¹⁷O测定精确度可达到0.19‰，与真实值差值最小可达0.04‰。本方法具有灵敏度高、测定精确度高、测定速度快、前处理步骤简单、实验流程安全的优点。本方法在0.4 μg N低浓度水平样品测定时Δ¹⁷O测定精确度可达到0.6‰， δ¹⁵N测定精确度可达到0.3‰，因此，在适用于大气气溶胶样品的Δ¹⁷O及δ¹⁵N测定的同时，调整样品处理方法后，本方法也可用于雨水、雪水等低浓度大气环境样品的Δ¹⁷O及δ¹⁵N测定。

关键词:

English

Determination of ¹⁷O Anomaly in Atmospheric Aerosol Nitrate

Center for Atmospheric Environment, Joint Laboratory of International Cooperation on Climate and Environmental Change, Collaborative Innovation Center for Meteorological Disaster Forecasting and Assessment/Key Laboratory of Meteorological Disasters, Ministry of Education, Nanjing University of Information Science and Technology, Nanjing 210044, China

Corresponding author: ZHANG Yan-Lin, dryanlinzhang@outlook.com

Received Date: 08 August 2020
Revised Date: 11 November 2020
Fund Project:
Supported by the National Natural Science Foundation of China (No.41977305), the National Key Research and Development Project of China (No. 2017YFC0212704), the Natural Science Foundation of Jiangsu Province, China (No.BK20180040) and the Project of Jiangsu Enovation & Entrepreneurship Team.

Abstract: A novel method for rapid determination of ¹⁷O anomaly in atmospheric aerosol samples was developed. With this method, the measurement was completed in 15 min with higher analytical precision and lower detection limit. This method required a minimum of 0.4 μg N for achieving an analytical precision of 0.6‰, and 0.8 μg N was selected in this work. The nitrate in atmospheric aerosol samples was converted to nitrous oxide by optimized bacterial denitrification process within 4 h. After that a thermal decomposition of nitrous oxide in sample gas was carried out in a gold tube at 800℃ after separation and purification, followed by gas chromatographic separation and isotope analysis of oxygen. The experiment result showed that the analytical precision of Δ¹⁷O by this method could reach 0.19‰ at a sample content of 0.8 μg N, and δ¹⁵N could reach 0.15‰ at same time. This method was not only suitable for determination¹⁷O anomaly in atmospheric aerosol samples, but also for the other atmospheric environmental samples such as rain and snow samples with low concentrations.

Key words:

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沈阳化工大学材料科学与工程学院沈阳 110142

大气气溶胶硝酸盐氧同位素异常值测定方法

通讯作者: 章炎麟,E-mail:dryanlinzhang@outlook.com

English

Determination of ¹⁷O Anomaly in Atmospheric Aerosol Nitrate

Corresponding author: ZHANG Yan-Lin, dryanlinzhang@outlook.com

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通讯作者: 陈斌, bchen63@163.com

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大气气溶胶硝酸盐氧同位素异常值测定方法

通讯作者: 章炎麟,E-mail:dryanlinzhang@outlook.com

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Corresponding author: ZHANG Yan-Lin, dryanlinzhang@outlook.com

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