基于MAX-DOAS观测的鹤山地区对流层甲醛廓线反演研究

doi:10.3964/j.issn.1000-0593(2024)06-1781-08

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摘要：甲醛（HCHO）是大气中一种十分重要的痕量气体，它不仅与人类健康和环境密切相关，还在对流层光化学反应中扮演着极其重要的角色。近年来，我国珠三角地区的秋季对流层臭氧及甲醛污染问题较为严重，而对流层甲醛也是分析边界层臭氧形成机理的关键性指标之一，因此，在珠三角地区开展甲醛观测实验具有十分重要的意义。利用多轴差分吸收光谱技术（MAX-DOAS）反演了鹤山超级站2019年9月20日至10月3日期间的氧气二聚体（O₄）与HCHO的差分斜柱浓度（DSCD），使用几何近似法得到了甲醛的大气质量因子（AMF），进而获得了对流层甲醛的垂直柱浓度（VCD）。结果显示，观测期间的对流层甲醛VCD在4.99×10¹³～6.48×10¹⁶ molec·cm^-2之间波动，平均值为2.18×10¹⁶ molec·cm^-2。将MAX-DOAS反演的对流层甲醛VCD与TROPOMI结果进行了对比，结果表明，MAX-DOAS与TROPOMI结果近乎一致，相关性系数R为0.80，但9月25日与28日的TROPOMI结果偏低了约25%，这可能是由于观测方式不同所导致的。此外，该研究还基于反演的O₄与甲醛DSCD，使用基于最优估计算法的海德堡大学廓线反演算法（HEIPRO）反演了观测期间的对流层气溶胶及甲醛廓线，结果表明，甲醛污染主要集中在近地面0～800 m内，观测期间的甲醛污染主要来源于当地的工业及机动车尾气排放。将MAX-DOAS技术反演的近地面甲醛结果与2,4-二硝基苯肼色谱技术测量结果进行了对比，结果表明，两种技术的近地面甲醛结果的一致性较高，均观测到了9月27至29日的近地面甲醛高值（峰值达到了14.31 μg·m^-3），且相关性系数R为0.88，斜率为0.98，验证了MAX-DOAS技术反演的近地面甲醛结果的可靠性。MAX-DOAS技术可实现对流层甲醛VCD的实时监测，可作为验证星载观测结果的一种重要手段，结合最优估计算法，MAX-DOAS技术还可以实现对流层甲醛廓线的反演。

关键词：多轴差分吸收光谱技术；对流层甲醛；最优估计算法；鹤山；卫星校验

Abstract：Formaldehyde (HCHO) is one of the most important trace gases in the atmosphere.It's closely related to human health and the environment and plays an extremely important role in tropospheric photochemical reactions. In recent years, the autumn tropospheric ozone and HCHO pollution problems in the Pearl River Delta (PRD) region of China have become more serious, and the tropospheric HCHO is one of the key indicators for analyzing the formation mechanism of the boundary ozone. Therefore, it is of great importance for us to carry out the HCHO observation experiments in the PRD region. This study retrieved the differential slant column density (DSCD) of O₄ and HCHO at HeShan Observatory from September 20 to October 3, 2019 using the multi-axis differential optical absorption spectroscopy (MAX-DOAS) technique. The air mass factor (AMF) of HCHO was calculated using the geometric approximation method, thus obtaining the tropospheric HCHO vertical column density (VCD). The results showed that the tropospheric formaldehyde VCD fluctuated between 4.99×10¹³ and 6.48×10¹⁶ molec·cm^-2 during the observation period, with an average value of 2.18×10¹⁶ molec·cm^-2. The retrieved tropospheric HCHO VCD was almost consistent with that from TROPOspheric Monitoring Instrument (TROPOMI), with a correlation coefficient (R) of 0.80. However, the tropospheric HCHO VCD from TROPOMI on 25 and 28 September was lower (about 25%) than that from MAX-DOAS, which may be caused by the different observation methods. In addition, the retrieved O₄ and HCHO DSCD and HEIdelberg PROfile (HEIPRO) algorithms based on the optimal estimation method were used to retrieve the tropospheric aerosol and HCHO profiles during the observation period. The results showed that the HCHO pollution was mainly concentrated near the surface (0～800 m), and the HCHO pollution during the observation period mainly came from the local industrial and motor vehicle emissions. The retrieved surface HCHO from MAX-DOAS was compared with that from 2,4-dinitrophenylhydrazine chromatography technique. The surface HCHO from MAX-DOAS showed similar trends with that from the 2,4-dinitrophenylhydrazine chromatography technique. The high values (up to 14.31 μg·m^-3) of surface HCHO from 27 to 29 in September were simultaneously monitored, with the correlation coefficient (R) and slope of 0.88 and 0.98, respectively, which validates the reliability of surface HCHO results retrieved from MAX-DOAS technique.The results of this study show that the MAX-DOAS technique can realize the real-time monitoring of tropospheric HCHO VCD, which can be used as an important means to verify satellite-based measurements. The tropospheric HCHO profiles can be retrieved using the MAX-DOAS technique.

Key words：Multi-axis differential optical absorption spectroscopy; Tropospheric formaldehyde; Optimal estimation method; Heshan; Satellite calibration

收稿日期: 2023-06-25 修订日期: 2023-07-25

中图分类号:

X831

基金资助: 国家自然科学基金青年科学基金项目（61905256）资助

通讯作者: 司福祺 E-mail: sifuqi@aiofm.ac.cn

作者简介: 钱园园，1996年生，中国科学院安徽光学精密机械研究所博士研究生 e-mail: qyyqdd@mail.ustc.edu.cn

引用本文:

钱园园，罗宇涵，周海金，窦科，常振，杨太平，奚亮，汤付颖，徐自强，司福祺. 基于MAX-DOAS观测的鹤山地区对流层甲醛廓线反演研究[J]. 光谱学与光谱分析, 2024, 44(06): 1781-1788.
QIAN Yuan-yuan, LUO Yu-han, ZHOU Hai-jin, DOU Ke, CHANG Zhen, YANG Tai-ping, XI Liang, TANG Fu-ying, XU Zi-qiang, SI Fu-qi. Research on Retrieval of Tropospheric Formaldehyde Profiles in Heshan Area From MAX-DOAS Measurements. SPECTROSCOPY AND SPECTRAL ANALYSIS, 2024, 44(06): 1781-1788.

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