Quantification of iodine monoxide based on incoherent broadband cavity enhanced absorption spectroscopy

Zhang He-Lu; Qin Min; Fang Wu; Tang Ke; Duan Jun; Meng Fan-Hao; Shao Dou; Hua Hui; Liao Zhi-Tang; Xie Pin-Hua

doi:10.7498/aps.70.20210312

Abstract

The quantitative method of iodine monoxide radical (IO) using incoherent broadband cavity enhanced absorption spectroscopy (IBBCEAS) in the 435–465 nm band is described in this paper. In order to obtain the concentration of IO accurately, the parameters such as the mirror reflectivity, effective cavity length and sample loss of the IBBCEAS system are evaluated. Using the difference of Rayleigh scattering between nitrogen and helium, the reflectivity curve of the high-reflection mirror is obtained. The reflectivity R of the mirror at 436.1 nm of the IO absorption peak is about 0.99982, and the effective absorption optical path reaches 3.83 km under vacuum condition. According to the absorption of O₄, the effective cavity length of the modified system is 60.7 cm. The Allan deviation is used to evaluate the performance of the system, and the standard deviation is used to analyze the detection sensitivity of the system. When the time resolution is 60 s, the detection sensitivity (2σ) of the system for IO and NO₂ are 1.9 pptv and 20 pptv (part per trillion by volume), respectively. The iodine dissolved in potassium iodide (KI) solution is taken out by the bubbling method and react with ozone after photolysis to produce a stable concentration of IO sample gas. The IO loss in the sampling tube is calibrated, and the results show that the sampling tube has no significant effect on the IO loss. The IBBCEAS system is used to determine the linearity of IO, and the correlation coefficient R² between the measured concentration of IO and the proportioned concentration in a concentration range from 39 to 530 pptv is 0.99. The IO produced by the reaction of iodine released from kelp with ozone is measured.

Keywords:

Authors and contacts

1.
Anhui Institute of Optics and Fine Mechanics, Hefei Institute of Material Science, Chinese Academy of Sciences, Key Laboratory of Environmental Optics and Technology, Chinese Academy of Sciences, Hefei 230031, China
2.
University of Science and Technology of China, Hefei 230026, China

Corresponding author: Qin Min, mqin@aiofm.ac.cn

Funds: Project supported by the National Natural Science Foundation of China (Grant Nos. 41875154, U19A2044) and the Anhui Provincial Key R&D Program, China (Grant No. 202104i07020010)

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References

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Cited By

图 1 基于蓝光LED的非相干宽带腔增强吸收光谱系统组成示意图

Figure 1. Schematic of the incoherent broadband cavity-enhanced absorption spectrometer based on blue LED.

DownLoad: Full-Size Img PowerPoint

图 2 (a)镜片反射率标定曲线, 黑线为镜片反射率曲线, 红线为氦气谱, 蓝线为氮气谱; (b) 435—465 nm波段主要吸收成分IO, NO₂, H₂O, O₄的吸收截面

Figure 2. (a) Reflectivity calibration of the mirror reflectivity. The blue and red curves represent intensity spectrum when the cavity is filled with N₂ and He, respectively. The black line represents derived mirror reflectivity curve. (b) Cross sections of NO₂ (sky blue line), H₂O (grey line), IO (red line) and O₄ (black line) in the 435–465 nm band.

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图 3 依次关闭和开启N₂吹扫时测量的O₂浓度时间序列图

Figure 3. Temporal variation of O₂ concentration with and without N₂ purge gas.

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图 4 IBBCEAS系统的评估　(a)和(b)分别是测量N₂背景下光谱反演的NO₂和IO的浓度时间序列; (c)和(d)分别是NO₂和IO的艾伦方差及标准偏差随平均时间的变化曲线

Figure 4. Evaluation of the performance of IBBCEAS instrument. Panels (a) and (b) are the time series of NO₂ and IO concentrations with 3 s acquisition time when the cavity is filled with N₂. Panels (c) and (d) are the variation curves of Allan and standard deviation plots for NO₂ and IO with mean time, respectively

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图 5 三套系统测量的NO₂浓度时间序列图, 黑线为中心波长为436 nm的IBBCEAS系统的NO₂浓度时间序列, 红线为中心波长为368 nm的IBBCEAS系统的NO₂浓度时间序列, 蓝线为LP-DOAS系统的NO₂浓度时间序列

Figure 5. Comparison of NO₂ concentration measured by three different instruments. The black, red and blue dotted lines denote the NO₂ concentrations measured by IBBCEAS (center wavelength: 368 nm and 436 nm) and LP-DOAS, respectively.

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图 6 (a) IBBCEAS (中心波长368 nm)和IBBCEAS (中心波长436 nm)测量的NO₂浓度的相关性; (b) IBBCEAS (中心波长436 nm)和LP-DOAS测量的NO₂浓度的相关性

Figure 6. (a) Correlation analysis of NO₂ concentrations measured by two IBBCEAS instruments (center wavelength: 368 nm and 436 nm); (b) correlation of NO₂ concentrations measured by IBBCEAS instrument (center wavelength: 436 nm) and LP-DOAS.

DownLoad: Full-Size Img PowerPoint

图 7 实验室IO的测量示意图

Figure 7. Schematic diagram of laboratory IO measurement system.

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图 8 IO采样损耗标定, 黑点表示采用10 m PFA采样管测得的IO, 红点表示采用3 m PFA采样管测得的IO

Figure 8. Measurements of IO loss in the sampling tube, black dots correspond to the IO measured with the 10 m PFA sample tube, red dots correspond to the IO measured with the 3 m PFA sample tube.

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图 9 (a)线性实验下IO的浓度时间序列图; (b)测量IO的浓度与配比浓度的相关性

Figure 9. (a) Different concentrations of IO measured by IBBCEAS; (b) the correlation analysis between the average of these concentration gradients and the normalized mixing ratio.

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图 10 随时间变化的不同浓度的IO反演实例, 最底层是反应时间为137.5 min的光谱反演的拟合残差

Figure 10. Example of retrieved absorption spectra of different IO concentrations varying with time, the fitting residuals of spectral retrieved with reaction time of 137.5 min is showed in the bottom of the figure.

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图 11 (a) IO的浓度时间序列图, 红色三角形代表海带的F_v/F_m值; (b) NO₂的浓度时间序列图, 阴影部分面积表示测量浓度的2σ拟合误差

Figure 11. (a) Time series of IO concentrations measured by the IBBCEAS. The red triangle denote the F_v/F_m of luminaria; (b) time series of NO₂ concentrations, and the shadow area represent the 2σ deviation error.

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表 1 相关IO测量仪器检测限和时间分辨率对比

Table 1. Comparison of detection limit and time resolution of correlated IO measuring instruments.

系统	时间分辨率	检测限(2σ)	参考文献
LP-DOAS	60 s	1.25 pptv	Commane等^[2] (2011)
MAX-DOAS	60 s	1.3 × 10¹³ molecule·cm^–2	Coburn等^[6] (2011)
LIF	300 s	0.6 pptv	Gravestocket等^[8] (2010)
CRDS	30 s	10 pptv	Wada等^[9] (2007)
ML-CEAS	300 s	20 ppqv	Grilli等^[10] (2012)
IBBCEAS	60 s	30 pptv	Vaughan等^[14] (2008)
IBBCEAS	60 s	4.4 pptv	Ashu-Ayem等^[12] (2012)
IBBCEAS	22 min	0.6 pptv	Thalman等^[13] (2010)
IBBCEAS	60 s	1.9 pptv	This work

DownLoad: CSV

[1]	Seitz K, Buxmann J, Pohler D, Sommer T, Tschritter J, Neary T, O'Dowd C, Platt U 2010 Atmos. Chem. Phys. 10 2117 Google Scholar
[2]	Commane R, Seitz K, Bale C S E, Bloss W J, Buxmann J, Ingham T, Platt U, Pöhler D, Heard D E 2011 Atmos. Chem. Phys. 11 6721 Google Scholar
[3]	Furneaux K L, Whalley L K, Heard D E, Atkinson H M, Bloss W J, Flynn M J, Gallagher M W, Ingham T, Kramer L, Lee J D, Leigh R, McFiggans G B, Mahajan A S, Monks P S, Oetjen H, Plane J M C, Whitehead J D 2010 Atmos. Chem. Phys. 10 3645 Google Scholar
[4]	Gómez Martín J C, Mahajan A S, Hay T D, Prados-Román C, Ordóñez C, MacDonald S M, Plane J M C, Sorribas M, Gil M, Paredes Mora J F, Agama Reyes M V, Oram D E, Leedham E, Saiz-Lopez A 2013 J. Geophys. Res.: Atmospheres 118 887 Google Scholar
[5]	Mahajan A S, Shaw M, Oetjen H, Hornsby K E, Carpenter L J, Kaleschke L, Tian-Kunze X, Lee J D, Moller S J, Edwards P, Commane R, Ingham T, Heard D E, Plane J M C 2010 J. Geophys. Res. 115 D20303 Google Scholar
[6]	Coburn S, Dix B, Sinreich R, Volkamer R 2011 Atmospheric Measurement Techniques 4 2421 Google Scholar
[7]	Alicke B, Hebestreit K, Stutz J, Platt U 1999 Nature 397 572 Google Scholar
[8]	Gravestock T J, Blitz M A, Heard D E 2010 Phys. Chem. Chem. Phys. 12 823 Google Scholar
[9]	Wada R, Beames J M, Orr-Ewing A J 2007 J. Atmos. Chem. 58 69 Google Scholar
[10]	Grilli R, Mejean G, Kassi S, Ventrillard I, Abd-Alrahman C, Romanini D 2012 Environ. Sci. Technol. 46 10704 Google Scholar
[11]	Whalley L K, Furneaux K L, Gravestock T, Atkinson H M, Bale C S E, Ingham T, Bloss W J, Heard D E 2007 J. Atmos. Chem. 58 19 Google Scholar
[12]	Ashu-Ayem E R, Nitschke U, Monahan C, Chen J, Darby S B, Smith P D, O'Dowd C D, Stengel D B, Venables D S 2012 Environ. Sci. Technol. 46 10413 Google Scholar
[13]	Thalman R, Volkamer R 2010 Atmospheric Measurement Techniques 3 1797 Google Scholar
[14]	Vaughan S, Gherman T, Ruth A A, Orphal J 2008 Phys. Chem. Chem. Phys. 10 4471 Google Scholar
[15]	Barbero A, Blouzon C, Savarino J, Caillon N, Dommergue A, Grilli R 2020 Atmospheric Measurement Techniques 13 4317 Google Scholar
[16]	Wei N, Hu C, Zhou S, Ma Q, Mikuska P, Vecera Z, Gai Y, Lin X, Gu X, Zhao W, Fang B, Zhang W, Chen J, Liu F, Shan X, Sheng L 2017 RSC Adv. 7 56779 Google Scholar
[17]	Duan J, Qin M, Ouyang B, Fang W, Li X, Lu K, Tang K, Liang S, Meng F, Hu Z, Xie P, Liu W, Häsler R 2018 Atmospheric Measurement Techniques 11 4531 Google Scholar
[18]	凌六一, 秦敏, 谢品华, 胡仁志, 方武, 江宇, 刘建国, 刘文清 2012 物理学报 61 140703 Google Scholar Ling L Y, Qin M, Xie P H, Hu Z R, Fang W, Jiang Y, Liu J G, Liu W Q 2012 Acta Phys. Sinc. 61 140703 Google Scholar
[19]	Spietz P, Martin J C G, Burrows J P 2005 J. Photoch. Photobio. A 176 50 Google Scholar
[20]	Voigt S, Orphal J, Burrows J P 2002 J. Photoch. Photobio. A 149 1 Google Scholar
[21]	Rothman L S, Gordon I E, Babikov Y, Barbe A, Benner D C, Bernath P F, Birk M, Bizzocchi L, Boudon V, Brown L R, Campargue A, Chance K, Cohen E A, Coudert L H, Devi V M, Drouin B J, Fayt A, Flaud J M, Gamache R R, Harrison J J, Hartmann J M, Hill C, Hodges J T, Jacquemart D, Jolly A, Lamouroux J, Le Roy R J, Li G, Long D A, Lyulin O M, Mackie C J, Massie S T, Mikhailenko S, Muller H S P, Naumenko O V, Nikitin A V, Orphal J, Perevalov V, Perrin A, Polovtseva E R, Richard C, Smith M A H, Starikova E, Sung K, Tashkun S, Tennyson J, Toon G C, Tyuterev V G, Wagner G 2013 J. Quant. Spectrosc. Radiat. Transf. 130 4 Google Scholar
[22]	Washenfelder R A, Langford A O, Fuchs H, Brown S S 2008 Atmospheric Chem. Phys. 8 7779 Google Scholar
[23]	Liang S, Qin M, Xie P, Duan J, Fang W, He Y, Xu J, Liu J, Li X, Tang K, Meng F, Ye K, Liu J, Liu W 2019 Atmospheric Measurement Techniques 12 2499 Google Scholar
[24]	Thalman R, Volkamer R 2013 Phys. Chem. Chem. Phys. 15 15371 Google Scholar
[25]	Axson J L, Washenfelder R A, Kahan T F, Young C J, Vaida V, Brown S S 2011 Atmospheric Chem. Phys. 11 11581 Google Scholar
[26]	Tang K, Qin M, Fang W, Duan J, Meng F, Ye K, Zhang H, Xie P, He Y, Xu W, Liu J, Liu W 2020 Atmospheric Measurement Techniques 13 6487 Google Scholar
[27]	覃志松, 赵南京, 殷高方, 石朝毅, 甘婷婷, 肖雪, 段静波, 张小玲, 陈双, 刘建国, 刘文清 2017 光学学报 37 0730002 Qin Z S, Zhao N J, Yin G F, Shi C Y, Gan T T, Xiao X, Duan J B, Zhang X L, Chen S, Liu J G, Liu W Q 2017 Acta Opt. Sin. 37 0730002
[28]	刘晶, 刘文清, 赵南京, 张玉均, 马明俊, 殷高方, 戴庞达, 王志刚, 王春龙, 段静波, 余晓娅, 方丽 2013 光谱学与光谱分析 33 2443 Google Scholar Liu J, Liu W, Zhao N, Zhang Y, Ma M, Yin G, Dai P, Wang Z, Wang C, Duan J, Yu X, Fang L 2013 Spectrosc Spect Anal. 33 2443 Google Scholar

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Vol. 70, Issue 15 - 2021-08-05

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