High precision measurement of spectroscopic parameters of H<sub>2</sub>S in 6320—6350 cm<sup>–1</sup> band

Tian Si-Di; Du Yan-Jun; Li Ji-Dong; Ding Yan-Jun; Peng Zhi-Min; Lü Jun-Fu; Pan Chao; Feng Xiao-Ya

doi:10.7498/aps.72.20221855

Abstract

As a highly corrosive and highly toxic gas, hydrogen sulfide (H₂S) is an important intermediate product or pollutant in many fields such as chemical industry, energy and environment. Accurate online measurement of its concentration is of great significance for process control and production safety. Tunable diode laser absorption spectroscopy (TDLAS), as a quantitative absorption spectroscopy technique, is suitable for high-precision on-line measurement of H₂S concentration in atmospheric environmental monitoring and industrial processes control. Considering that most of the spectroscopic parameters of H₂S in the HITRAN2020 database are mainly calculated based on semi-empirical theoretical model and the experimental data to support them are lacking. In this work, direct absorption spectroscopy (DAS) method is firstly used to measure the absorption spectra of H₂S in the band of 6320–6350 cm^–1. Six groups of characteristic lines with strong absorption and relative independence are selected as the target transitions for experimental measurement. Then, the wavelength modulation-direct absorption (WM-DAS) method with no calibration and high signal-to-noise ratio is used to measure the absorbances of the six groups of transitions under different pressures. Voigt, Raution and quadratic speed-dependent Voigt profiles fit the measured absorbances by least squares method in order to obtain the spectroscopic parameters such as the collision broadening coefficient, line strength and Dicke narrowing coefficient. And the minimum standard deviation of residual error of absorbances is 7×10^–5. The measurement uncertainty of each line strength is less than 2%, and the uncertainty of collision broadening coefficients, Dicke narrowing coefficients and the speed-dependent coefficients are all less than 10%. This work is helpful in improving the H₂S spectral database and providing the spectral data basis for the high-precision measurement of H₂S concentration.

Keywords:

hydrogen sulfide /
wavelength modulation-direct absorption spectrum /
collisional broadening /
line strength

Authors and contacts

1.
State Key Laboratory of Power Systems, Department of Energy and Power Engineering, Tsinghua University, Beijing 100084, China
2.
School of Control and Computer Engineering, North China Electric Power University, Beijing 102206, China
3.
State Key Laboratory of Clean and Efficient Coal-fired Power Generation and Pollution Control, National Energy Group Science and Technology Research Institute Co. LTD, Nanjing 210046, China

Corresponding author: Peng Zhi-Min, apspect@tsinghua.edu.cn

Funds: Project supported by the National Key R&D Program of China (Grant No. 2019YFB2006002) and the National Natural Science Foundation of China (Grant No. 51906120).

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References

[1]	Zhang C, Wang X, Liu H, Liu C, Li S, Xue J, Zeng X 2020 Fuel 269 117233 Google Scholar
[2]	Li S, Huo F, Yin C 2022 Dyes. Pigm. 197 109825 Google Scholar
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[9]	Shao L, Fang B, Zheng F, Qiu X, He Q, Wei J, Li C, Zhao W 2019 Spectrochim. Acta, Part A 222 117118 Google Scholar
[10]	Wang Z, Tian C, Qian S, Yu Y, Chang J, Zhang Q, Feng Y, Li H, Feng Z 2022 Opt. Laser Technol. 145 107483 Google Scholar
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[23]	Galatry L 1961 Phys. Rev. 122 1218 Google Scholar
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[25]	Peng Z M, Du Y J, Ding Y J 2020 Sensors 20 616 Google Scholar
[26]	Du Y J, Peng Z M, Ding Y J 2018 Opt. Express 26 9263 Google Scholar
[27]	Reid J, Labrie D 1981 Appl. Phys. B: Lasers Opt. 26 203
[28]	Sur R, Spearrin R M, Peng W Y, Strand C L, Jeffries J B, Enns G M, Hanson R K 2016 J. Quant. Spectrosc. Radiat. Transfer 175 90 Google Scholar
[29]	Li J D, Ding Y J, Li Z, Peng Z M 2021 J. Quant. Spectrosc. Radiat. Transfer 276 107901 Google Scholar

Cited By

图 1 WM-DAS方法示意图, 测量信号为1 kHz的正弦波, 其中Etalon表示经过干涉仪的信号, FSR表示干涉仪的自由光谱区

Figure 1. Schematic diagram of WM-DAS method. The measured signal is a sine wave of 1 kHz. Etalon is the light signal through the interferometer, FSR is free spectral range.

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图 2 H₂S谱线参数测量实验装置示意图

Figure 2. Schematic diagram of experimental setup for measuring the spectroscopic parameters of H₂S.

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图 3 H₂S, CO₂, H₂O分子谱线线强度分布

Figure 3. The distribution of line strengths of H₂S, CO₂ and H₂O.

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图 4 H₂S在6320—6350 cm^–1光谱测量结果和基于HITRAN2020数据的仿真结果, α为吸收率, ν为波数

Figure 4. Measured absorption spectra of H₂S in the range of 6320—6350 cm^–1 and simulation results based on HITRAN2020. α is absorbance and ν is wave number.

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图 5 H₂S特征谱线吸收率测量结果和基于HITRAN2020数据库的仿真结果以及残差

Figure 5. Measured absorbance of H₂S transitions, simulation results based on HITRAN2020 database and the residuals.

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图 6 不同压力下ν₀ = 6344.000 cm^–1谱线的吸收率测量结果和qSDVP对吸收率拟合的结果以及由VP, RP和qSDVP拟合所得残差

Figure 6. Measured absorbance and the qSDVP best-fit results and the residuals for VP, RP and qSDVP of the transition centered at 6344.000 cm^–1 at different pressures.

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图 7 (a) ν₀ = 6344.000 cm^–1的谱线Δν_L和IA与压力的线性拟合结果, 分别由VP, RP和qSDVP得到; (b) ν_H与压力的线性拟合结果, 由RP得到; γ₂与压力的线性拟合结果, 由qSDVP得到

Figure 7. For the transition centered at 6344.000 cm^–1 : (a) The linear fitting results of Δν_L and IA with pressure, which were obtained by VP, RP and qSDVP respectively; (b) the linear fitting results of ν_H and pressure, for RP; the linear fitting results of γ₂ and pressure, for qSDVP.

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表 1 H₂S在6320—6350 cm^–1波段谱线的光谱常数测量结果

Table 1. Measured spectroscopic parameters of the H₂S transitions in the range of 6320—6350 cm^–1.

ν₀/cm^–1	φ	${\gamma _{ { {\text{H} }_{\text{2} } }{\text{S-air} } } }\left( { {T_0} } \right)$ /(10^–2 cm^–1·atm^–1)		${\beta _0}\left( {{T_0}} \right)$/ (10^–2 cm^–1·atm^–1)	${\gamma _2}\left( {{T_0}} \right)$/ (10^–3 cm^–1·atm^–1)	S (T₀) / (10^–3 cm^–2·atm^–1)
ν₀/cm^–1	φ	Meas.	Ref.	${\beta _0}\left( {{T_0}} \right)$/ (10^–2 cm^–1·atm^–1)	${\gamma _2}\left( {{T_0}} \right)$/ (10^–3 cm^–1·atm^–1)	Meas.	Ref.
6320.605	VP	8.99 ^c	8.81			2.57 ^a	2.63
	RP	9.18 ^b		2.80 ^c		2.65 ^a
	qSDVP	9.18 ^b			7.85 ^c	2.65 ^a
6328.883	VP	8.62 ^b	8.79			3.19 ^a	3.35
	RP	8.81 ^b		1.75 ^c		3.24 ^a
	qSDVP	8.83 ^b			5.89 ^c	3.26 ^a
6336.617	VP	7.87 ^b	8.26			4.26 ^a	3.49
	RP	8.08 ^b		1.05 ^c		4.31 ^a
	qSDVP	8.13 ^b			4.52 ^b	4.32 ^a
6340.432	VP	9.07 ^b	10.4			2.43 ^a	2.66
	RP	9.18 ^b		2.38 ^b		2.49 ^a
	qSDVP	9.16 ^b			7.00 ^b	2.49 ^a
6344.000	VP	7.79 ^b	6.96			4.22 ^a	3.27
	RP	8.00 ^a		2.18 ^a		4.33 ^a
	qSDVP	7.96 ^a			7.36 ^b	4.34 ^a
6347.749	VP	8.62 ^b	8.40			2.24 ^a	2.36
	RP	8.79 ^a		2.40 ^b		2.29 ^a
	qSDVP	8.75 ^a			7.80 ^c	2.30 ^a
注: ^a不确定度0—2%; ^b不确定度2%—5%; ^c不确定度5%—10%.

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[1]	Zhang C, Wang X, Liu H, Liu C, Li S, Xue J, Zeng X 2020 Fuel 269 117233 Google Scholar
[2]	Li S, Huo F, Yin C 2022 Dyes. Pigm. 197 109825 Google Scholar
[3]	Mohammed A, Devi P (Singh J, et al. ed) 2021 Hazardous Gases (Academic Press) pp209–223
[4]	Chen L, Li W, Zhao Y, Zhou Y, Zhang S, Meng L 2022 Bioresour. Technol. 345 126557 Google Scholar
[5]	Malone Rubright S L, Pearce L L, Peterson J 2017 Nitric Oxide 71 1 Google Scholar
[6]	GB/T 33443–2016 p12
[7]	Brown M D, Hall J R, Schoenfisch M H 2019 Anal. Chim. Acta 1045 67 Google Scholar
[8]	王振, 杜艳君, 丁艳军, 彭志敏 2020 物理学报 69 064205 Google Scholar Wang Z, Du Y J, Ding Y J, Peng Z M 2020 Acta Phys. Sin. 69 064205 Google Scholar
[9]	Shao L, Fang B, Zheng F, Qiu X, He Q, Wei J, Li C, Zhao W 2019 Spectrochim. Acta, Part A 222 117118 Google Scholar
[10]	Wang Z, Tian C, Qian S, Yu Y, Chang J, Zhang Q, Feng Y, Li H, Feng Z 2022 Opt. Laser Technol. 145 107483 Google Scholar
[11]	彭志敏, 贺拴玲, 周佩丽, 杜艳君, 王振, 丁艳军, 吴玉新, 吕俊复 2022 热力发电 51 145 Peng Z M, He S L, Zhou P L, Du Y J, Wang Z, Ding YJ, Wu YX, Lv J F 2022 Thermal Power Generat. 51 145
[12]	Lan L J, Ding Y J, Peng Z M, Du Y J, Liu Y F, Li Z 2014 Appl. Phys. B Lasers Opt. 117 543 Google Scholar
[13]	Azzam A a A A, Yurchenko S N, Tennyson J, Martin-Drumel M-A, Pirali O 2013 J. Quant. Spectrosc. Radiat. Transfer 130 341 Google Scholar
[14]	Gordon I E, Rothman L S, Hargreaves R J, et al. 2022 J. Quant. Spectrosc. Radiat. Transfer 277 107949 Google Scholar
[15]	Mouelhi M, Cuisset A, Hindle F, Jellali C, Galalou S, Aroui H, Bocquet R, Mouret G, Rohart F 2020 J. Quant. Spectrosc. Radiat. Transfer 247 106955 Google Scholar
[16]	Naumenko O V, Polovtseva E R 2019 J. Quant. Spectrosc. Radiat. Transfer 236 106604 Google Scholar
[17]	Ciaffoni L, Cummings B L, Denzer W, Peverall R, Procter S R, Ritchie G A D 2008 Appl. Phys. B:Lasers Opt. 92 627 Google Scholar
[18]	Yan T, Kochanov R V, Rothman L S, Gordon I E https:// zenodo.org/record/345381#.YmpMA4VBx3h [2022-4-25 ]
[19]	Dicke R H 1952 Phys. Rev. 89 472
[20]	Boone C D, Walker K A, Bernath P F 2007 J. Quant. Spectrosc. Radiat. Transfer 105 525 Google Scholar
[21]	Armstrong B H 1967 J. Quant. Spectrosc. Radiat. Transfer 7 61 Google Scholar
[22]	Li J D, Peng Z M, Ding Y J 2020 Opt. Lasers Eng. 126 105875 Google Scholar
[23]	Galatry L 1961 Phys. Rev. 122 1218 Google Scholar
[24]	Peng Z M, Du Y J, Ding Y J 2020 Sensors 20 681 Google Scholar
[25]	Peng Z M, Du Y J, Ding Y J 2020 Sensors 20 616 Google Scholar
[26]	Du Y J, Peng Z M, Ding Y J 2018 Opt. Express 26 9263 Google Scholar
[27]	Reid J, Labrie D 1981 Appl. Phys. B: Lasers Opt. 26 203
[28]	Sur R, Spearrin R M, Peng W Y, Strand C L, Jeffries J B, Enns G M, Hanson R K 2016 J. Quant. Spectrosc. Radiat. Transfer 175 90 Google Scholar
[29]	Li J D, Ding Y J, Li Z, Peng Z M 2021 J. Quant. Spectrosc. Radiat. Transfer 276 107901 Google Scholar

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High precision measurement of spectroscopic parameters of H₂S in 6320—6350 cm^–1 band

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Corresponding author: Peng Zhi-Min, apspect@tsinghua.edu.cn

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High precision measurement of spectroscopic parameters of H2S in 6320—6350 cm–1 band

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Corresponding author: Peng Zhi-Min, apspect@tsinghua.edu.cn

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High precision measurement of spectroscopic parameters of H₂S in 6320—6350 cm^–1 band