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混合气体测量中重叠吸收谱线交叉干扰的分离解析方法

王前进 孙鹏帅 张志荣 张乐文 杨曦 吴边 庞涛 夏滑 李启勇

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混合气体测量中重叠吸收谱线交叉干扰的分离解析方法

王前进, 孙鹏帅, 张志荣, 张乐文, 杨曦, 吴边, 庞涛, 夏滑, 李启勇

Separation and analysis method of overlapping absorption spectra with cross interference in gas mixture measurement

Wang Qian-Jin, Sun Peng-Shuai, Zhang Zhi-Rong, Zhang Le-Wen, Yang Xi, Wu Bian, Pang Tao, Xia Hua, Li Qi-Yong
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  • 在基于可调谐二极管激光吸收光谱技术(tunable diode laser absorption spectroscopy, TDLAS)进行多种组分混合气体测量时, 经常会遇到吸收谱线之间存在相互干扰的现象, 这也是使用该技术测量过程中的主要“瓶颈”. 比如在前期的应用中: 微量一氧化碳(CO)和甲烷气体(CH4)在同时检测时两者的吸收谱线存在严重的重叠干扰现象, 特别是在高浓度CH4存在的环境下, 微量CO气体吸收信号会被干扰甚至湮没, 无法实现有效解调, 这是通过谱线选取所不能解决的问题. 因此, 针对此问题本文提出了基于支持向量回归模型, 以CO和CH4吸收谱线的严重重叠干扰问题为例, 通过选择线性核函数建立CO支持向量回归模型和CH4支持向量回归模型, 可对CO和CH4的混合气体吸收谱线进行解调, 最终获得两种气体浓度的准确测量结果. 通过实验分别实现了四种不同浓度CH4环境下微量CO气体的检测, 得到的CO和CH4浓度(气体的体积分数)测量的绝对误差分别小于2 × 10–6和0.2 × 10–2; 通过不同浓度的固定配比实验分析, CO和CH4气体的测量值与实际值之间的相关系数分别达到了0.998和0.9995, 且CO和CH4气体测量结果的绝对误差分别不超过2 × 10–6和0.1 × 10–2, 完全满足了混合气体的精确测量, 为实现多场合混合气体目标的实时监测提出了解决方案.
    The interference between overlapping gas absorption lines often occurs in the measurement of multi-component gas mixture with using tunable diode laser absorption spectroscopy (TDLAS). This is also the main problem of the technology in some applications. For instance, in the early application of multi-component gas mixture measurement in coal mines, we found that the absorption lines of carbon monoxide (CO) and methane (CH4) seriously overlapped. The absorption signal of trace CO gas was annihilated and could not be effectively demodulated, especially in the presence of high concentration of CH4. This problem could not be solved just by accurately selecting the spectral lines due to the band absorption of CH4. Therefore, in this paper, we introduce the support vector regression (SVR) model to deal with the interference between CO and CH4 absorption lines. The spectral signals of 14 groups of mixed gases with different concentrations of CO and CH4 are used as the training sets, and the five-fold cross-validation is adopted to prevent the model from overfitting. After 15 iterations in 30 seconds, the optimal regression model of CO and CH4 can be obtained respectively. Furthermore, it is worth noting that based on the experimental data, the linear kernel function is selected to construct the two gas SVR models, and the parameters of the SVR models are optimized by the sequential minimal optimization(SMO) algorithm. With the assistance of the SVR models, the absorption spectra of the two gases can be demodulated effectively, and finally the accurate measurement results are obtained. The measurement results show that the absolute error of trace CO and CH4 concentration(volume fraction of gas) are less than 2 × 10–6 and 0.2 × 10–2 respectively. Meanwhile, the correlation coefficient between the measured values and the actual values of CO and CH4 are 0.998 and 0.9995, respectively. In addition, the dynamic stability for each of the two regression models is fully verified by the experiment of the inflation process. Consequently, this method can eliminate the interference between the overlapping spectra, and can fully meet the requirements for accurately measuring the gas mixture. We hope that the SVR model can provide an effective solution for the real-time monitoring of multi-component gas mixture, and thus greatly improving the adaptability of TDLAS technology in the future.
      通信作者: 张志荣, zhangzr@aiofm.ac.cn
    • 基金项目: 国家自然科学基金(批准号: 11874364, 41877311, 42005107)、国家重点研发计划(批准号: 2017YFC0805004)、安徽省重点研究与开发计划项目(批准号: 201904c03020005)和中国科学院合肥研究院“火花”基金项目(批准号: YZJJ2020QN8)资助的课题
      Corresponding author: Zhang Zhi-Rong, zhangzr@aiofm.ac.cn
    • Funds: Project supported by the National Natural Science Foundation of China (Grant Nos. 11874364, 41877311, 42005107), the National Key Research and Development Program of China (Grant No. 2017YFC0805004), the Key Research and Development Projects of Anhui Province, China (Grant No. 201904c03020005), and the "Spark" Fund Project of Hefei Institutes of Physics Science, Chinese Academy Sciences, China (Grant No. YZJJ2020QN8)
    [1]

    Zhang Z R, Pang T, Yang Y, Xia H, Cui X J, Sun P S, Wu B, Wang Y, Sigrist M W, Dong F Z 2016 Opt. Express 24 A943Google Scholar

    [2]

    Wang F P, Chang J, Wang Q, Wei W, Qin Z G 2017 Sens. Actuators A 259 152Google Scholar

    [3]

    Avetisov V, Bjoroey O, Wang J, Geiser P, Paulsen K G 2019 Sensors 19 5313Google Scholar

    [4]

    Nwaboh J A, Werhahn O, Ortwein P, Schiel D, Ebert V 2013 Meas. Sci. Technol. 24 015202Google Scholar

    [5]

    Vallon R, Soutade J, Verant J L, Meyers J, Paris S, Mohamed A 2010 Sensors 10 6081Google Scholar

    [6]

    夏滑, 吴边, 张志荣, 庞涛, 董凤忠, 王煜 2013 物理学报 62 214208Google Scholar

    Xia H, Wu B, Zhang Z R, Pang T, Dong F Z, Wang Y 2013 Acta Phys. Sin. 62 214208Google Scholar

    [7]

    Zhang L W, Zhang Z R, Sun P S, Pang T, Xia H, Cui X J, Guo Q, Sigrist M W, Shu C M, Shu Z F 2020 Spectrochim. Acta, Part A 239 118495Google Scholar

    [8]

    He Q X, Dang P P, Liu Z W, Zheng C T, Wang Y D 2017 Opt. Quantum Electron. 49 115Google Scholar

    [9]

    Kluczynski P, Gustafsson J, Lindberg A M, Axner O 2001 Spectrochim. Acta, Part B 56 1277Google Scholar

    [10]

    Wang F, Wu Q, Huang Q X, Zhang H D, Yan J H, Cen K F 2015 Opt. Commun. 346 53Google Scholar

    [11]

    Lin X, Yu X L, Li F, Zhang S H, Xin J G, Chang X Y 2013 Appl. Phys. B: Lasers Opt. 110 401Google Scholar

    [12]

    Köhring M, Huang S, Jahjah M, Jiang W, Ren W, Willer U, Caneba C, Yang L, Nagrath D, Schade W, Tittel F K 2014 Appl. Phys. B 117 445Google Scholar

    [13]

    Zhang T, Kang J, Meng D, Wang H, Mu Z, Zhou M, Zhang X, Chen C 2018 Sensors 18 4295Google Scholar

    [14]

    张志荣, 吴边, 夏滑, 庞涛, 王高旋, 孙鹏帅, 董凤忠, 王煜 2013 物理学报 62 234204Google Scholar

    Zhang Z R, Wu B, Xia H, Pang T, Wang G X, Sun P S, Dong F Z, Wang Y 2013 Acta Phys. Sin. 62 234204Google Scholar

    [15]

    Gabrysch M, Corsi C, Pavone F S, Inguscio M 1997 Appl. Phys. B 65 75Google Scholar

    [16]

    Cai T D, Gao G Z, Wang M R 2016 Opt. Express 24 859Google Scholar

    [17]

    Malegori C, Marques E J N, Freitas S T d, Pimentel M F, Pasquini C, Casiraghi E 2017 Talanta 165 112Google Scholar

    [18]

    张志荣, 夏滑, 董凤忠, 庞涛, 吴边 2013 光学精密工程 21 2771Google Scholar

    Zhang Z R, Xia H, Dong F Z, Pang T, Wu B 2013 Opt. Precis. Eng. 21 2771Google Scholar

    [19]

    Shao L G, Fang B, Zheng F, Qiu X B, He Q S, Wei J L, Li C L, Zhao W X 2019 Spectrochim. Acta, Part A 222 117118Google Scholar

    [20]

    Qu J, Chen H Y, Liu W Z, Zhang B, Li Z B 2015 Proceedings of the 2015 International Conference on Intelligent Systems Research and Mechatronics Engineering Zhengzhou, PRC, April 11−13, 2015 p2111

    [21]

    Laref R, Losson E, Sava A, Adjallah K, Siadat M 2018 2018 Ieee International Conference on Industrial Technology (Icit) Lyon, France, February 19−22, 2018 p1335

    [22]

    Reid J, Labrie D 1981 Appl. Phys. B 26 203

    [23]

    Smola A J, Scholkopf B 2004 Stat. Comput. 14 199Google Scholar

    [24]

    Gordon I E, Rothman L S, Hill C, et al. 2017 J. Quant. Spectrosc. Radiat. Transfer 203 3Google Scholar

  • 图 1  DFB激光器电流-波长调谐性能曲线

    Fig. 1.  Current-wavelength tuning curve of DFB laser.

    图 2  实验系统原理图

    Fig. 2.  Schematic diagram of the experimental system.

    图 3  CO (20 × 10–6, 400 × 10–6)和CH4 (1 × 10–2)的模拟吸收光谱图

    Fig. 3.  Simulated absorption spectra of CO (20 × 10–6, 400 × 10–6) and CH4 (1 × 10–2).

    图 4  三组气体(Group 1、Group 4、Group 10)的2f/1f信号

    Fig. 4.  2f/1f signals of three groups of gases (Group 1, Group 4, Group 10).

    图 5  CO和CH4浓度设置值和测试值对比 (a) CO浓度值; (b) CH4浓度值

    Fig. 5.  Comparisons between set and test values: (a) CO concentration; (b) CH4 concentration.

    图 6  设置值和测量值之间相关性及测量误差 (a) CO相关性; (b) CH4相关性; (c) CO测量误差; (d) CH4测量误差

    Fig. 6.  Correlation and test errors between set and average values: (a) CO correlation; (b) CH4 correlation; (c) CO errors; (d) CH4 errors.

    图 7  不同浓度CH4对CO测量结果的干扰

    Fig. 7.  Interference on CO measurement results by different concentrations of CH4.

    图 8  第一组充气过程中CO和CH4浓度变化

    Fig. 8.  Concentration measured of CO and CH4 during the first set of inflation.

    图 9  第二组充气过程中CO和CH4浓度变化

    Fig. 9.  Concentration measured of CO and CH4 during the second set of inflation.

    表 1  训练数据集

    Table 1.  Training data set.

    Group
    Standard gas
    category and
    concentration
    Ratio
    Gas category and
    concentration in
    multi-pass cell
    CO/10–6CH4/10–2CO/10–6CH4/10–2
    119.3019.30
    254.0054.00
    3102.00102.00
    400.5000.50
    501.0401.04
    602.0202.02
    705.0205.02
    854.01.041∶127.00.52
    9102.01.041∶151.00.52
    1019.31.041∶19.60.52
    1119.30.501∶19.60.25
    1219.35.021∶19.62.51
    1319.32.021∶19.61.01
    1419.38.501∶19.64.25
    下载: 导出CSV

    表 2  SVR模型主要参数

    Table 2.  Optimal parameters of SVR model.

    CO-SVRmodelCH4-SVRmodel
    BoxConstraint(C )0.34430.0180
    KernelScale0.06170.9205
    ε0.171065.1810
    Total function evaluations1515
    Total elapsed time in seconds26.254512.5730
    下载: 导出CSV
  • [1]

    Zhang Z R, Pang T, Yang Y, Xia H, Cui X J, Sun P S, Wu B, Wang Y, Sigrist M W, Dong F Z 2016 Opt. Express 24 A943Google Scholar

    [2]

    Wang F P, Chang J, Wang Q, Wei W, Qin Z G 2017 Sens. Actuators A 259 152Google Scholar

    [3]

    Avetisov V, Bjoroey O, Wang J, Geiser P, Paulsen K G 2019 Sensors 19 5313Google Scholar

    [4]

    Nwaboh J A, Werhahn O, Ortwein P, Schiel D, Ebert V 2013 Meas. Sci. Technol. 24 015202Google Scholar

    [5]

    Vallon R, Soutade J, Verant J L, Meyers J, Paris S, Mohamed A 2010 Sensors 10 6081Google Scholar

    [6]

    夏滑, 吴边, 张志荣, 庞涛, 董凤忠, 王煜 2013 物理学报 62 214208Google Scholar

    Xia H, Wu B, Zhang Z R, Pang T, Dong F Z, Wang Y 2013 Acta Phys. Sin. 62 214208Google Scholar

    [7]

    Zhang L W, Zhang Z R, Sun P S, Pang T, Xia H, Cui X J, Guo Q, Sigrist M W, Shu C M, Shu Z F 2020 Spectrochim. Acta, Part A 239 118495Google Scholar

    [8]

    He Q X, Dang P P, Liu Z W, Zheng C T, Wang Y D 2017 Opt. Quantum Electron. 49 115Google Scholar

    [9]

    Kluczynski P, Gustafsson J, Lindberg A M, Axner O 2001 Spectrochim. Acta, Part B 56 1277Google Scholar

    [10]

    Wang F, Wu Q, Huang Q X, Zhang H D, Yan J H, Cen K F 2015 Opt. Commun. 346 53Google Scholar

    [11]

    Lin X, Yu X L, Li F, Zhang S H, Xin J G, Chang X Y 2013 Appl. Phys. B: Lasers Opt. 110 401Google Scholar

    [12]

    Köhring M, Huang S, Jahjah M, Jiang W, Ren W, Willer U, Caneba C, Yang L, Nagrath D, Schade W, Tittel F K 2014 Appl. Phys. B 117 445Google Scholar

    [13]

    Zhang T, Kang J, Meng D, Wang H, Mu Z, Zhou M, Zhang X, Chen C 2018 Sensors 18 4295Google Scholar

    [14]

    张志荣, 吴边, 夏滑, 庞涛, 王高旋, 孙鹏帅, 董凤忠, 王煜 2013 物理学报 62 234204Google Scholar

    Zhang Z R, Wu B, Xia H, Pang T, Wang G X, Sun P S, Dong F Z, Wang Y 2013 Acta Phys. Sin. 62 234204Google Scholar

    [15]

    Gabrysch M, Corsi C, Pavone F S, Inguscio M 1997 Appl. Phys. B 65 75Google Scholar

    [16]

    Cai T D, Gao G Z, Wang M R 2016 Opt. Express 24 859Google Scholar

    [17]

    Malegori C, Marques E J N, Freitas S T d, Pimentel M F, Pasquini C, Casiraghi E 2017 Talanta 165 112Google Scholar

    [18]

    张志荣, 夏滑, 董凤忠, 庞涛, 吴边 2013 光学精密工程 21 2771Google Scholar

    Zhang Z R, Xia H, Dong F Z, Pang T, Wu B 2013 Opt. Precis. Eng. 21 2771Google Scholar

    [19]

    Shao L G, Fang B, Zheng F, Qiu X B, He Q S, Wei J L, Li C L, Zhao W X 2019 Spectrochim. Acta, Part A 222 117118Google Scholar

    [20]

    Qu J, Chen H Y, Liu W Z, Zhang B, Li Z B 2015 Proceedings of the 2015 International Conference on Intelligent Systems Research and Mechatronics Engineering Zhengzhou, PRC, April 11−13, 2015 p2111

    [21]

    Laref R, Losson E, Sava A, Adjallah K, Siadat M 2018 2018 Ieee International Conference on Industrial Technology (Icit) Lyon, France, February 19−22, 2018 p1335

    [22]

    Reid J, Labrie D 1981 Appl. Phys. B 26 203

    [23]

    Smola A J, Scholkopf B 2004 Stat. Comput. 14 199Google Scholar

    [24]

    Gordon I E, Rothman L S, Hill C, et al. 2017 J. Quant. Spectrosc. Radiat. Transfer 203 3Google Scholar

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出版历程
  • 收稿日期:  2021-02-07
  • 修回日期:  2021-03-11
  • 上网日期:  2021-07-16
  • 刊出日期:  2021-07-20

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