差分吸收光谱技术在环境监测中的理论和应用研究
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摘要
环境监测伴随着全球环境问题的日益突出和环境保护事业的兴起而逐步发展成为一项独立的、多学科相互渗透的综合性科学事业。保护环境实现可持续发展成为新世纪经济发展的主题。大气中痕量气体和污染源排气的监测技术及仪器开发是环境治理的重要前提。本文根据光谱法测量大气中痕量气体的原理和技术,论述了差分光学吸收光谱技术(DOAS)在环境空气质量自动监测系统(AQMS)和烟气污染源排放自动监测系统中(CEMS)的理论与应用。
本文主要完成的创造性工作有以下几个方面:
1.差分光学吸收光谱法的关键技术之一是“宽带吸收”和“窄带吸收”的分离,本文在DOAS光谱差分分离技术中,首次采用了Savitzky -Golay数字滤波技术,与多项式分离技术相比,Savitzky -Golay方法不仅提高了气体浓度反演的准确度,而且将运算时间缩短了约8%,对实时监测很有利。
2.提出了一种新的浓度反演算法——差分吸收面积拟合法。由DOAS理论的基本公式推导出:测量的差分吸收光谱和参考差分吸收截面光谱所包含的面积具有线性关系。直接用差分吸收面积拟合法代替最小二乘方法,从而避免了光谱不同分辨率,光谱漂移、拉伸或压缩等因素对测量结果造成的误差,同时具有计算量小,处理速度快等特点。
3.原理性研究影响烟气CEMS测量结果的两个主要问题-温度对吸收截面的影响和Lambert-Beer定律非线性偏离,设计了一套有效的测量气体吸收截面的实验系统,并在实验研究的基础上,提出了可应用到实际系统中的经验公式。
4.从光学、机械、电子学和软件等方面的设计入手,完成了AQMS和CEMS两套监测系统的设计并投入生产。最后对研制的系统进行了现场测量和长时间的对比实验,给出仪器准确性、重复性、线性度的评价。
Environmental monitoring is developing an independent comprehensive discipline, with the development of industry, making the environmental pollution more and more serious, bringing great hazard to human beings’living circumstance. Nowadays environmental protection for realization of sustainable development has become the key point of current economic development, and thus technology and instrument exploitation of monitoring system for detecting trace gases in the air and pollutant source is an important prerequisite for bettering our environment. Based on the principle of trace gas monitoring with UV spectroscopy, the theory and application of Differential Optical Absorption Spectroscopy (short as DOAS) in Air Quality Monitoring System (short as AQMS) and Continuous Emission Monitoring System (short as CEMS) are presented.
The main content of my thesis is listed as follows.
Firstly, the one of key technology of DOAS is the divide of“narrow absorption”and“broad absorption”. Instead of polynomial approximation, Savitzky–Golay digital filter technique was applied for the first in DOAS filtering process. Experiments showed that by using the digital filter, retrieval accuracy was improved and the operation time was reduced by almost 8 percent, which was prefered to real-time monitoring.
Secondly, a novel calculation method- Differential Area Fitting Method (DAFM) was put forward for the first time to improve the accuracy of retrieval. According to the basic theory of DOAS, a linear relation between differential absorption cross-section and differential absorption spectrum is deduced. For using the area of absorption peak instead of points of spectrum to calculate the gas concentration, the effects of resolution factor, spectrum drift, stretch and compression are avoided. It needs less computation time.
Thirdly, the factors about absorption spectrum of the gases been measured, which affect on the measurement precision of DOAS, was studied deeply. The experimental equation of temperature was given to correct the effects of temperature on absorption cross-section. An easy operation measurement system was designed which can measure absorption cross-section of trace gases under different temperature. Based on the experimental system, the parameters of temperature compensation function were determined.
Finally, AQMS and CEMS based on optics, mechanics, electronics and software were performed under the air and flue gas condition. Especially, the multi-channel optical spectromecter with photodiode array (PDA) as the detector was used in this system. The accuracy, reproducibility and linearity of instruments were evaluated by comparison experiment.
本文主要完成的创造性工作有以下几个方面:
1.差分光学吸收光谱法的关键技术之一是“宽带吸收”和“窄带吸收”的分离,本文在DOAS光谱差分分离技术中,首次采用了Savitzky -Golay数字滤波技术,与多项式分离技术相比,Savitzky -Golay方法不仅提高了气体浓度反演的准确度,而且将运算时间缩短了约8%,对实时监测很有利。
2.提出了一种新的浓度反演算法——差分吸收面积拟合法。由DOAS理论的基本公式推导出:测量的差分吸收光谱和参考差分吸收截面光谱所包含的面积具有线性关系。直接用差分吸收面积拟合法代替最小二乘方法,从而避免了光谱不同分辨率,光谱漂移、拉伸或压缩等因素对测量结果造成的误差,同时具有计算量小,处理速度快等特点。
3.原理性研究影响烟气CEMS测量结果的两个主要问题-温度对吸收截面的影响和Lambert-Beer定律非线性偏离,设计了一套有效的测量气体吸收截面的实验系统,并在实验研究的基础上,提出了可应用到实际系统中的经验公式。
4.从光学、机械、电子学和软件等方面的设计入手,完成了AQMS和CEMS两套监测系统的设计并投入生产。最后对研制的系统进行了现场测量和长时间的对比实验,给出仪器准确性、重复性、线性度的评价。
Environmental monitoring is developing an independent comprehensive discipline, with the development of industry, making the environmental pollution more and more serious, bringing great hazard to human beings’living circumstance. Nowadays environmental protection for realization of sustainable development has become the key point of current economic development, and thus technology and instrument exploitation of monitoring system for detecting trace gases in the air and pollutant source is an important prerequisite for bettering our environment. Based on the principle of trace gas monitoring with UV spectroscopy, the theory and application of Differential Optical Absorption Spectroscopy (short as DOAS) in Air Quality Monitoring System (short as AQMS) and Continuous Emission Monitoring System (short as CEMS) are presented.
The main content of my thesis is listed as follows.
Firstly, the one of key technology of DOAS is the divide of“narrow absorption”and“broad absorption”. Instead of polynomial approximation, Savitzky–Golay digital filter technique was applied for the first in DOAS filtering process. Experiments showed that by using the digital filter, retrieval accuracy was improved and the operation time was reduced by almost 8 percent, which was prefered to real-time monitoring.
Secondly, a novel calculation method- Differential Area Fitting Method (DAFM) was put forward for the first time to improve the accuracy of retrieval. According to the basic theory of DOAS, a linear relation between differential absorption cross-section and differential absorption spectrum is deduced. For using the area of absorption peak instead of points of spectrum to calculate the gas concentration, the effects of resolution factor, spectrum drift, stretch and compression are avoided. It needs less computation time.
Thirdly, the factors about absorption spectrum of the gases been measured, which affect on the measurement precision of DOAS, was studied deeply. The experimental equation of temperature was given to correct the effects of temperature on absorption cross-section. An easy operation measurement system was designed which can measure absorption cross-section of trace gases under different temperature. Based on the experimental system, the parameters of temperature compensation function were determined.
Finally, AQMS and CEMS based on optics, mechanics, electronics and software were performed under the air and flue gas condition. Especially, the multi-channel optical spectromecter with photodiode array (PDA) as the detector was used in this system. The accuracy, reproducibility and linearity of instruments were evaluated by comparison experiment.
引文
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