温室气体及其稳定同位素排放通量测量技术和方法研究
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摘要
大气中温室气体浓度的增加引起的全球变暖已经成为全世界面临的重要的环境问题。为了控制温室气体的排放,需要更好地理解自然界碳源与碳汇的分布规律,更好地理解生态系统主要温室气体排放的基本过程和变化规律,这就需要温室气体源排放与生态通量的主动测量技术。13C和D等环境稳定同位素在大气圈、水圈和生物圈中广泛存在,可以利用稳定同位素来研究温室气体的形成、转移和消耗等动态过程。因此对于生态通量监测,除了多种温室气体之外,还应该考虑这些稳定同位素的测量。
论文的研究是基于傅里叶变换红外光谱(FTIR)技术的多组分温室气体测量新方法,发展温室气体源排放与生态通量监测的分析方法和关键技术。研究工作基于开放光程傅里叶变换红外光谱的温室气体分析系统,研究了多种温室气体(CO2、水汽、CH4和N2O)以及CO2和水汽的稳定同位素的浓度实时反演方法；构建了温室气体排放通量反演模型,研究生态系统温室气体排放通量测量技术和稳定同位素通量的测量方法,并对温室气体及其稳定同位素排放通量测量的系统和方法进行了实验验证。
首先,以气体分子中红外光谱独特的吸收特征为基础,研究温室气体及其大气稳定同位素的测量方法。讨论了温室气体及其稳定同位素浓度反演时光谱波段的选择原则,并确定了反演各成分时选择的红外光谱波段。研究了开放光程FTIR系统测量参数的确定,包括在实验室环境和外场环境下进行的实验和测试,并给出了整个测量系统和方法测量环境大气的准确度和精度。
在此基础上,把开放光程FTIR系统和基于后向拉格朗日随机扩散(bLS)模式的逆扩散技术相结合,构建了温室气体排放通量反演模型。在模型构建的基础上,进行了实验仿真和高纯度样气释放的外场实验,研究了模式应用中的假设引起的排放计算误差,为复杂排放源的研究确定合理的传感器布局,并验证了测量系统和通量反演模型测量温室气体排放的可行性和准确性。
在约半个月的外场实验中,连续测量环境大气中温室气体以及CO2和水汽的稳定同位素,研究环境大气中CO2和水汽的同位素以及同位素比值δ13C和δD随时间的变化规律。采用Keeling图方法在不同的时间尺度上对CO2和水汽的稳定同位素时间序列进行分析,得到了地表蒸散的氘同位素特征。并对C02同位素12CO2和13CO2的地表排放通量进行了初步的计算,在研究生态系统同位素通量方法上做了新的尝试。外场实验的结果,验证了我们的温室气体及其稳定同位素测量技术和方法的可行性,证明了我们的测量系统长期、连续、无人值守测量环境大气和源排放的潜力。
Global warming due to the increase in the atmospheric greenhouse gases has become a serious environmental problem facing the world.In order to control the emissions of the greenhouse gases, we need to better understand the distributions of natural carbon sources and sinks, as well as the basic processes and variation of the emissions of the greenhouse gases in the ecosystem, so the active techniques for measuring the emissions of greenhouse gases from ecosystem sources are required. Such environmental stable isotopes as carbon thirteen and deuterium are widespread in the atmosphere, hydrosphere, and biosphere,and can be used to research the dynamic processes of the formation, transfer, and consumption of greenhouse gases. Therefore, in addition to multiple greenhouse gases, the stable isotopes should be considered for monitoring ecological emission.
The focus of the paper is development of key methods and techniques for monitoring emissions of greenhouse gases from ecosystem sources,based on new methods of Fourier transform infrared spectrometry(FTIR) for measurement of multi-component greenhouse gases.In our work,the real time methods of concentration retrieval for multiple greenhouse gases(carbon dioxide,water vapor, methane,nitrous oxide) and the stable isotopes of carbon dioxide and water vapor have been studied using an open-path FTIR system. Also,a model for retrieval of emissions of greenhouse gases are developed,and the methods for measurement of emissions of greenhouse gases and the isotopic flux are examined.Furthermore, experimental verification has been conducted for our measurement system and methods.
Firstly, the methods for detecting greenhouse gases and their stable isotopes have been deliberated, based on the unique absorption features of gas species in infrared spectral region. The criteria in selection of wavelength region for retrieval of greenhouse gases and stable isotopes are discussed, and the spectral windows for analysis of each gas component of interest are determined.As well, the measurement parameters of the open-path FTIR system are studied,including experiments and tests carried out in a laboratory environment and field environment.The measurement accuracy and precision of the whole system for detecting the ambient air are given.
On this basis, a model for retrieval of emissions of greenhouse gases are constructed, which combines an inverse dispersion technique based on a backward Lagrangian stochastic (bLS)model with an open-path FTIR system. Then, numerical simulations and a field experiment of release of high purity sample gas are conducted, in which emission-calculation errors caused by the assumption in application of the bLS model are discussed, and a reasonable sensor configuration for complex sources is identified. The experimental results show the feasibility and accuracy of the measurement system in conjunction with the model for measuring emissions of greenhouse gases.
Finally, greenhouse gases and stable isotopes of CO2and H2O in ambient air are continuously measured in a half-month field experiment, and the variation of stable isotopes of CO2and water vapor as well as the isotopic ratios δ13C and δD are investigated. The time series of stable isotopes of CO2and water vapor are analyzed on different time scales by Keeling plot methods, and the deuterium isotopic characteristics of evapotranspiration are determined. Moreover, the surface flux of12CO2and13CO2are calculated preliminarily, and this is a new attempt to measure isotopic flux in ecosystem. The results of the field experiment indicate the feasibility of our measurement techniques and methods for detecting greenhouse gases and stable isotopes.Also,the outcomes demonstrate the potential of our measuring system for long term, continuous, unattended measurement of ambient air and source emissions.
论文的研究是基于傅里叶变换红外光谱(FTIR)技术的多组分温室气体测量新方法,发展温室气体源排放与生态通量监测的分析方法和关键技术。研究工作基于开放光程傅里叶变换红外光谱的温室气体分析系统,研究了多种温室气体(CO2、水汽、CH4和N2O)以及CO2和水汽的稳定同位素的浓度实时反演方法；构建了温室气体排放通量反演模型,研究生态系统温室气体排放通量测量技术和稳定同位素通量的测量方法,并对温室气体及其稳定同位素排放通量测量的系统和方法进行了实验验证。
首先,以气体分子中红外光谱独特的吸收特征为基础,研究温室气体及其大气稳定同位素的测量方法。讨论了温室气体及其稳定同位素浓度反演时光谱波段的选择原则,并确定了反演各成分时选择的红外光谱波段。研究了开放光程FTIR系统测量参数的确定,包括在实验室环境和外场环境下进行的实验和测试,并给出了整个测量系统和方法测量环境大气的准确度和精度。
在此基础上,把开放光程FTIR系统和基于后向拉格朗日随机扩散(bLS)模式的逆扩散技术相结合,构建了温室气体排放通量反演模型。在模型构建的基础上,进行了实验仿真和高纯度样气释放的外场实验,研究了模式应用中的假设引起的排放计算误差,为复杂排放源的研究确定合理的传感器布局,并验证了测量系统和通量反演模型测量温室气体排放的可行性和准确性。
在约半个月的外场实验中,连续测量环境大气中温室气体以及CO2和水汽的稳定同位素,研究环境大气中CO2和水汽的同位素以及同位素比值δ13C和δD随时间的变化规律。采用Keeling图方法在不同的时间尺度上对CO2和水汽的稳定同位素时间序列进行分析,得到了地表蒸散的氘同位素特征。并对C02同位素12CO2和13CO2的地表排放通量进行了初步的计算,在研究生态系统同位素通量方法上做了新的尝试。外场实验的结果,验证了我们的温室气体及其稳定同位素测量技术和方法的可行性,证明了我们的测量系统长期、连续、无人值守测量环境大气和源排放的潜力。
Global warming due to the increase in the atmospheric greenhouse gases has become a serious environmental problem facing the world.In order to control the emissions of the greenhouse gases, we need to better understand the distributions of natural carbon sources and sinks, as well as the basic processes and variation of the emissions of the greenhouse gases in the ecosystem, so the active techniques for measuring the emissions of greenhouse gases from ecosystem sources are required. Such environmental stable isotopes as carbon thirteen and deuterium are widespread in the atmosphere, hydrosphere, and biosphere,and can be used to research the dynamic processes of the formation, transfer, and consumption of greenhouse gases. Therefore, in addition to multiple greenhouse gases, the stable isotopes should be considered for monitoring ecological emission.
The focus of the paper is development of key methods and techniques for monitoring emissions of greenhouse gases from ecosystem sources,based on new methods of Fourier transform infrared spectrometry(FTIR) for measurement of multi-component greenhouse gases.In our work,the real time methods of concentration retrieval for multiple greenhouse gases(carbon dioxide,water vapor, methane,nitrous oxide) and the stable isotopes of carbon dioxide and water vapor have been studied using an open-path FTIR system. Also,a model for retrieval of emissions of greenhouse gases are developed,and the methods for measurement of emissions of greenhouse gases and the isotopic flux are examined.Furthermore, experimental verification has been conducted for our measurement system and methods.
Firstly, the methods for detecting greenhouse gases and their stable isotopes have been deliberated, based on the unique absorption features of gas species in infrared spectral region. The criteria in selection of wavelength region for retrieval of greenhouse gases and stable isotopes are discussed, and the spectral windows for analysis of each gas component of interest are determined.As well, the measurement parameters of the open-path FTIR system are studied,including experiments and tests carried out in a laboratory environment and field environment.The measurement accuracy and precision of the whole system for detecting the ambient air are given.
On this basis, a model for retrieval of emissions of greenhouse gases are constructed, which combines an inverse dispersion technique based on a backward Lagrangian stochastic (bLS)model with an open-path FTIR system. Then, numerical simulations and a field experiment of release of high purity sample gas are conducted, in which emission-calculation errors caused by the assumption in application of the bLS model are discussed, and a reasonable sensor configuration for complex sources is identified. The experimental results show the feasibility and accuracy of the measurement system in conjunction with the model for measuring emissions of greenhouse gases.
Finally, greenhouse gases and stable isotopes of CO2and H2O in ambient air are continuously measured in a half-month field experiment, and the variation of stable isotopes of CO2and water vapor as well as the isotopic ratios δ13C and δD are investigated. The time series of stable isotopes of CO2and water vapor are analyzed on different time scales by Keeling plot methods, and the deuterium isotopic characteristics of evapotranspiration are determined. Moreover, the surface flux of12CO2and13CO2are calculated preliminarily, and this is a new attempt to measure isotopic flux in ecosystem. The results of the field experiment indicate the feasibility of our measurement techniques and methods for detecting greenhouse gases and stable isotopes.Also,the outcomes demonstrate the potential of our measuring system for long term, continuous, unattended measurement of ambient air and source emissions.
引文
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