直射太阳光红外吸收光谱技术遥测大气中二氧化碳柱浓度

大气中二氧化碳浓度持续增高导致环境和气候变化等问题成为人们关注的焦点. 为了实时遥测二氧化碳气体柱浓度, 研究了一种地基低分辨遥测系统和实时光谱数据反演分析方法. 利用该系统在合肥地区进行了连续观测, 从太阳吸收光谱中实时获取了整层大气透过率. 采用逐线积分非线性最小二乘光谱反演算法, 从整层大气透过率中反演了二氧化碳柱浓度和氧气柱浓度, 并以氧气柱浓度为内标函数获得了二氧化碳干空气柱体积混合比, 精密度优于3%. 将2012年9月25日12时到15时本系统测量的二氧化碳干空气柱体积混合比均值与此时段过境本站点区域的日本温室气体卫星观测结果进行了比较, 两者偏差小于1%.可见, 该系统和方法具有很高的精密度和准确度, 是一种有效的温室气体观测手段. 关键词： 红外吸收光谱技术 遥测 二氧化碳 柱浓度     

可在线校准的大气CO_2浓度光声光谱监测系统研究

Fs光声光谱系统的谐振频率和池常数通常在实验室由标准气体标定得到,但在实际应用中,由于标准气体本身的不确定度以及与被测气体成分的不同、环境温湿度的变化,使得现场测量中谐振频率和池常数与实验室标定结果有偏差,从而导致测量结果不准确。为了解决以上问题,提出了基于大气中氧气的在线校准技术,并将该技术用于检测大气中二氧化碳浓度的光声光谱系统。大气中氧气浓度恒定为20.964%,通过探测氧气在763.73nm附近的扫频信号及峰值信号,实现共振频率和池常数的在线校准。该系统中光声池为直径6mm,长度100mm的一阶纵向共振模式结构。理论上分析了环境温湿度、气体成分对光声池性能的影响,同时给出了用标准气体、室内空气和室外空气标定的谐振频率和池常数,在标定结果的基础上,测量得到室内和室外的二氧化碳浓度值。实验结果显示,与校准过的气体分析仪的测量值相比,用被测大气中的氧气标定的谐振频率和池常数计算的二氧化碳浓度更准确,相对误差小于1%,远小于实验室标准气体标定计算的浓度相对误差。创新处在于,直接利用大气中的氧气对光声池的池常数和共振频率进行在线校准,有效的减小了标准气体标定带来的误差,以及环境变化带来系统漂移,提高光声系统在线监测的准确性和可靠性。     

小球藻溶液浓度与吸收系数的同时测量

为得到高准确度的小球藻浓度,利用空芯金属包覆波导作为测量腔对小球藻进行测量.利用自由空间耦合技术激发含有小球藻溶液的空芯金属包覆波导中超高阶导模,通过检测超高阶导模的衰减全反射吸收峰位置和反射极小值Rmin的变化,实现了小球藻溶液浓度和吸收系数的同时测量.该方法不仅可检测10-9 mol量级的小球藻浓度,而且具有测量成本低、操作方便等优点.     

利用电化学微分质谱在燃料电池的阴极研究碳载体的氧化

利用电化学微分质谱,在双薄层流动电解池中,通过检测二氧化碳产物的信号研究氧气与铂纳米粒子对碳载体氧化机理与动力学的影响．研究发现,碳载体可以在不同的电位区间内被氧化;氧气可以加速碳的氧化,在相同的电位下碳氧化生成二氧化碳产物的速率在氧气饱和溶液中是在氮气饱和溶液中的两倍;铂纳米粒子可以催化碳的氧化,在碳电极上,担载的铂纳米粒子可以大大降低碳氧化的过电势．讨论了铂与氧气促进碳氧化的机理．     

基于声谐振驱动的氢气流量检测系统设计与实现

氢气在空气中的爆炸极限浓度较低,当前电化学传感器氢气检测中容易受到电磁干扰引起爆炸,安全系数低;设计并实现了一种基于声谐振频率驱动的氢气流量检测系统设计方法,通过检测不同浓度的氢气通过传感器后引起的传感器谐振频率的变化反应氢气的浓度变化,系统基于S3C2410模块设计,设计了外围的信号调理电路,对芯片进行了Linux系统移植,安全性和准确性都有很大提高;最后进行仿真实验,实验工具包括传感器与探头,芯片搭建的硬件电路,USB数据采集卡;型号分别为1%,2.54%,3.05%,4.1%的经过国家标准检验的氢气,型号为0.513%的一氧化碳,型号为100%的二氧化碳与氧气;实验结果表明,系统能在10 s内对超浓度的氢气流量监控报警,误差在小于0.015,不同的交叉气体下系统的氢气流量检测准确度高达98%,具有很强的实用性。     

封装西林药瓶残留氧气检测中的谐波基线校正和去噪方法

可调谐激光二极管吸收光谱(TDLAS)技术的成熟和快速非接触气体浓度测量的优点,十分适合用于对封装西林药瓶内残留氧气进行浓度检测。采用TDLAS技术对封装西林药瓶内残留氧气进行浓度检测,检测系统的光路经过空气和玻璃药瓶,玻璃瓶壁对激光的散射和衰减是检测系统的主要干扰,给二次谐波信号的稳定性带来了很大影响。设计和搭建了基于TDLAS的封装西林药瓶残氧量检测系统。针对从系统中提取出的二次谐波信号,提出了一种基于小波变换的基线消除和噪声滤除方法, 解决在残留氧气浓度检测过程中基线漂移和噪声干扰问题,克服玻璃瓶壁对二次谐波信号的干扰,效果明显。选用“sym6”小波,将实验测得的信号进行五层小波分解,根据每一层小波分解得到的低频分量求出相应的基线斜率,对五个基线斜率进行加权平均得到原始信号的基线斜率。由求得的基线斜率,对原始信号经过去基线处理,再进行小波分解和软阈值处理后得到重构信号。对氧气浓度为21%的西林瓶的测量结果表明,处理后谐波信号和理论信号之间的相对误差由处理前的1.26%下降到了0.12%,证明了此方法可以很好地解决在残留氧气浓度检测过程中基线漂移和噪声干扰问题,克服玻璃瓶壁对二次谐波信号的干扰,为氧气浓度测量提供很高质量的信号。     

基于多模二极管激光吸收光谱的氧气浓度测量

可调谐二极管激光吸收光谱技术(TDLAS)具有高灵敏度、高选择性和快速响应等特点, 被广泛应用于环境监测、工业生产监控和生物医疗等众多领域。为克服传统TDLAS技术成本高以及长时间工作过程中由于中心波长偏移造成的稳定性差等问题, 提出了利用多模二极管激光关联光谱和谐波检测技术实现氧气浓度在线监测的研究。以Fabry-Perot(FP)激光器为光源, 通过对760 nm附近氧气分子的多条吸收谱线的探测, 实现了对氧气浓度的测量。输出光束被分光系统分成两路信号, 分别经过样品池和测量池, 双路接收采集含有气体浓度信息的光信号送后级处理, 通过测量信号和参考信号之间的相关性及比例关系对氧气浓度进行反演, 其中关联光谱技术和谐波检测技术被用于提高系统稳定性和信噪比。结果表明, 在1个大气压条件下, 系统的探测极限为280 ppm·m, 对同一样品在30 min内的30次连续测量的标准偏差为0.056%, 表明了系统良好的稳定性。该系统在软、硬件上的设计可以满足氧气的在线监测, 且系统稳定性高、装置简单、易用, 便于复杂环境应用。     

基于多模二极管激光吸收光谱的氧气浓度测量

可调谐二极管激光吸收光谱技术(TDLAS)具有高灵敏度、高选择性和快速响应等特点,被广泛应用于环境监测、工业生产监控和生物医疗等众多领域。为克服传统TDLAS技术成本高以及长时间工作过程中由于中心波长偏移造成的稳定性差等问题,提出了利用多模二极管激光关联光谱和谐波检测技术实现氧气浓度在线监测的研究。以Fabry-Perot(FP)激光器为光源,通过对760 nm附近氧气分子的多条吸收谱线的探测,实现了对氧气浓度的测量。输出光束被分光系统分成两路信号,分别经过样品池和测量池,双路接收采集含有气体浓度信息的光信号送后级处理,通过测量信号和参考信号之间的相关性及比例关系对氧气浓度进行反演,其中关联光谱技术和谐波检测技术被用于提高系统稳定性和信噪比。结果表明,在1个大气压条件下,系统的探测极限为280 ppm·m,对同一样品在30 min内的30次连续测量的标准偏差为0.056%,表明了系统良好的稳定性。该系统在软、硬件上的设计可以满足氧气的在线监测,且系统稳定性高、装置简单、易用,便于复杂环境应用。     

基于简单碰撞理论煤粉燃烧动力学模型的研究--PART Ⅱ:颗粒表面的氧气浓度分布模型

为了较准确地预报炉内煤粉燃烧速率,正确区分TGA中滞止煤粉表面与炉内载流煤粉表面氧气浓度的变化规律是非常关键的。从TGA中非稳态条件下坩埚内颗粒表面氧气浓度分布的数理解知,煤样的氧化过程是同时进行的,只是上部的氧化速率大一些,底部的氧化速率小一些;同一样品,同一升温速率,试样的堆积厚度的差异,会影响实验结果的重复性。分析表明,在初始和反应结束时,坩埚内颗粒表面氧气浓度等于环境浓度;反应速率达到最大值时,颗粒表面氧气浓度达到最小值。颗粒在炉内流动燃烧过程中,环境中氧气浓度值是单调减少的,煤焦表面氧的浓度是非线性变化的。     

中红外二氧化碳传感器的研制及在农业中的应用

利用二氧化碳气体分子在4.25μm处的基频吸收带,研制了一种差分式中红外二氧化碳检测系统.系统的光路部分由热辐射红外光源、双通道热释电探测器和球面反射镜构成,电路部分主要包括信号处理、光源驱动及主控模块.采用Tracepro软件对气室结构进行仿真和优化设计,使气体吸收光程达到30cm,改善了系统的性能.实验研究了系统对不同浓度二氧化碳气体样品的传感特性.实验结果表明,由拟合曲线得到的浓度与实际浓度误差较小,在0~5 000ppm范围内,测得二氧化碳浓度的标准差小于45ppm,而在500ppm以下,测量浓度的标准差小于5ppm;对浓度为0ppm的二氧化碳气体样品连续测量2h,测量结果的标准差约为2.8ppm;根据Allan方差分析得到系统的1σ检测下限为2.5ppm.在每个二氧化碳传感器上增加无线模块nRF24L01,构成传感器节点,在选定的日光温室大棚中构建了无线传感器网络,采集了温室大棚中的二氧化碳浓度信息,验证了所研制的传感器性能.     

Modeling the process of chemical regeneration of air in airtight habitable facilities

Physical experiments and mathematical modeling are used to study the kinetics of the reactions of carbon dioxide and water with potassium superoxide accompanied by oxygen release at various values of the temperature and humidity of the breathing gas mixture. The kinetics of the chemisorption is demonstrated to be limited by the rate of air regeneration in an airtight habitable facility. Experimental and analytical approaches are applied to determine the kinetic coefficients of the chemical reactions using the experimental data and a mathematical model of chemisorption kinetics. To perform the above chemical reactions, an original-design chemisorption reactor was developed, which contains plates with potassium superoxide nanocrystalline fixed on the fibers and pore surface of a fibrous polymer matrix. A mathematical model of chemical air regeneration is developed to calculate the guaranteed values of the parameters of the reactor and the protective effect time of the chemisorbent during which, at a given load, the reactor provides the appropriate concentrations of oxygen and carbon dioxide in the breathing gas mixture in an airtight habitable.     

方解石纳米孔隙内二氧化碳毛细凝聚的分子模拟

在二氧化碳地质封存、增产非常规油气以及孔隙材料表征测量方面,纳米孔隙中二氧化碳相态的准确预测具有重要意义.然而,由于纳米尺度下毛细力、分离压等作用力占据主导因素,流体在孔隙中的相行为与体相流体存在根本不同.已有实验和模拟表明,Kelvin毛细凝聚理论无法预测特征尺度10 nm下的,孔隙内流体凝聚压力与体相饱和蒸气压的偏...     

Structural and Parametric Optimization of S–CO2 Nuclear Power Plants

The transition to the use of supercritical carbon dioxide as a working fluid for power generation units will significantly reduce the equipment′s overall dimensions while increasing fuel efficiency and environmental safety. Structural and parametric optimization of S–CO₂ nuclear power plants was carried out to ensure the maximum efficiency of electricity production. Based on the results of mathematical modeling, it was found that the transition to a carbon dioxide working fluid for the nuclear power plant with the BREST–OD–300 reactor leads to an increase of efficiency from 39.8 to 43.1%. Nuclear power plant transition from the Rankine water cycle to the carbon dioxide Brayton cycle with recompression is reasonable at a working fluid temperature above 455 °C due to the carbon dioxide cycle′s more effective regeneration system.     

Simulation of front motion in a reacting condensed two phase mixture

The computational technique is developed in order to provide the scale capturing for numerical simulation of the thermal processes. The thermal front motion and gas flow dynamics as well as the rate of particle growth during the Carbon Combustion Synthesis of Oxides (CCSO) were predicted using the numerical simulation. In CCSO the exothermic oxidation of carbon nanoparticles generates a self-sustained thermal reaction front that propagates through the solid reactant mixture converting it to the desired complex oxides. The combusted carbon is emitted from the sample as carbon dioxide and its high rate of release increases the product porosity and friability. It was shown that the complicated finger front instability can be developed during the carbon combustion synthesis. This phenomenon results from a vortex gas flow in the reaction zone fed by the carbon dioxide co-flow and oxygen counter-flow filtration.     

Studies on the Decomposition of Carbon Dioxide in a Low-Temperature Plasma

The decomposition of carbon dioxide was studied in an argon plasma jet, generated by a direct-current arc discharge. The decomposition degree of carbon dioxide was up to 0,4 at an effective energy consumption lower than 1 MJ/mole CO. The efficiency of high-temperature decomposition of carbon dioxide to carbon monoxide and oxygen is essentially dependent both on the quenching intensity of the products, which prevents from the reverse oxidation reaction in the system, as well as on the proper conditions of plasma-substrate mixing.     

Evolution of disturbances in the shock layer on a flat plate in the flow of a mixture of vibrationally excited gases

The results of the numerical and experimental investigations of the evolution of the disturbances in a hypersonic shock layer on a flat plate streamlined by a flow of the mixture of vibrationally excited gases are presented. The experimental study was conducted in the hot-shot high-enthalpy wind tunnel IT-302 of the ITAM SB RAS. The numerical simulation was carried out with the aid of the ANSYS Fluent package using the solution of the unsteady two-dimensional Navier?Stokes equations with the incorporation of the user-created modules and enabling the consideration of the vibrational non-equilibrium of the carbon dioxide molecules within the framework of the model of the two-temperature aerodynamics. It was obtained that an increase in the carbon dioxide concentration in the mixture with air leads to a reduction of the intensity of pressure disturbances on the surface. The efficiency (up to 20 %) of the method of sound absorbing coatings in the vibrationally excited flows of the mixture of the carbon dioxide and air has been shown.     

Regeneration of the active aluminum oxide catalyst in supercritical carbon dioxide

The nature of the compounds inactivating the active aluminum oxide catalyst is studied. The results of the catalyst regeneration by pure supercritical carbon dioxide and by the supercritical carbon dioxide modified with a polar additive (2 wt % dimethyl sulfoxide) are presented.     

Modelling and simulation of countercurrent fractional extraction with supercritical solvents

Fractionating fluid mixtures by supercritical fluid extraction has received increasing attention within the last few years. In this paper, a simulation model of a countercurrent fractional extraction column operated with supercritical fluids is presented. The model is based on ideal separation stages and incorporates the equation of state due to Redlich-Kwong and Soave for describing phase equilibria.Simulation studies were performed on the separation of a binary feed using supercritical carbon dioxide as extraction solvent. The system is also used when treating a reaction mixture from an enzymatic conversion effected in supercritical carbon dioxide. To achieve a symmetric fractionation with equal purities in both top and bottom product flow of the column, the reflux ratio has to be set to a distinct ‘optimal’ value. All other column parameters remaining unchanged, the optimal reflux ratio increases as the solvent flow is increased. As a consequence, product purities also increase.     

Electrochemical promotion of Pt during the oxidation of ethanol

The reaction of ethanol oxidation has been examined over a Pt polycrystalline film deposited on an yttria stabilized zirconia (YSZ) electrochemical reactor. Experiments were carried out at 325 °C at atmospheric total pressure and under open and closed circuit conditions. It was found that the electrochemically-induced change in the catalytic rate of ethanol consumption is four orders of magnitude higher than the rate of ion transport through the solid electrolyte. The galvanostatic transient behavior of the consumption rates of ethanol and oxygen and of the formation rates of carbon dioxide and acetaldehyde have been also recorded. Paper presented at the 7th Euroconference on Ionics, Calcatoggio, Corsica, France, Oct. 1–7, 2000.