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β—蒎烯与臭氧的大气化学行为的初步实验室模拟研究 总被引:9,自引:1,他引:8
使用长光程傅里叶变换红外光谱系统对β-蒎烯与臭氧的大气化学行为进行初步的实验室模拟研究,测定了β-蒎烯及其与臭氧氧化反应的主要产物不蒎酮的气态红外谱图, 特征峰的红外吸光系数。 相似文献
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在(298±3)K的温度下,采用相对速率法测得了3-甲基丁酮与OH自由基在气相中的反应速率常数:k=(2·6±0·4)×10~(-12)cm~3·molecule~(-1)·s~(-1).该结果与根据结构活性法估算的结果相一致.实验中还测定了该反应的主要产物:丙酮、甲醛和过氧乙酰基硝酸酯(PAN),讨论了该气体在NOx存在下与OH自由基反应的机理.根据上述实验结果讨论了3-甲基丁酮对对流层臭氧浓度的影响:3-甲基丁酮在大气对流层中的氧化反应活性不高,它的主要氧化产物丙酮同样具有低的反应活性.因此,3-甲基丁酮对大气中臭氧生成的贡献不是很大. 相似文献
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大气CO2体积分数升高环境温度与土壤水分对农田土壤呼吸的影响 总被引:2,自引:0,他引:2
植物-土壤生态系统土壤呼吸与温度、水分环境因子的关系对评价目前大气CO2浓度持续升高背景下陆地生态系统土壤碳库的变化趋势具有重要意义.依托FACE(free air carbon dioxide enrichment)技术平台,利用阻断根法,采用LI-6400红外气体分析仪(IRGA)-田间原位测定的方法,研究了大气CO2体积分数升高对稻(Oryza sativa L.)/麦(Triticum aestivum L.)轮作制中麦田的土壤呼吸、基础土壤呼吸和呼吸主要影响因子,分析了大气CO2体积分数升高后温度与水分对土壤呼吸的影响.结果表明,在整个测定期间,土壤呼吸与基础土壤呼吸速率呈明显的季节变化,与气温和土壤温度季节变化趋势基本一致,呼吸速率与温度具有显著的相关性,是影响土壤呼吸的控制性因素;呼吸速率与土壤含水量无显著的相关性,土壤水分是研究区麦田土壤CO2排放的非限制性因素,且温度与土壤含水量间的交互效应对土壤呼吸的影响不显著.基础土壤呼吸比作物下的土壤呼吸更易受温度影响,土壤温度比气温能更好地解释土壤CO2排放的季节性变化.而CO2体积分数增加降低了温度与呼吸速率间的相关系数和Q10,表明温度对土壤CO2排放的影响程度下降.但高CO2体积分数环境中植物-土壤生态系统的土壤呼吸对温度增加敏感性的降低,有利于减缓土壤碳分解损失的速度.结果有助于评价未来高CO2体积分数气候变暖背景下植物-土壤系统下的农田生态系统土壤碳的固定潜力. 相似文献
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北京低山区森林土壤中CH4排放通量的研究 总被引:5,自引:0,他引:5
CH4是大气中一种重要的温室气体,与土壤圈有着频繁的交换过程。用静态箱式技术原位测定了北京西山低山区油松人工林地土壤中CH4的排放通量,结果显示北京西山森林土壤为大气CH4重要的汇。年平均吸收值为20.47 g(m-2(h-1,变动范围0~44.8 g(m-2(h-1。 吸收值有一定的季节变化规律, 冬季的吸收值最小,几乎为0,春秋季较高,夏季最高。影响吸收的外界环境因素主要有地表下5 cm处的土壤温度。原状土壤氧化CH4的模拟实验表明吸收过程为纯生物化学过程,吸收作用主要发生在0~5 cm的矿质土层,而枯落物层和20 cm以下的层次基本无吸收反应。CH4的氧化速率在开始的12 h内可用一级反应动力学方程 C =C 0e-kt很好地模拟 。 相似文献
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《环境化学》2015,(9)
采用环境烟雾箱模拟实验,在近大气条件下研究了α-蒎烯气相臭氧氧化反应.通过气体与气溶胶膜采样进样口FIGAERO(Filter Inlet for Gas and AEROsols)与高分辨率飞行时间化学电离质谱(HRTo F-CIMS)联用对颗粒相产物进行了鉴别,鉴别结果表明,颗粒相产物中浓度最高的是蒎酮醛,其它主要产物包括蒎酮酸、蒎醛酸、降蒎酮酸、降蒎醛酸和蒎酸.采用扫描电迁移率粒径谱仪(SMPS)、气溶胶质量分析仪(APM)与云凝结核计数器(CCNC)联用考察了臭氧氧化反应生成的二次有机气溶胶(SOA)的粒径谱分布、密度、产率以及云凝结核活性发现,随着臭氧氧化反应的进行,SOA的密度、质量浓度以及云凝结核活性均呈上升趋势.同时研究了重要的大气物种SO2对α-蒎烯臭氧氧化反应的影响,实验结果表明,SO2能大大促进气溶胶成核,气溶胶数浓度、质量浓度和产率均提高,同时云凝结核活性也显著增强,其可能的机制是反应中稳定化的Criegee中间体与SO2反应生成硫酸. 相似文献
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James Franklin 《毒物与环境化学》2013,95(3):169-182
The present paper reviews the existing literature on the atmospheric degradation and impact of perchloro‐ethylene (PER). Topics covered are: assessment of the relative importance of primary reactions of PER with OH, Cl, O3 and other reactive species; other tropospheric sinks for PER; estimated tropospheric lifetime, observed concentrations and atmospheric budget calculations; breakdown mechanisms leading to the formation of phosgene, and possibly trichloroacetyl chloride and carbon tetrachloride; contribution of PER to atmospheric chlorine loading; impact of PER on tropospheric ozone formation; uptake and hydrolysis of degradation products by clouds, rainwater and the oceans; contribution of PER to chloride and acidity in rainwater; potential contribution of PER to trichloroacetic acid in the hydrosphere, soil and the biosphere. 相似文献
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天然草地利用方式改变对土壤排放CO2 和吸收CH4的影响 总被引:1,自引:0,他引:1
1997年~ 1998年在内蒙古达拉特旗中国农业科学院草原研究所草原生态试验站对天然草地、天然草地转变为人工草地、玉米和土豆地后 ,土壤 CO2 排放和 CH4 吸收通量进行了测定。天然草地、人工草地和旱地农田均为大气中甲烷的吸收汇 ,天然草地转变为农田后 ,增强了土壤的 CO2 排放量 ,减少了土壤对大气中甲烷的吸收。天然草地和玉米地的 CO2 排放通量与 5cm处土壤温度呈线性相关 ,土壤对甲烷的吸收率与土壤含水量呈线性负相关 ,与土壤温度没有相关关系 相似文献
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Several reaction schemes, based on the conserved scalar theory, are implemented within a stochastic Lagrangian micromixing model to simulate the dispersion of reactive scalars in turbulent flows. In particular, the formulation of the reaction-dominated limit (RDL) reaction scheme is here extended to improve the model performance under non-homogeneous conditions (NHRDL scheme). The validation of the stochastic model is obtained by comparison with the available measurements of reactive pollutant concentrations in a grid-generated turbulent flow. This test case describes the dispersion of two atmospheric reactant species (NO and O3) and their reaction product (NO2) in an unbounded turbulent flow. Model inter-comparisons are also assessed, by considering the results of state-of-the-art models for pollutant dispersion. The present validation shows that RDL reaction scheme provides a systematic overestimation (relative error of ca. 85% around the centreline) in computing the local reactant consumption/production rate, whereas the NHRDL scheme drastically reduces this gap (relative error lower than 5% around the centreline). In terms of NO2 production (or reactant consumption), neglecting concentration fluctuations determines overestimations of the product mean of around 100% and a NO2 local production of one order of magnitude higher than the reference simulation. In terms of standard deviations, the concentration fluctuations of both the passive and reactive scalars are generally of the same order of magnitude or up to 1 or 2 orders of magnitudes higher than the corresponding ensemble mean values, except for the background reactant close to the plume edges. The study highlights the importance of modelling pollutant reactions depending on the instantaneous instead of the mean concentrations of the reactants, thus quantifying the role of the turbulent fluctuations of concentration, in terms of scalar statistics (mean, standard deviation, intensity of fluctuations, skewness and kurtosis of concentration, segregation coefficient, simulated reaction rate). This stochastic particle method represents an efficient numerical technique to solve the convection–diffusion equation for reactive scalars and involves several application fields: micro-scale air quality (urban and street-canyon scales), accidental releases, impact of odours, water quality and fluid flow industrial processes (e.g. combustion). 相似文献
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大气CO2体积分数升高对植物N素吸收的影响 总被引:3,自引:0,他引:3
从影响植物N素吸收的因素来看,大气CO2体积分数升高条件下植物净光合作用增强,碳同化产物增多,利于改善N素吸收的能量和物质基础:植物根系生长增强,生物量增多且空间分布加大,有利于N素吸收;但土壤有效N供应能力的变化存在增强和减弱两种观点。从植物N素吸收的实际情况来看,大气CO2体积分数升高条件下植物N吸收总量并末增加,植物体内N质量分数普遍降低,某些种类植物N吸收形态也发生了改变。因此要阐明大气CO2体积分数升高对植物N素吸收的影响机制,必须探明土壤有效N供应能力的变化:CO2体积分数升高条件下N矿化作用是否增强,微生物和植物间是否存在对有效N的竞争,此外,CO2体积分数升高条件下植物根系形态特征变化和N素吸收(包括主动和被动吸收)的生理机制及其与环境因素的关系也值得进一步研究。 相似文献
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作物地上部氨排放及对大气氮沉降的吸收 总被引:1,自引:0,他引:1
为研究作物地上部分氨排放以及对大气氮沉淀的吸收情况,以水稻(Oryza saliva L.)品种武运粳7号和小麦(Triticumaestivum L.)品种扬麦15为例.在盆栽条件下,利用~15N同位素示踪技术,采用探索性的研究方法,初步分析了水稻成熟期植株NH_3排放和小麦植株直接吸收的大气沉降氮.结果表明,土培的水稻品种武运粳7号地上部植株成熟期排放氨氮(NH_3-N)量约占当季总施氮(N)量的(0.50±0.21)%;收获后水稻植株不同部位~(15)N丰度值以根部最高,茎叶次之,籽粒最低,这与植株体内养分的运移顺序变化一致;贫化~(15)N小麦砂培试验测定的包括植株直接吸收在内的大气氮沉降数量为N(14.8±4.3)kg·hm~(-2),低于国外类似方法以其它作物作为研究对象的测定结果. 相似文献
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为了研究稻田生态系统中土壤钙、镁元素生物地球化学循环对大气CO2浓度升高的响应。利用中国稻/麦轮作FACE(Free Air Carbon-dioxide Enrichment)试验平台,研究大气CO2浓度升高(比周围大气高200μmol mol-1)对2007年稻季各生育期不同深度土壤溶液ρ(Ca)、ρ(Mg)的影响。结果表明,大气CO2浓度升高降低了5 cm处土壤溶液ρ(Ca)、ρ(Mg),有增加稻季30、60和90 cm处土壤溶液ρ(Ca)的趋势,其增幅分别为18.3%、12.4%和15.3%;大气CO2浓度升高会增加稻季Ca淋溶损失风险;稻季不同深度土壤溶液ρ(Ca)、ρ(Mg)对大气CO2浓度升高的响应有所不同。稻田生态系统不同深度土壤Ca、Mg循环对大气CO2浓度升高的响应值得深入研究。 相似文献
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This study delineated the mathematical forms for the reactions involved in the mass balance of As in cropland soils. Even
mathematically simplified, many model parameters are required to define the reactive processes involved. Example simulations
were conducted based on the range of parameter values and initial conditions derived from published literature. The outcomes
showed that the As inputs due to fertilizers and irrigation water caused total As content of the root zone to gradually increase
over time. The plant uptake and leaching were equally important as pathways for removal of the added As. In turn, the dissolution
kinetics of the mineral phase and the distribution coefficient of the adsorbed phase affected the availability of the As for
plant uptake and leaching. Parameters based on laboratory-derived data on the dissolution of As mineral phase, mineralization
and oxidation of As(III), and the As plant uptake however appeared to overestimate the As transformations in soils. While
the development of mathematical model was a straightforward process, its application to realistic situations was hindered
by difficulties of defining model parameter values with confidence. Current knowledge on the processes and reactions of As
transformation in the soil–plant system is inadequate to calibrate or validate the model. Studies are needed to understand
the kinetics of soil As mineral dissolution and precipitation and the dynamics of root growth and As uptake by plant in soils. 相似文献
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In large-eddy simulations of atmospheric boundary layer turbulence, the lumped coefficient in the eddy-diffusion subgrid-scale
(SGS) model is known to depend on scale for the case of inert scalars. This scale dependence is predominant near the surface.
In this paper, a scale-dependent dynamic SGS model for the turbulent transport of reacting scalars is implemented in large-eddy
simulations of a neutral boundary layer. Since the model coefficient is computed dynamically from the dynamics of the resolved
scales, the simulations are free from any parameter tuning. A set of chemical cases representative of various turbulent reacting
flow regimes is examined. The reactants are involved in a first-order reaction and are injected in the atmospheric boundary
layer with a constant and uniform surface flux. Emphasis is placed on studying the combined effects of resolution and chemical
regime on the performance of the SGS model. Simulations with the scale-dependent dynamic model yield the expected trends of
the coefficients as function of resolution, position in the flow and chemical regime, leading to resolution-independent turbulent
reactant fluxes. 相似文献