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1.
An O3 episode observed at Dorset, a rural site in central Ontario, during a stagnant high pressure period of the intensive Eulerian Model Evaluation Field Study (EMEFS), in the summer of 1988, is simulated using a photochemical box model with a two-layer treatment. In the model analysis, natural hydrocarbon chemistry is simulated based on an isoprene-only scenario. Sensitivity tests indicate that local isoprene emissions are an important contributor to local O3 production, relative to anthropogenic hydrocarbons (AHCs), during the event.The model calculated isoprene contribution to the local O3 production, defined as the ratio of the O3 amount formed in the absence of AHCs to that in the presence of AHCs, is characterized by a strong NOx dependence. A minimum value (∼50%) of the contribution was found at a NOx level of ∼ 6 ppbv for the representative hydrocarbon composition during the episode. At this NOx level, O3 production was strongly influenced by the presence of AHCs. At significantly higher or lower NOx levels, isoprene is more important than AHCs in the local O3 production.  相似文献   

2.
Results of modelled and observed deposition velocities (Vd) for O3, SO2 and NO2 for time-averaged diurnal cycles and sometimes for a collection of hourly values taken from different days are discussed for different seasons. From the observations, it was found that the O3Vd values over a deciduous forest had a daytime representative value of 1.0 cm s−1 in the summer and 0.3 cm s−1 in the winter. For SO2 over the same forest and over a carrot field the daytime values ranged from 0.0 to 0.65 cm s−1 in the autumn, and for SO2 over a snow surface the Vd ranged from 0.0 to 0.15 cm s−1. The NO2Vd was mostly negative over the forest and the carrot field in the autumn and had a range of 0.0-0.15 cm s−1 over snow. From the model, it was found that for the three seasons the Vd values over all the land-use types were much larger than the observations. The model could not simulate the observed negative values of the NO2Vd. The impact of the Vd model and its modified version on the concentrations of O3 and SO2 were tested with a comprehensive Eulerian air quality model.  相似文献   

3.
The rate constants for the gas-phase reactions of sabinene and camphene, two monoterpenes emitted from vegetation, with OH and NO3 radicals and O3 have been determined at 296±2 K and one atmosphere total pressure of air. The OH and NO3 radical reaction rate constants were determined using relative rate techniques. Using rate constants of k(OH + isoprene) = 1.01 × 10−10 cm3 molecule−1 s−1, k(NO3 + trans-2-butene) = 3.87 × 10−13 cm3 molecule−1 s−1 and k(NO3 + 2-methyl-2-butene) = 9.33 × 10−12 cm3 molecule−1 s−1, the following OH and NO3 radical reaction rate constants (in cm3 molecule−1 s−1 were obtained: OH radical reaction; sabinene, 1.17 × 10−10 and camphene, 5.33 × 10−11; NO3 radical reaction; sabinene, 1.01 × 10−11, and camphene, 6.54 × 10−13. The absolute O3 reaction rate constants determined were (in cm3 molecule−1 s−1 units): sabinene, 8.07 × 10−17, and camphene, 9.0 × 10−19. These rate constants are compared to literature data for other structural-related alkenes and monoterpenes.  相似文献   

4.
齐震  孙也  樊星  朱天乐 《环境科学学报》2014,34(12):3133-3137
分别采用Na Cl O2和Na2SO3溶液作为氧化液和吸收液,在自行设计的鼓泡塔反应系统进行了液相氧化-吸收脱除模拟烟气NOx的研究,考察了气相SO2浓度、Na Cl O2和Na2SO3投加量以及p H值等因素对NO氧化和NOx脱除的影响.结果表明,SO2会优先于NO与氧化剂反应,从而增大氧化剂消耗量.偏酸性条件有利于NO氧化,但酸性太强会导致Na Cl O2分解为Cl O2逸出.碱性吸收液对NO几乎不具吸收脱除效果,但共存NO2能促进NO的吸收脱除.SO2对NO2吸收脱除具有促进作用.  相似文献   

5.
支流已经成为辽河干流的重要污染源,在支流河口建设大型人工湿地可以阻控支流污染物.为揭示辽河保护区七星湿地的净污效果,在对七星湿地水质、水量进行监测的基础上,采用内梅罗污染指数法对其有机物和营养物状况进行评价,并计算污染物在湿地中的去除量,最后利用归趋模型对污染物变化情况进行模拟.结果表明:内梅罗污染指数在支流河入口处较高,万泉河污染最严重;支流水体在经过湿地净化后,水体污染程度有所下降.植物生长期内(5—10月)七星湿地对COD去除总量为26.83 t,削减率为35.3%;对氨氮的去除总量为2.63 t,削减率为37.9%;对总磷的去除总量为0.40 t,削减率为52.9%.衰减方程模型对于COD、TP及不同形态氮拟合效果一般;多元参数回归模型及Monod机制模型较好地模拟了湿地Cout(NH+4-N)和Cout(NO-3-N)的变化.对Monod机制模型参数进行计算可得:kNH+4=24.987 L·m-2·d-1,kmax,NO-2=77.696 mg·m-2·d-1,KS,NO-2=0.114 mg·L-1.相关模型参数可用于湿地氨氮与硝氮浓度的预测.因此,多元参数回归模型及Monod机制模型可应用于类似湿地Cout(NH+4-N)和Cout(NO-3-N)变化的模拟及预测.  相似文献   

6.
邹宇  邓雪娇  李菲  殷长秦 《环境科学》2019,40(4):1634-1644
通过对广州番禺大气成分站(GPACS)的光化学相关污染物(O3、PAN、VOCs、NO2、NO)以及气象要素进行观测,分析2010~2016年期间发生在广州地区一次典型光化学污染过程.结果表明,该光化学污染过程期间,O3和PAN总体体积分数比较高,最大O3小时体积分数为140.6×10-9,而最大PAN小时体积分数为4.7×10-9.NO整体体积分数较低,对O3的化学滴定和PAN的去除影响较小.NO2整体体积分数较高、辐射较强和风速较低则有利于O3和PAN的形成和积累.PAN和O3具有一定的线性关系(R2=0.55),而形成PAN和O3前体物VOCs物种不完全相同影响着它们的线性关系,在生成PAN的VOCs物种中,乙烯、丙烷、异戊二烯和甲苯所占的比例较大,而对臭氧生成潜势较大的物种有异戊二烯、1,3,5-三甲苯、丙烯、间,对-二甲苯以及甲苯.对PA自由基体积分数进行估算,发现它的日均值体积分数在0.11×10-12~0.16×10-12范围变化,远高于其它地区,表明此次发生的光化学反应较为强烈.  相似文献   

7.
采用赤子爱胜蚓(Eisenia fetida)为测试生物,人工土壤为测试介质,Pb(NO3)2为土壤污染物,研究土壤老化对赤子爱胜蚓生长及繁殖的影响.结果表明,与对照组相比,污染土壤中赤子爱胜蚓体重随土壤中Pb(NO3)2浓度的升高呈现降低的趋势.Pb(NO3)2在人工土壤中老化0、7、28和84 d后,不同老化时间,Pb(NO3)2抑制赤子爱胜蚓的生长也不相同,影响最明显的是1 000 mg·kg-1和1 500 mg·kg-1试验组.不同老化时间的Pb(NO3)2对赤子爱胜蚓繁殖的影响有很大差异,其产茧量的半数有效浓度(EC50)分别为1 085.10、1 163.32、1 666.86和1 606.94 mg·kg-1;幼蚓孵化量的EC50分别为700.01、703.88、1 031.34和1 017.89 mg·kg-1.Pb(NO3)2在人工土壤中经过不同老化时间后,其对赤子爱胜蚓生长及繁殖的影响有很大的差异,这种差异影响到对土壤Pb(NO3)2污染的毒性评估,因此,进行Pb(NO3)2毒性试验时应考虑其在土壤中的老化作用.此研究结果可为老化土壤中污染物的生态风险评估以及土壤环境质量标准的制定提供科学依据.  相似文献   

8.
Oxidation-absorption technology is a key step for NOx removal from low-temperature gas. Under the condition of low O3 concentration (O3/NO molar ratio = 0.6), F-TiO2 (F-TiO2), which is cheap and environmentally friendly, has been prepared as ozonation catalysts for NO oxidation. Catalytic activity tests performed at 120°C showed that the NO oxidation efficiency of F-TiO2 samples was higher than that of TiO2 (about 43.7%), and the NO oxidation efficiency of F-TiO2-0.15 was the highest, which was 65.3%. Combined with physicochemical characteristics of catalysts and the analysis of active species, it was found that there was a synergistic effect between F sites and oxygen vacancies on F-TiO2, which could accelerate the transformation of monomolecular O3 into multi-molecule singlet oxygen (1O2), thus promoting the selective oxidation of NO to NO2. The oxidation reaction of NO on F-TiO2-0.15 follows the Eley-Rideal mechanism, that is, gaseous NO reacts with adsorbed O3 and finally form NO2.  相似文献   

9.
对菌株YB3进行了16S rRNA基因序列进化分析,并分别以NH_4Cl、NaNO_2、NaNO_3、尿素和蛋白胨为单一氮源,配制了5种低氮源浓度培养基,研究YB3在与养殖水体相近营养水平条件下的生长与氨氮去除特性.结果显示,菌株YB3属于蜡样芽孢杆菌(Bacullis cereus),在5种培养基中均能够生长,菌悬液(吸光度OD600为1.0)接种量为1.0%(v/v)时,OD600由0.010增长到0.100~0.117.在NH_4Cl培养基中,YB3的氨氮去除速率为1.23 mg·L~(-1)·d~(-1),去除率为93.5%.在尿素、蛋白胨等有机氮源培养基中,YB3将首先导致氨氮的积累,累积倍数分别为51.69和3.38,之后开始去除,去除速率为1.56和0.29 mg·L~(-1)·d~(-1),去除率为93.7%和26.8%.结果也表明,提高YB3接种量至8.0%(v/v),可以使蛋白胨培养基氨氮累积倍数下降至2.02,去除速率提高至1.07 mg·L~(-1)·d~(-1),去除率最终达到98.4%.NaNO_2和NaNO_3培养基中均未检测到氨氮,而NH_4Cl、尿素和蛋白胨培养基中也未检测到NO_2~--N和NO_3~--N,表明YB3的硝化、亚硝化和反硝化作用均不强烈,去除氨氮的同时将不会造成NO_2~--N和NO_3~--N等的大量积累.本文为菌株YB3在养殖水体调控与净化中的应用研究提供了实验基础和理论支持.  相似文献   

10.
Volatile organic compounds (VOCs) were measured at six sites in Beijing in August, 2004. Up to 148 VOC species, including C3 to C12 alkanes, C3 to C11 alkenes, C6 to C12 aromatics, and halogenated hydrocarbons, were quantified. Although the concentrations differed at the sites, the chemical compositions were similar, except for the Tongzhou site where aromatics were significantly high in the air. Based on the source profiles measured from previous studies, the source apportionment of ambient VOCs was preformed by deploying the chemical mass balance (CMB) model. The results show that urban VOCs are predominant from mobile source emissions, which contribute more than 50% of the VOCs (in mass concentrations) to ambient air at most sites. Other important sources are gasoline evaporation, painting, and solvents. The exception is at the Tongzhou site where vehicle exhaust, painting, and solvents have about equal contribution, around 35% of the ambient VOC concentration. As the receptor model is not valid for deriving the sources of reactive species, such as isoprene and 1,3-butadiene, other methodologies need to be further explored.  相似文献   

11.
大气NOx测量准确性问题分析   总被引:1,自引:1,他引:0  
采用美国热电公司的NO-N02-NOx分析仪(Model 42i TL)和NOy分析仪(Model 42i NOy),在2011年1月-10月期间,对北京城市大气中的NO、NOx和NOy进行了连续在线测量.两台仪器对NO的测量结果具有较高的一致性(r>0.998,p<0.01),说明两台仪器测量精度基本一致.将NOy分析仪(Model 42i NOy)采样口处安装和不安装颗粒物过滤膜两种条件下测量的NOy结果与NO-NO2-NOx分析仪所测的NOx结果分别进行了相关性分析([NOy] =0.989x[NOx],R2 =0.993;[NOy] =1.134 ×[NOx],R2=0.959),得出以下两个结论:①以颗粒态硝酸盐为代表的颗粒物是造成NOx与NOy偏差的主要原因,其所占比例在10%左右;②目前Model 42i-TL所测NOx的浓度水平较真实值偏高,其测量值更接近气态NOy的浓度水平.为估算NO2测值被高估的程度(以2011年8月6日-15日观测数据为例),用扣除部分气态NOz物种(HONO、HNO3、PAN、PPN)的修正方法,推论出在夏季N02被高估约7%(R2=0.968).  相似文献   

12.
龚巍巍  栾胜基 《环境科学》2012,33(11):4006-4011
气溶胶NH3和气体NOx是大气颗粒物和降水的主要成分,是形成气溶胶的关键物种.田间集约化氮肥施用是气溶胶NH3和气体NOx的一个重要来源,目前该领域的研究鲜有报道.2010年5月~2010年10月,在线监测了稻田施用尿素后气溶胶NH3和气体NOx的排放情况.监测系统的时间分辨率设置为1 h.在4次稻田施肥试验中,施肥后对气溶胶NH3排放和相应的气象因子连续采样20 d.在第4次施肥试验中,施肥后连续采样47 d,进而研究气体NOx的排放规律及其与气象因子的关系.结果表明,气溶胶NH3的排放因子分别为2.6%、5.5%、4.0%和1.6%,相应的排放通量分别为3.97、2.08、1.52和1.22 kg·hm-2.温度(空气温度和土壤温度)是影响稻田施肥气溶胶NH3排放的主要因子,而空气湿度和土壤水分对其排放的影响却不明确.通过分析监测数据可知,稻田施肥后NO2-N排放量与NO-N排放量的比值为9/4,气体NOx的排放因子和排放通量分别为0.14%和0.30 kg·hm-2.气象因子与气体NOx排放通量的关系也进行了初步探讨.  相似文献   

13.
Wet scrubbing combined with ozone oxidation has become a promising technology for simultaneous removal of SO2 and NOx in exhaust gas. In this paper, a new 20-species, 76-step detailed kinetic mechanism was proposed between O3 and NOx. The concentration of N2O5 was measured using an in-situ IR spectrometer. The numerical evaluation results kept good pace with both the public experiment results and our experiment results. Key reaction parameters for the generation of NO2 and N2O5 during the NO ozonation process were investigated by a numerical simulation method. The effect of temperature on producing NO2 was found to be negligible. To produce NO2, the optimal residence time was 1.25 sec and the molar ratio of O3/NO about 1. For the generation of N2O5, the residence time should be about 8 sec while the temperature of the exhaust gas should be strictly controlled and the molar ratio of O3/NO about 1.75. This study provided detailed investigations on the reaction parameters of ozonation of NOx by a numerical simulation method, and the results obtained should be helpful for the design and optimization of ozone oxidation combined with the wet flue gas desulfurization methods (WFGD) method for the removal of NOx.  相似文献   

14.
生物营养物去除(BNR)工艺模型参数校正与验证方法   总被引:2,自引:0,他引:2  
研究了结合活性污泥系统物料平衡的生物营养物去除(BNR)工艺模型参数校正与验证方法.首先采用代尔夫特理工大学开发的TUD模型及其参数缺省值进行初步模拟,并将模拟结果与实测数据进行对比以明确模拟偏差.同时,对原始运行数据进行物料平衡衡算,以消除测量误差并获得TP排放量、反硝化量及氧的净消耗量等平衡计算值,为模型校正提供依据.初步模拟结果显示,TP排放量(3913mg·d-1,以P计)和反硝化量(16170mg·d-1,以N计)均超出了平衡计算值的误差范围(分别为(3762.0±43.1)mg·d-1和(14150±237)mg·d-1),且沿程溶解性COD(SCOD)、PO34--P、NH4+-N、NO3--N不能完全与实测数据吻合,表明工艺模型参数的默认值需得到必要的校正.结合TP平衡,先修正污泥龄(SRT)的计算误差;应用平衡后的运行数据,将SRT由初始值10.3d调整为10d.SRT调整后,再次模拟得出的TP排放量为3750mg·d-1,已在平衡计算结果的范围之内,TP平衡得到了闭合.将发酵过程最大反应速率常数qfe从3d-1提高到15d-1后,沿程及PO43--P拟合结果同时得到了显著改善.通过调整DO及NH4+-N的亲和系数KNH4(从1mg·L-1至0.2mg·L-1),沿程NH4+-N得到了拟合.出水及沿程NO3--N的拟合通过调整氧的亲和系数KO2从0.7至0.1mg·L-1)得以实现.最后校核反硝化负荷及氧的净消耗量,模拟计算的反硝化负荷为14090mg·d-1,氧的净消耗量为126900mg·d-1,均在平衡计算值的误差范围之内(分别为(14150±237)mg·d-1和(129700±2910)mg·d-1),说明校正过程合理、可靠.  相似文献   

15.
Outdoor smog chamber experiments were used to study the sensitivity of the yields of two important nitrogen-containing pollutants, nitric acid (HNO3) and peroxyacetyl nitrate (PAN) to changes in nonmethane hydrocarbon (HC) and nitrogen oxide (NOx) concentrations in Los Angeles. The experiments were conducted at two sites in the Los Angeles Basin using eight chambers filled with morning Los Angeles air on 33 days. At least one chamber was unchanged and served as a control, while the initial HC and/or NOx concentrations were changed by 25–50% in up to seven chambers to simulate O3 control strategies and to broaden the range of HC - NOx conditions studied. Empirical models that predict the maximum yields of HNO3 and PAN were used to determine the response of these pollutants to three possible ozone control strategies. All three strategies (reductions in HC, NOx or both HC and NOx) reduced PAN while only NOx reductions decreased HNO3. However, reducing NOx increased the HC reductions required to attain lower O3 levels. Thus, there is a conflict between the O3 and HNO3 control strategies.  相似文献   

16.
利用Williams等和Guenther等的模型估计中国地区NOx和VOC的自然源排放.所得清单显示土壤NOx排放总量(以N计)为225.75 Gg;植被VOC年排放总量(以C计)为13.23 Tg,其中异戊二烯、单萜烯、其它VOC分别为7.77、1.86、3.60 Tg;排放有明显季节变化和空间变化.运用中尺度气象模式MM5以及光化学模式Calgrid研究这些排放在不同季节对对流层化学的影响.结果表明,O3、NOx、HNO3和PAN的全国平均浓度在土壤NOx排放影响下分别增加15.3%、15.7%、25.5%和6.5%;在植被VOC排放影响下改变5.6%、-4.9%、-19.3%和142.3%;在两者综合影响下增加26.1%、8.8%、4.3%和177.9%;浓度变化在夏季明显强于其它季节.自然源对中国地区光化学污染物空间分布有不同程度的影响,这种影响同区域气象条件、源排放和NMHC/NOx比值等因素有关.NOx和VOC的自然源排放对光化学特性影响显著,在光化学模拟过程中不容忽视.  相似文献   

17.
A field campaign on air quality was carried out in Shanghai in winter of 2012. The concentrations of NO, NO2, NOx, SO2, CO, and PM2.5 increased during haze formation. The average masses of SO42-, NO3- and NH4+ were 10.3, 11.7 and 6.7 μg/m3 during the haze episodes, which exceeded the average (9.2, 7.9, and 3.4 μg/m3) of these components in the non-haze days. The mean values for the aerosol scattering coefficient (bsp), aerosol absorption coefficient (bap) and single scattering albedo (SSA) were 288.7, 27.7 and 0.91 Mm-1, respectively. A bi-peak distribution was observed for the mass concentrations of CO, NO, NO2, and NOx. More sulfate was produced during daytime than that in the evening due to photochemical reactions. The mass concentration of NH4+ achieved a small peak at noontime. NO3- showed lower concentrations in the afternoon and higher concentrations in the early morning. There were obvious bi-peak diurnal patterns for bsp and bap as well as SSA. bsp and bap showed a positive correlation with PM2.5 mass concentration. (NH4)2SO4, NH4NO3, organic mass, elemental carbon and coarse mass accounted for 21.7%, 19.3%, 31.0%, 9.3% and 12.3% of the total extinction coefficient during non-haze days, and 25.6%, 24.3%, 30.1%, 8.1% and 8.2% during hazy days. Organic matter was the largest contributor to light extinction. The contribution proportions of ammonium sulfate and ammonium nitrate to light extinction were significantly higher during the hazy time than during the non-haze days.  相似文献   

18.
张柏发  陈丁江 《环境科学》2014,35(8):2911-2919
以浙江某典型流域为研究对象,基于1980~2010年的水质水量和氮源数据及LOADEST模型,估算了逐年河流NO-3-N通量和净人类活动氮输入(NANI),分析了河流NO-3-N通量和NANI的年际演化特征及其动态响应关系,探讨了每年NANI、滞留氮库、自然背景源对河流NO-3-N通量的贡献.结果表明,1980~2010年,河流NO-3-N通量和NANI总体上都呈现出先增后减的抛物线型变化趋势,均在1998年左右分别达到峰值5.74 kg·(hm2·a)-1和77.5 kg·(hm2·a)-1;过去31 a,河流NO-3-N通量和NANI分别净增加了~42%和~77%.化肥氮和大气氮沉降是NANI的主要来源,分别占了NANI的~48%和~40%.河流NO-3-N通量的年际变化不仅与NAIN(R2=0.27**)和化肥氮输入量(R2=0.32**)显著相关,而且与河流年均流量(R2=0.79**)或降雨量(R2=0.63**)具有更强的相关性,意味着河流NO-3-N的来源除了当年的NAIN,还受滞留氮库的影响.所建立的以NANI和流量为自变量的回归模型能很好地模拟河流NO-3-N通量变化(R2=0.94**).该模型预测结果显示,在NANI和流量分别降低30%的情况下,河流年均NO-3-N通量将分别减少~21%和~30%;每年的NANI、滞留氮库、自然背景源对河流当年NO-3-N通量的贡献率分别为~53%、~24%、~23%.河流NO-3-N通量长期的年际变化是NANI和水文要素共同作用的结果;但是,由于滞留氮库的影响,与源控制方式相比,增加"汇"景观应该能更加快速地削减河流NO-3-N通量.  相似文献   

19.
在一台装备有电控单体泵增压中冷系统柴油机的进气管上,加装甲醇喷射装置并向进气道喷入定量的纯甲醇,结合废气再循环(EGR)技术并使用氧化催化转化器(DOC)组合微粒氧化催化器(POC)后处理系统,使其常规排放能满足国五排放法规基础上,全面研究了柴油甲醇双燃料(Diesel Methanol Dual Fuel,DMDF)发动机的非常规排放特性.在采用国五排放法规标准规定的ESC(稳态13点工况)测试方法条件下,利用FTIR(傅里叶变换红外检测法)对DMDF发动机的检测结果表明:该机非常规排放物主要为甲醇、甲醛、1,3-丁二烯、苯、甲苯和SO2,非常规排放物的全工况加权比排放为19.532 g·kW~(-1)·h~(-1),其中,甲醇的全工况加权比排放为11.395 g·kW~(-1)·h~(-1),甲醛的全工况加权比排放为5.927g·kW~(-1)·h~(-1),SO2的全工况加权比排放为0.053 g·kW~(-1)·h~(-1),其余排放物为痕量水平.在催化氧化装置处理后非常规排放物全工况加权比排放为0.115 g·kW~(-1)·h~(-1),降幅为99.41%.催化氧化装置对甲醇、1,3-丁二烯、苯和甲苯的消除率为100%,对甲醛的消除率为99.04%.  相似文献   

20.
两种微藻胞外分泌物与NO2-、NO3-对2,4-D光解的影响   总被引:1,自引:1,他引:0  
在模拟太阳光照射下,利用旋转式光化学反应装置,研究了海水小球藻(Chlorella vulgaris)和新月菱形藻(Nitzschia closterium)的胞外分泌物(EOM),以及分别在NO-2或(和)NO-3共存条件下对2,4-二氯苯氧乙酸(2,4-D)光解的影响.实验结果表明,2,4-D在海水小球藻和新月菱形藻EOM及分别在NO-2、NO-3共存下的光解过程均符合准一级动力学反应.研究发现,2,4-D的光解速率随海水小球藻和新月菱形藻EOM浓度的增加而减小,表明这两种微藻EOM可抑制海水中2,4-D的光解.当在微藻EOM溶液中分别加入不同浓度的NO-2或NO-3后,微藻EOM对2,4-D光解的抑制作用减弱,且随着NO-2和NO-3浓度的增加,2,4-D光解速率明显增加.特别是当微藻EOM与NO-2或NO-3三者共存时,可进一步促进2,4-D的光解.  相似文献   

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