利用逆向轨迹反演模式估算北京地区甲烷源强

利用连续监测的大气甲烷浓度数据和拉格朗日逆向轨迹反演模式估算出北京甲烷源排放强度，并与根据最新调查数据建立的北京地区甲烷源排放清单进行了比较。排放清单结果表明，北京地区甲烷排放总量为296．4Gg/a，其中，最主要的甲烷排放源为城市垃圾和化石燃料，反映了北京作为一特大城市甲烷排放以人为源为主的特点。利用2000年6月至12月连续观测的有湿合层代表性的北京大气甲烷浓度，通过奇异值分解法（Singular Value Decomposition，SVD）反演出模拟区域的甲烷排放源强度和分布。模式计算与排放清单在甲烷源定性分布上对应较好，定量结果也是合理的。但由于可输入的气象数据有限，轨迹在整个模拟区域内覆盖不均匀，反演出的源块位置有偏差，其中偏差最大的为煤矿的甲烷排放。     

Calculation of long-term averaged and episodic oxidant concentrations for the Netherlands

Ground-level ozone and oxidant (sum of O₃ and NO₂) concentrations in The Netherlands are calculated during the growing season (May–September) by means of a Lagrangian long-range transport model. Two air parcels—one representative of the mixed layer, the other representative of the polluted layer above the mixed layer (aged smog layer)—are followed along 96 h back trajectories. Long-term averaged and 98 percentile values of hourly averaged concentrations are estimated on the basis of concentrations calculated for four arrival times per day for all days in the period considered.In a number of sensitivity runs the influence of European anthropogenic NO_x and VOC emissions on the oxidant concentrations in The Netherlands has been investigated. In general, the influence of European emissions on the 98-percentile values is 2–3 times as large as on the averaged concentrations. This indicates that long-term averaged concentrations more strongly depend on the concentrations in the free troposphere whereas the episodic concentrations are determined by photochemical production over Europe. VOC emission reduction is more effective in lowering episodic concentrations than NO_x emission reduction. For long-term averaged concentrations, however, NO_x and VOC emission reduction of 50% or more are nearly equally effective.     

Quantification of carbon dioxide and methane emissions in urban areas: source apportionment based on atmospheric observations

Anthropogenic emissions of carbon dioxide (CO₂) and methane (CH₄) in the atmosphere constitute an important component of the related carbon budget. The main source of anthropogenic CO₂ is burning of fossil fuels, especially in densely populated areas. Similar emissions of CH₄ are associated with the agricultural sector, coal mining, and other human activities, such as waste management and storage and natural gas networks supplying methane to large urban, industrial centers. We discuss several methods aimed at characterizing and quantifying atmospheric loads and fluxes of CO₂ and CH₄ in Krakow, the second largest city in Poland. The methods are based on atmospheric observations of mixing ratios as well as isotopic composition of the investigated gases. Atmospheric mixing ratios of CO₂ and CH₄ were measured using gas chromatography (GC) and cavity ring-down spectroscopy (CRDS). The isotopic composition of CO₂ and CH₄ was analyzed using isotope ratio mass spectrometry (IRMS), accelerator mass spectrometry (AMS), and CRDS techniques. These data, combined with auxiliary information characterizing the intensity of vertical mixing in the lower atmosphere (height of the nocturnal boundary layer [NBL] and atmospheric ²²²Rn concentration), were further used to quantify emission rates of CO₂ and CH₄ in the urban atmosphere of Krakow. These methods provide an efficient way of quantifying surface emissions of major greenhouse gases originating from distributed sources, thus complementing the widely used bottom-up methodology based on emission statistics.

     

Calculation of long term averaged ground level ozone concentrations

Seasonal averaged ground level concentrations for O₃ have been calculated for The Netherlands by means of a two-layer Lagrangian long-range transport (LRT) model. The model includes emissions, nonlinear atmospheric chemistry, dry deposition, exchange between boundary layer (BL) and free troposphere (FT) and fumigation between a mixed layer and an aged smog layer. Concentrations of primary and secondary pollutants in the FT are obtained from a two-dimensional global model developed by Isaksen.In the reference calculation the modelled concentrations of Ox (sum of O₃ and NO₂) and O₃ are in fair agreement with measurements. The NO_x (sum of NO and NO₂) and NO₂ concentrations are under-estimated by the model but there is a good temporal correlation between calculated and measured concentrations. Validation of other components involved in the chemical scheme is hardly possible due to the paucity of measured data. It can only be stated that the results presented in this paper are not in disagreement with measured or modelled data presented in the literature.In a number of sensitivity runs the influence of European anthropogenic emissions of NO_x and volatile organic compounds (VOC) has been investigated. The calculations indicate that the influence of European emissions on the growing season, daytime averaged (May–September, 10–17 h) O₃ concentrations in The Netherlands is small. For European reductions in the order of tens of per cents a VOC emission reduction is more effective than a NO_x emission reduction in lowering the O₃ concentrations. For strong reductions (about 70%) VOC and NO_x are equally effective. The effects of the modelled underprediction of NO_x concentrations on the production of O₃ on a European scale are probably small. On a local scale the effects are more pronounced due to the NO/O₃ titration (photostationary equilibrium). Therefore, an empirical correction is applied on the modelled O₃ concentrations. After this correction, it is shown that daytime O₃ levels during the growing season increase when European NO_x emissions are reduced (2.0–7.7.% increase at 50% NO_x emission reduction). A reduction in VOC emission leads to decreasing O₃ levels (9% reduction for 40% VOC emission reduction, 16% reduction for 70% VOC emission reduction). For a combined reduction of both VOC and NO_x slightly decreasing ground level O₃ concentrations are expected.     

A non-local closure model for vertical mixing in the convective boundary layer

A simple non-local closure model for vertical mixing in Convective Boundary Layers (CBL) has been developed specifically for application in regional or mesoscale atmospheric chemistry models. The model, named the Asymmetrical Convective Model (ACM), is based on the concept that vertical transport within the CBL is inherently asymmetrical. Upward transport by buoyant plumes originating in the surface layer is simulated by mixing from the lowest model layer directly to all other layers in the CBL. Downward transport, however, proceeds only to the next layer in order to emulate gradual compensatory subsidence. The ACM is similar to the model developed by Blackadar (1978, 4th Symp. on Atmospheric Turbulence, Diffusion and Air Quality, pp. 443–447, Reno, Am. Meteorol. Soc.) but differs in its treatment of downward transport. The realism of the ACM is tested through comparisons to large-eddy simulations of several idealized test cases. These tests show that while the ACM shares the Blackadar model's ability to simulate rapid transport upward from the surface layer to all levels in the CBL, it is clearly superior in its treatment of material emitted from elevated sources either within or above the CBL. The ACM is also tested in the context of the Regional Acid Deposition Model (RADM) both to determine sensitivity to different CBL mixing schemes and to compare to vertically resolved aircraft measurements. These tests demonstrate quicker upward transport of ground-level emissions by the ACM as compared to the eddy diffusion scheme currently used in RADM. The ACM also affects ozone photochemistry in the boundary layer resulting in lower ozone concentrations in areas of high NO_x emissions.     

华北地区典型机场清单建立及空气质量影响

基于利用AMDAR数据确定大气混合层高度进而对飞机不同工作状态下的时间进行修正的计算方法，核算了2017年华北地区6座典型机场大气污染物排放量.结果显示，6座机场NO_x、CO、VOC、SO₂与PM_2.5的排放总量分别为21504.2，7074.8，1424.0，1283.6和323.2t.飞机源NO_x、CO、VOC与SO₂的排放量远高于机场内其他污染源，而对PM_2.5的排放贡献相差较小.HC与CO的排放主要集中在滑行阶段，占比分别为90.6%与90.2%，而NO_x、SO₂与PM_2.5的排放主要集中在爬升阶段，排放占比分别为58.9%、38.7%和43.5%.6座机场1月份污染物排放量较低，在8月份达到峰值.基于本研究建立的天津滨海国际机场大气污染物排放清单，利用WRF-CAMQ模型研究机场排放对周边区域PM_2.5浓度的影响.结果表明机场区域小时最大贡献浓度为3.24μg/m³；距离机场5km处的年均贡献浓度与小时最大贡献浓度分别为0.08和2.84μg/m³.     

2015年中国地区大气甲烷排放估计及空间分布

CH₄是仅次于CO₂的重要温室气体,也是重要的化学活性气体.定量估算我国甲烷的排放量及分析其空间分布特征,对于控制温室气体排放,减缓温室效应具有重要意义.本文以2015年中国官方统计年鉴资料为基础,利用IPCC排放清单指南、国内外排放因子研究结果及动力学模型方法,从能源活动（煤炭开采和油气系统）、农业活动（反刍动物、稻田排放和秸秆露天燃烧）、自然源排放（自然湿地和植被排放）、废弃物处理（固体废弃物、工业污水和生活污水）和人工湿地等几个主要方面,对中国地区的CH₄排放进行定量估计.结果表明：中国地区2015年CH₄排放总量为61.59 Tg,其中以农业活动和能源活动为主要排放源,排放量分别达到20.42 Tg和20.39 Tg,占总排放量比例分别约为33.2%和33.1%.CH₄自然源考虑了植被和自然湿地排放,排放量为11.77 Tg,占比为19.1%;废弃物处理产生的CH₄排放量为8.64 Tg,占比为14.0%;人工湿地排放量为0.37 Tg,占比为0.6%.从空间分布来看,CH₄排放具有较明显的不均匀性,大值区主要集中在华北、西南及东南地区,而西北地区的排放量则相对较低,主要与各地的资源环境、人口密度和经济情况密切相关.     

风帽在准好氧填埋的应用及对填埋初期的影响

首次将风帽应用于准好氧填埋,以2 m×1 m×2 m的准好氧模拟箱为对象,考察了风帽对准好氧填埋环境形成过程的影响,比较了不同风速条件下二氧化碳和甲烷的浓度变化,并对风帽应用于准好氧填埋的作用原理进行了分析,以期为设计和优化准好氧填埋结构提供参考.结果表明,风帽可以加快准好氧环境的形成,将传统的准好氧环境的形成期由常规的50 d以上提前到40 d左右.通过比较风帽先拆后装二氧化碳和甲烷的浓度变化,表明风帽可以促进甲烷向二氧化碳的转化,减少甲烷的排放.卸下风帽后二氧化碳的浓度由最初的16.67%降为15.88%,甲烷从6.14%增大到16.12%;装上后二氧化碳的浓度增至19.18%,甲烷降为10.05%.考察了风速为2.0、3.5、5.0、6.5、8.0 m/s 5种条件下导气管出口处的甲烷排放情况,表明风速可以加强风帽的作用,有利于甲烷的减排,当风速增至8 m/s时,甲烷浓度由最初的15%以上降为5%以下.     

Development of the Pasture Simulation Model for assessing livestock production under climate change

To simulate climate change impacts on pastures and domestic herbivores as well as feedbacks to the atmosphere in terms of greenhouse gas emissions, we have improved a process-based biogeochemical pasture model, PaSim. The overall aim was to simulate the meat and milk production of cattle (suckler cows with their calves, dairy cows and heifers) in response to climate and management, as well as feedbacks to the atmosphere through enteric methane emissions. Herbage intake at grazing was calculated from animal characteristics, herbage availability, diet digestibility and air temperature. With suckler cows, milk production and changes in daily liveweight and body condition were calculated from net energy balance. The net energy intake of dairy cows and their body reserves at turnout to pasture were used to simulate milk production at pasture, daily liveweight and body condition changes, taking into account cow energy requirements and intake capacity. Heifer growth was determined from heifer net energy intake and liveweight. Net energy intake was used to assess enteric methane production through a conversion factor, which depends both on the energy level of the diet and on the herbivore type. The model was assessed against experimental data for animal performance and methane emissions at grazing. Predictions show good agreement with observations. On average, the root mean square error was 6.5, 4 and 2.5% for the liveweights of suckler cows, suckler calves and heifers, respectively, 18% for dairy milk production and 12% for enteric methane emissions. By comparing this new version of the PaSim model to the previous version, we show that a greater accuracy in animal performance modelling improves the sensitivity of the model to interannual climate variability. However, long term (30 years) projections of climate change impacts on grasslands and of radiative feedbacks to the atmosphere are not significantly modified. The originality and the validity domain of the model are discussed.     

Hydrogen peroxide levels in Los Angeles: A screening-level evaluation

The major factors affecting the diurnal variation of gaseous hydrogen peroxide were studied using a one-dimensional vertical gas-phase chemistry/transport screening model. The model which included diurnal variations of the inversion layer, surface emissions, dry deposition of air pollutants, and meteorological conditions such as solar radiation, temperature, relative humidity and wind speed, was used to evaluate the influence of the ratio of NMHC/NO_x, the emission rates of NO_x and NMHC, the deposition velocity of H₂O₂, and the height of inversion layer on the ground level gaseous H₂O₂ concentrations. The model was found to yield reasonable agreement with field data from the Carbonaceous Species Methods Comparison Study at Glendora, California, in 11–21 August 1986. Specifically, model predictions and field results all indicated that during clear skies, ambient H₂O₂ concentration was highest at about early afternoon when O₃ concentration was highest and NO_x was lowest. It was concluded that the predicted gaseous H₂O₂ concentration is most sensitive to the emission rate of NO_x and the ratio of NHMC/NO_x, but it is less sensitive to the deposition velocity, height of inversion layer, and the emission rate of NMHC.     

Using a biological aerated filter to treat mixed water-borne volatile organic compounds and assessing its emissions

A biological aerated filter (BAF) was evaluated as a fixed-biofilm process to remove water-borne volatile organic compounds (VOCs) from a multiple layer ceramic capacitor (MLCC) manufacturing plant in southern Taiwan. The components of VOC were identified to be toluene, 1,2,4-trimethylbenzene, 1,3,5-trimethylbenzene, bromodichloromethane and isopropanol (IPA). The full-scale BAF was constructed of two separate reactors in series, respectively, using 10- and 15-cm diameter polypropylene balls as the packing materials and a successful preliminary bench-scale experiment was performed to feasibility. Experimental results show that the BAF removed over 90% chemical oxygen demand (COD) from the influent with (1188 605) mg/L of COD. A total organic loading of 2.76 kg biochemical oxygen demand (BOD)/(m3 packing d) was determined for the packed bed, in which the flow pattern approached that of a mixed flow. A limited VOC concentration of (0.97 0.29) ppmv (as methane) was emitted from the BAF system. Moreover, the emission rate of VOC was calculated using the proposed formula, based on an air-water mass equilibrium relationship, and compared to the simulated results obtained using the Water 9 model. Both estimation approaches of calculation and model simulation revealed that 0.1% IPA (0.0031–0.0037 kg/d) were aerated into a gaseous phase, and 30% to 40% (0.006–0.008 kg/d) of the toluene were aerated.     

2008北京残奥会期间大气黑碳气溶胶污染特征

利用单颗粒黑碳光度计(SP2)对2008年残奥会期间北京市黑碳(BC)气溶胶的质量浓度、粒径分布及单颗粒混合态进行连续在线观测.结果表明:观测期间BC浓度均值为1.65μg/m3,低于往年同期水平;质量粒径分布呈单峰型,峰值位于207nm;内混态BC比例平均为56.1%,高于其他国内外城市,说明本地源排放贡献相对较小.随大气边界层高度及本地源排放变化,BC浓度在上午8:00和午夜0:00出现2个峰值,内混态BC比例日变化趋势与之相反.风向风速分析表明,残奥会期间来自五环外未限行区域的机动车排放对市区BC浓度有明显影响.     

建筑施工扬尘排放因子定量模型研究及应用

选择天津某建筑施工工地,现场采集大气中PM10、气象、路面积尘及机动车数等数据,并确定施工扬尘排放的主要影响因素.利用FDM模型,计算施工扬尘排放因子,将计算得到的扬尘排放因子和各影响因素进行非线性拟合,建立施工扬尘PM10排放因子定量模型,并结合ISC3模型,模拟计算2003年11~12月间,天津市建筑施工过程中的PM10排放浓度.结果表明,施工产生的PM10平均浓度为20.3μg/m3,占大气PM10浓度的13.3%.     

中国区域反应性气体排放源清单

反应性气体是形成气溶胶及酸雨、光化学烟雾等环境问题的重要前体物,采用政府部门公布的基础数据(包括社会－经济数据、化石燃料和生物质燃料消耗、废物处理数据等,绝大部分为县级水平)及一些较新的、中国特有的排放因子,计算了中国大陆2007年高时空分辨率的关键反应性气体SO2、NOx、CO、NH3、VOCs的排放源清单.计算出的全国和各地区的排放量使用了0.5°×0.5°的网格来显示,结果表明,各反应性气体的估算年排放量分别为:SO2 3158.4万t,主要是燃煤所致;NOx、CO分别为2492.6,15785.2万t,均主要来源于燃煤和生物质燃烧;NH3 1601.7万t,主要源于动物排放和农田化肥的使用;VOCs 3709.8万t,主要源于溶剂挥发、废物处理、交通源等.本研究计算的排放结果比以前的清单稍高,主要是由于部分排放量以前被低估了;东部地区的排放量比西部高.反应性气体的排放具有较强的季节性,主要是由于自然因素及居民采暖、农业秸秆的露天焚烧的季节性等所致.     

基于卫星数据研究兰州市NO2时空分布特征以及冬季NOx排放通量

搭载在EOS AURA卫星上的OMI探测器由于其较高时空分辨率在大气痕量气体(O3,NO2,SO2)探测中得到广泛应用.利用2010~2012年OMI NO2柱浓度数据产品重构了兰州市以及周边地区NO2柱浓度分布,分析了其时空变化特征,并利用西南风场下NO2空间分布特征采用拟合方法研究了NOx冬季排放通量以及寿命.研究表明,NO2柱浓度空间分布呈现以兰州市为中心,浓度向四周扩散的特征;兰州市NO2柱浓度的年变化特征为12月达到最大浓度,8月达到最小浓度;2010~2012年NO2寿命分别为10.6,9.9,9.1h,NOx冬季排放通量分别为175.3, 183.7,179.9mol/s.其排放通量与兰州环境公报提供的氮氧化物排放通量数量级之间具有较好的一致性,说明利用卫星数据估算兰州的NOx通量方法的有效性.     

Impact analysis of drought, water excess and salinity on grass production in The Netherlands using historical and future climate data

The coupled SWAP-WOFOST model was used to study the effects of increasing salinity of groundwater, drought and water excess on grass production in The Netherlands. WOFOST simulates crop growth and SWAP simulates transport of water, solutes and heat in the vadose zone. The model was tested using several datasets from field experiments. We applied the models at regional scale where we quantified the impact of various groundwater salinity levels on grass growth and production using historical weather data (1971-2000). The salt concentrations in the subsoil were derived from the National Hydrological Instrument. The results show that salinity effects on grass production are limited. In wet years the excess rainfall will infiltrate the soil and reduce salt water seepage. In a next step we used future weather data for the year 2050, derived from 3 Global Circulation Models. From each model we used data from two CO₂ emission scenarios. As expected higher temperatures increased drought stress, however, the production reduction as a result of salt water in the root zone is limited. Salt stress mainly occurred when irrigation was applied with saline water. The increased CO₂ concentration in combination with the limited drought stress resulted in increasing simulated actual and potential yields. Overall conclusion for grassland in The Netherlands: drought stress is stronger than stress caused by water excess which on its turn is stronger than salinity stress. Future water demand for irrigation may increase by 11-19% and result in water scarcity if water supply is insufficient.     

机动车排放车载实验及模型模拟研究

研究机动车的排放特征及获得排放因子,是建立机动车排放清单和制定相应控制策略的基础,而路上的机动车排放车载测试被认为是实验室台架测试的一个重要补充.本研究利用AVL DiGas 4000 light五气分析仪,在澳门典型路段上对7辆汽油轿车样本开展了尾气排放车载实验.研究发现安装电喷加三元催化转化系统的车辆(以下称电喷车)在气态污染物排放上比旧的化油器车有显著降低,化油器车HC、CO和NO排放的体积浓度平均值分别为227×10^-6、1.57%和1477×10^-6,而电喷车则分别为33×10^-6、0.21%和131×10^-6,约是前者的1/11～1/7.但电喷车在冷启动阶段会出现高排放;对电喷车的CO和NO排放浓度做算术平均,其绝对值主要由出现频率少的高浓度值所贡献.研究进一步估算了汽油轿车的排放因子,同时利用MOBILE5模型计算了澳门2000年汽油轿车的平均排放因子,模型计算值和实验数据估算结果的比值在59%～139%之间,如果仅比较年平均排放因子,这个比值则在68%～132%之间.结果表明,车辆采用电喷加催化转化系统,对控制污染物排放的作用显著,但催化设备存在冷启动时起燃缓慢的问题;对电喷车的技术改进,减少其在行驶过程中出现高浓度的污染物排放,将能进一步大大降低平均排放水平;应用修正的MOBILE5模型计算澳门地区汽油轿车的排放因子,结果是比较可信的.     

组合灰色预测模型应用于山东省碳排放预测

根据山东省2000—2012年工业、建筑业和交通运输业能源消费数据测算得到碳排放量,基于GM(1,1)模型、Verhulst模型和SCGM(1,1)c模型建立组合灰色预测模型,运用预测有效度方法确定组合预测模型的权重系数。选用2000—2009年三大碳排放行业的实际值作为原始数据,利用各预测模型预测2010—2012年碳排放量。结果表明:组合灰色预测模型比单一预测模型具有更高的预测精度。利用组合模型预测山东省2013—2017年各行业碳排放量,为相关部门制定节能减排政策提供理论及方法借鉴。     

Nitrogen source-receptor matrices and model results for eastern Canada

The long-range transport sulphur/nitrogen model of the Atmospheric Environment Service of Environment Canada was used to compute nitrogen source-receptor matrices for 1980 at 12 receptor sites in eastern Canada and 3 in the eastern U.S.A. There were 40 emission regions used to produce the 40 × 15 matrices of concentration and deposition of nitrogen species. The model used nonlinear chemical reactions and the nonlinear effects could be estimated by running each emission region regions combined. For wet deposition the nonlinear effects were less than 10%. For the total annual deposition (wet and dry), the nonlinearity was less than 5%.At each receptor, the matrices showed the contribution to nitrogen concentration and deposition from each emission region. The Canadian contribution to nitrogen concentration/deposition was greatest at Gander, Newfoundland (60–70%) and least at Algoma, Ontario (7–12%). Of the total North American emissions, Canada contributed about 8–9%. Model results that were compared to the limited amount of observed data showed reasonably good agreement (within factors of 2–3).In spite of the model nonlinearities, deficiencies and uncertainties, these matrices provide a first quantitative estimate of the magnitude and relative contributions of Canadian and U.S. source regions to the nitrogen concentration and deposition at several receptors in eastern Canada.     

北京市沥青搅拌站VOCs排放清单研究

定量化的排放清单是环境管理和研究工作的重要抓手,由于行业规模小、活动水平数据匮乏、测试难度大,沥青混合料生产过程的VOCs排放研究国内文献报导极少.本文构建了一套沥青混凝土搅拌站VOCs排放量核算方法,依据排放特点分环节分别核算VOCs排放量,分析排放量的时空分布特征,定量分析排放清单的不确定性,并基于目前的污染控制水平和未来行业管控规划,预估2030年北京市沥青混合料生产行业的VOCs排放量,以期为北京市VOCs总量减排和精细化管理提供依据.结果表明：2017年北京市沥青搅拌站VOCs总排放量为25.9 t,不确定度为25.6%,其中,沥青储罐的排放量最大,占总排放量的87.2%;顺义、昌平、通州3个区的排放量位居前三,分别占行业总排放量的16.2%、14.4%和14.1%;在时间分布上,5—7月沥青混合料产量最高、VOCs排放量最大;通过情景分析,本研究认为通过出台行业标准和绿色生产技术指南,可大幅削减沥青混合料生产行业的VOCs排放量.