Evaluation of Modeled Spatially and Temporarily Highly Resolved Emission Inventories of Photosmog Precursors for the City of Augsburg: The Experiment EVA and Its Major Results

Emission inventories of NO_x, CO, and individual volatile organic compounds (VOC), highly resolved in space and time, belong to the most important input parameters for chemistry and transport models (CTM) used for ozone prediction. Because of the decisive influence of the input quality on the outcome of CTM simulations, the quality of emission inventories has to be assessed. This paper presents an experimental evaluation of the highly resolved emission inventories for the city of Augsburg. The emissions of the city, determined in March and October 1998 using mass balance and tracer techniques, and derived from the measured receptor concentration ratios, were compared with emissions modeled from an emission inventory. The modeled CO emissions were in agreement with the measured ones within the combined experimental and model uncertainties. More detailed CO emission model simulations suggest that the tendency of calculated CO emissions being smaller than the measured ones may be due to higher traffic activity in Augsburg. Modeled NO_x emissions were in agreement with the measured ones within the combined experimental and model uncertainties. Large deviations between modeled and measured values have been found for some individual NMHC compounds. The measured NMHC emission fingerprints were dominated by mobile sources. Substantial model predicted NMHC emissions from the solvent use could not be detected by measurements suggesting that they may not be correctly represented by the emission model.     

不同人为源排放清单对大气污染物浓度数值模拟的影响:以浙江省为例

应用大气化学模式WRF-Chem(Weather Research and Forecast-Chemistry),分别选用亚洲排放源清单INTEX-B(Intercontinental Chemical Transport Experiment-Phase B)、REASv2.1(Regional Emission inventory in Asia version 2.1)以及全球排放源清单HTAP_v2(Hemispheric Transport of Air Pollution version 2),对浙江省2013年12月进行模拟,分别记为IN、RE和HT试验,研究人为源排放清单对大气污染物浓度数值模拟的影响。结果表明,3组试验合理的反映出PM2.5(空气动力学当量直径小于等于2.5μm的颗粒物,即细颗粒物)、PM10(空气动力学当量直径小于等于10μm的颗粒物,即可吸入颗粒物)和NO_2近地面浓度的时空分布特征,相关系数为0.5~0.8,85%以上的模拟值落在观测值的0.5~2倍范围内,但对SO_2近地面浓度模拟较差。IN、RE、HT试验对PM2.5和PM10的模拟偏差均成递减趋势,约为30%、16%和6%,HT试验的模拟值更加接近观测。INTEX-B清单中PM2.5的一次排放与二次气溶胶前提物SO_2均高于REAS与HTAP清单,因此会导致更多的硫酸盐生成,从而进一步增加PM2.5浓度。HTAP_v2清单中较低的NH3排放会抑制硝酸盐的生成,从而有助于降低PM2.5浓度。3个清单的基准年与模拟年的差异对SO_2浓度模拟的准确性影响更大,INTEX-B清单中SO_2排放量明显高于REASv2.1与HTAP_v2清单,尤其在浙北和沿海工业发达地区,导致IN试验模拟的SO_2在这些地区存在明显高估。3组试验模拟的NO_2浓度偏差最小且更为接近(-8%~4%),主要原因是3个清单在浙江省的NOx排放十分一致。从3组试验结果之间的差异程度来看,浙江省范围内PM2.5、PM10、SO_2和NO_2逐日浓度模拟值之间的平均差异程度分别约为14%、15%、51%和16%,最大差异程度分别为69%、78%、137%和132%。月均浓度与逐日浓度的平均差异程度基本一致,但最大差异程度明显更低。总体来看3组试验模拟的PM2.5、PM10与NO_2的差异程度明显低于SO_2。     

Biogenic Volatile Organic Compounds (VOC): An Overview on Emission, Physiology and Ecology

This overview compiles the actual knowledge of the biogenic emissions of some volatile organic compounds (VOCs), i.e., isoprene, terpenes, alkanes, alkenes, alcohols, esters, carbonyls, and acids. We discuss VOC biosynthesis, emission inventories, relations between emission and plant physiology as well as temperature and radiation, and ecophysiological functions. For isoprene and monoterpenes, an extended summary of standard emission factors, with data related to the plant genus and species, is included. The data compilation shows that we have quite a substantial knowledge of the emission of isoprene and monoterpenes, including emission rates, emission regulation, and biosynthesis. The situation is worse in the case of numerous other compounds (other VOCs or OVOCs) being emitted by the biosphere. This is reflected in the insufficient knowledge of emission rates and biological functions. Except for the terpenoids, only a limited number of studies of OVOCs are available; data are summarized for alkanes, alkenes, carbonyls, alcohols, acids, and esters. In addition to closing these gaps of knowledge, one of the major objectives for future VOC research is improving our knowledge of the fate of organic carbon in the atmosphere, ending up in oxidation products and/or as aerosol particles.     

Investigating the Changes in Air Pollutant Emissions over the Beijing-Tianjin-Hebei Region in February from 2014 to 2019 through an Inverse Emission Method

In recent years, China has implemented several measures to improve air quality. The Beijing-Tianjin-Hebei(BTH)region is one area that has suffered from the most serious air pollution in China and has undergone huge changes in air quality in the past few years. How to scientifically assess these change processes remain the key issue in further improving the air quality over this region in the future. To evaluate the changes in major air pollutant emissions over this region, this paper employs ens...     

RMAPS_Chem V1.0系统SO2排放清单优化效果评估

RMAPS_Chem V1.0系统是基于WRF_Chem模式建立的服务于华北区域雾霾等污染预报业务的模式系统,该研究着重针对系统中污染排放清单不确定性带来的SO₂浓度预报偏差较大问题,采用EnKF源反演和误差统计订正相结合的方法对排放清单进行了改进,形成了一套优化后的华北区域SO₂排放清单。通过输入初始清单和优化清单对2017年10月进行模拟,并与华北地区616个地面环境监测站观测值进行对比,结果表明:EnKF源反演结合误差统计订正的排放清单优化方法适用于SO₂排放清单的改进,有效降低了清单系统性偏差,针对主要区域及重点城市的检验显示模拟结果接近观测值;排放清单优化后模拟误差显著降低,如河北南部、山东西部至北京一带模式预报均方根误差与归一化平均绝对误差明显下降,区域内站点模拟误差呈正态分布特征,误差分布范围、最大概率出现范围均明显变窄,且最大误差概率明显上升。     

Regional adjustment of emission strengths via four dimensional data assimilation

The Four-Dimensional Data Assimilation was performed to evaluate source emission strengths over the United States. The USEPA Models-3 system (CMAQ/MM5/SMOKE) and ridge regression are used as the forward and inverse models, respectively. The continental US is divided into six regions, and data assimilation is performed for each region in July 2001 and January 2002. In addition, two separate scaling factors are calculated for weekdays and weekends. Results show that base emissions for CO and SO₂ sources are relatively accurate. Base emissions for PEC source are overestimated 100%, but those for POA source are underestimated up to 70% when compared with the adjusted emissions. Emissions for NH₃, NO _x , and PMFINE sources are relatively accurate in July 2001, but those in January 2002 are around 100% higher than the adjusted emissions. Base VOC emissions in July 2001 are similar to the adjusted emissions but those in January 2002 are underestimated up to 70% when compared with the adjusted emissions. Though the emission adjustment itself improves the overall air quality model performance, a better improvement is expected with the modification of speciation profiles and temporal allocations in the Models-3 system, as well.     

Emission of nitrous oxide from temperate forest soils into the atmosphere

N₂O emission rates were measured during a 13-month period from July 1981 till August 1982 with a frequency of once every two weeks at six different forest sites in the vicinity of Mainz, Germany. The sites were selected on the basis of soil types typical for many of the Central European forest ecosystems. The individual N₂O emission rates showed a high degree of temporal and spatial variabilities which, however, were not significantly correlated to variabilities in soil moisture content or soil temperatures. However, the N₂O emission rates followed a general seasonal trend with relatively high values during spring and fall. These maxima coincided with relatively high soil moisture contents, but may also have been influenced by the leaf fall in autumn. In addition, there was a brief episode of relatively high N₂O emission rates immediately after thawing of the winter snow. The individual N₂O emission rates measured during the whole season ranged between 1 and 92 g N₂O-N m^–2 h^–1. The average values were in the range of 3–11 g N₂O-N m^–2 h^–1 and those with a 50% probability were in the range of 2–8 g N₂O-N m^–2 h^–1. The total source strength of temperate forest soils for atmospheric N₂O may be in the range of 0.7–1.5 Tg N yr^–1.     

农田生态系统温室气体排放研究进展

自1985年起,中国科学院大气物理研究所利用自行设计制造的自动观测仪器系统,历时十六年先后对我国四大类主要水稻产区的甲烷排放规律及其与土壤、气象条件和农业管理措施的关系进行了系统野外观测实验,并对稻田甲烷产生、转化和输送机理进行了理论研究,探讨了控制稻田甲烷排放的实用措施,建立了估算和预测稻田甲烷排放的数值模型.在甲烷排放的时空变化规律和转化率研究方面有一系列新的发现,在稻田甲烷产生率、排放率及其与环境条件的关系方面取得一系列新的成果,以充分证据改变了国际上关于全球和中国稻田甲烷排放总量的估算.在对稻田甲     

中国大陆黑碳气溶胶排放清单

The detailed high-resolution emission inventory of black carbon (BC) from China in the year 2000 was calculated. The latest fuel consumption data including fossil and biomass fuels, and socio-economic statistics used were obtained from government agencies, mostly at the county level, and some new emission factors (Efs) from local measurements were also used. National and regional summaries of emissions were presented at 0.2°×0.2°resolution. Total BC emission was 1499.4 Gg in 2000, mainly due to the burning of coal and biomass. The BC emission estimated here is higher than those in previous studies, mainly because the emissions from coal burning by rural industries and residences were previously underestimated. More BC aerosols were emitted from eastern China than western China. A strong seasonal dependence was observed for BC emissions, with peaks in January and December and low emissions in July and August; and this seasonality is mainly due to patterns in residential heating and the open burning of crop residues.     

基于排放源的中国城市垃圾填埋场甲烷排放研究

利用全国垃圾填埋场的点源数据,基于实际调研和实验室分析建立中国不同区域、不同规模、不同填埋时间的排放因子矩阵,采用IPCC推荐的一级降解动力学（FOD）方法自下而上地核算了中国2107个垃圾填埋场在2007年的甲烷（CH₄）排放量。针对不同区域和类型的填埋场,分别就城市垃圾组分、可降解有机碳、CH₄修正因子、CH₄氧化系数、填埋场CH₄收集率等进行了深入研究。结果显示,中国2007年填埋场CH₄排放量为118.61万t,与《中华人民共和国气候变化第二次国家信息通报》2005年填埋场排放量（220万t）差异较大,其主要原因是城市垃圾填埋场统计数据的差异,例如填埋场个数及垃圾填埋量。中国绝大部分填埋场CH₄年排放量在700 t以下,超过1000 t的有279个,超过1万t的仅10个。江苏省的CH₄排放量最高,达到9.87万t;西藏的排放量最小,仅为0.21万t。东部江苏、广东、浙江等省的整体排放量较高,西部地区西藏、宁夏、青海等地的排放水平较低。     

武汉市道路扬尘源排放清单及空间分布特征研究

参考AP-42方法的采样规范（USEPA,2011）,对武汉市13个城区的不同类型道路采集了137个扬尘样,并记录采样面积、车流情况、车道状况、地理位置、周围环境以及气象数据要素信息,得到了不同类型道路的积尘负荷,估算了其扬尘排放因子和排放量.结果表明：武汉总城区尘负荷由大到小顺序为支路 > 次干道 > 主干道 > 快速路,其中支路平均尘负荷为2.396 g/m²,快速路为0.852 g/m²,远城区平均尘负荷是主城区平均尘负荷的2倍左右.各类型道路不同粒径范围的道路交通扬尘排放因子大小顺序为支路 > 次干路 > 主干路 > 高速路,与尘负荷大小趋势一致.2016年道路交通扬尘源TSP的年排放量为156 931.4 t,PM₁₀的年排放量为39 868.7 t,PM_2.5的年排放量为11 574.8 t,其不确定性范围分别为-24.7%~31.4%、-31.3%~32.9%、-31.8%~30.5%.其中主干道扬尘排放量最大,其TSP、PM₁₀和PM_2.5的年排放量分别为64 447.1、16 372.9和4 753.4 t.     

基于WRF模式的京津冀地区地表大气CO2浓度的模拟研究

在“双碳”目标背景下,从国家层面到地方层面,区域、城市、行业企业都在制定和实施双碳目标行动计划。CO₂模拟因其客观性和高时空分辨率等优势,在城市碳排放研究中深受重视。本研究以京津冀地区为研究区域,采用Picarro仪器高精度观测的2019—2020年CO₂数据,利用WRF模式进行CO₂传输模拟,分析了CO₂浓度变化的季节特征,评估了模式在城区中心、城郊及背景3个观测站点的模拟效果,并对边界层高度及化石燃料碳排放等可能影响CO₂浓度的因素进行了研究。3个观测站点分别为北京中国科学院大气物理研究所325 m气象塔观测站(北京站)、河北香河观测站(香河站)和上甸子区域本底观测站(上甸子站)。模拟结果表明：上甸子站优于香河站,香河站优于北京站,在冬季尤其明显;CO₂浓度的高值区主要分布在城区、电厂和工业区,尤其是唐山、石家庄和邯郸地区,大量交通、工业排放导致CO₂浓度明显上升,且高值区的范围在冬季最大;就日平均变化和日变化而言,边界层高度与C...     

Trace elements in tropical African savanna biomass burning aerosols

As a part of the FOS/DECAFE experiment, aerosol particles emitted during prescribed savanna fires were collected in January 1991 at Lamto (Ivory Coast), either close to the emission or in ambient air. Analytical transmission electron microscopy pointed out the presence of sub-micrometer soots, salt condensates, vegetation relicts and soil derived particles. The samples were also analyzed for their total particulate matter (TPM) content and elemental composition by PIXE or XRF. At the emission, high concentrations of soil derived elements (Fe and Al) pointed out an intense remobilization process during the fires. Biomass burning emissions contributed to more than 90% of the measured concentrations, of P, Cl, S, K, Cu and Zn, which were found primarily in the fine fraction with the exception of P. Near the emission, K was mainly present as KCl, evolving to K₂SO₄ in the ambient samples. Trace elements emission factors were obtained for the first time for the African savanna burning and their annual emissions were estimated: our median K emission factor (0.78 g/kg of C) is higher than estimates for other ecosystems (0.2–0.58 g/kg of C); Zn emissions (0.008 Tg/year) account for 4 to 11% of the global anthropogenic emissions.     

一次引发华北和北京沙尘(暴)天气起沙机制的数值模拟研究

在对气象背景场进行诊断分析的基础上,集中对一次沙尘(暴)天气的起沙机制进行了数值模拟.具体做法是先将澳大利亚新南威尔士大学(UNSW)邵亚平博士发展的具有清晰物理概念的起沙数值模式(非参数化方案),与PSU/NCAR的中尺度气象预报模式MM5进行耦合.使用该模式系统,根据陆面状况和大气条件,定量模拟出沙尘(暴)起沙的过程.对2000年4月6～7日发生在华北和北京的一次沙尘暴过程的数值试验结果表明,该模式对沙尘天气的起沙过程有较好的模拟能力.     

Evaluation of the use of photochemical indicators to assess ozone—NOx—VOC sensitivity in the Southwestern Iberian Peninsula

Understanding the chemical links between ozone (O₃) and its two main precursors, nitrogen oxides (NOx) and volatile organic compounds (VOC), is important for designing effective photochemical smog reduction strategies. This chemical relationship will determine which precursor (NOx or VOC) emission reduction will be more effective for decreasing the ozone formation. Under certain conditions, ozone levels decrease as a result of a reduction in NOx emissions but do not respond significantly to changes in VOC emissions (NOx-sensitive condition), while under other conditions ozone concentrations decrease in response to reductions in VOCs and may even increase when NOx emissions are reduced (VOC-sensitive conditions). Indicator species can be used to assess the sensitivity of ozone to changes in the emissions of its precursors. These indicators are species or species ratios involved in ozone photochemistry which reflect the primary chemical process through which the ozone was formed. In this work we use the MM5-CAMx model system to explore the behaviour of various indicator species during two meteorological situations featuring different atmospheric conditions in a complex terrain area. The results show that indicators based on nitrogen compounds (i.e,. NOy and NOz) are suitable for defining the transition range from VOC- to NOx-sensitive chemistry, and that despite the uncertainties associated with the use of chemical indicators, the ratios O₃/NOy and O₃/NOz may provide a simple and useful way to summarize the response of ozone to changes in NOx and VOC emissions in Southwestern Spain.     

Competing impact of anthropogenic emissions and meteorology on the distribution of trace gases over Indian region

The spatial distribution of trace gases exhibit large spatial heterogeneity over the Indian region with an elevated pollution loading over densely populated Gangetic Plains (IGP). The contending role and importance of anthropogenic emissions and meteorology in deciding the trace gases level and distribution over Indian region, however, is poorly investigated. In this paper, we use an online regional chemistry transport model (WRF/Chem) to simulate the spatial distribution of trace gases over Indian region during one representative month of only three meteorological seasons namely winter, spring/summer and monsoon. The base simulation, using anthropogenic emissions from SEAC⁴RS inventory, is used to simulate the general meteorological conditions and the realistic spatial distribution of trace gases. A sensitivity simulation is conducted after removing the spatial heterogeneity in the anthropogenic emissions, i.e., with spatially uniform emissions to decouple the role of anthropogenic emissions and meteorology and their role in controlling the distribution of trace gases over India. The concentration levels of Ozone, CO, SO₂ and NO₂ were found to be lower over IGP when the emissions are uniform over India. A comparison of the base run with the sensitivity run highlights that meteorology plays a dominant role in controlling the spatial distribution of relatively longer-lived species like CO and secondary species like Ozone while short-lived species like NO_X and SO₂ are predominantly controlled by the spatial variability in anthropogenic emissions over the Indian region.     

Gas Chromatographic Determination of Extractable Compounds Composition and Emission Rate of Volatile Terpenes from Larch Needle Litter

A combination of solid-phase microextraction (SPME) and gas chromatography can be successfully used both for establishing the qualitative composition of volatile organic compounds (VOC) emitted by leaf litter and for determining their emission rates. Taking as an example European larch litter, it is shown that dead plant material contains considerable amounts of volatile components as well as non-volatile compounds that can be VOC precursors formed as a result of enzymatic reactions. It is proposed to include the determination of extractable compounds into the methodology of studying litter as a source of atmospheric VOC. Some data on litter mass are reported and it is concluded that this data may be included into special models for emission evaluation. In this work the distribution coefficients of monoterpene hydrocarbons between the gas phase and polydimethylsiloxane fiber coating necessary for quantitative determinations in SPME were estimated.     

Comparability of Biogenic VOC Emission Rate Measurements under Laboratory and Ambient Conditions at the Example of Monoterpene Emissions from Scots Pine (Pinus sylvestris)

Laboratory experiments under controlled environmental conditions are a useful tool to investigate the influence of different environmental parameters on VOC emissions from plants individually. Before using the obtained results to interpret measurements under ambient conditions, it has to be ensured that the laboratory system is suitable for performing emission rate measurements under ambient-like conditions to derive algorithms describing the emissions of volatile organic compounds as a function of physical variables like temperature and light intensity. Here we compare results from monoterpene emission rate measurements with Scots pines (Pinus sylvestris L.) under both ambient environmental conditions using a mobile plant enclosure chamber, and under controlled laboratory conditions in a continuously stirred tank reactor. The different analytical instruments to quantify monoterpene emissions were compared in an intercalibration experiment. Measurements of the mixing ratios of -pinene, -pinene, 3-carene, camphene, and limonene on the order of some hundred parts per trillion differed by less than 20%. The laboratory system has proven capable of providing ambient-like conditions and results of monoterpene emission rate measurements under laboratory conditions could be extrapolated to the natural environment. Monoterpene emission rate measurements with identical specimens of Scots pines conducted within small temporal differences under similar laboratory and outdoor conditions agreed well. Both laboratory and outdoor experiments clearly showed that distinct and constant values neither exist for the standard emission rates nor for the emission pattern of monoterpenes from Scots pine. Temporal variations in the standard emission rates from identical specimens and plant-to-plant variations were on the order of one magnitude.     

Emission of aliphatic amines from animal husbandry and their reactions: Potential source of N2O and HCN

We measured the emissions of volatile aliphatic amines and ammonia produced by the manure of beef cattle, dairy cows, swine, laying hens and horses in livestock buildings. The amine emissions consisted almost exclusively of the three methylamines and correlated with those of ammonia. The molar emission ratios of the methylamines to ammonia, and data on NH₃ emissions from animal husbandry in Europe, together with global statistics on domestic animals, were used to estimate the global emissions of amines. Annual global methylamine-N input to the atmosphere from animal husbandry in 1988 was 0.15±0.06 TgN (Tg=10¹² g). Almost 3/4 of these emissions consisted of trimethylamine-N. This represents about half of all methylamine emissions to the atmosphere. Other sources are marine coastal waters and biomass burning.Possible reaction pathways for atmospheric methylamines are shown. Among various speculative but possible products N₂O and HCN are of interest because the emission of methylamines could contribute to the global budgets of these compounds. Maximum atmospheric N₂O production from methylamines are below 0.4 Tg N/year, which is less than 10% of the annual N₂O growth rate. Although we do not expect the methylamine emissions to contribute in a major way to the atmospheric N₂O budget, more studies are needed to establish this conclusion beyond doubt. Similar conclusions hold for HCN.