基于空气质量模拟的江苏省大气污染物排放清单比较研究

大气污染物排放清单是空气质量模拟和空气污染治理的重要依据.本研究比较分析了两套覆盖江苏省的2017年大气污染物排放清单，即分别由上海市环境科学研究院、江苏省环境科学研究院编制的"长三角清单"和"江苏省清单"，并结合区域空气质量模型CMAQ评估不同清单对长三角地区2017年1、4、7、10月的空气质量模拟的影响.清单比较结果表明，除二氧化硫（SO₂）以外，江苏省清单估算的各污染物排放量较长三角清单低.通过与观测数据比较，发现两套清单对SO₂、氮氧化物（NO_x）、臭氧（O₃）和细颗粒物（PM_2.5）的模型模拟性能均较好.江苏省清单与长三角清单两者的模拟结果空间分布接近，其中江苏省清单模拟的PM_2.5和O₃在长三角多数地区略低于长三角清单的模拟结果（1月O₃除外）.江苏省清单与长三角清单均能够用于空气质量模式模拟，可为江苏地区的细颗粒物和光化学烟雾污染的控制策略制定提供参考.     

Analysis of summertime atmospheric transport of fine particulate matter in Northeast Asia

In Northeast Asia, the effect of long-range transport of air pollutants is generally pronounced in spring and winter, but can be important even in summer. This study analyzed summer-time atmospheric transport of elemental carbon (EC) and sulfate (SO₄ ^2?) with the Community Multiscale Air Quality (CMAQ) model driven by the Weather Research and Forecasting (WRF) model. The WRF/CMAQ modeling system was applied to regions ranging from Northeast Asia to the Greater Tokyo Area in Japan in summer 2007. In terms of EC, while the model simulated well the effect of long-range transport, the simulation results indicated that domestic emissions in Japan dominantly contributed (85%) to EC concentrations in the Greater Tokyo. In terms of SO₄ ^2?, the simulation results indicated that both domestic emissions (62%) and long-range transport from the other countries (38%) substantially contributed to SO₄ ^2? concentrations in the Greater Tokyo. Distinctive transport processes of SO₄ ^2? were associated with typical summer-time meteorological conditions in the study region. When a Pacific high-pressure system covered the main island of Japan, domestic emissions, including volcanic emission, dominantly contributed to SO₄ ^2? concentrations in the Greater Tokyo. When a high-pressure system prevailed over the East China Sea and low-pressure systems passed north of Japan, synoptic westerly winds associated with this pressure pattern transported a large amount of SO₄ ^2? from the continent to Japan. In addition, although heavy precipitation and strong wind decreased SO₄ ^2? concentrations near the center of a typhoon, peripheral typhoon winds occasionally played an important role in long-range transport of SO₄ ^2?.     

Impact of precursor levels and global warming on peak ozone concentration in the Pearl River Delta Region of China

The relationship between the emission of ozone precursors and the chemical production of tropospheric ozone(O3) in the Pearl River Delta Region(PRD) was studied using numerical simulation.The aim of this study was to examine the volatile organic compound(VOC)-or nitrogen oxide(NOx =NO+NO2)limited conditions at present and when surface temperature is increasing due to global warming,thus to make recommendations for future ozone abatement policies for the PRD region.The model used for this application is the U.S.Environmental Protection Agency’s(EPA’s) third-generation air-quality modeling system;it consists of the mesoscale meteorological model MM5 and the chemical transport model named Community Multi-scale Air Quality(CMAQ).A series of sensitivity tests were conducted to assess the influence of VOC and NOx variations on ozone production.Tropical cyclone was shown to be one of the important synoptic weather patterns leading to ozone pollution.The simulations were based on a tropicalcyclone-related episode that occurred during 14-16 September 2004.The results show that,in the future,the control strategy for emissions should be tightened.To reduce the current level of ozone to meet the Hong Kong Environmental Protection Department(EPD) air-quality objective(hourly average of 120 ppb),emphasis should be put on restricting the increase of NOx emissions.Furthermore,for a wide range of possible changes in precursor emissions,temperature increase will increase the ozone peak in the PRD region;the areas affected by photochemical smog are growing wider,but the locations of the ozone plume are rather invariant.     

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。     

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。     

Accounting for CO<Subscript>2</Subscript> variability over East Asia with a regional joint inversion system and its preliminary evaluation

A regional surface carbon dioxide (CO₂) flux inversion system, the Tan-Tracker-Region, was developed by incorporating an assimilation scheme into the Community Multiscale Air Quality (CMAQ) regional chemical transport model to resolve fine-scale CO₂ variability over East Asia. The proper orthogonal decomposition-based ensemble four-dimensional variational data assimilation approach (POD-4DVar) is the core algorithm for the joint assimilation framework, and simultaneous assimilations of CO₂ concentrations and surface CO₂ fluxes are applied to help reduce the uncertainty in initial CO₂ concentrations. A persistence dynamical model was developed to describe the evolution of the surface CO₂ fluxes and help avoid the “signal-to-noise” problem; thus, CO₂ fluxes could be estimated as a whole at the model grid scale, with better use of observation information. The performance of the regional inversion system was evaluated through a group of single-observation-based observing system simulation experiments (OSSEs). The results of the experiments suggest that a reliable performance of Tan-Tracker-Region is dependent on certain assimilation parameter choices, for example, an optimized window length of approximately 3 h, an ensemble size of approximately 100, and a covariance localization radius of approximately 320 km. This is probably due to the strong diurnal variation and spatial heterogeneity in the fine-scale CMAQ simulation, which could affect the performance of the regional inversion system. In addition, because all observations can be artificially obtained in OSSEs, the performance of Tan-Tracker-Region was further evaluated through different densities of the artificial observation network in different CO₂ flux situations. The results indicate that more observation sites would be useful to systematically improve the estimation of CO₂ concentration and flux in large areas over the model domain. The work presented here forms a foundation for future research in which a thorough estimation of CO₂ flux variability over East Asia could be performed with the regional inversion system.     

Tropospheric NO2 Columns over Northeastern North America： Comparison of CMAQ Model Simulations with GOME Satellite Measurements

We present comparisons of the NO2 regional Chemical Transport Model （CTM） simulations over North-eastern North America during the time period from May to September, 1998 with hourly surface NO2 observations and the NO2 columns retrieved from the GOME （Global Ozone Monitoring Experiment） satellite instrument. The model calculations were performed using the Mesoscale Meteorological Model 5 （MM5）, Sparse Matrix Operator Kernal Emissions （SMOKE）, and Community Multiscale Air Quality （CMAQ） modeling systems, using the emission data from the National Emissions Inventory （NEI） databases of 1996 （U.S.） and 1995 （Canada）. The major objectives were to assess the performance of the CMAQ model and the accuracy of the emissions inventories as they affected the simulations of this important short-lived atmospheric species. The modeled （NcMAQ） and measured （NGOME） NO2 column amounts, as well as their temporal variations, agreed reasonably well. The absolute differences （NcMAQ-NGOME） across the domain were between ±3.0×10^15 molecules cm^-2, but they were less than ±1.0×10^15 molecules cm^-2 over the majority （80%） of the domain studied. The overall correlation coefficient between the measurements and the simulations was 0.75. The differences were mainly ascribed to a combination of inaccurate emission data for the CTM and the uncertainties in the GOME retrievals. Of these, the former were the more easily identifiable.     

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...     

基于极端随机树方法的WRF-CMAQ-MOS模型研究

随着城市化、工业化的快速发展,空气污染已经成为了公众最关注的问题之一。为了提高空气质量预报的准确度,以多尺度空气质量模型（Community Multi-Scale Air Quality,CMAQ）为工具,结合中尺度WRF（Weather Research and Forecast Model）气象预报数据、气象观测数据、污染物浓度观测数据,基于极端随机树方法建立了WRF-CMAQ-MOS（Weather Research and Forecast Model-Community Multi-Scale Air Quality-Model Output Statistics）统计修正模型。结果表明,结合WRF气象预报的CMAQ-MOS方法明显修正了由于模型非客观性产生的模式预报偏差,提高了预报效果。使用线性回归方法不能获得较好的优化效果,选取极端随机树方法和梯度提升回归树方法对模型进行改进和比较,发现极端随机树方法对结合WRF气象要素的CMAQ-MOS模型有较大的提升。针对徐州地区空气质量预报,进一步使用基于极端随机树方法的WRF-CMAQ-MOS模型对2016年1、2、3月的空气质量指数（AQI）及PM_2.5、PM₁₀、NO₂、SO₂、O₃、CO六种污染物优化试验进行验证,发现优化效果最为明显的两种污染物分别是NO₂及O₃,2016年1、2、3月整体相关系数NO₂由0.35升至0.63,O₃由0.39升至0.79,均方根误差NO₂由0.0346减至0.0243 mg/m3,O₃由0.0447减至0.0367 mg/m3。文中发展的WRF-CMAQ-MOS统计修正模型可以有效提升预报精度,在空气质量预报中具有很好的应用前景。      

蒙特卡罗不确定性分析在O3模拟中的初步应用

利用蒙特卡罗不确定性分析方法,分析了嵌套网格空气质量模式系统(NAQPMS/IAP)中154个模式输入变量不确定性对臭氧模拟的影响,量化了模式在北京奥运会期间臭氧模拟的不确定性,并确定出了主要不确定性因子。结果表明:(1)在奥运会期间(2008年8月8日～2008年8月24日),北京城区臭氧模拟的平均不确定性为19ppb,不确定性存在明显的日变化特征,白天不确定性大,夜间不确定性小。(2)在白天,北京城区近地层臭氧模拟最重要的不确定性来源是局地前体物排放,其次是NO2光解系数、风向、北京周边前体物排放和垂直扩散系数。另外,地面约150m以上,对臭氧模拟影响最大的不确定性因子是风向和北京周边前体物排放;夜间,北京城区近地层臭氧模拟的最大不确定性来源是局地NOx排放和垂直扩散系数。     

Application of satellite data in a regional model to improve long-term ozone simulations

To investigate an alternative technique of providing background and transboundary transport inputs for ozone (O₃) simulations on a regional scale, the EPA’s Community Multi-scale Air Quality (CMAQ) model was integrated with high spectral resolution data from the Tropospheric Emission Spectrometer (TES) aboard the NASA’s Aura satellite. This study presents a comprehensive model evaluation of O₃ for the entire year of 2009 over the contiguous United States with a focus on the State of Texas using both ozonesonde and ground measurements. While improving model performance in the upper atmosphere, CMAQ’s initial and boundary conditions (IC/BC) derived from the original TES data do not improve model performance in the troposphere because the satellite data exaggerated concentration of tropospheric O₃. With a 10-ppb deduction of O₃ concentration from TES, the IC/BC derived from the adjusted TES improves model performance from ground level through the upper atmosphere. The mean bias of daily maximum 8-h average concentration of O₃ (MDA8) from the ground monitored in Texas decreased from 7 ppb to 4 ppb. Model results also show small influences of O₃ from the upper troposphere on the concentrations at the ground level. With a complete exclusion of stratospheric layers, changes of annual mean MDA8 of O₃ concentrations at ground-level were smaller than 1.1 % in Dallas and Houston. In addition, limitations of satellite data are discussed and recommendations are provided regarding the future application of satellite data in regional O₃ simulations.     

复杂地形上气象场对空气质量数值模拟 结果影响的研究

利用WRF模式三种边界层参数化方案(YSU、MYJ、ACM2)产生的气象场分别驱动多尺度空气质量模式CMAQ,对兰州市西固区冬季2005年1月27日至2月2日期间SO₂和NO₂浓度进行了数值模拟,将模拟结果与同期监测的污染物浓度进行对比分析,结果表明:WRF模式不同边界层参数化方案模拟输出的气象场驱动CMAQ模式所模拟的SO₂和NO₂浓度均可以反映出污染物的时空变化特征,CMAQ模式具有模拟复杂下垫面高分辨率污染物输送特征的能力;WRF模式的边界层参数化方案选为局地与非局地闭合方案(ACM2)时,模拟的气象场驱动CMAQ模式得到的空气污染物浓度分布特征最优,这主要是由于ACM2的湍流输送机制较为合理,模拟的边界层低层气象场更接近实际,从而可以较好地模拟污染物的输送特征;当CMAQ模式的垂直混合方案与WRF模式的湍流输送方案一致时(均采用ACM2方案),模式间的兼容性好.     

污染源反演对重点城市群夏季O3模拟的改进效果评估

在嵌套网格空气质量预报模式系统(NAQPMS)的基础上,采用污染源反演方法优化以中国多尺度排放清单(MEIC)为主的先验排放清单中臭氧(O₃)前体物排放量估计。分析时段为2019年6～8月,重点评估了污染源反演对我国“2+26”城市、长三角、珠三角、成渝4个重点城市群O₃模拟的改进效果。评估结果表明,污染源反演获得的“2+26”城市、长三角、珠三角的氮氧化物(NO_x)排放速率整体低于先验清单的排放速率约0.6μg m_-2 s_-1,但反演的挥发性有机物(VOCs)排放速率在“2+26”城市整体上高于先验清单的排放速率约0.5μg m_-2 s_-1。利用反演的NO_x和VOCs排放量和NAQPMS模式对4个城市群O₃进行模拟,发现反演排放数据可以显著改进夏季O₃模拟性能,使得O₃日最大8小时平均值(MDA8-O₃)模拟的均方根误差(R...     

A Retrospective Analysis of Ozone Formation in the Lower Fraser Valley,British Columbia,Canada. Part II: Influence of Emissions Reductions on Ozone Formation

A mechanistic exploration of how ozone formation in the Lower Fraser Valley (LFV) has changed over a 20-year (1985–2005) retrospective period was performed using numerical models, observations, and emissions data from four key episodes selected from the 20-year period. The motivation for this study was the observed differences in trends in summertime episodic ozone concentrations recorded at various monitoring stations within the valley; stations in the western part of the valley have generally shown a noticeable reduction in episodic ozone concentrations whereas stations in the eastern part of the valley have shown little or no improvement in their maximum 8-hour averaged ozone concentrations. Concurrent with these air quality changes, there has been a well-documented reduction in ozone precursor emissions along with an observed shift in the population patterns within the valley over the 20-year period. Ozone formation for four episodes, encompassing the different meteorological regimes that occur during LFV ozone events and spanning the retrospective period, were investigated using the Weather Research and Forecasting (WRF)-Sparse Matrix Operator Kernel Emission (SMOKE)-Community Multiscale Air Quality (CMAQ) modelling system. For each episode, two simulations, intended to isolate the effects of emission changes from meteorological changes, were performed: one with emissions set at the 1985 level and the other with emissions set at the 2005 level. Based on analysis of the model output, observational data, and precursor emission inventories, we find that the Port Moody station in the western LFV remains a volatile organic compound (VOC)-sensitive location; the central part of the LFV around the town of Chilliwack has generally changed from being VOC-limited to being NO_x-limited; the easternmost part of the valley around the town of Hope has been and remains NO_x-limited. Furthermore, based on the observational data and numerical model output, ozone production efficiency as a function of NO has increased noticeably at Chilliwack and likely in the other eastern parts of the valley. This efficiency increase has likely offset some of the benefits resulting from local NO_x emission reductions.

RÉSUMÉ?[Traduit par la rédaction] Nous avons effectué une exploration mécaniste de la façon dont la formation de l'ozone dans la vallée du bas Fraser (VBF) a changé au cours d'une période rétrospective de 20 ans (1985–2005) en nous servant de modèles numériques, d'observations et de données sur les émissions pour quatre épisodes clés choisis dans la période de 20 ans. Ce sont les différences observées entre les tendances dans les concentrations épisodiques d'ozone enregistrées à certaines stations de surveillance dans la vallée qui ont motivé cette étude : les stations dans la partie ouest de la vallée ont généralement affiché une réduction notable des concentrations épisodiques d'ozone alors que les stations dans la partie est de la vallée n'ont montré que peu ou pas d'amélioration dans les valeurs maximales des concentrations moyennes d'ozone sur 8 heures. Concurremment avec ces changements dans la qualité de l'air, il s'est produit une réduction bien documentée dans les émissions de précurseurs de l'ozone en même temps qu'un déplacement observé dans les configurations de population dans la vallée au cours de la période de 20 ans. Nous avons étudié la formation d'ozone au cours de quatre épisodes, englobant les différents régimes météorologiques survenus lors des événements d'ozone dans la VBF et couvrant la période rétrospective, à l'aide du système de modélisation SMOKE (Sparse Matrix Operator Kernel Emissions) – CMAQ (Community Multiscale Air Quality) du WRF (Weather Research and Forecasting). Pour chaque épisode, nous avons effectué deux simulations visant à isoler l'effet des changements dans les émissions de l'effet des changements météorologiques, l'une avec les émissions réglées au niveau de 1985 et l'autre avec les émissions réglées au niveau de 2005. En nous basant sur l'analyse de la sortie du modèle, les données d'observation et les inventaires des émissions de précurseurs, nous trouvons que la stations de Port Moody dans l'ouest de la VBF demeure un endroit sensible aux composés organiques volatiles (COV); la partie centrale de la VBF, autour de la ville de Chilliwack, a généralement changé de « limitée par les COV » à « limitée par les NO_x »; la partie la plus à l'est de la vallée, autour de la ville de Hope, était et est restée « limitée par les NO_x ». De plus, d'après les données d'observation et la sortie du modèle numérique, l'efficacité de la production d'ozone en fonction de NO a notablement augmenté à Chilliwack et vraisemblablement dans les autres parties de l'est de la vallée. Cette augmentation d'efficacité a probablement annulé certains gains provenant des réductions dans les émissions locales de NO_x.     

Impacts of Seasonal Fossil and Ocean Emissions on the Seasonal Cycle of Atmospheric CO2

The seasonal cycle of atmospheric CO2 at surface observation stations in the northern hemisphere is driven primarily by net ecosystem production (NEP) fluxes from terrestrial ecosystems. In addition to NEP from terrestrial ecosystems, surface fluxes from fossil fuel combustion and ocean exchange also contribute to the seasonal cycle of atmospheric CO2. Here the authors use the Goddard Earth Observing System-Chemistry (GEOS-Chem) model (version 8-02-01), with modifications, to assess the impact of these fluxes on the seasonal cycle of atmospheric CO2 in 2005. Modifications include monthly fossil and ocean emission inventories. CO2 simulations with monthly varying and annual emission inventories were carried out separately. The sources and sinks of monthly averaged net surface flux are different from those of annual emission inventories for every month. Results indicate that changes in monthly averaged net surface flux have a greater impact on the average concentration of atmospheric CO2 in the northern hemisphere than on the average concentration for latitudes 30-90°S in July. The concentration values differ little between both emission inventories over the latitudinal range from the equator to 30°S in January and July. The accumulated impacts of the monthly averaged fossil and ocean emissions contribute to an increase of the total global monthly average of CO2 from May to December.An apparent discrepancy for global average CO2 concentration between model results and observation was because the observation stations were not sufficiently representative. More accurate values for monthly varying net surface flux will be necessary in future to run the CO2 simulation.     

气象预报模式参数化方案对重污染过程PM2.5浓度预报效果的影响

针对北京市2016年12月16～21日的重污染过程,基于嵌套网格空气质量模式预报系统(NAQPMS),面向气象驱动模式WRF中7类物理过程的参数化方案,通过单扰动和组合扰动方式构建了51组不同的WRF模式运行配置,对比分析不同方案配置下NAQPMS对这次重污染过程细颗粒物(PM2.5)浓度预报的性能.结果表明:在重污染...     

非结构网格空气质量模式对东亚强沙尘暴的初步模拟研究

基于中国科学院大气物理研究所自主研发的嵌套网格空气质量数值预报模式(NAQPMS)和英国帝国理工学院应用计算与建模小组(AMCG)研制的有限元流体模式(Fluidity),构建了非结构网格沙尘传输模式(Fluidity-Dust),并模拟再现了2010年3月19~22日东亚强沙尘暴整个暴发、演变的三维立体动态过程,从整体上对这次沙尘事件有了全新的直观认识和了解。通过利用FY-2D卫星沙尘反演资料及MODIS(Moderate Resolution Imaging Spectroradiometer)卫星反演的气溶胶光学厚度(AOD)资料,可对模拟结果进行整体上对比验证;同时,利用中国9个城市站点的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)地面观测资料以及日本多个站点的激光雷达资料,逐一对比分析了不同地区PM10的时空分布以及沙尘传输经过时的垂直分布情况;并与NAQPMS模式的沙尘模拟结果进行了模式间的对比分析。对比结果均表明:该模式具有较好的模拟能力,能很好地模拟再现整个沙尘暴过程,为今后进一步运用自适应变网格技术以实现对沙尘暴的高精度追踪模拟奠定了基础。不同模式比较是量化模拟不确定性的重要方法。以往沙尘输送模式比较研究表明:起沙量模拟的不确定性是沙尘暴数值模拟的最大不确定来源。本文通过两个具有相同起沙方案的模式对同一沙尘事件的模拟,发现不同的平流方案以及不同的沉降计算也会对沙尘过程模拟产生重要影响。     

基于CMAQ-MCM模型的长三角地区夏季臭氧和大气氧化性影响的研究

传统的空气质量模型多使用简化的光化学反应机制来模拟大气污染物的形成.这些机制主要基于烟雾箱实验拟合的反应速率和产物来模拟二次产物（如臭氧（O₃））前体物的氧化反应,具有一定的不确定性,导致模拟结果产生偏差.针对该问题,本研究将详细的大气化学机理（MCMv3.3.1）与美国国家环境保护局研制的第三代空气质量预报和评估系统CMAQ相结合（CMAQ-MCM）,模拟研究长三角地区2015年8月27—9月5日臭氧高发时段的空气质量.CMAQ-MCM模型可以较好地模拟长三角地区6个代表城市O₃和其前体物随时间的变化趋势.对模拟的O₃日最大8 h平均浓度的统计分析表明,徐州表现最好（标准平均误差=-0.15,标准平均偏差=0.23）.在长三角地区,居民源对挥发性有机物（VOCs）的贡献最大,占39.08%,其次是交通运输（33.25%）和工业（25.56%）.能源对总VOCs的贡献最小,约为2.11%.对活性氧化氮（NO_y）的分析表明,其主要组分是NO_x（80%）,其次是硝酸（HNO₃）（<10%）.O₃的空间分布与NO_y和NO_x非常相似.HCHO等其他氧化产物的分布与NO_x相似,这很可能是由于在高NO_x条件下VOCs氧化产生的产物.甲基乙烯基酮（MVK）和甲基丙烯醛（MACR）的空间分布与自然源VOCs （BVOCs）非常相似,表明长三角地区MVK和MACR主要由BVOCs氧化生成.长三角地区受到人为源和自然源排放相互作用的影响.     

Accounting for CO_2 Variability over East Asia with a Regional Joint Inversion System and Its Preliminary Evaluation

A regional surface carbon dioxide(CO_2) flux inversion system, the Tan-Tracker-Region, was developed by incorporating an assimilation scheme into the Community Multiscale Air Quality(CMAQ) regional chemical transport model to resolve fine-scale CO_2 variability over East Asia. The proper orthogonal decomposition-based ensemble four-dimensional variational data assimilation approach(POD-4 DVar) is the core algorithm for the joint assimilation framework, and simultaneous assimilations of CO_2 concentrations and surface CO_2 fluxes are applied to help reduce the uncertainty in initial CO_2 concentrations. A persistence dynamical model was developed to describe the evolution of the surface CO_2 fluxes and help avoid the "signal-to-noise" problem; thus, CO_2 fluxes could be estimated as a whole at the model grid scale, with better use of observation information. The performance of the regional inversion system was evaluated through a group of single-observation-based observing system simulation experiments(OSSEs). The results of the experiments suggest that a reliable performance of Tan-Tracker-Region is dependent on certain assimilation parameter choices, for example, an optimized window length of approximately 3 h, an ensemble size of approximately 100, and a covariance localization radius of approximately 320 km. This is probably due to the strong diurnal variation and spatial heterogeneity in the fine-scale CMAQ simulation, which could affect the performance of the regional inversion system. In addition, because all observations can be artificially obtained in OSSEs, the performance of Tan-Tracker-Region was further evaluated through different densities of the artificial observation network in different CO_2 flux situations. The results indicate that more observation sites would be useful to systematically improve the estimation of CO_2 concentration and flux in large areas over the model domain. The work presented here forms a foundation for future research in which a thorough estimation of CO_2 flux variability over East Asia could be performed with the regional inversion system.     

A Three-Dimensional Simulation of HO x Concentrations Over East Asia During TRACE-P

The Models-3 Community Multi-scale Air Quality modeling system (CMAQ) coupled with the Regional Atmospheric Modeling System (RAMS) is used to simulate three-dimensional concentration distributions of hydroxyl (OH) and hydroperoxyl (HO₂) radicals over the western Pacific Ocean during the NASA Transport and Chemical Evolution over the Pacific (TRACE-P) field campaign. Modeled values of OH and HO₂ and their closely related chemical species and photolysis rates are compared with observational data collected onboard the DC-8 aircraft. Comparison shows that the model reasonably reproduced these observed values over a broad range of conditions with an overall tendency to overestimate the measured OH and HO₂ by a factor of 1.56 and 1.24, respectively. A case study of OH, HO₂ and their closely related chemical species and photolysis rates along the DC-8 flights 11 and 12 conducted on 17–18 March 2001 shows that the model reproduces the temporal and spatial variations reasonable well, and produces more reliable OH and HO₂ concentrations in the polluted environment than in the clean marine boundary layer.