武汉市2018年4—9月臭氧及其前体物非线性关系研究

近年来武汉市臭氧污染日益严峻,成为影响空气质量达标的瓶颈,弄清臭氧及其前体物非线性关系是臭氧防控的关键和基础.本研究基于武汉中心城区2018年4—9月臭氧及其前体物在线观测数据,分析出武汉市臭氧浓度受前体物和气象条件等因素的共同影响,呈较为明显的季节变化和日变化特征.观测期间武汉市大气挥发性有机物（VOCs）平均体积分数为32.5×10^-9,烷烃是武汉市VOCs的主要组分,其次是含氧VOCs （OVOCs）和卤代烃.利用基于观测的模型定量分析臭氧与前体物之间的关系,发现削减VOCs会引起臭氧生成潜势的显著下降,而削减氮氧化物则会使臭氧生成潜势升高,说明武汉市臭氧生成处于VOCs控制区.在人为源VOCs中,间/对二甲苯和邻二甲苯的相对增量反应活性（RIR）最高,是影响臭氧生成的关键组分.     

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。     

不同时间尺度下汾渭平原臭氧浓度变化及气象环境影响

汾渭平原作为中国大气环境治理的第三大重点区域,由挥发性有机物和氮氧化物等前体物排放增加导致光化学反应加剧进而引发的近地面臭氧(O_3)污染已成为迫切需要面对的关键问题。本文基于汾渭平原11个重点城市2015-2019年近地面大气O_3及前体物观测数据结合同期气象监测资料,总结归纳其时空变化特征,利用Global Moran's I和Getis-Ord Gi*指数方法分析空间集聚效应和冷热点区域,运用KZ(Kolmogorov-Zurbenko)滤波方法揭示了不同时间尺度的排放和气象环境对O_3浓度变化的影响。结果表明:近5年汾渭平原O_3污染以轻度为主,超标率逐年增加且夏季最高春季次之,其中6月超标37%以上,前体物中NO_2年际差异不大CO浓度逐年减少。空间分布上,O_3空间集聚特征逐年增强,高浓度聚集区分布在临汾、运城、三门峡和洛阳的三角区域。从气象环境的影响看,O_3浓度主要受到前体物排放及气象条件的季节分量和短期分量影响,贡献率分别达到40%和24%。原始序列及各分量除与气压成负相关外,与气温和日照均呈显著正相关且对不同区域影响较为一致,而相对湿度和风速对各分量的影响具有显著的区域性差异。     

人类活动对气候影响的研究Ⅰ.温室气体和气溶胶

近5年来中国在温室气体源和汇,碳循环,气溶胶以及对流层臭氧等方面都进行了大量的研究.作者着重介绍农田温室气体排放,碳循环模式,亚洲沙尘气溶胶,对流层臭氧前体物的来源以及大气有机化合物的浓度观测等方面的主要研究成果,特别是关于稻田甲烷排放和沙尘气溶胶的物理化学特性方面的研究成果.     

中国东部地区典型臭氧污染过程防控敏感性及减排情景研究

近年来,我国东部地区夏季臭氧污染问题日渐凸显,成为影响空气质量、环境改善的重要因素之一,为量化评估臭氧前体物减排对臭氧污染的影响,本文以2021年6月19—30日中国东部地区臭氧污染过程为例,应用空气质量模型CMAQ-DDM方法与卫星遥感反演算法分析了东部地区臭氧浓度对人为源前体物排放敏感性的响应程度,并对臭氧前体物设置不同削减比例开展减排情景模拟,结果表明:1)2021年6月19—30日中国东部出现了一次长时间区域性臭氧污染过程,大部分城市达轻度至中度污染水平;2)整个污染时段东部地区主要以VOCs(Volatile Organic Compounds,挥发性有机物)控制区或VOCs与NO_x协同控制区为主,模型模拟与卫星反演结果具有较好的一致性,污染过程前段(19—25日)东部地区对VOCs敏感性较高,污染后段(26—30日)大部分地区转为VOCs和NO_x协同控制区,特别是河南、安徽、江苏部分地区,对NO_x敏感性提高较为显著;3)在相同减排比例条件下(VOCs∶NO_x=2∶1),减排幅度越大,臭氧降幅越大,当VOCs削减比例由20％提高到40％时,臭氧浓度降幅由1.7％增大至3.6％;由VOCs和NO_x协同减排(2∶1)过渡为强化NO_x减排(1∶1)的分阶段控制优于单一的减排控制方案,臭氧改善率平均增强0.1％;仅削减高架源NO_x对臭氧降幅不显著。     

当前对流层臭氧数值模式研究中的若干问题

对当前对流层臭氧(O3)数值模式研究中存在的若干问题以及需要重点研究的方向进行了评述,内容包括O3前体物的生态源及其模拟、对流层化学机制、大气化学研究中的气象模式以及大气化学模式与气象模式的相容性等.     

2017年8—9月湖州市臭氧污染特征及其生成机制研究

近年来近地面臭氧问题日益凸显,成为影响空气质量持续改善的瓶颈.本研究基于2017年8—9月在湖州市城区开展的为期1个月的臭氧及其前体物挥发性有机物（VOCs）和氮氧化物（NO_x）在线观测数据,分析了臭氧及其前体物污染特征,利用正矩阵因子分析（PMF）解析了VOCs来源,并采用基于观测的模型（OBM）对臭氧生成机制进行研究.研究结果表明：1）观测期间湖州市VOCs平均体积分数为（24.78±9.10）×10^-9,其中占比最高的组成为烷烃、含氧VOCs （OVOCs）和卤代烃;2）在臭氧非超标时段,湖州市臭氧生成处于VOCs控制区,而在臭氧重污染期间湖州市处于以VOCs控制为主的过渡区;3）在臭氧超标时段,对臭氧生成潜势（OFP）贡献最大的是芳香烃（39.6%）,其次是烯烃（21.5%）和OVOCs （19.4%）,排名前三的关键组分为甲苯、乙烯和间/对二甲苯;4）源解析结果显示观测期间湖州市VOCs的主要来源是溶剂使用（27.0%）、交通排放（22.7%）、背景+传输（19.3%）、工业排放（16.9%）、汽油挥发（7.7%）和植物排放（6.4%）,重污染过程期间对OFP贡献最大的两类源是交通排放源和溶剂使用源,贡献百分比分别为35.1%和30.5%.因此,对交通排放和溶剂使用方面进行控制管理对湖州市大气臭氧污染防控有重要意义.     

城市交通废气与低层大气臭氧形成和分布的数值模拟

建立了一个三维的边界层光化学模式，气象过程的模拟舍弃了静力近似的假定，模式由细网格、高分辨率并取湍流能量（E－ε）闭合的气象模式，提供较为细致的气流场和湍流场。文章中以汽车尾气和植物排放为光化学反应前体物的源，模拟了不同季节南京市的光化学过程以及臭氧随时间和空间的分布。结果表明，夏季南京市的地面臭氧浓度远远高于冬季，臭氧分布有所不同。并且在不少地方出现较高的O3浓度值，超过国家二级标准，气流对污染物浓度分布的影响在较高的高度上显得尤其明显。     

解析北京郊区一次典型臭氧污染的物理化学过程

臭氧污染是我国当前面临的重要大气环境问题,其不仅取决于大气化学反应过程,而且会受大气物理过程和各气象要素的影响,因此需要从化学和物理两个方向来研究近地面臭氧污染问题。本研究结合外场观测和欧拉光化学模式,解析了2022年秋季北京怀柔城区的一次光化学污染周期内的物理和化学过程。给出了温度、湿度和风速等气象因子,以及臭氧及其前体物挥发性有机物(VOCs)和氮氧化物(NO_x,x=1、2)在此期间的日变化特征。通过源解析得到VOCs主要来源为交通排放(46%)、植物源(25%)、溶剂挥发(23%)和燃烧源(9%)。通过欧拉光化学模式确定了区域传输和本地VOCs对臭氧的贡献,结果显示强北风天气条件下,怀柔区臭氧以外来水平输送为主(贡献超过70%);当以弱的南风或东南风为主时,天气处于稳定状态,臭氧主要来自VOCs和NO_x的二次转化。根据VOCs的臭氧潜势,在所有VOCs中对臭氧贡献最大的物质为烯烃,其贡献为67%,其次为芳香烃(16%)。通过敏感度分析,发现臭氧生成对物理因子中的光强、温度和边界层高度最敏感;在臭氧前体物中,活性较强的烯烃类物质的敏感度最...     

临安秋季近地层臭氧的形成及其前体物特征

应用浙江临安1999年秋季观测数据,分析了臭氧及其前体物特征与气象条件的关系。结果表明,该地区臭氧前体物丰富,在合适的天气条件、充足的日照下可以生成高浓度的臭氧;CO、NOx*等一次污染物浓度与大尺度大气扩散稀释能力有关;观测期间临安CO浓度很高;NMHCs以芳香烃含量最高,烷烃、烯烃、炔烃次之,生物排放的烃最少。以观测为基础的光化学模式计算表明,临安光化学臭氧生成率比损失率大一个数量级,中午净臭氧生成率最大可达14.8×10-9h-1。     

Global air quality change during the COVID-19 pandemic: Regionally different ozone pollution responses COVID-19: 疫情期间全球空气质量变化:臭氧响应的区域间差异

The explosive spread of the 2019 novel coronavirus (COVID-19) provides a unique chance to rethink the relationship between human activity and air pollution. Though related studies have revealed substantial reductions in primary emissions, obvious differences do exist in the responses of secondary pollutants, like ozone (O₃) pollution. However, the regional disparities of O₃ responses and their causes have still not been fully investigated. To better elucidate the interrelationship between anthropogenic emissions, chemical production, and meteorological conditions, O₃ responses caused by lockdowns over different regions were comprehensively explored at a global scale. Observational signals of air-quality change were derived from multi-year surface measurements and satellite retrievals. With similar substantial drops in nitrogen dioxide (NO₂), ozone shows rising signals in most areas of both East Asia and Europe, even up to ∼14 ppb, while a non-negligible declining signal exists in North America, by about 2–4 ppb. Furthermore, the drivers behind the different O₃ responses are discussed based on meteorological analysis and O₃ sensitivity diagnosis. On the one hand, O₃ responses to NO₂ declines can be affected by the primary dependence on its precursors. On the other hand, it is also highly dependent on meteorological factors, especially temperature. Our study further highlights the great importance of taking into consideration both the regional disparities and synergistic effects of precursor reductions and meteorological influence for scientific mitigation of O₃ pollution.摘要疫情期间全球各地一次排放大幅削减, 而臭氧等二次污染的响应则存在着区域间差异.结合地面和卫星观测发现, 同在氮氧化物大幅下降的情况下,臭氧在东亚和欧洲呈现出可达14ppb的上升信号, 而北美则下降为主 (约2–4ppb) .我们结合气象分析和臭氧敏感性进一步讨论了臭氧响应差异性的原因, 一方面受臭氧与前体物间关系的影响;另一方面来自于气象, 尤其是温度.研究明晰了人为排放,化学和气象三者的内在关联, 强调了在臭氧控制过程中考虑前体物削减和气象条件协同的重要性.     

鼎湖山森林地区臭氧及其前体物的变化特征和分析

通过对鼎湖山森林地区近地面O3和NOx浓度、太阳辐射、气象参数等为期一年的观测和资料分析,给出了地面O3和NOx浓度、太阳辐射的变化规律及其相互之间的关系.地面O3、NOx、CO、SO2浓度以及紫外辐射、太阳总辐射等有明显的日变化和季节变化.不同因子对O3的敏感性试验结果表明,晴天和实际天气,O3浓度对NO、NO2浓度的变化最为敏感,其次是水汽、气溶胶,最后是紫外辐射.所有因子的变化均引起O3在湿季比干季更大的变化率,因此在研究臭氧化学和光化学时,应该考虑水汽以及OH自由基的重要作用.对于晴天和实际天气的逐时值和日平均值而言,O3浓度与NO2/NO之间存在很好的正相关关系,比值NO2/NO可以作为判断O3峰值出现的一个指标.O3极值的出现既受NO和NOx影响,也受气象因素(温湿度、云、风、雾、降雨)和辐射的影响.周末O3、NOx浓度及NO2/NO有规律的增大,表明实验地点的大气受到人为污染源的影响.     

Changes in air pollutants during the COVID-19 lockdown in Beijing:Insights from a machine-learning technique and implications for future control policy

基于2015-2020年北京35个环境空气站和20个气象站观测资料,应用机器学习方法(随机森林算法)分离了气象条件和源排放对大气污染物浓度的影响.结果发现,为应对疫情采取的隔离措施使北京2020年春节期间大气污染物浓度降低了35.1％-51.8％;其中,背景站氮氧化物和一氧化碳浓度的降幅最大,超过了以往报道较多的交通站点.同时,2020年春节期间的气象条件不利于污染物扩散,导致多次霾污染事件发生.为进一步改善北京空气质量,未来需要优化减排策略.     

Climate change, ambient ozone, and health in 50 US cities

We investigated how climate change could affect ambient ozone concentrations and the subsequent human health impacts. Hourly concentrations were estimated for 50 eastern US cities for five representative summers each in the 1990s and 2050s, reflecting current and projected future climates, respectively. Estimates of future concentrations were based on the IPCC A2 scenario using global climate, regional climate, and regional air quality models. This work does not explore the effects of future changes in anthropogenic emissions, but isolates the impact of altered climate on ozone and health. The cities’ ozone levels are estimated to increase under predicted future climatic conditions, with the largest increases in cities with present-day high pollution. On average across the 50 cities, the summertime daily 1-h maximum increased 4.8 ppb, with the largest increase at 9.6 ppb. The average number of days/summer exceeding the 8-h regulatory standard increased 68%. Elevated ozone levels correspond to approximately a 0.11% to 0.27% increase in daily total mortality. While actual future ozone concentrations depend on climate and other influences such as changes in emissions of anthropogenic precursors, the results presented here indicate that with other factors constant, climate change could detrimentally affect air quality and thereby harm human health.     

人为和生物排放量对春季东亚地面臭氧的协同贡献

臭氧O3的生成是多因子影响的复杂非线性过程, 一个因子在其他因子起作用时的贡献可以分为纯贡献与协同贡献。本文采用因子分离方法和改进后的区域空气质量模式 (RAQM) 计算了人为氮氧化物 (NOx＝NO+NO2)、人为可挥发性有机化合物(AVOCs)以及生物可挥发性有机化合物(BVOCs)对春季东亚地区地面臭氧浓度的协同贡献及总贡献(＝纯贡献+协同贡献)。结果表明, AVOCs、BVOCs与NOx对O3生成量的贡献依赖于AVOCs、BVOCs排放量的相对大小。AVOCs或BVOCs排放量显著偏高的地区, 其总贡献主要来源于其与NOx的协同贡献。从区域角度 (1°×1°) 来看, BVOCs对东亚春季地面O3浓度的贡献较小, BVOCs排放量明显偏高的个别地区除外。BVOCs总贡献有很强的日变化特征, BVOCs总贡献有可能小于其协同贡献。个例研究的成果应用于O3调控对策的制定和实施很可能达不到预期的效果。我国北方 (30°N以北) 应控制人为源; 我国南方BVOCs排放量显著偏高的地区, 生物源和人为源的贡献都必须考虑。     

Evaluating the Effects of Radiative Forcing Feedback in Modelling Urban Ozone Air Quality in Portland,Oregon: Two-Way Coupled MM5–CMAQ Numerical Model Simulations

We summarize an on-line coupled meteorological–emissions–photochemical modelling system that allows feedback from air-quality/chemistry to meteorology via radiative forcing. We focus on the radiative-forcing impacts (direct effects) of ozone. We present an application of the coupled modelling system to the episode of 23–31 July 1998 in Portland, Oregon, U.S.A. Results suggest that the inclusion of radiative-forcing feedback produces small but accountable impacts. For this region and episode, stand-alone radiative transfer simulations, i.e., evaluating the effects of radiative forcing independently of changes in meteorology or emissions, suggest that a change of 1 ppb in ground-level ozone is approximately equivalent to a change of 0.017 W m⁻² in radiative forcing. In on-line, coupled, three-dimensional simulations, where the meteorological dependencies are accounted for, domain-wide peak ozone concentrations were higher by 2–4 ppb (relative to a simulated peak of 119.4 ppb) when including the effects of radiative-forcing feedback. A scenario of 10% reduction in anthropogenic emissions produced slightly larger decreases in ozone, an additional 1 ppb in local-peak reductions, relative to scenarios without feedback.     

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.     

Surface ozone concentrations in Agra: links with the prevailing meteorological parameters

Measurements of surface ozone (O₃), nitric oxide (NO), nitrogen dioxide (NO₂), oxides of nitrogen (NO_x=NO+NO₂) and meteorological parameters have been made at Agra (North Central India, 27°10??N, 78°05??E) in post monsoon and winter season. The diurnal variation in O₃ concentration shows daytime in situ photochemical production with diurnal maximum in noon hours ranging from 51 to 54 ppb in post monsoon and from 76 to 82 ppb in winter, while minimum (16?C24 ppb) during nighttime and early morning hours. Average 8-h O₃ concentration varied from 12.4 to 83.9 ppb. The relationship between meteorological parameters (solar radiation intensity, temperature, relative humidity, wind speed and wind direction) and surface O₃ variability was studied using principal component analysis (PCA), multiple linear regression (MLR) and correlation analysis (CA). PCA and MLR of daily mean O₃ concentrations on meteorological parameters explain up to 80 % of day to day ozone variability. Correlation with meteorology is strongly emphasized on days having strong solar radiation intensity and longer sunshine time.     

Studies of Oxidant Production at the Weybourne Atmospheric Observatory in Summer and Winter Conditions

Detailed studies have been made of the behaviour of gases and radicals involved in the production of oxidants at the Weybourne Atmospheric Observatory in both summertime and wintertime conditions. In June 1995 the range of meteorological conditions experienced varied such that ozone destruction was observed in clean northerly air flows reaching Weybourne down the North Sea from the Arctic, and ozone production was observed in varying degrees in air with different loadings of nitrogen oxides and other precursors. The transition point for ozone destruction to ozone production occurred at a nitric oxide concentration of the order of 50 pptv. Plumes of polluted air from various urban areas in the U.K. were experienced in the June campaign at Weybourne. Quantitative studies of ozone production in a plume from the Birmingham conurbation on 18 June 1995 showed that the measurement of ozone production agreed well with calculated production rates from the product of the nitric oxide and peroxy radical concentrations (r2=0.9). In wintertime conditions (October–November 1994) evidence was also found for oxidant production, defined as the sum of O3+NO2. At this time of year the peroxy radical concentrations (RO2) were much lower than observed in the summertime and the nitric oxide (NO) was much higher. There was still sufficient RO2 during the day, however, for a slow accumulation of oxidant. Confirmatory evidence for this comes from the diurnal co-variance of (O3+NO2) with PAN, an excellent tracer of tropospheric photochemistry. The same type of covariance occurs in summer between PAN and ozone. The results obtained in these series of measurements are pertinent to understanding the measures necessary to control production of regional photochemical air pollution, and to the production of ozone throughout the northern hemisphere in winter.