ROx Budgets and O3 Formation during Summertime at Xianghe Suburban Site in the North China Plain

Photochemical smog characterized by high concentrations of ozone (O3) is a serious air pollution issue in the North China Plain (NCP) region, especially in summer and autumn. For this study, measurements of O3, nitrogen oxides (NOx), volatile organic compounds (VOCs), carbon monoxide (CO), nitrous acid (HONO), and a number of key physical parameters were taken at a suburban site, Xianghe, in the NCP region during the summer of 2018 in order to better understand the photochemical processes leading to O3 formation and find an optimal way to control O3 pollution. Here, the radical chemistry and O3 photochemical budget based on measurement data from 1-23 July using a chemical box model is investigated. The daytime (0600-1800 LST) average production rate of the primary radicals referred to as ROx (OH + HO2+ RO2) is 3.9 ppbv h-1. HONO photolysis is the largest primary ROx source (41％). Reaction of NO2 + OH is the largest contributor to radical termination (41％), followed by reactions of RO2 + NO2 (26％). The average diurnal maximum O3 production and loss rates are 32.9 ppbv h-1 and 4.3 ppbv h-1, respectively. Sensitivity tests without the HONO constraint lead to decreases in daytime average primary ROx production by 55％ and O3 photochemical production by 42％, highlighting the importance of accurate HONO measurements when quantifying the ROx budget and O3 photochemical production. Considering heterogeneous reactions of trace gases and radicals on aerosols, aerosol uptake of HO2 contributes 11％ to ROx sink, and the daytime average O3 photochemical production decreases by 14％. The O3-NOx-VOCs sensitivity shows that the O3 production at Xianghe during the investigation period is mainly controlled by VOCs.     

西固工业区光化学烟雾的数值模拟

本文给出了一个半拉格朗日形式的大气扩散模式。模式除考虑污染物在大气中的输送、弥散过程外,还加入了光化学反应过程。我们用此模式计算了1983年8月中旬兰州市西固地区的光化学烟雾浓度。计算结果和监测资料的对比表明,模式对这一地区O_3最大浓度值有较好的模拟能力,对O_3浓度的日变化及地理分布也有一定的模拟能力。     

金华地区夏秋大气中过氧乙酰硝酸酯的污染特征

过氧乙酰硝酸酯（PAN）是由VOCs和NO_x的光化学反应生成的一种典型二次污染物,比O₃更适合作为光化学污染的指示剂.2019年6—10月对浙江中部盆地金华市大气中PAN进行了在线监测,并对影响其体积分数变化的因素进行了分析,同时还分析了一次典型的光化学污染过程.结果表明,观测期间PAN的平均体积分数为0.656×10^-9,最高体积分数为4.348×10^-9,日均体积分数水平在0.130×10^-9~2.203×10^-9之间.PAN日变化特征显著,9月为明显的双峰变化,其他月份均为单峰.受气象条件的影响,夏季的污染程度显著低于秋季.9月27—30日典型污染时段内,PAN的小时均值是整个观测期均值的2.8倍,污染以本地积累为主.前体物浓度水平差异与去除机制的不同是影响PAN和O₃相关性的重要因素,此外NO/NO₂的比值是影响PAN生成速率的重要因素,PAN的峰值基本出现在NO/NO₂比值较低的时段.在生成PAN的VOCs物种中,丙烷、乙烷和间/对二甲苯所占比例较大.     

A Review of Atmospheric Chemistry Research in China: Photochemical Smog, Haze Pollution, and Gas-Aerosol Interactions

In this paper we present a review of atmospheric chemistry research in China over the period 2006-2010, focusing on tropospheric ozone, aerosol chemistry, and the interactions between trace gases and aerosols in the polluted areas of China. Over the past decade, China has suffered severe photochemical smog and haze pollution, especially in North China, the Yangtze River Delta, and the Pearl River Delta. Much scientific work on atmospheric chemistry and physics has been done to address this large-scale, complex environmental problem. Intensive field experiments, satellite data analyses, and model simulations have shown that air pollution is significantly changing the chemical and physical characters of the natural atmosphere over these parts of China. In addition to strong emissions of primary pollutants, photochemical and heterogeneous reactions play key roles in the formation of complex pollution. More in-depth research is recommended to reveal the formation mechanism of photochemical smog and haze pollution and their climatic effects at the urban, regional, and global scales.     

北京城市重烟尘雾与水雾过程的边界层结构

分析1999年11月1日至12月20日北京城市雾综合性观测试验中5次雾过程的实测资料，对如何区分重烟尘雾与水雾过程给出了判定方法，并对重烟尘雾与水雾过程的边界层结构特征作了探讨。主要结论为：从能见度、相对湿度、长波辐射平衡3个方面可以区分重烟尘雾过程和水雾过程；由于重烟尘雾和水雾的物理化学性质差异很大，对城市大气边界层结构产生的影响也不同，因此造成它们在相对湿度逆温层、风速分布、水汽变化等方面也有很大差异。     

光化学烟雾的控制试验

利用MM5与RADM的耦合模式,设计了3个削减源排放的试验,用以探讨控制光化学污染的有效途径。试验结果表明,在NMHC/NOx比值很大的前提条件下,NOx地面源排放的削减对降低大气中O3含量的作用最显著,而削减NMHC对降低大气中PAN含量的作用明显,同时削减NMHC和NOx是降低大气光化学污染强度的最佳途径。     

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.     

The photo-oxidations of propyl acetates in synthetic air-HONO-NO x mixtures: Product formation studies and proposed kinetic mechanisms

The formation of products following the hydroxyl radical initiated photo-oxidations of n-and isopropyl acetates has been studied. Mixtures of synthetic air containing a few ppm of nitrous acid, nitric oxide, nitrogen dioxide and one of the propyl acetates were irradiated with sunlamps in a Teflon bag smog chamber. The decay of reactants and the formation of products was monitored by chemiluminescent analysis or by gas chromatography. The major primary products from the photo-oxidation of n-propyl acetate are acetaldehyde and propionaldehyde while from isopropyl acetate they are acetone and methyl nitrate. It was not possible to analyse for formaldehyde, an expected primary product in these systems. The nature and distribution of products indicate that a significant fraction of primary products arise from decomposition reactions of the alkoxy-type radicals generated following the initial attack of hydroxyl radicals on the esters. The derived reaction stoichiometries (molecules of NO oxidised per molecule of ester reacted) are also consistent with the proposed mechanisms.     

造成北京PM10重污染的二类典型天气形势

利用北京空气质量监测资料和NCEP再分析资料,分析了北京发生PM10重污染的天气形势。研究表明:1)虽然北京地区PM10重污染(API指数3级以上)每年只有10 d左右,但与之关联的轻微或轻度空气污染(API指数3级)天数,却可能占全年3级污染总天数的40%-50%。因此,分析研究造成北京PM10重污染的天气形势,对于空气污染的预警预报以及污染源的控制和管理,都具有十分重要意义。2)通过海平面气压场的主观分析,确定了二类北京PM10重污染的典型天气形势,即高压南下东移阻滞型和与北上台风(或热带低压)相关联的弱高压控制型,并指出了后者在2008年奥运会期间,对开展北京空气污染预报和污染控制的指导作用。     

Intercomparison of NO<Subscript><Emphasis Type="Italic">x</Emphasis></Subscript>, SO<Subscript>2</Subscript>, O<Subscript>3</Subscript>, and aromatic hydrocarbons measured by a commercial DOAS system and traditional point monitoring techniques

A field-based intercomparison study of a(DOAS) instrument (OPSIS AB, Sweden) andcommercial Differential Optical Absorption Spectroscopydifferent point-sample monitoring techniques (PM, basedon an air monitoring station, an air monitoring vehicle, and various chemical methods) was conducted inBeijing from October 1999 to January 2000. The mixing ratios of six trace gases including NO, NO2, SO2,03, benzene, and toluene were monitored continuously during the four months. A good agreement betweenthe DOAS and PM data was found for NO2 and SO2. However, the concentrations of benzene, toluene,and NO obtained by DOAS were significantly lower than those measured by the point monitors. Theozone levels monitored by the DOAS were generally higher than those measured by point monitors. Theseresults may be attributed to a strong vertical gradient of the NO-O3-NO2 system and of the aromatics atthe measurement site. Since the exact data evaluation algorithm is not revealed by the manufacturer ofthe DOAS system, the error in the DOAS analysis can also not be excluded.     

北京市房山区大气污染物时空分布特征及气象影响因素分析

利用北京市房山区良乡镇和琉璃河镇内的区域自动气象站和环境监测站观测数据,对2013年至2015年PM_(2. 5)、PM_(10)、NO_2、SO_2、CO 5种大气污染物浓度变化特征进行了统计分析。结果显示,近3年来,两个镇综合污染物指数呈现逐年下降趋势,各污染物对房山区整体大气污染的贡献率从大至小依次为PM_(2. 5)、PM_(10)、SO_2、NO_2、CO,PM_(2. 5)已取代传统大气污染物SO_2成为房山区的主要大气污染贡献体。两个站点各污染物浓度均表现出明显的季节、月、日变化特征。在不同季节条件下,局地气象要素与污染天气发生概率之间有着很好的相关关系。因此,可根据气象要素分级方法找出各季节污染天气发生时最敏感的气象因素,为局地污染天气预报提供参考指标,也为防范空气污染、制定科学的综合管理措施提供科学参考。     

Intercomparison of NO_x, SO_2, O_3, and Aromatic Hydrocarbons Measured by a Commercial DOAS System and Traditional Point Monitoring Techniques

A field-based Intercomparison study of a commercial Differential Optical Absorption Spectroscopy (DOAS) instrument (OPSIS AB, Sweden) and different point-sample monitoring techniques (PM, based on an air monitoring station, an air monitoring vehicle, and various chemical methods) was conducted in Beijing from October 1999 to January 2000. The mixing ratios of six trace gases including NO, NO2, SO2, O3, benzene, and toluene were monitored continuously during the four months. A good agreement between the DOAS and PM data was found for NO2 and SO2. However, the concentrations of benzene, toluene, and NO obtained by DOAS were significantly lower than those measured by the point monitors. The ozone levels monitored by the DOAS were generally higher than those measured by point monitors. These results may be attributed to a strong vertical gradient of the NO-O3-NO2 system and of the aromatics at the measurement site. Since the exact data evaluation algorithm is not revealed by the manufacturer of the DOAS sys     

Photooxidation of dimethyl sulfide and dimethyl disulfide. II: Mechanism evaluation

The mechanisms for atmospheric photooxidation of CH₃SCH₃ and CH₃SSCH₃ developed in Part I are evaluated by a series of outdoor smog chamber experiments. Measured product yields, including SO₂, H₂SO₄, CH₃SO₃H and HCHO, are reported. The predictions of the mechanisms developed in Part I are found to be in substantial agreement with the measured concentrations from the smog chamber. By comparison of mechanism predictions and observations, critical uncertainties in the mechanism are identified.     

汾渭平原CUACE模式空气质量预报性能的检验订正及环境评估

利用2019年1—6月地面环境监测资料和PM_2.5气象条件评估指数，结合滚动偏差订正方法，对汾渭平原CUACE空气质量预报产品进行了检验订正，并对气象条件和污染减排影响进行了评估。结果表明：CUACE模式对空气质量指数(AQI)、PM_2.5和SO₂浓度预报值较接近观测值，PM₁₀、CO和NO₂预报值小于观测值，O₃预报值大于观测值；对首要污染物O₃和PM_2.5及重度和严重等级污染的预报的TS评分最高，漏报率和空报率最小，预报偏差最接近1；滚动偏差订正方法对改善CUACE空气质量预报效果较为明显，尤其是对PM₁₀、O₃和NO₂改善最为明显；汾渭平原2019年上半年气象条件变化使PM_2.5浓度较2018年同期和过去5年同期分别上升了18.26%和11.18%，减排措施使PM_2.5浓度较2018年同期和过去5年...     

嵌套网格空气质量预报模式系统的发展与应用

主要综述中国科学院大气物理研究所自主开发的嵌套网格空气质量预报模式系统(NAQPMS,Nested Air Quality Prediction Modeling System)的历史发展与应用情况.模式发展伊始为欧拉污染物输送实用模型,利用其研究东亚硫氧化物的跨国输送问题,得出中国对于周边国家的输送量不大的结论; 在系统中嵌入适合东亚的起沙机制模块,用来模拟沙尘发生、输送及沉降等过程,估算亚洲大陆沙尘气溶胶对海洋地区的输送与沉降通量,为研究海洋生物地球化学循环提供基础数据; 利用该系统研究沙尘及其土壤粒子对酸雨的中和作用,发现沙尘输送对东亚酸雨的分布影响很大; 发展城市尺度高分辨率气象和空气质量预报技术,使模式水平分辨率达到500 m,并应用于台北高浓度臭氧和PM10的模拟; 研究和集成区域及城市尺度大气污染预报理论和模拟技术,研制成目前的嵌套网格空气质量预报模式系统,以探讨不同尺度各种污染(如沙尘暴、城市光化学烟雾、酸雨、高浓度悬浮颗粒物等)的变化规律.在模式系统中初步建立资料同化模块,开展大气化学成分及沙尘输送模拟的资料同化研究.系统已经在北京、上海、深圳、郑州等城市环境监测中心实施空气质量的实时预报.未来,系统将集成到全球环境大气输送模式(GEATM),以实现从城市群到全球具有双向耦合功能的模式系统.     

2008年北京奥运会期间污染控制效果数值模拟——以个例分析为例

利用2007和2008年北京地区空气质量监测资料和NCEP再分析资料,分析了北京地区空气动力学当量直径小于等于10μm颗粒物(PM10)污染过程与天气形势及天气系统之间的关系。结果表明:西太平洋热带气旋路径对北京地区发生PM10污染具有预示作用,即当热带气旋北上并在朝鲜半岛或日本登陆的情况下,北京地区一般受持续均压场等弱中尺度天气系统控制,这种中尺度天气系统不利于污染物的扩散,因此北京地区经常发生区域性的PM10空气污染事件。在2007年9次台风北上登陆朝鲜半岛或日本的过程中,北京地区伴随发生了9次PM10污染过程,预示准确率达100%,2008年的预示准确率也达到了80%以上。为了说明北京奥运会期间污染控制措施对改善北京空气质量有实际效果,利用中国科学院大气物理研究所区域空气质量模式NAQPMS,采用无控制措施源和有控制措施源,对2008年北京残奥会期间一次西太平洋北上型热带气旋天气条件下的空气质量状况进行了数值模拟试验,揭示了此次过程北京地区未发生PM10空气污染的原因。     

2004年北京市沙尘天气对空气质量影响的对比分析

北京市环保局近几年的空气质量监测报告表明：PMIO污染显著，一直居高不下，是最主要的污染物，全年中其占首要污染物的天数超过90％；SO2的污染趋势已经得到控制；NO2的污染状况改善相对较小，但整体呈现缓慢下降的趋势。通过对2004年春季北京市发生的3次沙尘天气过程的分析与比较，结合北京市3月份的空气污染物浓度（或指数）的变化情况，总结了沙尘天气对空气质量的影响情况，为今后北京地区沙尘天气的空气质量预报提供参考。     

北京地区严重大气污染的气象和化学因子

利用北京３２５ ｍ 气象塔进行了大气污染物臭氧、氮氧化物、一氧化碳和气象要素的同步观测, 对影响大气污染的气象和化学因子进行了分析,探讨大气污染物变化的规律, 为城市空气污染预报提供理论基础。     

The EUMAC Zooming Model,a tool for local-to-regional air quality studies

Summary The EUMAC Zooming Model (EZM) is a comprehensive model system for simulations of wind flow and air pollutant transport and transformation at the local-to-regional scale. Core models of the EZM are the nonhydrostatic mesoscale model MEMO and the photochemical dispersion model MARS. Manifold air quality studies, primarily for large urban agglomerations, have been already performed with the EZM. In most of these studies the results of the EZM agree fairly well with available observations. An example for a successful study with the EZM is its application to simulate the formation of photochemical smog in the case of stagnant meteorological conditions in Athens. By applying a suitable nesting technique, MEMO reproduces satisfactorily the observed diurnal wind pattern in Athens. The results of MARS elucidate the characteristics of a severe photosmog episode in Athens and are in general very similar to available observations.With 17 Figures     

冬季采暖优化对北京地区空气质量的影响

空气污染能够影响人体健康、交通运输、农业生产等,会对国家经济造成损失。多年来,北京一直是空气污染严重地区,而冬季燃煤采暖是一个重要的原因。2016～2017年,北京大力优化采暖的能源结构,旨在改善空气质量。本文通过分析5个位于北京不同区域的空气质量监测站的PM2.5、PM10、SO₂、NO₂和CO污染物浓度,对比了2018年和2015年的空气质量变化情况。结果显示:2018年5个站5种污染物浓度较2015均下降,平均下降幅度为37.3%,而5个站降幅最大的污染物浓度都是SO₂,平均降幅为59.2%。进一步分析表明,两年5种污染物浓度的差距主要来自冬季的取暖时期。2018年冬季5个站重空气污染（PM2.5浓度>150 μg/m3）天数较2015年平均下降率高达91.3%,比其他季节多了41.3%。相较于2015年,5个站平均的2018年冬季5种污染物浓度平均下降值是其他季节的4.8倍,平均下降的幅度是其他季节的2.3倍。逐小时数据分析显示,2018年较2015年冬季污染物浓度下降比较大的时刻主要来来自暖更多的时间段。结合气象条件分析表明,北京冬季采暖优化很大程度地提高了空气质量,这为有相似采暖方式的城市的空气污染治理提供借鉴和参考。