A review of gas-phase chemical mechanisms commonly used in atmospheric chemistry modelling

The atmospheric chemical mechanism is an essential component of airshed models used for investigating the chemical behaviors and impacts of species. Since the first tropospheric chemical mechanism was proposed in the 1960s, various mechanisms including Master Chemical Mechanism (MCM), Carbon Bond Mechanism (CBM), Statewide Air Pollution Research Center (SAPRC) and Regional Atmospheric Chemistry Mechanism (RACM) have been developed for different research purposes. This work summarizes the development and applications of these mechanisms, introduces their compositions and lumping methods, and compares the ways the mechanisms treat radicals with box model simulations. CBM can reproduce urban pollution events with relatively low cost compared to SAPRC and RACM, whereas the chemical behaviors of radicals and the photochemical production of ozone are described in detail in RACM. The photolysis rates of some oxygenated compounds are low in SAPRC07, which may result in underestimation of radical levels. As an explicit chemical mechanism, MCM describes the chemical processes of primary pollutants and their oxidation products in detail. MCM can be used to investigate certain chemical processes; however, due to its large size, it is rarely used in regional model simulations. A box model case study showed that the chemical behavior of OH and HO₂ radicals and the production of ozone were well described by all mechanisms. CBM and SAPRC underestimated the radical levels for different chemical treatments, leading to low ozone production values in both cases. MCM and RACM are widely used in box model studies, while CBM and SAPRC are often selected in regional simulations.     

2007年春节期间北京大气颗粒物中多环芳烃的污染特征

利用大流量颗粒物采样器分昼夜采集了2007年春节前后大气气溶胶中PM₁₀和PM_2.5样品，并采用气相色谱-质谱技术对PM_2.5样品中的多环芳烃进行了检测.春节期间大气颗粒物中PM₁₀和PM_2.5夜间平均质量浓度为232 μg·m^-3和132 μg·m^-3,分别高于白天的PM₁₀(194 μg·m^-3)和PM_2.5(107 μg·m^-3)；除夕后颗粒物日平均质量浓度为252.3 μg·m^-3 (PM₁₀)和123.8 μg·m^-3 (PM_2.5)，分别高于除夕前的166.7 μg·m^-3(PM₁₀)和106.8 μg·m^-3(PM_2.5)；同时夜间PM_2.5中多17种多环芳烃(PAHs)的总浓度都高于相应白天的总浓度，且除夕前多环芳烃日均总浓度为95.9 ng·m^-3，高于除夕后的58.9 ng·m^-3.结果表明，除了受一定的气象条件的影响外，大量燃放烟花爆竹会对大气颗粒物浓度有影响，但对大气中的多环芳烃影响不大，而春节期间工业及交通污染排放的减少削减了排放到大气中的PAHs.根据荧蒽/芘等比值指标判别北京PAHs主要以燃煤为主、交通为次的混合局地源污染.     

同位素方法在大气甲烷研究中的应用

通过对大气甲烷研究的同位素方法理论基础及其研究进展的综述，概括介绍了现有的大气甲烷同位素研究方法和所取得的成果，讨论分析了在中国开展该项研究的意义和前景。     

Comprehensive and high-resolution emission inventory of atmospheric pollutants for the northernmost cities agglomeration of Harbin-Changchun, China: Implications for local atmospheric environment management

Using a bottom-up estimation method, a comprehensive, high-resolution emission inventory of gaseous and particulate atmospheric pollutants for multiple anthropogenic sectors with typical local sources has been developed for the Harbin-Changchun city agglomeration (HCA). The annual emissions for CO, NOx, SO₂, NH₃, VOC_S, PM_2.5, PM₁₀, BC and OC during 2017 in the HCA were estimated to be 5.82 Tg, 0.70 Tg, 0.34 Tg, 0.75 Tg, 0.81Tg, 0.67 Tg, 1.59 Tg, 0.12 Tg and 0.26 Tg, respectively. For PM₁₀ and SO₂, the emissions from industry processes were the dominant contributors representing 54.7% and 49.5%, respectively, of the total emissions, while 95.3% and 44.5% of the total NH₃ and NOx emissions, respectively, were from or associated with agricultural activities and transportation. Spatiotemporal distributions showed that most emissions (except NH₃) occurred in November to March and were concentrated in the central cities of Changchun and Harbin and the surrounding cities. Open burning of straw made an important contribution to PM_2.5 in the central regions of the northeastern plain during autumn and spring, while domestic coal combustion for heating purposes was significant with respect to SO₂ and PM_2.5 emissions during autumn and winter. Furthermore, based on Principal Component Analysis and Multivariable Linear Regression model, air temperature, relative humidity, electricity and energy consumption, and the urban and rural population were optimized to be representative indicators for rapidly assessing the magnitude of regional atmospheric pollutants in the HCA. Such indicators and equations were demonstrated to be useful for local atmospheric environment management.     

Identification of close relationship between atmospheric oxidation and ozone formation regimes in a photochemically active region

Understanding ozone (O₃) formation regime is a prerequisite in formulating an effective O₃ pollution control strategy. Photochemical indicator is a simple and direct method in identifying O₃ formation regimes. Most used indicators are derived from observations, whereas the role of atmospheric oxidation is not in consideration, which is the core driver of O₃ formation. Thus, it may impact accuracy in signaling O₃ formation regimes. In this study, an advanced three-dimensional numerical modeling system was used to investigate the relationship between atmospheric oxidation and O₃ formation regimes during a long-lasting O₃ exceedance event in September 2017 over the Pearl River Delta (PRD) of China. We discovered a clear relationship between atmospheric oxidative capacity and O₃ formation regime. Over eastern PRD, O₃ formation was mainly in a NO_x-limited regime when HO₂/OH ratio was higher than 11, while in a VOC-limited regime when the ratio was lower than 9.5. Over central and western PRD, an HO₂/OH ratio higher than 5 and lower than 2 was indicative of NO_x-limited and VOC-limited regime, respectively. Physical contribution, including horizontal transport and vertical transport, may pose uncertainties on the indication of O₃ formation regime by HO₂/OH ratio. In comparison with other commonly used photochemical indicators, HO₂/OH ratio had the best performance in differentiating O₃ formation regimes. This study highlighted the necessities in using an atmospheric oxidative capacity-based indicator to infer O₃ formation regime, and underscored the importance of characterizing behaviors of radicals to gain insight in atmospheric processes leading to O₃ pollution over a photochemically active region.     

南宁市区交通环境空气颗粒物中碳组分的污染特征分析研究

含碳颗粒物是大气颗粒物的重要组成部分,对人体健康产生很大的威胁.分别于2012年夏季及2013年冬季在南宁市选取六条主要交通干道采集了PM10、PM2.5样品,分析测定了其中的碳组分.结果表明,碳组分浓度季节变化明显.碳组分在细颗粒物中占有比重比在可吸入颗粒物中大.存在二次有机碳污染.对8种碳组分丰度分析说明南宁市大气颗粒物中碳组分的主要来源是燃煤、机动车尾气及生物质样品燃烧.     

西安市一次严重霾污染天气特征及气象条件分析

为了解西安市气象条件对霾污染天气的影响,利用西安市13个测点PM2.5逐时监测资料和气温(T)、风向(WD)、风速(WS)、相对湿度(RH)、气压(p)以及能见度(VIS)等地面气象观测数据,对西安市2013年12月16—26日发生的一次严重霾污染过程进行分析。结果表明:此次霾污染过程中,西安市PM2.5日均值浓度最高达744μg/m3,超过国家二级标准近10倍,能见度最低降至0.42 km,重霾污染期间PM2.5/PM10在64%~80%。分析认为高相对湿度、低风速和主导风向不明显以及大气层结稳定是造成本次霾污染天气的主要气象因素,其中大气能见度与风速和大气压呈正相关,其相关系数(r)分别为0.3162、0.3479,能见度与温度的相关系数r=0.0825,呈微弱正相关,能见度和相对湿度的相关系数r=-0.7465,呈显著负相关。细颗粒物对能见度的影响非常明显,二者之间的相关系数为-0.7290,细颗粒污的消光系数最高达9.2 km-1。     

超细颗粒物PM25控制技术综述

PM2.5由于其较小的粒径、巨大的比表面积、较大的危害等特点受到世界各国的广泛研究。对此从亚微米粒子的来源、性质、危害等方面进行阐述,对比和总结国内外目前常用的控制技术,详细叙述了静电和其他除尘器相结合以及交流凝并技术脱出超细颗粒物的原理。交流凝并是一种适合收集亚微米粒子的有效方法,这种方法收集效果好,经济实用,适用于去除炼钢、焊接、煤炭燃烧后产生的悬浮性粉尘粒子等方面。研究粒子的荷电、凝并对继续完善荷电凝并理论,提高亚微米粒子的收集效果是十分必要的。     

机动车行驶过程道路扬尘影响因素试验研究

机动车行驶过程道路扬尘是城区颗粒物污染的主要因素,其贡献率可达30％-50％。城市路面积尘是机动车行驶过程道路扬尘的主要尘源。路面尘受机动车车轮积压作用、机车行驶过程诱导气流、热射流等综合尘化作用的影响,再次扬向空中并扩散,造成空气中颗粒污染物TSP、PM10浓度增高。实验模拟单车行驶,研究道路粉尘负荷、车速、排放源距离对总悬浮颗粒物（TSP）、可吸入颗粒物（PM10）浓度的影响,结果显示：TSP、PM10浓度与机动车行驶速度呈显著正相关;同一车速下与路面粉尘负荷呈对数变化规律;与排放源距离呈负相关。     

燃煤电厂排放细颗粒物的水溶性无机离子特征综述

当前我国面临严重的大气细颗粒物(PM2.5)污染,燃煤电厂是大气中PM2.5的重要来源之一.为了实现国家"十一五"和"十二五"规划对二氧化硫(SO2)和氮氧化物(NOx)的总量减排目标,燃煤电厂大规模安装烟气脱硫和脱硝设施,这虽然减少了气态污染物转化生成的二次PM2.5,但另一方面也会对烟气中PM2.5的物理化学特征产生影响,有可能增加一次PM2.5的排放.本文综述了燃煤电厂排放PM2.5及其水溶性离子的粒径分布特征,重点介绍了脱硫和脱硝这两种烟气处理设施对燃煤电厂排放PM2.5的影响原理及相关研究结果,特别是对细颗粒物中水溶性离子(如SO2-4、Ca2+和NH+4)的影响.在目前我国PM2.5污染十分严重和燃煤电厂大量安装脱硫和脱硝装置的背景下,定量研究脱硫和脱硝对PM2.5排放特征的影响具有十分重要的意义.