2003年夏季临安地区大气气溶胶离子成分的尺度分布特征

文中利用2003年夏季在浙江临安大气本底污染监测站观测的资料,分析了临安的气溶胶质量浓度、离子成分的尺度分布特点及主要离子间的相互关系。初步结果显示,该期间临安气溶胶主要以粒径小于2.1μm的细粒子为主,约占总质量浓度的66%,其中粒径小于0.65μm的粒子可达总质量浓度的50%,远高于其他各级尺度段上的粒子浓度。与质量浓度分布相似,可溶性无机离子成分主要集中在粒径小于2.1μm(记为PM2.1)的细粒子中,PM2.1粒子中可溶性无机离子约占所有尺度段(包括所有5级)离子质量浓度总和的88%。其中粒径小于0.65μm的亚微米粒子中的离子质量浓度是细粒子的主要部分,占所有尺度段上离子质量浓度总和的77%。SO42-,NH4+和K+是PM2.1中决定性的离子成分。相关分析和离子平衡表明,PM2.1中SO42-与NH4+和K+有很高的相关,在粒径小于0.65μm的亚微米粒子中,非海盐硫酸盐(Nss-SO42-)主要为(NH4)2SO4,由气-粒转化产生;而在粒径为0.65~2.1μm尺度段,Nss-SO42-除(NH4)2SO4外,可能还有K2SO4,Na2SO4等存在。     

广州市气溶胶质量谱和水溶性成分谱分析

对2006年9月—2007年1月在广州市采集的气溶胶粒子的质量谱和水溶性成分进行分析表明,广州市各测点的气溶胶质量谱基本呈双峰或三峰分布,细粒子浓度占气溶胶总浓度的四成到六成;在气溶胶水溶性离子成分中,浓度最高的阴离子是SO42-和NO3-,浓度最高的阳离子是NH4+和Na+;各离子多呈三峰或是双峰分布,但不同离子的峰值不尽相同;广州市的粉尘污染逐渐减少,而NH4+浓度迅速增大;相对土壤,只有Na+和NH4+富集度比较大,SO42-和K+有一定富集;相对海洋,F-的富集度非常大,其他离子则无明显富集;Cl-被严重耗损;致酸离子以SO42-为主,NO3-作用较弱些;SO42-和NH4+谱分布有很好的相关性,并且在细粒子和巨粒子粒径范围有共同的来源。     

采暖期和非采暖期西安大气颗粒物中水溶性组分的化学特征

为了探讨采暖期和非采暖期西安大气颗粒物水溶性组分的化学特征和来源,分别于2005年冬季(2005年12月-2006年2月)和2006年夏季(6～8月)采集西安大气PM2.5和TSP样品,分析其中Na+、NH4+、K+、Mg2+、Ca2+、F-、Cl-、Br-、NO-2、NO-3和SO2-4共11种水溶性离子的浓度,并对其季节特征和来源进行了研究.结果显示,采暖期西安大气PM2.5和TSP中11种水溶性离子的平均浓度分别为53.2μg·m-3和110.3μg·m-3,非采暖期分别为51.3 μg·m-3和89.3μg·m-3.SO2-4、NO-3和NH+4在PM2.5和TSP中均为最主要的离子组分,浓度之和在采暖期分别占到PM2.5和TSP总离子浓度的78%和76%,在非采暖期则占到88%和76%.PM2.5和TSP中,NH+4、SO2-4和NO-3三者之间都有很好的相关性,其在颗粒物中的主要结合形式为(NH4)2SO4、NH4 HSO4和NH4 NO3.硫的转化率(SOR)和氮的转化率(NOR)在非采暖期明显大于采暖期,揭示SO2-4和NO-3的形成机制为气相氧化,主要受温度的控制.阴阳离子平衡和pH值测定的结果表明西安市大气PM2.5稍偏酸性,TSP为碱性,无论是粗、细粒子采暖期比非采暖期更偏酸性.对比10年前的研究结果,显示西安市大气污染控制措施大大降低了采暖期气溶胶中二次组分的污染程度,但主要污染排放源已逐渐由燃煤型向机动车排放转化.     

北京奥运期间气溶胶中水溶性无机离子浓度特征及来源解析

2008年7—10月在中国科学院大气物理研究所采集气溶胶样品,用离子色谱进行水溶性无机离子分析,并对其组成、质量浓度变化特征、相关性及存在形式、来源解析等方面进行研究。结果显示,整个采样期间,SO42-、NO3-和NH4＋是最主要的水溶性离子,主要以（NH4）2SO4和NH4NO3形式存在;SO42-、NO3-和NH4＋、Ca2＋和Mg2＋的相关系数都较高,具有很好的同源性。NO3-/SO42-质量浓度比值表明,奥运前,固定源（燃煤）对水溶性离子的贡献大于流动源（机动车）,而奥运期间和奥运后则相反。因子分析表明,交通、燃煤、土壤、建筑尘和生物质燃烧源是采样期间北京大气污染的主要来源。     

安徽省雾、霾、晴空天气的气象条件对比分析

使用2008~2012年逐日地面观测资料,揭示了安徽不同地区雾、霾、晴空天气气象条件的差异,指出不同地区要根据本地特点建立雾、霾预报指标和预报方法。3类天气差异最大的地面气象要素是能见度和相对湿度。根据3种天气前一日和当日能见度和相对湿度分布特征,全省站点可以分为3类:1)从雾、霾到晴空,能见度递增、相对湿度递减,且差异显著,如合肥站;2)雾、霾天的能见度和相对湿度均很接近,但与晴空天差别较大,如阜阳站;3)能见度在雾、霾天无明显差别,但相对湿度在雾、霾天差异显著,如安庆站。地级市测站雾后即霾的可能性较大(大于50%),县城测站雾后即霾的可能性较低(低于25%)。垂直方向,雾时相对湿度随高度下降很快,850 h Pa中位值已降到20%(安庆)和45%(阜阳)以下,霾时相对湿度随高度下降缓慢,850 h Pa中位值仍在60%左右;另外,霾天边界层中上部风切变较小,雾天和晴空天边界层中上部都存在较大的风切变。     

敦煌莫高窟大气颗粒物中水溶性离子变化及来源解析

为探明莫高窟大气颗粒物污染特征,采集了2014年4-12月第16窟及72窟外环境中大气颗粒物PM2.5和PM10~2.5样品,对比分析了样品中水溶性离子变化及影响因素,通过主成分分析法解析了其主要来源。结果表明:(1)窟区主风向为南风,起沙风频率仅为0.01%,不利于污染物的扩散;(2)窟外PM2.5和PM10~2.5、窟内PM2.5和PM10~2.5中水溶性离子总浓度分别为6.1±4.0μg·m^-3、12.2±9.1μg·m^-3、3.7±0.8μg·m^-3和7.5±1.6μg·m^-3,SO₄^2-、Ca²⁺、NO3^-、Na⁺及Cl^-是主要组成,SO42-、NO3-和Ca2+之和在窟外和窟内PM2.5和PM10~2.5中占总离子比例分别为79.24%,76.81%,80.61%及77.74%,二次离子主要来自固定污染源;(3)PM2.5与PM10~2.5中各离子浓度的比值在窟外、内分别为0.33~0.88、0.25~0.94,9种水溶性离子在不同粒径粒子中富集程度有所差异,3-5月的沙尘、7-9月的降雨、11月农村农作物秸秆燃烧及冬季取暖燃煤等对水溶性离子都有一定影响,窟内PM2.5中游客数量与NH4+和NO^3-有一定的相关性(R2=0.27、0.35)、PM10~2.5中游客数量与NH4+有一定的相关性(R2=0.31);(4)沙尘天气下窟外和窟内的PM2.5与PM10-2.5中Cl-、SO₄^2-、Na⁺、K+和Ca²⁺的浓度增加,窟区微环境主要受区域环境气象因素影响,建议极端沙尘天气关闭洞窟;(5)莫高窟大气环境呈碱性;(6)PM2.5和PM10~2.5主要来源于当地秸秆燃烧、二次污染源、土壤沙尘及干涸的大泉河。     

天津大气气溶胶化学组分的粒径分布和垂直分布

2006年8月在天津气象铁塔的10、120、220 m 3个不同高度.利用Andersen分级采样器同步进行大气气溶胶采样,样品用离子色谱和电感耦合等离子体质谱仪进行分析.结果表明,K元素主要集中在细粒子,Mg、Ca、Al、Fe元素主要集中在粗粒子,Na元素则具有双峰结构;总离子浓度随着高度的升高有增加的趋势,SO42-、N3-、NH4+、Ca2+是最主要的水溶性尤机离子;二次源是水溶性离子重要的贡献源.NO3-、SO42-、NH4+随着高度升高,浓度有向小粒径集中的趋势;各层气溶胶阴阳离子平衡值小于1,表明气溶胶偏碱性,与天津地处北方,土壤偏碱性,且非采暖期地面扬尘是主要的气溶胶来源有关;各层NO3-/SO42-平均值为0.48,表明非采暖期固定排放源(燃煤)仍然是天津大气细粒子中水溶性离子的主要来源.     

乌鲁木齐市不同天气条件下TSP水溶性离子特征分析

利用2009年乌鲁木齐4个大气总悬浮颗粒物（TSP）观测站点样品,采用离子色谱仪测定了不同天气条件下TSP中水溶性离子成分,分析了水溶性离子变化特征及影响因素,结果表明：不同天气条件对乌鲁木齐市TSP中的NH4 、Ca2 、NO3-和SO42-浓度具有明显的影响。降水对离子有清除作用,使其在TSP中浓度减小。大风及沙尘天气使TSP中Ca2 浓度大幅增加,其它离子增加幅度很小。连续污染日,各离子在大气中累积至较高浓度,是同期晴天条件下的2-7倍。气象因素对采暖期TSP离子浓度变化影响较大。非采暖期乌鲁木齐市TSP离子浓度主要受到自然因素引起的土壤尘和建筑尘的影响。     

南京气溶胶水溶性离子粒径分布及其随高度的变化

2009年1月对南京市河西生活区距地面1．5、54和80m3处同步进行了大气颗粒物采样,并用离子色谱对样品进行了分析。结果显示,随着高度的增加,PM10和PM2.1的质量浓度逐渐降低,而总离子浓度随高度增加而增大。气溶胶中最主要的3种水溶性离子分别为N03、SO4 2-、Ca2＋,且3个高度的NO3-与SO4 2-浓度之比均大于1,表明该生活区移动排放源已经成为大气气溶胶离子的主要来源。3个高度处各离子粒径分布规律为：SO4 2-、NO3-、K＋在0．43-1．1um出现峰值;Ca2＋、Mg2＋、NO2-在4．7～5．8um出现峰值;Na＋、Cl-、F-在0．43～1．1um和4．7～5．8um出现双峰。     

一次罕见的辐射-平流雾研究(Ⅱ)——雾水化学性质分析

利用2006年12月24-27日南京市持续浓雾的雾水样品资料,结合雾滴谱仪观测的雾的微物理结构和系留气球探测的边界层资料,分析了本次浓雾雾水的化学特征.结果表明:酸雾的频率达61.5%,平均pH值为5.63;雾水中主要阳离子是NH+4、Na+、Ca2+,主要阴离子是SO42-、NO-3,其次是Cl-;雾水中总离子和SO2-4浓度水平较高,说明本次过程大气污染比较严重;雾水的Na+/Cl-为3.09,明显高于其它地区,Cl-亏损严重,主要是因为此次雾是辐射-平流雾,受到东南海面上吹来的暖湿平流的影响;雾水中的离子浓度远高于雨水中的浓度,但雨水比雾水更酸;雾水离子总浓度与雾滴粒径呈反相关趋势(r=-0.71);浓雾发展过程中,pH值先升后降,前后出现三次起伏,其趋势与各离子和总离子浓度的变化大体相反.     

Using hourly measurements to explore the role of secondary inorganic aerosol in PM2.5 during haze and fog in Hangzhou,China

This paper explores the role of the secondary inorganic aerosol （SIA） species ammonium,NH4＋,nitrate,NO3-,and sulfate,SO24-,during haze and fog events using hourly mass concentrations of PM2.5 measured at a suburban site in Hangzhou,China.A total of 546 samples were collected between 1 April and 8 May 2012.The samples were analyzed and classified as clear,haze or fog depending on visibility and relative humidity （RH）.The contribution of SIA species to PM2.5 mass increased to ～50％ during haze and fog.The mass contribution of nitrate to PM2.5 increased from 11％ during clear to 20％ during haze episodes.Nitrate mass exceeded sulfate mass during haze,while near equal concentrations were observed during fog episodes.The role of RH on the correlation between concentrations of SIA and visibility was examined,with optimal correlation at 60％-70％ RH.The total acidity during clear,haze and fog periods was 42.38,48.38 and 45.51 nmol m-3,respectively,indicating that sulfate,nitrate and chloride were not neutralized by ammonium during any period.The nitrate to sulfate molar ratio,as a function of the ammonium to sulfate molar ratio,indicated that nitrate formation during fog started at a higher ammonium to sulfate molar ratio compared to clear and haze periods.During haze and fog,the nitrate oxidation ratio increased by a factor of 1.6-1.7,while the sulfur oxidation ratio increased by a factor of 1.2-1.5,indicating that both gaseous NO2 and SO2 were involved in the reduced visibility.     

2016—2017年中国中东部本底地区PM10化学特性

对中国中东部3个区域大气本底观测站2015年12月—2017年12月PM₁₀质量浓度及其化学成分空间分布与季节变化特征进行研究,结果显示:研究期间龙凤山站、临安站和金沙站平均PM₁₀质量浓度分别为57.5,62.2 μg·m-3和57.6 μg·m-3。其中临安站和金沙站2017年PM₁₀质量浓度较2016年有所下降,但龙凤山站有所上升。与2013年相比,临安站和金沙站平均PM₁₀质量浓度分别降低29.3%和26.2%。临安站SO₄2-,NO₃-和NH₄+平均质量浓度分别为9.9,8.2 μg·m-3和3.7 μg·m-3,金沙站分别为10.2,6.7 μg·m-3和2.6 μg·m-3,均高于龙凤山站的5.9,4.9 μg·m-3和2.1 μg·m-3,其中龙凤山站和临安站的NO₃-与SO₄2-质量浓度比值较高（0.9和0.8）,金沙站较低（0.6）。龙凤山站的有机碳（OC）和元素碳（EC）质量浓度分别为10.1 μg·m-3和2.7 μg·m-3,临安站为6.7 μg·m-3和3.1 μg·m-3,金沙站为4.7 μg·m-3和2.3 μg·m-3,即龙凤山站OC最高,金沙站最低,3个站点的EC基本相当,临安站略高。与2013年相比,研究期间临安站SO₄2-,NH₄+和OC分别下降38.1%,26.0%和55.6%,金沙站分别下降46.3%,51.9%和44.7%,但临安站和金沙站的NO₃-分别上升12.3%和15.5%;临安站EC下降27.9%,金沙站EC上升4.5%。3个站点夏季PM₁₀,NO₃-,EC质量浓度及NO₃-与SO₄2-质量浓度比值均最低。     

天津雾和霾自动观测与人工观测的对比评估

为适应地面气象观测业务调整方向,提高新型自动气象站观测资料的质量及可用性,研究中对天津地区10个地面气象站1951—2014年历年2月人工观测及2014年2月自动观测和人工观测的轻雾、雾、霾现象进行对比评估。结果表明:天津地区历年2月轻雾的平均日数为10 d,雾和霾均为2 d,轻雾和霾同期出现的日数占有天气现象的7.4%,而雾和霾同期出现日数仅占0.7%;平行观测期的对比分析得到人工观测轻雾日数比自动观测多11 d,雾日数和霾日数均比自动观测少6 d,其中,轻雾和雾的判别差异集中出现在每日08:00(北京时,下同),霾则基本出现在每日08:00,14:00,17:00,20:00;通过对比自动观测和人工观测的能见度数据发现,二者相对偏差达25.1%,能见度小于15.0 km时,自动观测的能见度有60%~76%数值偏小,特别是08:00和20:00, 因此,在相对湿度满足条件的情况下,能见度的判别误差是导致自动观测与人工观测轻雾、雾、霾现象判别差异的重要原因。     

A Comparative Analysis of Chemical Properties and Factors Impacting Spring Sea Fog over the Northwestern South China Sea

In the present study, we analyzed the chemical properties and factors impacting the sea fog water during two sea fog events over the northwestern South China Sea in March 2017, and compared our results with those of other regions. The sea fog water during these two events were highly acidic and their average pH was below 3, which was related to the high initial acidifying potential and large amounts of NO3- and SO42- not involved in the neutralization reaction. The dominant cations in the sea fog water were Na+ and NH4+. The primary anions in the sea fog water over the South China Sea were Cl- and NO3-, while that over the North Pacific Ocean was mainly SO42-, and ratios of the three fog water ions near the Donghai Island were similar. Ions in the sea fog water during the two events were mainly derived from marine aerosols, while the difference was that the first low-level sea fog airflow trajectory passed over Hainan Island. Therefore, the proportion of K+ in the first sea fog was much higher than that in sea water and the second. Sulfate was the key to fog water nucleation, which made ion concentration in the sea fog water during the second event higher than that during the first. A decrease in average diameter during the first sea fog formation led to an ion concentration increase, while the average diameter of sea fog water during the second event was lower than that during the first, which corresponded with a moderate ion concentration increase.     

The influences of macro- and microphysical characteristics of sea-fog on fog-water chemical composition

ABSTRACT During a sea-fog field observation campaign on Donghai Island in the spring of 2011, fog-water, visibility, meteorological elements, and fog droplet spectra were measured. The main cations and anions in 191 fog-water samples were Na＋, NH2, H＋, NO3, C1- and SO] , and the average concentrations of cations and anions were 2630 and 2970 p-eq L 1, respectively. The concentrations of Na＋ and C1- originated from the ocean were high. The enhancement of anthropogenic pollution might have contributed to the high concentration of NH＋, H＋, and NO^-3. The average values ofpH and electrical conductivity （EC） were 3.34 and 505 uS cm-1, respectively, with a negative correlation between them. Cold fronts associated with cyclonic circulations promoted the decline of ion loadings. Air masses from coastal areas had the highest ion loadings, contrary to those from the sea. The ranges of wind speed, wind direction and temperature corresponding to the maximum total ion concentration （TIC） were 3.5-4 m s-1, 79°-90° and 21°C-22°C, respectively. In view of the low correlation coefficients, a new parameter Lr was proposed as a predictive parameter for TIC and the correlation coefficient increased to 0.74. Based on aerosol concentrations during the sea-fog cases in 2010, we confirmed that fog-water chemical composition also depended on the species and sizes of aerosol particles. When a dust storm passed through Donghai Island, the number concentration of large aerosol particles （with diameter 〉 1 p-m） increased. This caused the ratio of CaZ＋/Na＋ in fog-water to increase significantly.     

霾观测判识标准定量化对雾霾观测记录的影响

为研究霾观测判识标准定量化对雾霾观测记录的影响,选取2006—2012年湖北省18个基准站、基本站和一般站三类国家级地面气象观测站的资料,对已记录和按照相对湿度判识标准统计的雾、轻雾和霾天数进行分析,结果表明:判识标准定量化将使霾的观测记录明显增多,轻雾和雾观测记录略有减少,霾和轻雾观测记录将更趋合理,就湖北省而言,相对湿度在80%~95%之间,应以轻雾和雾为主;通过定时观测时次的能见度、相对湿度,以及日天气现象记录,可以得到历年按照相对湿度判识标准统计的霾和轻雾天数,实现对历史资料序列的订正,形成判识标准改变前后均一化的月年资料序列。判识标准定量化后,不能机械的硬套判识指标,观测员仍需熟练掌握轻雾和霾以及其他视程障碍现象的成因和特征,避免相对湿度在霾观测判识标准上下波动、轻雾处于消散过程阶段,轻雾与霾的频繁转记。     

一次持续性雾霾天气过程的阶段性特征及影响因子分析

应用常规与非常规气象观测资料及PM2.5浓度监测资料,对2013年1月20~24日山西区域一次持续性雾霾天气过程进行分析。研究发现：（1）本次雾霾天气过程具有明显的阶段性特征。2013年1月20日14时至23日11时,由于相对湿度的变化导致了3次轻雾转大雾过程;23日14~20时,由于PM2.5浓度的增大经历了1次轻雾转霾的天气过程。（2）地面弱的气压场和较小的风速以及PM2.5浓度的上升和相对湿度的增大为本次持续性雾霾天气过程的形成和发展提供了有利条件。（3）边界层逆温的存在是雾霾低能见度过程形成的必要条件,边界层有逆温层而不出现雾霾天气的条件是：相对湿度〈50%,PM2.5日均值浓度〈75μg·m-3;逆温层下相对湿度的大小是区别雾和霾天气的指标。（4）相对湿度和PM2.5是决定能见度大小的关键因子,其对能见度的影响体现出明显的阶段性特征,当相对湿度〈90%时,PM2.5浓度对能见度的作用强于相对湿度,是影响能见度变化的主要因子,但随着相对湿度的增大,其对能见度的影响相对增强,当能见度降至1 km以下时,相对湿度成为影响能见度变化的主要因子。     

Characteristics of Aerosol Pollution Under Different Visibility Conditions in Winter in a Coastal Mega-City in China

To investigate chemical profiles and formation mechanisms of aerosol particles in winter haze events,comprehensive measurements including hourly concentrations of PM2.5 and water-soluble inorganic ions and related gasphase precursors were conducted via an online monitoring system from January to March of 2016 in Shenzhen, a coastal mega-city in south China. In this study, high concentrations of PM2.5, NO2 and lower levels of O3 were observed during haze periods in comparison with clear days(Visibility15 km). The major secondary ionic species were NH+4、NO-3 and SO2-4, which varied significantly on haze and clear days. The ratio of NO-3/SO2-4 in haze days was greater than that on clear days and tended to be larger when air pollution became more serious. At the same time, compared with previous studies, it has been found that the ratio has been increasing gradually in Shenzhen, indicating that the motor vehicle exhaust emissions have a more and more important impact on air quality in Shenzhen. Sulfur oxidation rate(SOR) and nitrogen oxidation rate(NOR) was higher during the haze period than that in clean days, indicating efficient gas to particle conversion. Further analysis shows that high concentrations of sulfate might be explained by aqueous oxidation,but gas-phase reactions might dominate nitrate formation. This study also highlights that wintertime nitrate formation can be an important contributor to aerosol particles, especially during haze periods.