利用SPAMS研究南宁市四季细颗粒物的化学成分及污染来源

为研究南宁市四季大气颗粒物的化学成分及污染来源,利用单颗粒气溶胶质谱仪(single particle aerosol mass spectrometer,SPAMS)对南宁市2015年四季大气细颗粒物进行观测.SPAMS所测得4个观测阶段大气细颗粒物数浓度与细颗粒物质量浓度线性相关系数均在0.75以上,在一定程度上颗粒物数浓度可反映大气污染状况.南宁市四季大气细颗粒物平均质谱图体现出冬、春两季二次反应生成的污染物质较多.利用自适应共振神经网络分类方法对细颗粒物化学成分进行分类,南宁市细颗粒物各化学成分数浓度占比和污染来源在四季均有差异,且化学成分能体现污染来源.冬季元素碳最高,对应较高的燃煤源;秋季有机碳最高,对应较高的机动车尾气源;夏季富钾颗粒、左旋葡聚糖和矿物质较高,对应较高的生物质燃烧源和扬尘源;春季富钠颗粒和重金属略高.在污染升高过程,生物质燃烧源和燃煤源等贡献较大.     

喷泉产生的细菌气溶胶空间分布特性

为阐明喷泉产生的细菌气溶胶空间分布特性,利用大肠杆菌NK5449作为试验菌株,通过喷泉喷洒试验,使用安德森六级空气采样器采集喷泉周围空间的细菌气溶胶,研究各级细菌气溶胶的浓度和粒径分布特征和变化规律,并分析其与液滴直径的相关性.结果表明,在高度0.75~1.75 m,距离喷头0.5~3 m的范围内,细菌气溶胶总浓度在(38±15)~(676±92)CFU·m-3之间,并随着高度的增加和与喷头之间水平距离的增大而逐渐降低,且与液滴直径呈显著负相关(P0.05);随着与喷头水平距离的增大,粒径大于4.7μm的细菌气溶胶粒子所占比例出现先降后升的变化趋势;而粒径在2.1~4.7μm之间的粒子所占比例则是先升后降.与喷头水平距离0.5 m以外的各点,细菌气溶胶粒子的粒径大都集中在1.1~4.7μm范围内.距离喷泉较远处的人吸入小粒径细菌气溶胶的风险不容忽视.     

华北平原灰霾天气下大气气溶胶的单颗粒分析

为分析灰霾期间单颗粒气溶胶化学组成和混合状态,于2014年12月9日—2015年1月10日,使用单颗粒气溶胶质谱仪（SPAMS）表征华北平原郑州市中牟县的气溶胶颗粒.结果表明:灰霾期（H1:20141213T19:00—20141215T10:00;H2:20150102T10:00—20150106T03:00）和清洁期（C1:20141215T18:00—20141217T18:00;C2:20141231T16:00—20150101T20:00）大气颗粒物种类相同,主要分为有机碳（OC）、元素碳（EC）、生物质燃烧颗粒（BB）、元素碳有机碳（ECOC）、钾二次颗粒（K-Secondary）、矿尘（Dust）以及重金属颗粒（HM）7类.C1时间段,ECOC颗粒占比最高,占总颗粒数的49.8%;其次是OC和EC颗粒物,二者分别占总颗粒数的16.5%和10.8%.H1时间段,K-Secondary颗粒的占比（31.3%）最高;其次是OC和EC颗粒,二者分别占总颗粒数的23.1%和20.2%.清洁期与灰霾期质谱差分结果表明,清洁期颗粒物中含有C₃H+、C₄H₃+、C₅H₃+等有机碳碎片峰,而灰霾期颗粒物中NO₃-、HSO₄-、NO₂-等组分的信号强度显著大于清洁期.混合状态分析表明,从清洁期到灰霾期的过程中,主要颗粒物与NO₃-和HSO₄-的混合程度显著增强.清洁期与灰霾期单颗粒化学组成与混合状态的对比分析表明,清洁期新鲜排放的含碳气溶胶在灰霾期不断老化,单颗粒中二次无机组分增加,气溶胶整体老化严重.此外,灰霾期（H2）EC颗粒占总颗粒数的比例增至18.1%,并且与NO₃-、HSO₄-二次组分的混合状态增强,使平均能见度降低为4.0 km.研究显示,郑州大气能见度主要受化学组分、颗粒物混合状态和污染物质量浓度的影响.      

轻型汽油车排放颗粒物数浓度和粒径分布特征

我国机动车颗粒物排放研究多集中于重型柴油车,对于轻型汽油车的研究相对较少.本研究对3辆缸内直喷(GDI)汽车和1辆进气道喷射(PFI)汽车排放颗粒物的数浓度与粒径分布进行测试,并利用两台不同检测下限的颗粒物冷凝生长计数器(CPC)对轻型汽油车颗粒物实际排放水平进行了探究.结果表明,GDI汽车排放的颗粒物数浓度高于PFI汽车一个数量级,冷启动下颗粒物主要在测试循环前200 s大量产生,GDI汽车排放颗粒物数浓度与工况速度变化关系密切,而PFI汽车变化相对较小.GDI与PFI汽车排放的颗粒物粒径分布均具有核模态和积聚模态两个特征峰,核模态颗粒物峰值粒径约为20~27 nm,积聚模态约为80~95 nm.粒径检测下限为2.5 nm的UCPC测得的颗粒物数浓度比法规使用的粒径测量下限为23 nm的CPC测量结果分别高出35.0%(GDI)和50.4%(PFI).表明喷油技术是影响颗粒物数量排放水平的关键因素,法规测试会低估轻型汽油车实际颗粒物排放水平.     

Evaluation of the influence of El Niño–Southern Oscillation on air quality in southern China from long-term historical observations

•Strong ENSO influence on AOD is found in southern China region. •Low AOD occurs in El Niño but high AOD occurs in La Niña events in southern China. •Angstrom exponent anomalies reveals the circulation pattern during each ENSO phase. •ENSO exerts large influence (70.5%) on annual variations of AOD during 2002–2020. •Change of anthropogenic emissions is the dominant driver for AOD trend (2002–2020). Previous studies demonstrated that the El Niño–Southern Oscillation (ENSO) could modulate regional climate thus influencing air quality in the low-middle latitude regions like southern China. However, such influence has not been well evaluated at a long-term historical scale. To filling the gap, this study investigated two-decade (2002 to 2020) aerosol concentration and particle size in southern China during the whole dynamic development of ENSO phases. Results suggest strong positive correlations between aerosol optical depth (AOD) and ENSO phases, as low AOD occurred during El Niño while high AOD occurred during La Niña event. Such correlations are mainly attributed to the variation of atmospheric circulation and precipitation during corresponding ENSO phase. Analysis of the angstrom exponent (AE) anomalies further confirmed the circulation pattern, as negative AE anomalies is pronounced in El Niño indicating the enhanced transport of sea salt aerosols from the South China Sea, while the La Niña event exhibits positive AE anomalies which can be attributed to the enhanced import of northern fine anthropogenic aerosols. This study further quantified the AOD variation attributed to changes in ENSO phases and anthropogenic emissions. Results suggest that the long-term AOD variation from 2002 to 2020 in southern China is mostly driven (by 64.2%) by the change of anthropogenic emissions from 2002 to 2020. However, the ENSO presents dominant influence (70.5%) on year-to-year variations of AOD during 2002–2020, implying the importance of ENSO on varying aerosol concentration in a short-term period.     

Particle-bound polycyclic aromatic hydrocarbons in typical urban of Yunnan-Guizhou Plateau: Characterization,sources and risk assessment

• The sampling was conducted in city on the Yunnan-Guizhou Plateau for one year. • The groups of PAHs revealed their different environmental fates and migration paths. • Seasonal biomass burning could affect the concentration by long-distance transport. • Industrial sources and traffic emissions were the main contributor of PAHs. • Living in industrial areas or winter had higher health risk by exposure PAHs in PM_2.5. Monthly particle-phase ambient samples collected at six sampling locations in Yuxi, a high-altitude city on the edge of Southeast Asia, were measured for particle-associated PAHs. As trace substances, polycyclic aromatic hydrocarbons (PAHs) are susceptible to the influences of meteorological conditions, emissions, and gas-particulate partitioning and it is challenging job to precise quantify the source and define the transmission path. The daily concentrations of total PM_2.5-bound PAHs ranged from 0.65 to 80.76 ng/m³, with an annual mean of 11.94 ng/m³. Here, we found that the concentration of PM_2.5-bound PAHs in winter was significantly higher than that in summer, which was mainly due to source and meteorology influence. The increase of fossil combustion and biomass burning in cold season became the main contributors of PAHs, while precipitation and low temperature exacerbated this difference. According to the concentration variation trend of PM_2.5-bound PAHs and their relationship with meteorological conditions, a new grouping of PAHs is applied, which suggested that PAHs have different environmental fates and migration paths. A combination of source analysis and trajectory model supported local sources from combustion of fossil fuel and vehicle exhaust contributed to the major portion on PAHs in particle, but on the Indochina Peninsula the large number of pollutants emitted by biomass burning during the fire season would affect the composition of PAHs through long-range transporting. Risk assessment in spatial and temporal variability suggested that citizens living in industrial areas were higher health risk caused by exposure the PM_2.5-bound PAHs than that in other regions, and the risk in winter was three times than in summer.     

超大城市新粒子生成事件对云凝结核贡献分析

高浓度气溶胶在受人类活动影响的污染地区种类和组成非常复杂,因此,其环境和气候效应引起了广泛关注,但在超大城市背景下气溶胶粒子活化成为云凝结核的过程与边界层的相互作用尚不完全清楚.本研究基于北京（BJ）、上海（SH）、广州（GZ）的观测数据,选取3个城市的春季和冬季（北京冬季11月和广州冬季12月的连续观测,以及上海春季4月的加强观测）集成观测气溶胶数据和云凝结核同期观测的变化并结合其他污染物演化规律,对比分析了新粒子生成事件和环境变量演化对3个超大城市云凝结浓度形成的影响.结果表明,以用云凝结核（CCN）浓度与气溶胶（CN）数浓度的比值作为3个城市的活化率,北京CCN数浓度约为（500±200） #·cm^-3,CN最大浓度小于（1.0×10⁴±0.3×10⁴） #·cm^-3,活化率约为0.07%.上海CCN数浓度为（1500±500） #·cm^-3,CN最大浓度小于（98.0×10⁴±0.3×10⁴） #·cm^-3,最大活化率为0.05%.广州CCN数浓度为（150±30） #·cm^-3,CN最大浓度为（24.0×10³±0.3×10³） #·cm^-3,最大活化率为0.03%.本文旨在阐明气溶胶物理化学性质（粒子谱、化学成分、排放源等的时空演变特征）在不同排放源和大气边界层条件的影响下,造成不同类型的排放和输送过程对气溶胶活化率的影响,对比发现新粒子生成（NPF）期间CCN数浓度明显高于非新粒子生成（Non-NPF）时期,证明NPF发生时对CCN的活化率（AR）有显著的提升,在过饱和度SS=0.1%下,北京达到峰值在4×10^-3附近,广州的最大值约为17×10^-4,上海的最大值为3×10^-3.且在NPF期间气溶胶活化率显著增加,3个超大城市在NPF和Non-NPF期间,CCN数浓度与活化率的关系在上海尤其明显,化学成分包括有机物、硝酸盐和硫酸盐等物质也会影响超大城市地区气溶胶粒子的活化率,对比发现3个城市在NPF期间CCN数浓度和活化率都明显区别于其他时段.发现气溶胶的物理和化学性质以及与活化率的直接关系,可用以评估新粒子生成对区域大气环境（如霾）的影响,并估计气溶胶贡献为CCN的间接气候影响.     

负载过渡金属颗粒电极催化降解焦化废水尾水

制备以活性炭为载体,负载Ni、Fe、Co单元素和Ni-Fe、Co-Fe双元素的5种颗粒电极,用以降解模拟焦化废水尾水.结果显示,负载双元素的颗粒电极对模拟废水的处理效果要好于单元素,其中Ni-Fe/PAC降解性能最好,COD与TOC降解率可达70.1%和40.1%.Ni-Fe/PAC也具有最高的析氧电位和最低的Tafel斜率,分别为2.25V和86mV/dec;所负载的晶体结构为单质Ni和Fe,含有少量的铁氧化物.颗粒电极的添加,会导致出水呈碱性,Co的掺入导致碱性增大,而Fe的掺入有利于降低出水pH值.模拟废水中3类有机物在Ni-Fe/PAC上降解效果呈现为多环芳烃<杂环化合物<苯系物.Ni-Fe/PAC能催化·OH和新生态氢的产生,有机物的降解以间接氧化为主.     

南京雾过程对大气气溶胶谱分布及化学组成的影响

为探究南京地区雾过程对气溶胶粒子化学组成和尺度分布的影响,在2017年冬季的雾观测中平行收集了3级分档雾水和分粒径气溶胶样品,并对雾微物理量与气溶胶谱分布、3级分档雾水与雾前、雾中、雾后分粒径气溶胶化学组成对比分析。结果表明,2017年冬季南京第1次雾过程的雾滴液态水含量随粒径分布为不对称“V”型,最低值位于7μm处,第2次雾过程的雾滴液态水含量随粒径分布为3峰型,峰值分别位于5,15,21.5μm处。在雾形成、发展阶段,粒径<0.33μm的气溶胶质量浓度降低,粒径0.38μm气溶胶质量浓度升高,雾成熟阶段,气溶胶粒子质量浓度在全粒径段均达到最低,粒径0.38μm的气溶胶质量浓度大幅降低,与雾前相比,雾后气溶胶质量浓度峰值向大粒径方向移动。雾前,气溶胶水溶性离子组分富集在粒径<0.43μm的小粒子中,随着雾过程进行,成核作用和吸湿增长使得水溶性离子向较大粒径段富集。雾中新生成的气溶胶随着雾滴的蒸发被释放,导致雾后NO₃^-、SO₄^2-和NH₄⁺浓度升高。较小粒径的气溶胶中和率更高,雾形成初期的新生雾滴酸性较强,随着雾过程的进行逐渐中和,雾水pH值逐渐升高。     

四川盆地大气氨与氮氧化物排放对细颗粒物污染的影响及减排潜力

基于IASI、OMI与TROPOMI卫星数据识别了2008~2019年四川盆地氨与氮氧化物柱浓度的变化趋势,并进一步采用空气质量模型CMAQ对2019年冬季四川盆地氨排放的大气环境影响进行了研究,评估了氨与氮氧化物单独减排及氨与氮氧化物协同减排情景下对四川盆地颗粒物污染的影响.结果表明：2008~2012年四川盆地氮氧化物排放逐年升高随后在2013~2019年迅速下降,而氨柱浓度在2008~2013年期间较为稳定,自2014年起迅速增长.四川盆地氨排放的高值区主要集中在人为活动强烈的成都及周边地区和川南城市群以及农业源氨排放主导的川西北地区.铵根离子在川南城市群的PM_2.5当中占比高达11.4%,而对川西地区城市的PM_2.5贡献较低.敏感性实验结果表明,氨与氮氧化物协同减排50%能有效降低大气中硝酸铵与硫酸铵的浓度,从而减少细颗粒物污染,改善四川盆地区域环境空气质量.