北京大气中醛酮化合物污染特征与来源分析
Pollution Characterization and Source Analyses of Carbonyl Compounds in the Ambient Air in Beijing
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摘要: 利用2,4-二硝基苯肼(DNPH)采样管采样-高效液相色谱仪(HPLC)分析的测定方法,分别于2020年1月~12月对北京市城市评价点位车公庄大气中的13种醛酮化合物开展6天1次的常规监测;于2020年5月26日~5月29日9:00~19:00开展每小时1次的加密监测;于2020年9月17日~9月21日对北京城市评价点车公庄和城市边界点永乐店开展每天3次的同步监测。研究结果表明,2020年北京大气中醛酮化合物总浓度为25.1 μg/m3±8.5 μg/m3,主要组分为甲醛、乙醛和丙酮,丙酮>甲醛>乙醛;丙酮占比43%,甲醛占比31%,乙醛占比16%。臭氧生成潜势(OFP)甲醛>乙醛>丙酮,甲醛占比66%,乙醛占比23%。季节变化中,醛酮化合物总浓度呈现“夏季>春季>秋季>冬季”的污染特征,主要与夏季气温高、光照强,溶剂蒸发排放高于其他季节及夏季污染物气-颗分配系数低于冬季,醛酮化合物从气相转移到颗粒相的量随之减少有关。日变化中,甲醛和乙醛显现“双峰”特征,在12:00~15:00达到第一个峰值,与该时段温度和光照增强,且光化学反应生成醛酮化合物的速率高于消耗速率,甲醛和乙醛主要来自二次光化学反应有关;17:00~19:00出现第二个峰值,与交通晚高峰期间机动车排放有关。丙酮整体较稳定,交通晚高峰略有抬升,与其具有较长的大气寿命,在大气中逐步累积有关。5月29日数表明醛酮化合物除受光照和机动车影响外,还受温度、湿度和风速等气象因素影响。9月同步监测期间,城市评价点位车公庄和城市边界点位永乐店醛酮化合物总量分别为24.4 μg/m3±7.8 μg/m3和24.1μg/m3±7.5 μg/m3。车公庄点位的正丁醛和甲基丙烯醛占比均为4%,较永乐店均低2%,表明相对于车公庄受机动车及光化学反应影响稍大,永乐店受工业排放影响更大。从特征比值看,常规监测期间北京大气中C1/C2比值范围为0.8~3.6,春、夏、秋、冬C1/C2比值分别为1.9、2.4、1.7和1.2,年均值为1.7,与典型大城市大气比例特征一致,说明北京大气中醛酮化合物也主要来源于人类活动。Abstract: The concentrations of 13 kinds of carbonyl compounds in the ambient air in Beijing were measured by 2,4-dinitrophenylhydrazine(DNPH) and high performance liquid chromatography(HPLC),including routine monitoring once every 6 days,the hourly monitoring from 9:00 to 19:00 from May 26th to May 28th , 2020 ,where in Chegongzhuang which is an urban site; the synchronous monitoring three times a day from September 17th to September 21th, 2020 for Chegongzhuang and Yongledian site which is a boundary site of Beijing.Results were shown as follows,the total concentration of carbonyl compounds in the ambient air in Beijing was 25.1 μg/m3±8.5 μg/m3. The main components are formaldehyde, acetaldehyde and acetone, acetone > formaldehyde > acetaldehyde, in which acetone accounted for 43%, formaldehyde accounted for 31% and acetaldehyde accounted for 16%. Ozone generation potential (OFP) was formaldehyde > acetaldehyde > acetone, in which formaldehyde accounted for 66% and acetaldehyde accounted for 23%. In the seasonal variation,the total concentration of carbonyl compounds showed the characteristics of " summer > spring > autumn > winter" during 2020,which was mainly due to higher temperature,light intensity and more solvent evaporation emissions in summer than other seasons, at the same time gas particle partition coefficient of pollutants in summer is lower than in winter,the amount of carbonyl compounds transferred from the gas to the particle decreases accordingly.In the diurnal variation, formaldehyde and acetaldehyde showed "double peak" characteristics, the first peak appeared from 12:00 to 15:00, which was related to the enhancement of temperature and light, and the rate of photochemical reaction to produce aldehyde and ketone compounds was higher than the consumption.Formaldehyde and acetaldehyde mainly comed from the secondary photochemical reaction.The second peak appeared from17:00 to 19:00, which was related to motor vehicle emissions. Acetone is stable relatively and rises slightly at the traffic time in the afternoon, which was related to long atmospheric life and gradual accumulation. The data of May 29th indicated that carbonyl compounds are affected not only by light and motor vehicles, but also by meteorological factors such as temperature, humidity and wind speed.During the synchronous monitoring of Chegongzhuang and Yongledian in September, the concentrations of carbonyl compounds at the two stations were 24.4 μg/m3±7.8 μg/m3 and 24.1 μg/m3±7.5 μg/m3 respectively. The proportion of n-butyraldehyde and methacrolein at Chegongzhuang site is 4%, which is 2% lower than that of Yongledian site, it showed that Yongledian was more affected by industrial emissions compared to Chegongzhuang.The C1/C2 ratio in the ambient air in Beijing during the routine monitoring ranges from 0.8 to 3.6, and the C1/C2 ratios in spring, summer, autumn and winter were 1.9, 2.4, 1.7 and 1.2 respectively, the average value was 1.7. Consistent with the atmospheric proportion characteristics of typical large cities, the carbonyl compounds in the ambient air in Beijing also mainly come from human activities.
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Key words:
- Beijing /
- carbonyl compounds /
- pollution characterization /
- ozone generation potential
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