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天津冬季两个典型污染过程高浓度无机气溶胶成因及来源分析
摘要点击 3134  全文点击 77  投稿时间:2023-06-06  修订日期:2023-08-08
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中文关键词  无机气溶胶  气象因素  区域传输  化学过程  天津
英文关键词  inorganic aerosol  meteorological parameters  regional transport  chemical process  Tianjin
作者单位E-mail
卢苗苗 天津市环境气象中心, 天津 300074
中国气象局-南开大学大气环境与健康研究联合实验室, 天津 300074 
lumiaomiao1027@126.com 
韩素芹 天津市环境气象中心, 天津 300074
中国气象局-南开大学大气环境与健康研究联合实验室, 天津 300074 
sq_han@126.com 
刘可欣 南开大学环境科学与工程学院, 天津市城市交通污染防治研究重点实验室, 天津 300071  
唐晓 中国科学院大气物理研究所大气边界层物理和大气化学国家重点实验室, 北京 100029  
孔磊 中国科学院大气物理研究所大气边界层物理和大气化学国家重点实验室, 北京 100029  
丁净 天津市环境气象中心, 天津 300074
中国气象局-南开大学大气环境与健康研究联合实验室, 天津 300074 
 
樊文雁 天津市环境气象中心, 天津 300074
中国气象局-南开大学大气环境与健康研究联合实验室, 天津 300074 
 
王自发 中国科学院大气物理研究所大气边界层物理和大气化学国家重点实验室, 北京 100029
中国科学院大气物理研究所国际气候与环境科学中心, 北京 100029
中国科学院大学地球与行星科学学院, 北京 100049 
 
中文摘要
      无机气溶胶是天津冬季霾天出现的主要成分,研究挑选了2020年1月污染天中两个典型的高浓度无机气溶胶(SIA)过程(CASE1和CASE2),利用观测数据和耦合了在线污染物来源追踪方法的大气化学传输模式NAQPMS综合探究了气象要素、区域输送和化学过程的影响.两个过程的ρ(SIA)均值分别为76.8 μg·m-3和66.0 μg·m-3,硝酸盐浓度高于硫酸盐和铵盐,均为硝酸盐为主导的污染过程.气象条件影响了无机气溶胶的生成,CASE1过程ρ(SIA)>80 μg·m-3对应的温度和相对湿度区间分别是[-6℃,0℃]、[2℃,4℃]和[50%,60%]、[80%,100%];CASE2过程对应的温度和相对湿度区间分别是[2℃,4℃]和[60%,70%].外来源对CASE1和CASE2过程SIA的平均贡献率为62.3%和22.1%,分别为区域传输主导和局地生成主导过程.CASE1本地排放对硝酸盐和硫酸盐的贡献分别为16.2 μg·m-3和8.2 μg·m-3,均高于外来源的贡献(31.7 μg·m-3和8.8 μg·m-3);CASE2过程本地排放对硝酸盐和硫酸盐的贡献分别为29.3 μg·m-3和25.1 μg·m-3,而外来源的贡献为8.1 μg·m-3和9.4 μg·m-3.这表明CASE1本地生成和外来源输送贡献造成硝酸盐高于硫酸盐浓度,而CASE2仅本地源造成硝酸盐浓度高于硫酸盐.两个污染过程气相氧化反应是无机气溶胶生成的首要来源,贡献率分别为48.9%和57.8%;非均相反应也是重要过程,对SIA的贡献率分别为48.1%和42.2%;液相反应的影响小.
英文摘要
      Inorganic aerosol is the main component of haze days in winter over Tianjin. In this study, two typical high concentrations of secondary inorganic aerosol (SIA) processes, defined as CASE1 and CASE2, were selected during polluted days in January 2020 over Tianjin, and the effects of meteorological factors, regional transport, and chemical processes were comprehensively investigated combined with observations and numerical models (WRF-NAQPMS). The average SIA concentrations in CASE1 and CASE2 were 76.8 μg·m-3 and 66.0 μg·m-3, respectively, and the nitrate concentration was higher than that of sulfate and ammonium, which were typical nitrate-dominated pollution processes. Meteorological conditions played a role in inorganic aerosol formation. The temperature of approximately -6-0℃ and 2-4℃ and the relative humidity of 50%-60% and 80%-100% would be suitable conditions for the high SIA concentration (>80 μg·m-3) in CASE1, whereas the temperature of approximately 2-4℃ and the relative humidity of 60%-70% would be suitable in CASE2. The average contribution rates of external sources to SIA in the CASE1 and CASE2 processes were 62.3% and 22.1%, which were regional transport-dominant processes and local emission-dominant processes, respectively. The contribution of the local emission of CASE1 to nitrate and sulfate was 16.2 μg·m-3 and 8.2 μg·m-3, respectively, higher than that of external sources (31.7 μg·m-3 and 8.8 μg·m-3). the local contribution of CASE2 to nitrate and sulfate was 29.3 μg·m-3 and 25.1 μg·m-3, respectively, whereas the contribution from external sources was 8.1 μg·m-3 and 9.4 μg·m-3, respectively. The quantitative result indicated that local formation and regional transport resulted in higher nitrate concentration than sulfate in CASE1, in contrast to only local sources in CASE2. The gas phase reaction was the main source of inorganic aerosol formation, contributing 48.9% and 57.8% in CASE1 and CASE2, respectively, whereas the heterogeneous reactions were also important processes, with contribution rates of 48.1% and 42.2% to SIA. The effect of aqueous phase reaction was negligible.

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