城市和边远地区大气汞的浓度、形态及影响因素
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摘要
大气汞的来源、时空分布特征以及变化影响因素等是近年来大气化学和气溶胶研究的重点之一。为深入理解大气汞的背景浓度,时空分布特征,大气转化机制,源汇特征以及长距离输送,本文以中国城市包括地处海陆交界的大型城市和中型城市以及北极地区作为监测对象,开展对比研究。主要结论如下：
(1)合肥市采样期间(2009年1月至6月)大气气态总汞TGM平均浓度是2.53±1.36ng/m3,浓度范围是0.40-12.34ng/m3。大气总汞的日变化特征是最大值出现在上午07：00-09：00,最小值出现在下午14：00-16：00(本地时间)。采样期间(2009年1月至6月)合肥大气颗粒态总汞TPM的平均浓度是310pg/m3,浓度范围是160-580pg/m3。大气可吸入颗粒态汞Hg-PM10和Hg-PM2.5的平均浓度分别为350pg/m3和280pg/m3。Hg-PM2.5的平均浓度是大气Hg-PM10平均浓度的80%,显示大气颗粒态汞呈现出倾向于附着细颗粒的现象。颗粒总汞浓度与污染物标志性元素和离子(Se、Pb、K+)的相关关系显示大气颗粒态汞与燃煤有最密切的相关关系,其次是生物质燃烧,最后是汽车尾气。
(2)珠江三角洲中心的万顷沙镇采样期间(2008年11月23日-12月22日)的大气气态总汞TGM平均浓度是2.94±2.02ng/m3,浓度范围是0.50-18.67ng/m3.大气总汞的日变化特征是最大值出现在7：00-8：00,最小值出现在14：00-16：00(本地时间)。下午大气汞最小值。下午的气态总汞最小值的出现与大气垂直混合和臭氧氧化有关。臭氧与TGM呈现明显的负相关关系。早上6：00-7：00的TGM的突然增加可能是因为温度升高造成的地表汞释放引起的。类似的TGM和CO及SO2的变化显示了潜在的人为来源,更深入的风向玫瑰图显示,西风可能从中国西南或者当地人为排放源带来高浓度的TGM。
(3)厦门市采样期间(2011年3月23日-6月7日)大气气态总汞TGM的平均浓度是3.34±1.94ng/m3,浓度范围是0.29-14.99ng/m3。大气总汞的日变化特征是最大值出现在上午06：00-07：00,最小值出现在下午17：00(本地时间)。夜间(18：00-06：00)TGM平均浓度为3.39ng/m3,昼间(06：00-18：00)TGM平均浓度为3.17ng/m3,夜间浓度要高于昼间7%。采样期间高TGM浓度时段分析显示,本地源的浓度和频率占绝大部分。采样期间(2011年3月21日-4月22日)GEM、RGM和Hgp的平均浓度分别为3.05±1.08ng/m3、20.63±8.14pg/m3和36.58±14.78pg/m3。GEM占大气总汞的97.98%,RGM占大气总汞的0.845%,Hgp占大气总汞的1.175%。三种组分相互之间的相关系数分别是：R2(GEM-Hgp)=0.3311, R2(GEM-RGM)=0.5026, R2(RGM-Hgp)=0.5513。
(4)第四次北极考察走航期间(2010年7月1日-9月20)大气TGM平均浓度为1.99±0.89ng/m3。浓度范围是0.42-8.97ng/m3。不同海域去回程的大气气态总汞的浓度分别为：日本海去程和回程TGM浓度分别为0.89±0.16ng/m3和3.41±1.78ng/m3；鄂霍次克海去回程的平均浓度分别为0.764±0.15ng/m3和2.68±0.78ng/m3；白令海的去回程平均浓度分别为1.21±0.36ng/m3和2.62±0.38ng/m3；北极圈内开阔水域(N°66-N°75)的TGM平均浓度为1.85±0.53ng/m3；浮冰区(N°75-N°85)的平均浓度为2.12±0.54ng/m3；永久冰区(N°85-N°90)的平均浓度为2.034±0.52ng/m。日本海和鄂霍次克海去程TGM浓度水平分别为0.89±0.16ng/m3和0.76±0.15ng/m3,显示在这两个海域很可能是全球大气总汞的一个“汇”。北极圈内浮冰区TGM浓度值高于永久冰区和开阔水域,显示海冰融化可能是大气汞浓度高值的一个重要来源。
The source, temporal and influencing factor of atmospheric mercury is one of the research focuses on atmospheric chemistry and aerosols. In order to better understand the background concentration of atmospheric mercury, the spatial and temporal distribution characteristics of atmospheric transformation mechanism, characteristics and long-distance transmission of the sources and sinks, atmospheric mercury in large and medium-sized cities and the Arctic were selected to monitor and comparative study.The main conclusions are as follows:
(1) Atmospheric mercury in Hefei.TGM concentration in Hefei was2.53±1.36ng/m3and range was0.40-12.34ng/m3in the period January2009to June. The TGM concentration reaches its maximum in the morning07:00-09:00and minimize during14:00-16:00.The average concentration of atmospheric particulate total mercury (TPM) in Hefei was310pg/m3and ranged from160pg/m3to580pg/m3(January2009to June).The average concentration of inhalable particulate mercury (Hg-PM10and Hg-PM2.5) were350pg/m3and280pg/m3(April2008-2009May),the concentration of Hg-PM2.5accounting for80%of the concentration of Hg-PM10, this means that particulate mercury tend to be attached to the fine particles. In the sampling period, the largest contribution to particulate mercury is coal, followed by biomass burning, vehicle exhaust is the lowest. The correlation between TPM and TGM showed a positive from January to mid-March and a negative from mid-March to mid-May.
(2) Atmospheric mercury in the Pearl River Delta. The TGM concentration in the town of Wanqingsha was2.94±2.02ng/m3and ranged from0.50to18.67ng/m3(November23,2008to December22). The TGM concentration reaches its maximum in the morning07:00-08:00and down to its minimum in the afternoon14:00-16:00. The average concentration in the night (18:00-6:00) was3.12ng/m3and the average concentration in the daytime (6:00-18:00) was2.74ng/m3.42.55%of the high concentrations (>8ng/m3) was come from Dongguan direction and57.45%from the direction of Shenzhen and Hong Kong. The TGM and temperature showing a significant negative correlation (R2=0.8458). The TGM and ozone also showing a significant negative correlation (p<0.01, r=-0.864)
(3) Atmospheric mercury in Xiamen. The TGM average concentration in Xiamen was3.34±1.94ng/m3and ranged from0.29to14.99ng/m3(March23,2011to June7). The TGM concentration reached the maximum value in the morning06:00-07:00and the minimum value in the afternoon17:00. The TGM average concentration in night (18:00-06:00) was3.39ng/m3and in daytime (06:00-18:00) was3.17ng/m3, the former than the latter7%. In the sampling period, the high TGM concentrations were mostly from local source and few from the long-distance transmission source. In the sampling period (March21,2011to2011), the average concentration of GEM. RGM and Hgp were3.05±1.08ng/m3,20.63±8.14pg/m3and36.58±14.78pg/m3. GEM accounted for97.98%of the total atmospheric mercury, the RGM accounted for0.845%of the total atmospheric mercury, Hgp accounted for1.175%of the total atmospheric mercury. Correlation coefficient of GEM-Hgp, GEM-RGM and RGM-Hgp all showed a positive correlation. The R2(GEM-Hgp)=0.3311, the R2(GEM-RGM), R2(RGM-Hgp R2=0.5513.
(4) Atmosphere mecury in Fourth National Arctic Research Expedition. The TGM average concentration in the entire route (July1,2010to September20) was1.99±0.89ng/m3and ranged from0.42to8.97ng/m3. The TGM concentrations in Sea of Japan during the round-trip voyage were0.89±0.16ng/m3and3.41±1.78ng/m3respectively; The TGM concentrations in Sea of Okhotsk during the round-trip voyage were0.76±0.15ng/m3and2.68±0.78ng/m3respectively; The TGM concentrations in Bering Sea during the round-trip voyage were1.21±0.36ng/m3and2.62±0.38ng/m3respectively.The TGM concentration in open waters of the Arctic Circle (N°66-N°75) was1.85±0.53ng/m3. The TGM concentration in ice floes district (N°75-N°85) was2.12±0.54ng/m3. The TGM concentration in permanent ice(N°85-N°90) was2.03±0.52ng/m3. Sea of Japan and Okhotsk may be sinks of the TGM.The TGM concentration values in ice floes distrct was higher than these in permanent ice and open waters,which means that the sea ice melting might be an important reason of the high value of the TGM concentration.
(1)合肥市采样期间(2009年1月至6月)大气气态总汞TGM平均浓度是2.53±1.36ng/m3,浓度范围是0.40-12.34ng/m3。大气总汞的日变化特征是最大值出现在上午07：00-09：00,最小值出现在下午14：00-16：00(本地时间)。采样期间(2009年1月至6月)合肥大气颗粒态总汞TPM的平均浓度是310pg/m3,浓度范围是160-580pg/m3。大气可吸入颗粒态汞Hg-PM10和Hg-PM2.5的平均浓度分别为350pg/m3和280pg/m3。Hg-PM2.5的平均浓度是大气Hg-PM10平均浓度的80%,显示大气颗粒态汞呈现出倾向于附着细颗粒的现象。颗粒总汞浓度与污染物标志性元素和离子(Se、Pb、K+)的相关关系显示大气颗粒态汞与燃煤有最密切的相关关系,其次是生物质燃烧,最后是汽车尾气。
(2)珠江三角洲中心的万顷沙镇采样期间(2008年11月23日-12月22日)的大气气态总汞TGM平均浓度是2.94±2.02ng/m3,浓度范围是0.50-18.67ng/m3.大气总汞的日变化特征是最大值出现在7：00-8：00,最小值出现在14：00-16：00(本地时间)。下午大气汞最小值。下午的气态总汞最小值的出现与大气垂直混合和臭氧氧化有关。臭氧与TGM呈现明显的负相关关系。早上6：00-7：00的TGM的突然增加可能是因为温度升高造成的地表汞释放引起的。类似的TGM和CO及SO2的变化显示了潜在的人为来源,更深入的风向玫瑰图显示,西风可能从中国西南或者当地人为排放源带来高浓度的TGM。
(3)厦门市采样期间(2011年3月23日-6月7日)大气气态总汞TGM的平均浓度是3.34±1.94ng/m3,浓度范围是0.29-14.99ng/m3。大气总汞的日变化特征是最大值出现在上午06：00-07：00,最小值出现在下午17：00(本地时间)。夜间(18：00-06：00)TGM平均浓度为3.39ng/m3,昼间(06：00-18：00)TGM平均浓度为3.17ng/m3,夜间浓度要高于昼间7%。采样期间高TGM浓度时段分析显示,本地源的浓度和频率占绝大部分。采样期间(2011年3月21日-4月22日)GEM、RGM和Hgp的平均浓度分别为3.05±1.08ng/m3、20.63±8.14pg/m3和36.58±14.78pg/m3。GEM占大气总汞的97.98%,RGM占大气总汞的0.845%,Hgp占大气总汞的1.175%。三种组分相互之间的相关系数分别是：R2(GEM-Hgp)=0.3311, R2(GEM-RGM)=0.5026, R2(RGM-Hgp)=0.5513。
(4)第四次北极考察走航期间(2010年7月1日-9月20)大气TGM平均浓度为1.99±0.89ng/m3。浓度范围是0.42-8.97ng/m3。不同海域去回程的大气气态总汞的浓度分别为：日本海去程和回程TGM浓度分别为0.89±0.16ng/m3和3.41±1.78ng/m3；鄂霍次克海去回程的平均浓度分别为0.764±0.15ng/m3和2.68±0.78ng/m3；白令海的去回程平均浓度分别为1.21±0.36ng/m3和2.62±0.38ng/m3；北极圈内开阔水域(N°66-N°75)的TGM平均浓度为1.85±0.53ng/m3；浮冰区(N°75-N°85)的平均浓度为2.12±0.54ng/m3；永久冰区(N°85-N°90)的平均浓度为2.034±0.52ng/m。日本海和鄂霍次克海去程TGM浓度水平分别为0.89±0.16ng/m3和0.76±0.15ng/m3,显示在这两个海域很可能是全球大气总汞的一个“汇”。北极圈内浮冰区TGM浓度值高于永久冰区和开阔水域,显示海冰融化可能是大气汞浓度高值的一个重要来源。
The source, temporal and influencing factor of atmospheric mercury is one of the research focuses on atmospheric chemistry and aerosols. In order to better understand the background concentration of atmospheric mercury, the spatial and temporal distribution characteristics of atmospheric transformation mechanism, characteristics and long-distance transmission of the sources and sinks, atmospheric mercury in large and medium-sized cities and the Arctic were selected to monitor and comparative study.The main conclusions are as follows:
(1) Atmospheric mercury in Hefei.TGM concentration in Hefei was2.53±1.36ng/m3and range was0.40-12.34ng/m3in the period January2009to June. The TGM concentration reaches its maximum in the morning07:00-09:00and minimize during14:00-16:00.The average concentration of atmospheric particulate total mercury (TPM) in Hefei was310pg/m3and ranged from160pg/m3to580pg/m3(January2009to June).The average concentration of inhalable particulate mercury (Hg-PM10and Hg-PM2.5) were350pg/m3and280pg/m3(April2008-2009May),the concentration of Hg-PM2.5accounting for80%of the concentration of Hg-PM10, this means that particulate mercury tend to be attached to the fine particles. In the sampling period, the largest contribution to particulate mercury is coal, followed by biomass burning, vehicle exhaust is the lowest. The correlation between TPM and TGM showed a positive from January to mid-March and a negative from mid-March to mid-May.
(2) Atmospheric mercury in the Pearl River Delta. The TGM concentration in the town of Wanqingsha was2.94±2.02ng/m3and ranged from0.50to18.67ng/m3(November23,2008to December22). The TGM concentration reaches its maximum in the morning07:00-08:00and down to its minimum in the afternoon14:00-16:00. The average concentration in the night (18:00-6:00) was3.12ng/m3and the average concentration in the daytime (6:00-18:00) was2.74ng/m3.42.55%of the high concentrations (>8ng/m3) was come from Dongguan direction and57.45%from the direction of Shenzhen and Hong Kong. The TGM and temperature showing a significant negative correlation (R2=0.8458). The TGM and ozone also showing a significant negative correlation (p<0.01, r=-0.864)
(3) Atmospheric mercury in Xiamen. The TGM average concentration in Xiamen was3.34±1.94ng/m3and ranged from0.29to14.99ng/m3(March23,2011to June7). The TGM concentration reached the maximum value in the morning06:00-07:00and the minimum value in the afternoon17:00. The TGM average concentration in night (18:00-06:00) was3.39ng/m3and in daytime (06:00-18:00) was3.17ng/m3, the former than the latter7%. In the sampling period, the high TGM concentrations were mostly from local source and few from the long-distance transmission source. In the sampling period (March21,2011to2011), the average concentration of GEM. RGM and Hgp were3.05±1.08ng/m3,20.63±8.14pg/m3and36.58±14.78pg/m3. GEM accounted for97.98%of the total atmospheric mercury, the RGM accounted for0.845%of the total atmospheric mercury, Hgp accounted for1.175%of the total atmospheric mercury. Correlation coefficient of GEM-Hgp, GEM-RGM and RGM-Hgp all showed a positive correlation. The R2(GEM-Hgp)=0.3311, the R2(GEM-RGM), R2(RGM-Hgp R2=0.5513.
(4) Atmosphere mecury in Fourth National Arctic Research Expedition. The TGM average concentration in the entire route (July1,2010to September20) was1.99±0.89ng/m3and ranged from0.42to8.97ng/m3. The TGM concentrations in Sea of Japan during the round-trip voyage were0.89±0.16ng/m3and3.41±1.78ng/m3respectively; The TGM concentrations in Sea of Okhotsk during the round-trip voyage were0.76±0.15ng/m3and2.68±0.78ng/m3respectively; The TGM concentrations in Bering Sea during the round-trip voyage were1.21±0.36ng/m3and2.62±0.38ng/m3respectively.The TGM concentration in open waters of the Arctic Circle (N°66-N°75) was1.85±0.53ng/m3. The TGM concentration in ice floes district (N°75-N°85) was2.12±0.54ng/m3. The TGM concentration in permanent ice(N°85-N°90) was2.03±0.52ng/m3. Sea of Japan and Okhotsk may be sinks of the TGM.The TGM concentration values in ice floes distrct was higher than these in permanent ice and open waters,which means that the sea ice melting might be an important reason of the high value of the TGM concentration.
引文
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