华东高山背景点大气气态汞含量与传输特征
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摘要
利用高时间分辨率自动测汞仪(Tekran2537B)于2017年6月～2018年5月对武夷山气态元素汞(GEM)进行了连续1a的观测.结果表明,武夷山GEM年均浓度为(1.70±0.43)ng/m3,稍高于北半球背景值,表明武夷山受到一定程度的大气汞污染.GEM浓度表现为冬季>秋季>春季>夏季,季风和风速是影响武夷山GEM季节变化的主要因素.武夷山四季GEM表现为不同的日变化特征,早上8:00之后,春秋季GEM继续呈现下降趋势,其他季节则呈现先升后降再上升,并在晚上不同时刻出现峰值.GEM值白天低于晚上,这与风速和汞的长距离迁移有关.后向轨迹和浓度权重轨迹分析结果表明,偏西风背景下污染气团经江西向武夷山输送是大气汞迁移的主要路径,而江西和福建中北部为武夷山大气汞污染的潜在源区.△GEM/△CO值表明武夷山GEM汞污染主要来源于人为工业排放,生物质燃烧贡献较弱.
Gaseous elemental mercury(GEM) was monitored continuously at Wuyi Mountain using the high-resolution automatic atmospheric mercury vapor analyzer(Tekran 2537 B) from June 2017 to May 2018. The annual mean concentration of GEM was(1.70±0.43)ng/m3, slightly higher than background level in the northern hemisphere, suggesting that the atmosphere of the Wuyi Mountain was polluted to some extent. The GEM varied in different seasons, with the highest concentration observed in winter, followed by fall, spring, and summer. The monsoon and wind speed contributed mostly to the seasonal variation. Different diurnal variation characteristics of GEM were found in four seasons. In spring and autumn, GEM continued to decrease after 8:00 am, however, in other seasons, GEM showed "increase-decrease-increase" and peaked at different times in nighttime. The GEM in the daytime were generally higher than those in the nighttime, which may related to the wind speed and long distance transport of mercury. Backward trajectory and concentration-weighted trajectory indicated that polluted air masses to the Wuyi Mountain via Jiangxi province under westerly wind was the main path of atmospheric mercury migration. In addition, Jiangxi province and north-central Fujian province were the potential source areas of GEM at the Wuyi Mountain. The values of △GEM/△CO suggested that mercury pollution at the Wuyi Mountain was mainly affected by anthropogenic mercury emissions, while biomass burning did little contribution.
Gaseous elemental mercury(GEM) was monitored continuously at Wuyi Mountain using the high-resolution automatic atmospheric mercury vapor analyzer(Tekran 2537 B) from June 2017 to May 2018. The annual mean concentration of GEM was(1.70±0.43)ng/m3, slightly higher than background level in the northern hemisphere, suggesting that the atmosphere of the Wuyi Mountain was polluted to some extent. The GEM varied in different seasons, with the highest concentration observed in winter, followed by fall, spring, and summer. The monsoon and wind speed contributed mostly to the seasonal variation. Different diurnal variation characteristics of GEM were found in four seasons. In spring and autumn, GEM continued to decrease after 8:00 am, however, in other seasons, GEM showed "increase-decrease-increase" and peaked at different times in nighttime. The GEM in the daytime were generally higher than those in the nighttime, which may related to the wind speed and long distance transport of mercury. Backward trajectory and concentration-weighted trajectory indicated that polluted air masses to the Wuyi Mountain via Jiangxi province under westerly wind was the main path of atmospheric mercury migration. In addition, Jiangxi province and north-central Fujian province were the potential source areas of GEM at the Wuyi Mountain. The values of △GEM/△CO suggested that mercury pollution at the Wuyi Mountain was mainly affected by anthropogenic mercury emissions, while biomass burning did little contribution.
引文
[1]Schroeder W H,Munthe J.Atmospheric mercury-an overview[J].Atmospheric Environment.1998,32:809-822.
[2]Daniel Obrist,Yannick Agnan,Martin Jiskra,et al.Tundra uptake of atmospheric elemental mercury drives Arctic mercury pollution[J].Nature,2017,547:201-204.
[3]Fu X W,Feng X B,Zhu W Z,et al.Total gaseous mercury concentrations in ambient air in the eastern slope of Mt.Gongga,South-Eastern fringe of the Tibetan plateau,China[J].Atmospheric Environment,2008,42:970-979.
[4]Fu X W,Feng X B,Wang S F,et al.Temporal and spatial distributions of total gaseous mercury concentrations in ambient air in a mountainous area in southwestern China:implications for industrial and domestic mercury emissions in remote areas in China[J].Science of the Total Environment,2009,407:2306-2314.
[5]高志强,刘明,陈来国,等.广东南岭大气背景点气态元素汞含量变化特征[J].中国环境科学,2016,36(2):342-348.Gao Z Q,Liu M,Chen L G,et al.Variation characteristics of gaseous elemental mercury at Nanling mountain background station in Guangdong[J].China Environmental Science,2016,36(2):342-348.
[6]Fu X W,Feng X B,Dong Z Q,et al.Atmospheric gaseous elemental mercury(GEM)concentrations and mercury depositions at a high-altitude mountain peak in south China[J].Atmosphere Chemistry and Physics,2010,10:2425-2437.
[7]Fu X W,Feng X B,Liang P,et al.Temporal trend and sources of speciated atmospheric mercury at Waliguan GAW station,Northwestern China[J].Atmospheric Chemistry and Physics,2012,12:1951-1964.
[8]Wang X Zhang H,Lin C J,et al.Transboundary transport and deposition of Hg emission from springtime biomass burning in the Indo-China Peninsula[J].Journal of Geophysical Research:Atmospheres,2015,120:9758-9771,doi:10.1002/2015JD023525.
[9]Liu M,Chen L G,Xie D H,et al.Monsoon-driven transport of atmospheric mercury to the South China Sea from the Chinese mainland and Southeast Asia-Observation of gaseous elemental mercury at a background station in South China[J].Environment Science Pollution Research,2016,23:21631-21640.
[10]Ci Z J,Zhang X S,Wang Z W,et al.Atmospheric gaseous elemental mercury(GEM)over a coastal/rural site downwind of East China:Temporal variation and long-range transport[J].Atmospheric Environment,2011,45:2480-2487.
[11]Kim S H,Han Y J,Holsen T M,et al.Characteristics of atmospheric speciated mercury concentrations(TGM,Hg(II)and Hg(p)in Seoul,Korea[J].Atmospheric Environment,2009,43:3267-3274.
[12]Sheu G R,Lin N H,Wang J L,et al.Temporal distribution and potential sources of atmospheric mercury measured at a highelevation background station in Taiwan[J].Atmospheric Environment,2010,44:2393-2400.
[13]李舒,高伟,王书肖,等.上海崇明地区大气分形态汞污染特征[J].环境科学,2016,37(9):3290-3299.Li S,Gao W,Wang S X,et al.Characteristics of speciated atmospheric mercury in ChongMing island,Shanghai[J].Environmental Science,2016,37(9):3290-3299.
[14]Wang Y Q,Zhang X Y,Draxler R.TrajStat:GIS-based software that uses various trajectory statistical analysis methods to identify potential sources from long-term air pollution measurement data[J].Environ.Model&Soft,2009,24:938-939
[15]Cheng,I,Zhang,L,Blanchard,P,et al.Concentration-weighted trajectory approach to identifying potential sources of speciated atmospheric mercury at an urban coastal site in Nova Scotia,Canada[J].Atmospheric Chemistry and Physics,2013,13:6031-6048.
[16]Lindberg S,Bullock R,Ebinghaus R,et al.A synthesis of progress and uncertainties in attributing the sources of mercury in deposition[J].Ambio.,2007,36:19-32
[17]Valente R J,Shea C,Humes K,et al.Atmospheric mercury in the Great Smoky Mountains compared to regional and global levels[J].Atmospheric Environment,2007,41:1861-1873
[18]Fu X W,Feng X B,Shang L H,et al.Two years of measurements of atmospheric total gaseous mercury(TGM)at a remote site in Mt.Changbai area,Northeastern China[J].Atmospheric Chemistry and Physics,2012,12:4215-4226.
[19]Itsaso A M,álvaro C,Joseph W.B.Mercury Oxidation via Chlorine,Bromine,and Iodine under Atmospheric Conditions:Thermochemistry and Kinetics[J].The Journal of Physical and Chemistry A,2014,118(16):2959-2975
[20]Torbjorn B,Henning R.Oxidation of elemental mercury in the atmosphere,constraints imposed by global scale modelling[J].Journal of Atmospheric Chemistry,2001,40:191-212.
[21]Slemr F,Scheel H E.Trends in atmospheri c mercury concentrations at the summit of the Wank Mountain,southern Germany[J].Atmospheric Environment,1998,32(5):845-853.
[22]Holmes C D,Jacob D J,Corbitt E S,et al.Global atmospheric model for mercury including oxidation by bromine atoms[J].Atmosphere Chemistry and Physics,2010,10:12037-12057.
[23]苏彬彬.华东森林及高山背景区域臭氧变化特征及影响因素[J].环境科学,2013,34(7):2519-2525.Su B B.Characteristics and impact factors of O3 concentrations in Mountain background region of East China[J].Environmental Science,2013,34(7):2519-2525.
[24]苏彬彬,许椐洋,张若宇,等.区域传输对华东森林及高山背景点位大气污染物浓度的影响[J].环境科学,2014,35(8):2871-2877.Su B B,Xu J Y,Zhang R Y,et al.Influence of atmospheric transport on air pollution levels at mountain backround site of East China[J].Environmental Science,2014,35(8):2871-2877.
[25]Weiss-Penzias P,Jaffe D,Swartzendruber P,et al.Quantifying Asian and biomass burning sources of mercury using the Hg/CO ratio in pollution plumes observed at the Mount Bachelor Observatory[J].Atmospheric Environment,2007,41:4366-4379.
[26]Jaffe D,Prestbo E,Swartzendruber P,et al.Export of atmospheric mercury from Asia[J].Atmospheric Environment,2005,39:3029-3038.
[27]Fu X W,Zhang H,Lin C J,et al.Correlation slopes of GEM/CO,GEM/CO2,and GEM/CH4 and estimated mercury emissions in China,South Asia,the Indochinese peninsula,and Central Asia derived from observations in northwestern and southwestern China[J].Atmospheric Chemistry and Physics,2015,15:1013-1028.
[28]Weiss-Penzias P,Jaffe D,Swartzendruber P,et al.Observations of Asian air pollution in the free troposphere at Mount Bachelor Observatory during the spring of 2004[J].Journal of Geophysical Research,2006,111:D10304.doi:10.1029/2005JD06522.
[2]Daniel Obrist,Yannick Agnan,Martin Jiskra,et al.Tundra uptake of atmospheric elemental mercury drives Arctic mercury pollution[J].Nature,2017,547:201-204.
[3]Fu X W,Feng X B,Zhu W Z,et al.Total gaseous mercury concentrations in ambient air in the eastern slope of Mt.Gongga,South-Eastern fringe of the Tibetan plateau,China[J].Atmospheric Environment,2008,42:970-979.
[4]Fu X W,Feng X B,Wang S F,et al.Temporal and spatial distributions of total gaseous mercury concentrations in ambient air in a mountainous area in southwestern China:implications for industrial and domestic mercury emissions in remote areas in China[J].Science of the Total Environment,2009,407:2306-2314.
[5]高志强,刘明,陈来国,等.广东南岭大气背景点气态元素汞含量变化特征[J].中国环境科学,2016,36(2):342-348.Gao Z Q,Liu M,Chen L G,et al.Variation characteristics of gaseous elemental mercury at Nanling mountain background station in Guangdong[J].China Environmental Science,2016,36(2):342-348.
[6]Fu X W,Feng X B,Dong Z Q,et al.Atmospheric gaseous elemental mercury(GEM)concentrations and mercury depositions at a high-altitude mountain peak in south China[J].Atmosphere Chemistry and Physics,2010,10:2425-2437.
[7]Fu X W,Feng X B,Liang P,et al.Temporal trend and sources of speciated atmospheric mercury at Waliguan GAW station,Northwestern China[J].Atmospheric Chemistry and Physics,2012,12:1951-1964.
[8]Wang X Zhang H,Lin C J,et al.Transboundary transport and deposition of Hg emission from springtime biomass burning in the Indo-China Peninsula[J].Journal of Geophysical Research:Atmospheres,2015,120:9758-9771,doi:10.1002/2015JD023525.
[9]Liu M,Chen L G,Xie D H,et al.Monsoon-driven transport of atmospheric mercury to the South China Sea from the Chinese mainland and Southeast Asia-Observation of gaseous elemental mercury at a background station in South China[J].Environment Science Pollution Research,2016,23:21631-21640.
[10]Ci Z J,Zhang X S,Wang Z W,et al.Atmospheric gaseous elemental mercury(GEM)over a coastal/rural site downwind of East China:Temporal variation and long-range transport[J].Atmospheric Environment,2011,45:2480-2487.
[11]Kim S H,Han Y J,Holsen T M,et al.Characteristics of atmospheric speciated mercury concentrations(TGM,Hg(II)and Hg(p)in Seoul,Korea[J].Atmospheric Environment,2009,43:3267-3274.
[12]Sheu G R,Lin N H,Wang J L,et al.Temporal distribution and potential sources of atmospheric mercury measured at a highelevation background station in Taiwan[J].Atmospheric Environment,2010,44:2393-2400.
[13]李舒,高伟,王书肖,等.上海崇明地区大气分形态汞污染特征[J].环境科学,2016,37(9):3290-3299.Li S,Gao W,Wang S X,et al.Characteristics of speciated atmospheric mercury in ChongMing island,Shanghai[J].Environmental Science,2016,37(9):3290-3299.
[14]Wang Y Q,Zhang X Y,Draxler R.TrajStat:GIS-based software that uses various trajectory statistical analysis methods to identify potential sources from long-term air pollution measurement data[J].Environ.Model&Soft,2009,24:938-939
[15]Cheng,I,Zhang,L,Blanchard,P,et al.Concentration-weighted trajectory approach to identifying potential sources of speciated atmospheric mercury at an urban coastal site in Nova Scotia,Canada[J].Atmospheric Chemistry and Physics,2013,13:6031-6048.
[16]Lindberg S,Bullock R,Ebinghaus R,et al.A synthesis of progress and uncertainties in attributing the sources of mercury in deposition[J].Ambio.,2007,36:19-32
[17]Valente R J,Shea C,Humes K,et al.Atmospheric mercury in the Great Smoky Mountains compared to regional and global levels[J].Atmospheric Environment,2007,41:1861-1873
[18]Fu X W,Feng X B,Shang L H,et al.Two years of measurements of atmospheric total gaseous mercury(TGM)at a remote site in Mt.Changbai area,Northeastern China[J].Atmospheric Chemistry and Physics,2012,12:4215-4226.
[19]Itsaso A M,álvaro C,Joseph W.B.Mercury Oxidation via Chlorine,Bromine,and Iodine under Atmospheric Conditions:Thermochemistry and Kinetics[J].The Journal of Physical and Chemistry A,2014,118(16):2959-2975
[20]Torbjorn B,Henning R.Oxidation of elemental mercury in the atmosphere,constraints imposed by global scale modelling[J].Journal of Atmospheric Chemistry,2001,40:191-212.
[21]Slemr F,Scheel H E.Trends in atmospheri c mercury concentrations at the summit of the Wank Mountain,southern Germany[J].Atmospheric Environment,1998,32(5):845-853.
[22]Holmes C D,Jacob D J,Corbitt E S,et al.Global atmospheric model for mercury including oxidation by bromine atoms[J].Atmosphere Chemistry and Physics,2010,10:12037-12057.
[23]苏彬彬.华东森林及高山背景区域臭氧变化特征及影响因素[J].环境科学,2013,34(7):2519-2525.Su B B.Characteristics and impact factors of O3 concentrations in Mountain background region of East China[J].Environmental Science,2013,34(7):2519-2525.
[24]苏彬彬,许椐洋,张若宇,等.区域传输对华东森林及高山背景点位大气污染物浓度的影响[J].环境科学,2014,35(8):2871-2877.Su B B,Xu J Y,Zhang R Y,et al.Influence of atmospheric transport on air pollution levels at mountain backround site of East China[J].Environmental Science,2014,35(8):2871-2877.
[25]Weiss-Penzias P,Jaffe D,Swartzendruber P,et al.Quantifying Asian and biomass burning sources of mercury using the Hg/CO ratio in pollution plumes observed at the Mount Bachelor Observatory[J].Atmospheric Environment,2007,41:4366-4379.
[26]Jaffe D,Prestbo E,Swartzendruber P,et al.Export of atmospheric mercury from Asia[J].Atmospheric Environment,2005,39:3029-3038.
[27]Fu X W,Zhang H,Lin C J,et al.Correlation slopes of GEM/CO,GEM/CO2,and GEM/CH4 and estimated mercury emissions in China,South Asia,the Indochinese peninsula,and Central Asia derived from observations in northwestern and southwestern China[J].Atmospheric Chemistry and Physics,2015,15:1013-1028.
[28]Weiss-Penzias P,Jaffe D,Swartzendruber P,et al.Observations of Asian air pollution in the free troposphere at Mount Bachelor Observatory during the spring of 2004[J].Journal of Geophysical Research,2006,111:D10304.doi:10.1029/2005JD06522.