典型西南岩溶区工业城市降水酸化缓解原因探究——以柳州市为例
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摘要
利用柳州市环境保护监测站2013—2017年大气降水监测数据,分析近年来柳州岩溶区工业城市降水酸化缓解原因,并对离子来源进行探究.结果表明:①统计柳州近5年的降水pH值发现研究区降水酸化问题有了明显的改善,同时具有季节性差异,春冬季降水酸化相对夏秋季较重.②通过分析降水中主要离子组成及变化特征、计算中和因子(NF)和相对酸度(FA)发现,降水中主要离子浓度出现减少趋势,酸化类型逐渐向硫-硝酸混合型过渡,且99.97%的酸性离子被NH~+_4、Ca~(2+)等离子所中和,所以得出酸性物质的减少和碱性离子的中和作用可能是降水酸化改善的重要因素.③采用Hysplit模型对研究区降水酸化较严重的2016年(共60场)的降水水汽来源进行后向轨迹追踪及聚类分析,显示降水离子组成与浓度不仅与当地污染源有关,还与来自大陆内部西北和西南远距离物质输送有关.上述结果指示由于喀斯特化学风化作用、柳州市严格执行环保规定、大环境改善导致远程传输污染减弱等原因使得柳州市降水酸化情况得到极大改善.此外值得注意的是柳州市酸雨类型逐渐向硫-硝酸混合型过渡,指示随着工业污染的控制得到减弱,日益增长的机动车尾气排放或许成为研究区下一步治理重点方向.
According to the monitoring data of atmospheric precipitation in Liuzhou from 2013 to 2017, the effects of acid precipitation and its mitigation in the typical industrial karst areas of Southwest China were analyzed to trace the source of ions for the history of acidic precipitation. Our findings revealed that, in the past five years, the pH values increased slowly and had the obvious seasonal variation(pH values were lower in winter and spring than those in summer and fall). In this respect, the main ionic composition and variation of precipitation, the neutralization factor(NF) and the fractional acidity(AF) indicated that the ionic concentration of precipitation was still sulfur type with a reducing trend to sulfuric-nitrous mixed type and the 99.97% acid ions were neutralized by NH~+_4 and Ca~(2+) ions, suggesting that it might be the important factor to mitigating acid precipitation. Besides that, the Hysplit model was applied to trace and cluster the precipitation with 60 times in 2016. It was found that the compositions and concentrations of ions about Liuzhou precipitation were not only controlled by local pollution sources, but also were affected by the transmission distance of pollution sources from the northwest and southwest in the interior of continents. Talked together, our results revealed that the reduced acid precipitation in Liuzhou might be as a result of the combined action of karst chemical weathering, strict implementing environmental policy, and the reduction of long-term pollutant. It should be noted that the precipitation has a reducing trend to sulfuric-nitrous mixed type, suggesting that vehicle exhaust should be focused on the future.
According to the monitoring data of atmospheric precipitation in Liuzhou from 2013 to 2017, the effects of acid precipitation and its mitigation in the typical industrial karst areas of Southwest China were analyzed to trace the source of ions for the history of acidic precipitation. Our findings revealed that, in the past five years, the pH values increased slowly and had the obvious seasonal variation(pH values were lower in winter and spring than those in summer and fall). In this respect, the main ionic composition and variation of precipitation, the neutralization factor(NF) and the fractional acidity(AF) indicated that the ionic concentration of precipitation was still sulfur type with a reducing trend to sulfuric-nitrous mixed type and the 99.97% acid ions were neutralized by NH~+_4 and Ca~(2+) ions, suggesting that it might be the important factor to mitigating acid precipitation. Besides that, the Hysplit model was applied to trace and cluster the precipitation with 60 times in 2016. It was found that the compositions and concentrations of ions about Liuzhou precipitation were not only controlled by local pollution sources, but also were affected by the transmission distance of pollution sources from the northwest and southwest in the interior of continents. Talked together, our results revealed that the reduced acid precipitation in Liuzhou might be as a result of the combined action of karst chemical weathering, strict implementing environmental policy, and the reduction of long-term pollutant. It should be noted that the precipitation has a reducing trend to sulfuric-nitrous mixed type, suggesting that vehicle exhaust should be focused on the future.
引文
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Al-Khashman O A. 2005. Ionic composition of wet precipitation in thePetra Region, Jordan[J].Atmospheric Research, 78(1/2):1-12
Akkoyunlu B O, Tayanc M. 2003. Analyses of wet and bulk deposition in four different regions of Istanbul, Turkey[J]. Atmospheric Environment, 37(25):3571-3579
Araguás-Araguás L. 1998. Stable isotope composition of precipitation over southeast Asia[J]. Journal of Geophysical Research Atmospheres, 103(D22):28721-28742
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Báez A, Belmont R, García R, et al. 2007. Chemical composition of rainwater collected at a southwest site of Mexico City, Mexico[J]. Atmospheric Research, 86(1):61-75
Balasubramanian R, Victor T, Chun N. 2001. Chemical and statistical analysis of precipitation in singapore[J]. Water, Air, and Soil Pollution, 130(1/4):451-456
程新金,黄美元.1998.降水化学特性的一种分类分析方法[J].气候与环境研究,3(1): 82-88
丁国安,徐晓斌,王淑凤,等.2004.中国气象局酸雨网基本资料数据集及初步分析[J].应用气象学报,15(z1):85-94
董蕙青,黄海洪,高安宁,等.2005.影响广西酸雨的大气环流特征分析[J].气象,31(10):51-55
Das R, Das S N,Misra V N. 2005. Chemical composition of rainwater and dustfall at Bhubaneswar in the east coast of India[J]. Atmospheric Environment, 39(32):5908-5916
Ding G A, Xu X B, Fang X M, et al. 1997. Current status and future of acid rain in China[J]. Chinese Science Bulletin, 42 (24):2076-2076
郭雅思,于奭,黎泳珊,等.2016.桂林市酸雨变化特征及来源分析[J].环境科学,37(8):2897-2905
郭雅思.2017.柳州市酸雨化学特征分析及人为硫源对碳酸盐岩风化的影响[D].重庆:西南大学
Galloway J N, Likens G E, Edgerton E S. 1976. Acid precipitation in the Northeastern United States: pH and acidity[J]. Science (New York, N.Y.), 194(4266):722-724
Galloway J N, Savoie D L, Keene W C, et al. 1993. The temporal and spatial variability of scavenging ratios for NSS sulfate, nitrate, methanesulfonate and sodium in the Atmosphere over the North Atalantic Ocean[J]. Atmospheric Environment,27(2):235-250
Han G L, Liu C Q. 2004. Strontium isotope and chemical compositions of rainwaters from Guiyang, Guizhou Province, China[J]. Geochimica et Cosmochimica Acta,68(11):A461
Han G L, Tang Y, Wu Q X. 2010. Chemical and strontium isotope characterization of rainwater in karst virgin forest, Southwest China[J]. Atmospheric Environment, 44(2):174-181
Keene W C, Pszenny A A P, Galloway J N. 1986. Sea-salt corrections and interpretation of constituent ratios in marine precipitation[J]. Journal of Geophysical Research:Atmospheres, 91(D6): 6647-6658
Krupa S V. 2002. Sampling and physico-chemical analysis of precipitation:a review[J]. Environmental Pollution, 120(3):565-594
Kulshrestha U C, Kulshrestha M J, Sekar R. 2003. Chemical characteristics of rainwater at an urban site of south-central India[J]. Atmospheric Environment, 37(21):3019-3026
梁宏温,温远光,何斌,等.2002.柳州市中心酸雨化学特征与成因分析[J].广西农业生物科学,21(4):261-265
刘嘉麒.1996.降水背景值与酸雨定义研究[J].中国环境监测,(5):7-11
刘君峰,宋之光,许涛.2006.广州地区雨水化学组成与雨水酸度主控因子研究[J].环境科学,27(10):1998-2002
Lei X E, Han Z W, Zhang M G, et al. 1998. Physical, chemical, biological processes and mathematical model on air pollution[M]. Beijing:China Meteorological Press
Négrel P, Guerrot C, Millot R. 2007. Chemical and strontium isotopecharacterization of rainwater in France: influence of sources and hydrogeochemical implications[J]. Isotopes in Environmental and Health Studies, 43(3):179-196
牛彧文,何凌燕,胡敏.2008.深圳大气降水的化学组成特征[J].环境科学,29(4):1014-1019
Okuda T, Iwase T, Ueda H, et al. 2004. Long-term trend of chemical constituents in precipitation in Tokyo metropolitan area, Japan, from 1990 to 2002[J]. Science of the Total Environment, 339(1): 127-141
Possanzini M, Buttini P, Di Palo V. 1988. Characterization of a rural area in terms of dry and wet deposition[J]. Science of the Total Environment, 74:111-120
Rahn K A. 1976. Silicon and aluminum in atmospheric aerosols: Crust-air fractionation[J]. Atmospheric Environment, 10(8):597-601
Salam A, Bauer H, Kassin K, et al. 2003. Aerosol chemical characteristics of a mega-city in Southeast Asia (Dhaka-Bangladesh)[J]. Atmospheric Environment, 37(18):2517-2528
Sigg L, Stumm W, Zobrist J. 1987. The chemistry of fog:factors of regulating its composition[J]. Chimia International Journal for Chemistry, 41(41):159-165
Taylor S R. 1964. Abundance of chemical elements in the continental crust:a new table[J]. Geochimica Et Cosmochimica Acta, 28(8):1273-1285
王红梅.2005.浅析昆明市酸雨污染状况及变化[J].云南环境科学,24(3):51-54
王文兴.1994.中国酸雨成因研究[J].中国环境科学,14(5):323-329
王自发,高超,谢付莹.2007.中国酸雨模式研究回顾与所面临的挑战[J].自然杂志,29(2):78-82
韦翠云,蔡丽.2008.柳州酸雨分布特征分析[J].气象研究与应用,29(Z1):22
吴甫成,吴君维,王晓燕,等.2000.湖南酸雨污染特征[J].环境科学学报,20(6):807-809
吴起鑫,韩贵琳,陶发祥,等.2011.西南喀斯特农村降水化学研究:以贵州普定为例[J].环境科学,32(1):26-32
Wu Y, Xu Z F, Liu W J. 2016. Chemical compositions of precipitation at three non-urban sites of Hebei Province, North China: Influence of terrestrial sources on ionic composition[J]. Atmospheric Research, 181:115-123
Xu Z F, Li Y S, Tang Y. 2009. Chemical and strontium isotopecharacterization of rainwater at an urban site in Loess Plateau, northwest China[J]. Atmospheric Research, 94 (3):481-490
张红安,汤洁,于晓岚,等.2010.侯马市酸雨长期变化趋势分析[J].环境科学学报,30(5):1069-1078
郑凤琴,孙崇智,谢宏斌.2007.1991—2004年不同环流背景下南宁市降水化学成分变化特征的研究[J].热带气象学报,23(6):664-668
周晓得,徐志方,刘文景,等.2017.中国西南酸雨区降水化学特征研究进展[J].环境科学,38(10):4438-4446
Al-Momani I F, Aygun S, Tuncel G. 1998. Wet deposition of major ions and trace elements in the eastern Mediterranean basin[J]. Journal of Geophysical Research: Atmospheres, 103(D7): 8287-8299
Al-Khashman O A. 2005. Ionic composition of wet precipitation in thePetra Region, Jordan[J].Atmospheric Research, 78(1/2):1-12
Akkoyunlu B O, Tayanc M. 2003. Analyses of wet and bulk deposition in four different regions of Istanbul, Turkey[J]. Atmospheric Environment, 37(25):3571-3579
Araguás-Araguás L. 1998. Stable isotope composition of precipitation over southeast Asia[J]. Journal of Geophysical Research Atmospheres, 103(D22):28721-28742
程佳惠,李金娟,孙广权,等.2015.典型酸雨城市降水、降尘中阴阳离子分布特征及其相关性[J].环境科学学报,35(6):1676-1682
Báez A, Belmont R, García R, et al. 2007. Chemical composition of rainwater collected at a southwest site of Mexico City, Mexico[J]. Atmospheric Research, 86(1):61-75
Balasubramanian R, Victor T, Chun N. 2001. Chemical and statistical analysis of precipitation in singapore[J]. Water, Air, and Soil Pollution, 130(1/4):451-456
程新金,黄美元.1998.降水化学特性的一种分类分析方法[J].气候与环境研究,3(1): 82-88
丁国安,徐晓斌,王淑凤,等.2004.中国气象局酸雨网基本资料数据集及初步分析[J].应用气象学报,15(z1):85-94
董蕙青,黄海洪,高安宁,等.2005.影响广西酸雨的大气环流特征分析[J].气象,31(10):51-55
Das R, Das S N,Misra V N. 2005. Chemical composition of rainwater and dustfall at Bhubaneswar in the east coast of India[J]. Atmospheric Environment, 39(32):5908-5916
Ding G A, Xu X B, Fang X M, et al. 1997. Current status and future of acid rain in China[J]. Chinese Science Bulletin, 42 (24):2076-2076
郭雅思,于奭,黎泳珊,等.2016.桂林市酸雨变化特征及来源分析[J].环境科学,37(8):2897-2905
郭雅思.2017.柳州市酸雨化学特征分析及人为硫源对碳酸盐岩风化的影响[D].重庆:西南大学
Galloway J N, Likens G E, Edgerton E S. 1976. Acid precipitation in the Northeastern United States: pH and acidity[J]. Science (New York, N.Y.), 194(4266):722-724
Galloway J N, Savoie D L, Keene W C, et al. 1993. The temporal and spatial variability of scavenging ratios for NSS sulfate, nitrate, methanesulfonate and sodium in the Atmosphere over the North Atalantic Ocean[J]. Atmospheric Environment,27(2):235-250
Han G L, Liu C Q. 2004. Strontium isotope and chemical compositions of rainwaters from Guiyang, Guizhou Province, China[J]. Geochimica et Cosmochimica Acta,68(11):A461
Han G L, Tang Y, Wu Q X. 2010. Chemical and strontium isotope characterization of rainwater in karst virgin forest, Southwest China[J]. Atmospheric Environment, 44(2):174-181
Keene W C, Pszenny A A P, Galloway J N. 1986. Sea-salt corrections and interpretation of constituent ratios in marine precipitation[J]. Journal of Geophysical Research:Atmospheres, 91(D6): 6647-6658
Krupa S V. 2002. Sampling and physico-chemical analysis of precipitation:a review[J]. Environmental Pollution, 120(3):565-594
Kulshrestha U C, Kulshrestha M J, Sekar R. 2003. Chemical characteristics of rainwater at an urban site of south-central India[J]. Atmospheric Environment, 37(21):3019-3026
梁宏温,温远光,何斌,等.2002.柳州市中心酸雨化学特征与成因分析[J].广西农业生物科学,21(4):261-265
刘嘉麒.1996.降水背景值与酸雨定义研究[J].中国环境监测,(5):7-11
刘君峰,宋之光,许涛.2006.广州地区雨水化学组成与雨水酸度主控因子研究[J].环境科学,27(10):1998-2002
Lei X E, Han Z W, Zhang M G, et al. 1998. Physical, chemical, biological processes and mathematical model on air pollution[M]. Beijing:China Meteorological Press
Négrel P, Guerrot C, Millot R. 2007. Chemical and strontium isotopecharacterization of rainwater in France: influence of sources and hydrogeochemical implications[J]. Isotopes in Environmental and Health Studies, 43(3):179-196
牛彧文,何凌燕,胡敏.2008.深圳大气降水的化学组成特征[J].环境科学,29(4):1014-1019
Okuda T, Iwase T, Ueda H, et al. 2004. Long-term trend of chemical constituents in precipitation in Tokyo metropolitan area, Japan, from 1990 to 2002[J]. Science of the Total Environment, 339(1): 127-141
Possanzini M, Buttini P, Di Palo V. 1988. Characterization of a rural area in terms of dry and wet deposition[J]. Science of the Total Environment, 74:111-120
Rahn K A. 1976. Silicon and aluminum in atmospheric aerosols: Crust-air fractionation[J]. Atmospheric Environment, 10(8):597-601
Salam A, Bauer H, Kassin K, et al. 2003. Aerosol chemical characteristics of a mega-city in Southeast Asia (Dhaka-Bangladesh)[J]. Atmospheric Environment, 37(18):2517-2528
Sigg L, Stumm W, Zobrist J. 1987. The chemistry of fog:factors of regulating its composition[J]. Chimia International Journal for Chemistry, 41(41):159-165
Taylor S R. 1964. Abundance of chemical elements in the continental crust:a new table[J]. Geochimica Et Cosmochimica Acta, 28(8):1273-1285
王红梅.2005.浅析昆明市酸雨污染状况及变化[J].云南环境科学,24(3):51-54
王文兴.1994.中国酸雨成因研究[J].中国环境科学,14(5):323-329
王自发,高超,谢付莹.2007.中国酸雨模式研究回顾与所面临的挑战[J].自然杂志,29(2):78-82
韦翠云,蔡丽.2008.柳州酸雨分布特征分析[J].气象研究与应用,29(Z1):22
吴甫成,吴君维,王晓燕,等.2000.湖南酸雨污染特征[J].环境科学学报,20(6):807-809
吴起鑫,韩贵琳,陶发祥,等.2011.西南喀斯特农村降水化学研究:以贵州普定为例[J].环境科学,32(1):26-32
Wu Y, Xu Z F, Liu W J. 2016. Chemical compositions of precipitation at three non-urban sites of Hebei Province, North China: Influence of terrestrial sources on ionic composition[J]. Atmospheric Research, 181:115-123
Xu Z F, Li Y S, Tang Y. 2009. Chemical and strontium isotopecharacterization of rainwater at an urban site in Loess Plateau, northwest China[J]. Atmospheric Research, 94 (3):481-490
张红安,汤洁,于晓岚,等.2010.侯马市酸雨长期变化趋势分析[J].环境科学学报,30(5):1069-1078
郑凤琴,孙崇智,谢宏斌.2007.1991—2004年不同环流背景下南宁市降水化学成分变化特征的研究[J].热带气象学报,23(6):664-668
周晓得,徐志方,刘文景,等.2017.中国西南酸雨区降水化学特征研究进展[J].环境科学,38(10):4438-4446