青岛近岸区域典型海陆人为交互作用下酸雨的化学特征
Chemical characteristics of acid rain under the representative interaction among sea, land and anthropogenic activities in the coastal area of Qingdao
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摘要: 作为我国北方地区酸雨最为严重的城市之一,青岛及其近岸区域酸雨的研究对揭示典型海陆人为交互作用下酸雨形成机理具有典型的示范性.本文从酸雨的现状及变化、酸雨形成机制及影响因素、雨水中致酸/碱性成分的来源入手,系统总结了青岛近岸区域酸雨的化学特征.结果表明,青岛近岸区域自1981年以来酸雨状况有所减轻,但2006年以来又有加重的趋势,并由“硫酸型”酸雨向“硫-硝混合型”酸雨转变.局地人为源SO2和NOx的排放、区域外污染物的输送以及海上浮游生物释放的二甲基硫(DMS)是该地区大气致酸物质的3条重要输入途径.大气中致酸成分前体物的浓度和排放强度、气溶胶中酸化缓冲/碱性物质的含量以及复杂多变的气象条件是该区域酸雨形成的主要控制因素.人为源和地壳源分别是大气中致酸成分和碱性成分的主要来源,海盐源硫酸盐气溶胶会对降水酸性产生一定的稀释作用.今后的研究应特别重视:(1)降水pH的动态变化及与大气颗粒物的相互作用;(2)低分子有机弱酸、重金属及与污染有机物的复合污染作用机制对酸雨的影响;(3)优化酸沉降模型,精确量化解析不同来源对雨水酸性成分的贡献;(4)雾、露、霜等其它形式的酸沉降及沉降通量.深入研究青岛近岸区域酸雨的地球化学特征,不但有助于加深对海陆人为交互作用下我国东部沿海经济发达地区大气污染与酸沉降形成机理及其生态效应的认识,还可为科学制定酸雨防控对策提供理论依据.Abstract: As one of the most seriously suffered cities from acid rain in the north of China, Qingdao and its coastal area is typical for revealing the formation mechanism of acid rain under the representative interactions among sea, land and anthropogenic activities. In this paper, the chemical characteristics of acid rain in Qingdao coastal area were systematically summarized via the current status and variation, the formation mechanisms and its affecting factors, and the origins of acid/alkaline components in rainwater. The results indicated that the acidity and frequency of acid rain had been decreasing since 1981 but enhanced again from 2006, and the type of acid rain changed from "sulfuric acid" to "sulfuric-nitric acid mixture". The emissions of SO2 and NOx from the local anthropogenic activities, long-range transport of external atmospheric pollutants, and dimethylsulfide (DMS) released from marine planktons are the three major sources of acidic substances in the air of Qingdao coastal area. Meanwhile, concentrations and emission intensity of atmospheric acidic precursors, contents of buffer or alkaline substances as well as the changeable meteorological conditions are the three primary factors that control the formation of acid rain in this region. In the rainwater, the acidic components are mainly anthropogenic, but alkaline components are from crustal sources. The aerosol originated from sea salt may exert a dilution effect on the acidity of rainwater to a certain degree. Several suggestions for further studies on acid rain in Qingdao coastal area were put forward as follows:(1) to focus on the dynamic variation of pH in rainwater and its interaction with atmospheric suspended particles; (2) to focus on the combined effects of multiple pollutants of weak organic acids with low molecular weight, heavy metals and organic pollutants in acid rain; (3) to optimize the acid deposition models for accurately analyzing the contributions of different sources of acidic components in rainwater; (4) to strengthen the studies on other forms of acid deposition such as fog, dew and frost and their fluxes. Further studies on the geochemical characteristics of acid rain in Qingdao coastal areas are not only beneficial to getting a deeper insight into the formation mechanism as well as the ecological environmental effects of air pollution and acid deposition under the interactions among sea, land and anthropogenic activities in the developed eastern China coastal areas, but could also provide theoretical basis on scientific strategies of prevention and control of acid rain.
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Key words:
- acid rain /
- pH value /
- acidic component /
- alkaline component /
- anthropogenic activities /
- Qingdao coastal area
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[1] CHARLSON R, RODHE H. Factors controlling the acidity of natural rainwater[J]. Nature, 1982, 295:683-685. [2] CAO Y Z, WANG S Y, ZHANG G, et al. Chemical characteristics of wet precipitation at an urban site of Guangzhou, South China[J]. Atmospheric Research, 2009, 94(3):462-469. [3] WANG W X, WANG T. On the origin and the trend of acid precipitation in China[J]. Water, Air, and Soil Pollution, 1995, 85(4):2295-2300. [4] 宋少杰, 陈宁, 王建华, 等. 青岛地区酸沉降现状的研究[J]. 环境科学研究, 1996, 9(5):9-12. SONG S J, CHEN N, WANG J H, et al. Study on current situation of acid deposition in Qingdao area[J]. Research of Environmental Sciences, 1996, 9(5):9-12(in Chinese).
[5] 贾洪玉, 张巧显, 邓红兵, 等. 山东省主要城市酸沉降现状及影响因素分析[J]. 环境科学, 2006, 27(12):2453-2457. JIA H Y, ZHANG Q X, DENG H B, et al. Current situation and impact factors of acid deposition in main cities of Shandong Province[J]. Environmental Science, 2006, 27(12):2453-2457(in Chinese).
[6] 王俊英, 郝欣欣, 甄文栋, 等. 青岛市降水化学组成特征及相关性分析[J]. 山东大学学报, 2006, 36(3):56-59 , 107. WANG J Y, HAO X X, ZHEN W D, et al. Characteristics and correlative analysis of chemical composition of precipitation in Qingdao City[J]. Journal of Shandong University (Engineering Science), 2006, 36(3):56-59, 107(in Chinese).
[7] 刘宝章, 李金龙, 王敬云, 等. 青岛地区边界层特征及酸雨成因[J]. 环境科学学报, 1998, 18(1):39-44. LIU B Z, LI J L, WANG J Y, et al. Character of the boundary layer and cause of acid rain in the Tsingdao area[J]. Acta Scientiae Circumstantiae, 1998, 18(1):39-44(in Chinese).
[8] 张慧明, 应金生, 林小妍, 等. 青岛市酸雨污染的状况及发展趋势[J]. 环境科学进展, 1995, 3(2):61-69. ZHANG H M, YING J S, LIN X Y, et al. The present situation and the trend of acid rain pollution in Qingdao[J]. Advances in Environmental Science, 1995, 3(2):61-69(in Chinese).
[9] [10] 亓靓, 宋传真, 董君. 青岛市"十五"期间酸雨特征及成因浅析[J]. 环境科学与管理, 2007, 32(8):44-46. QI L, SONG C Z, DONG J. The analysis on the characteristic and causes of acid rain in Qingdao[J]. Environmental Science and Management, 2007, 32(8):44-46(in Chinese).
[11] 姜晓璐. 东、黄海的大气干、湿沉降及其对海洋初级生产力的影响[D]. 青岛:中国海洋大学, 2009:1-32. JIANG X L. Atmospheric dry and wet deposition of nutrient in East China Sea and Yellow Sea and its impact on marine primary production[D]. Qingdao:Ocean University of China, 2009:1 -32(in Chinese).
[12] 朱玉梅. 东、黄海大气沉降中营养盐的研究[D]. 青岛:中国海洋大学, 2011. ZHU Y M. Nutrients in atmospheric deposition of the Yellow and East China Sea[D]. Qingdao:Ocean University of China, 2011(in Chinese). [13] 张占峰, 王红磊, 德力格尔, 等. 瓦里关大气降水的化学特征[J]. 大气科学学报, 2014, 37(4):502-508. ZHANG Z F, WANG H L, DELI G E, et al. Chemical characteristics of atmospheric precipitation in Waliguan[J]. Transactions of Atmospheric Sciences, 2014,37(4):502-508(in Chinese).
[14] 王艳, 葛福玲, 刘晓环, 等. 泰山降水的离子组成特征分析[J]. 中国环境科学, 2006, 26(4):422-426. WANG Y, GE F L, LIU X H, et al. Analysis of ionic composition characteristics of precipitation at Mount Taishan[J]. China Environmental Science, 2006, 26(4):422-426(in Chinese).
[15] ZHANG X, JIANG H, ZHANG Q, et al. Chemical characteristics of rainwater in northeast China, a case study of Dalian[J]. Atmospheric Research, 2012, 116:151-160. [16] 王志春, 丁凌云, 刘尉, 等. 广州酸雨现状及影响因素分析[J]. 热带气象学报, 2011, 27(5):717-722. WANG Z C, DING L Y, LIU W, et al. Current status and causes of acid rain in Guangzhou[J]. Journal of Tropical Meteorology, 2011, 27(5):717-722(in Chinese).
[17] 薛德强, 鹿健, 郑全岭, 等. 青岛降水的酸性分析[J]. 山东气象, 1996, 16(1) 12-14. XUE D Q, LU J, ZHENG Q L, et al. The analysis of acidity of acid rain in Qingdao[J]. Journal of Shandong Meteorology, 1996, 16(1) 12-14(in Chinese).
[18] 毕言锋. 中国东部沿海的大气营养盐干、湿沉降及其对海洋初级生产力的影响[D]. 青岛:中国海洋大学硕士学位论文, 2006:1-55. BI Y F. Atmospheric nutrient deposition at the East China coast and its impact on marine primary production[D]. Qingdao:Thesis for Master Degree of Ocean University of China, 2006:1 -55(in Chinese).
[19] 张爱群, 徐晓峰, 徐文静, 等. 北京地区酸雨概况及特征分析//中国气象学会. 中国气象学会2008年年会大气环境监测、预报与污染物控制分会场论文集[C]. 北京:中国气象学会,2008:160-163. ZHANG A Q, XU X F, XU W J, et al. The general status and characteristics of acid rain in Beijing//Chinese Meteorological Society. Proceedings of Atmospheric Environmental Monitoring, Forecast and Controlling of Pollutants of Annual Symposium for Chinese Meteorological Society, 2008[C]. Beijing:Chinese Meteorological Society, 2008 :160-163(in Chinese).
[20] 吴起鑫, 韩贵琳. 三峡水库库首地区大气降水化学特征[J]. 中国环境科学, 2012, 32(3):385-390. WU Q X, HAN G L. Chemical characteristics of rainwater collected in the head region of Three Gorges Reservoir[J]. China Environmental Science, 2012, 32(3):385-390(in Chinese).
[21] ZHANG M Y, WANG S J, WU F C, et al. Chemical compositions of wet precipitation and anthropogenic influences at a developing urban site in southeastern China[J]. Atmospheric Research, 2007, 84(4):311-322. [22] 刘宝章, 王敬云. 青岛地区酸雨发展时空变化研究[J]. 环境科学学报, 2000, 20(增刊):34-39. LIU B Z, WANG J Y. Study on the spatiotemporal distribution of acid rain in Qingdao region[J]. Acta Scientiae Circumstantiae, 2000 , 20(suppl):34-39(in Chinese).
[23] TUNCER B, BAYAR B, YESILYURT C, et al. Ionic composition of precipitation at the Central Anatolia (Turkey)[J]. Atmospheric Environment, 2001, 35(34):5989-6002. [24] YANG F, TAN J, SHI Z B, et al. Five-year record of atmospheric precipitation chemistry in urban Beijing, China[J]. Atmospheric Chemistry and Physics, 2012, 12(4):2025-2035. [25] 程新金, 黄美元. 降水化学特性的一种分类分析方法[J]. 气候与环境研究, 1998, 3(1):83-89. CHENG X J, HUANG M Y. A Classification method to analyze the chemical characteristics of precipitation[J]. Climatic and Environmental Research, 1998, 3(1):83-89(in Chinese).
[26] 王文兴, 许鹏举. 中国大气降水化学研究进展[J]. 化学进展, 2009, 21(2/3):266 -281. WANG W X XU P J. Research progress in precipitation chemistry in China[J]. Progress in Chemistry, 2009, 21(2/3):266-281(in Chinese).
[27] 宋金明, 詹斌秋, 李鹏程. 中国酸性沉降物致酸机理的研究//中国科协首届青年学术年会论文集(理科分册)[C]. 北京:中国科技出版社, 1992:600-610. SONG J M, ZHAN B Q, LI P C. Study of acidification mechanism for acidic deposition in China//Proceedings of the Second Academic Conference of Young Scientists of China Association for Science and Technology (Science Fascicule)[C]. Beijing:China Science and Technology Press, 1992:600 -610(in Chinese).
[28] 殷美雪. 中国中东部地区大气湿沉降中的离子化学特征[D]. 上海:上海师范大学, 2015:1-60. YIN M X. Chemical characteristics of ions in atmospheric wet deposition in the mid-eastern China[D]. Shanghai:Shanghai Normal University, 2015:1 -60(in Chinese).
[29] FENG Z W, HUANG Y Z, FENG Y W, et al. Chemical composition of precipitation in Beijing area, Northern China[J]. Water, Air, and Soil Pollution, 2001, 125(1):345-356. [30] TANG A H, ZHUANG G S, WANG Y, et al. The chemistry of precipitation and its relation to aerosol in Beijing[J]. Atmospheric Environment, 2005, 39(19):3397-3406. [31] BAI L, WANG Z L. Anthropogenic influence on rainwater in the Xi'an City, Northwest China:Constraints from sulfur isotope and trace elements analyses[J]. Journal of Geochemical Exploration, 2014, 137:65-72. [32] XIAO J. Chemical composition and source identification of rainwater constituents at an urban site in Xi'an[J]. Environmental Earth Sciences, 2016, 75(3):1-12. [33] WANG Y S, YU W P, PAN Y P, et al. Acid neutralization of precipitation in Northern China[J]. Journal of the Air & Waste Management Association, 2012, 62(2):204-211. [34] 王文兴, 丁国安. 中国降水酸度和离子浓度的时空分布[J]. 环境科学研究, 1997, 10(2):1-7. WANG W X, DING G A. The geographical distribution of ion concentration in precipitation over China[J]. Research of Environmental Sciences, 1997, 10(2):1-7(in Chinese).
[35] 张新民, 柴发合, 王淑兰, 等. 中国酸雨研究现状[J]. 环境科学研究, 2010, 23(5):527-532. ZHANG X M, CHAI F H, WANG S L, et al. Research progress of acid precipitation in China[J]. Research of Environmental Sciences, 2010, 23(5):527-532(in Chinese).
[36] [37] [38] 魏巍. 青岛市酸雨影响因素分析及降水酸度预测[D]. 青岛:中国海洋大学, 2008:1-70. WEI W. The influencing factors analysis of acid rain and forecast of precipitation acidity in Qingdao[D]. Qingdao:Ocean University of China, 2008:1 -70(in Chinese).
[39] 宋金明, 李鹏程, 詹斌秋. 大气污染物质SO2对雾水酸度的控制作用[J]. 海洋科学, 1994, 18(5):44-49. SONG J M, LI P C, ZHAN B Q. Controlling effect of atmospheric pollutant SO2 on fogwater acidity[J]. Marine Sciences, 1994, 18(5):44-49(in Chinese).
[40] 刘宝章, 李金龙, 王敬云, 等. 青岛酸雨天气边界层气象特征[J]. 中国环境科学, 1997,17(2):103-107. LIU B Z, LI J L, WANG J Y, et al. Meteorological features of the boundary layer for the weather of acid rain in Qingdao[J]. China Environmental Science, 1997,17(2):103-107(in Chinese).
[41] 王文兴. 中国酸雨成因研究[J]. 中国环境科学, 1994, 14(5):323-328. WANG W X. Study on the origin of acid rain formation in China[J]. China Environmental Science, 1994, 14(5):323-328(in Chinese).
[42] 朱彤. 城市与区域大气复合污染//戴树桂. 环境化学进展[M]. 北京:化学工业出版社, 2005:1-17. ZHU T. Combined air pollution in city and region//. DAI S G. Advances in Environmental Chemistry[M]. Beijing:Chemical Industry Press, 2005:1 -17(in Chinese).
[43] 马奇菊, 胡敏, 田旭东, 等. 青岛近岸海域二甲基硫排放和大气中二甲基硫浓度变化[J]. 环境科学, 2004, 25(1):20-24. MA Q J, HU M, TIAN X D, et al. Dimethylsulfide emission in Qingdao near-shore waters and atmospheric dimethylsulfide concentration variation[J]. Environmental Science, 2004,25(1):20-24(in Chinese).
[44] 田旭东, 胡敏, 马奇菊. 青岛环境大气和海洋表层水中挥发性硫化物的测定[J]. 环境科学学报, 2005, 25(1):30-33. TIAN X D, HU M, MA Q J. Determination of volatile sulfur compounds in the atmosphere and surface seawater in Qingdao[J]. Acta Scientiae Circumstantiae, 2005, 25(1):30-33(in Chinese).
[45] 胡敏, 唐孝炎, 李金龙, 等. 胶州湾海水中二甲基硫的测定[J]. 环境科学学报, 1997, 17(1):110-115. HU M, TANG X Y, LI J L, et al. Dimethylsulfide in sea water in the Gulf of Jiaozhou[J]. Acta Scientiae Circumstantiae, 1997, 17(1):110-115(in Chinese).
[46] LU X W, LI L Y, LI N, et al. Chemical characteristics of spring rainwater of Xi'an city, NW China[J]. Atmospheric Environment, 2011, 45(28):5058-5063. [47] CAO J J, TIE X X, DABBERDT W F, et al. On the potential high acid deposition in northeastern China[J]. Journal of Geophysical Research:Atmospheres, 2013, 118(10):4834-4846. [48] XU Z F, WU Y, LIU W J, et al. Chemical composition of rainwater and the acid neutralizing effect at Beijing and Chizhou city, China[J]. Atmospheric Research, 2015, 164:278-285. [49] WU D, WANG S G, XIA J R, et al. The influence of dust events on precipitation acidity in China[J]. Atmospheric Environment, 2013, 79:138-146. [50] 刘素美, 黄薇文, 张经, 等. 青岛地区大气沉降物中化学成分研究2.常量组分[J]. 海洋环境科学, 1993, 12(3/4):89 -98. LIU S M, HUANG W W ZHANG J, et al. Study on the chemical components of atmospheric deposition matters in Qingdao 2. Bulk component[J]. Marine Environmental Science, 1993, 12(3/4):89-98(in Chinese).
[51] AL-KHASHMAN O A. Chemical characteristics of rainwater collected at a western site of Jordan[J]. Atmospheric Research, 2009, 91(1):53-61. [52] KEENE W C, PSZENNY A A P, GALLOWAY J N, et al. Sea-salt corrections and interpretation of constituent ratios in marine precipitation[J]. Journal of Geophysical Research:Atmospheres, 1986, 91(D6):6647-6658. [53] TAYLOR S. Abundance of chemical elements in the continental crust:a new table[J]. Geochimica et Cosmochimica Acta, 1964, 28(8):1273-1285. [54] LI Y C, ZHANG M, SHU M, et al. Chemical characteristics of rainwater in Sichuan basin, a case study of Ya'an[J]. Environmental Science and Pollution Research, 2016:23(13):13088-13099. [55] DAS R, DAS S N, MISRA V N. Chemical composition of rainwater and dustfall at Bhubaneswar in the east coast of India[J]. Atmospheric Environment, 2005, 39(32):5908-5916. [56] 肖辉, 沈志来, 黄美元. 西太平洋热带海域降水化学特征[J]. 环境科学学报, 1993, 13(2):143-149. XIAO H, SHEN Z L, HUANG M Y. Chemical characteristics of tropical western Pacific precipitation[J]. Acta Scientiae Circumstantiae, 1993, 13(2):143-149(in Chinese).
[57] 张金良, 于志刚, 张经, 等. 黄海西部大气湿沉降(降水)的pH与主要酸碱离子的关系[J]. 海洋环境科学, 2000, 19(3):30-34. ZHANG J L, YU Z G, ZHANG J, et al. Relation of pH and major acid and alkaline ions in atmospheric wet deposition (precipitation) of Western Yellow Sea[J]. Marine Environmental Science, 2000, 19(3):30-34(in Chinese).
[58] 武瑶, 徐志方. 大气降水中稳定同位素研究进展[J]. 地球与环境, 2013, 41(6):688-695. WU Y, XU Z F. Progress in research on stable isotopes in precipitation in China:A review[J]. Earth and Environment, 2013, 41(6):688-695(in Chinese).
[59] XIAO H W, XIE L H, LONG A M, et al. Use of isotopic compositions of nitrate in TSP to identify sources and chemistry in South China Sea[J]. Atmospheric Environment, 2015, 109:70-78. [60] 李亲凯, 杨周, 黄俊, 等. 大气颗粒物稳定同位素组成的研究进展[J]. 生态学杂志, 2016, 35(4):1063-1071. LI Q K, YANG Z, HUANG J, et al. A review of stable isotopic compositions of atmospheric particulate matter[J]. Chinese Journal of Ecology, 2016, 35(4):1063-1071(in Chinese).
[61] 李佩霖, 傅平青, 康世昌, 等. 大气气溶胶中的氮:化学形态与同位素特征研究进展[J]. 环境化学, 2016, 35(1):1-10. LI P L, FU P Q, KANG S C, et al. Research progress on nitrogen in atmospheric aerosol:Chemical speciation and isotopic characteristics[J]. Environmental Chemistry, 2016, 35(1):1-10(in Chinese).
[62] 宋宇然. 青岛地区大气湿沉降的研究[D]. 青岛:中国海洋大学, 2006:1-59. SONG Y R. The study on atmospheric wet deposition in Qingdao[D]. Qingdao:Thesis for Master Degree of Ocean University of China, 2006:1 -59(in Chinese).
[63] XU H, BI X H, FENG Y C, et al. Chemical composition of precipitation and its sources in Hangzhou, China[J]. Environmental Monitoring and Assessment, 2011, 183(1/4):581-592. [64] WANG H, HAN G L. Chemical composition of rainwater and anthropogenic influences in Chengdu, Southwest China[J]. Atmospheric Research, 2011, 99(2):190-196. [65] HUANG K, ZHUANG G S, XU C, et al. The chemistry of the severe acidic precipitation in Shanghai, China[J]. Atmospheric Research, 2008, 89(1):149-160. [66] 宋金明, 李鹏程, 詹斌秋. 青岛雾水中的氯离子[J]. 海洋环境科学, 1992, 11(4):14-22. SONG J M, LI P C, ZHAN B Q. The chloridion in fog of Qingdao[J]. Marine Environmental Science, 1992, 11(4):14-22(in Chinese).
[67] 宋金明. 海洋环境中硫的存在形式[J]. 环境化学, 1990, 9(6):59-64. SONG J M. Species of sulfur in marine environments[J]. Environmental Chemistry, 1990, 9(6):59-64(in Chinese).
[68] AVERY G B, KIEBER R J, WITT M, et al. Rainwater monocarboxylic and dicarboxylic acid concentrations in southeastern North Carolina, USA, as a function of air-mass back-trajectory[J]. Atmospheric Environment, 2006, 40(9):1683-1693. [69] 徐刚, 李心清, 吕迎春, 等. 大气降水中低分子有机酸的季节变化及对酸雨形成的贡献(以贵阳市和尚重镇为例)[J]. 科学通报, 2009, 54(17):2568-2573. XU G, LI X Q, LV Y C, et al. Seasonal variations of carboxylic acids and their contributions to the rainwater acidity:A case study of Guiyang City and Shangzhong Town, China[J]. Chinese Science Bulletin, 2009, 54(17):2568-2573(in Chinese).
[70] ZHANG Y L, LEE X Q, CAO F, et al. Seasonal variation and sources of low molecular weight organic acids in precipitation in the rural area of Anshun[J]. Chinese Science Bulletin, 2011, 56(10):1005-1010. [71] GALLOWAY J N, LIKENS G E, KEENE W C, et al. The composition of precipitation in remote areas of the world[J]. Journal of Geophysical Research:Oceans, 1982, 87(C11):8771-8786. -

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