中国东部陆架海大气气溶胶中主要化学组成与来源分析
发布时间：2018-09-18 15:00
【摘要】：受陆地和海洋地共同影响，中国东部陆架海大气气溶胶中主要化学组成及其来源非常复杂，不仅如此大气气溶胶还可通过直接和间接辐射等方式影响大气辐射平衡，影响全球环境。本文以中国黄渤海和东海为研究对象，分别对2012年春季和秋季黄渤海，2011年冬季、2012年夏季和秋季东海海域进行大气样品的采集，分析其主要水溶性离子、部分痕量金属元素和低分子量有机酸的浓度水平，探讨其分布和来源情况，主要研究结果如下： （1）在黄渤海海域春季和秋季调查航次采集的大气总悬浮颗粒物（TotalSuspended Particulates，TSP）的质量分别为（0.18±0.04）g和（0.05±0.03）g，其中主要水溶性离子的总浓度分别为（23.3±10.7）μg·m-3和（27.1±9.4）μg·m-3，二次离子浓度比例最大，分别为84.7%和63.7%。各离子平均浓度大小顺序是NO3- nss-SO42- NH4+ Cl- Na+ nss-K+ nss-Ca2+ Mg2+；秋季为NO3-nss-SO42- NH4+ Cl- Na+ nss-K+ nss-Ca2+ Mg2+。秋季痕量金属离子浓度整体略高于春季，在所有金属离子中Al和Fe浓度水平最高，表现为：春季，FeAlZnPbV CuCd；秋季，FeAlZnPbCuVCd。黄渤海春季大气气溶胶中甲基磺酸（methanesulfonic acid，MSA）浓度平均值为（22.0±18.2）ng·m-3，秋季黄渤海平均值为（11.4±9.6）ng·m-3。CH3COOH和HCOOH秋季浓度水平较高，分别为（472.5±147.3）ng·m-3和（264.2±131.0）ng·m-3，春季CH3COOH和HCOOH平均浓度水平分别为（74.9±47.2）ng·m-3、（55.6±39.5）ng·m-3。 （2）在东海夏季航次采集的TSP质量为（0.012±0.003）g，水溶性离子总浓度为（12.3±3.1）μg·m-3，，其中海盐离子的浓度较大，各离子平均浓度由大到小为Cl- Na+ NO3- nss-SO42- NH4+ Mg2+ nss-K+ nss-Ca2+，二次离子在水溶性离子中的比例为49.2%；秋季TSP的质量为（0.020±0.013）g，水溶性离子总浓度为（21.3±8.2）μg·m-3，各离子大小顺序为Cl- Na+ nss-SO42- NO3-NH4+ Mg2+ nss-K+ nss-Ca2+，二次离子占离子浓度的40.3%。东海冬季采样航次水溶性离子浓度水平最高，平均浓度为（40.9±13.2）μg·m-3，二次离子所占比例也最高，67%，各离子大小顺序nss-SO42- Cl- NH4+ NO3- Na+ Mg2+nss-K+ nss-Ca2+。东海航次中痕量金属元素浓度水平低于黄渤海，夏季各金属元素平均浓度大小为FeAlZn Pb V CuCd，秋季为FeAl Zn Pb Cu VCd。东海航次有机酸的浓度低于黄渤海，其中MSA秋季浓度最高，夏季次之，冬季最低，平均浓度依次为（5.8±1.5）、（5.0±3.1）、（1.9±0.3）ng·m-3。夏季航次CH3COOH和HCOOH平均值为（43.6±37.0）、（16.0±9.1）ng·m-3；秋季浓度水平相当，分别为（50.8±45.0）、（66.8±56.2）ng·m-3。 （3）总水溶性离子对TSP质量的贡献表现为夏季最高，秋季次之，春季最低。二次离子NH4+、nss-SO42-和NO3-相对于地壳源的富集因子非常大，且三者相关性显著，主要来自人为源，Mg2+主要来自海洋源，K+和Ca2+主要受地壳源控制；在富集因子基础上分别估算人为源和地壳源对痕量金属元素的贡献率，结果表明近岸黄渤海中人为源对金属元素的贡献要普遍高于东海，人为源对Cd、Zn和Pb的贡献最大，而Fe和V源于自然和人为源的共同贡献。 （4）依据nss-SO42-/MSA的质量比值计算生源硫酸盐（SO42-bio）对nss-SO42-的贡献率，得到结果为：黄渤海春季和秋季SO42-bio对nss-SO42-的贡献率比较接近，分别为5.5%和5.6%，东海夏季、秋季和冬季航次SO42-bio对nss-SO42-的贡献率分别是2.2%、2.8%和0.8%。春季生源硫酸盐比例较高，但整体来看中国东部近海海域大气气溶胶的组成和其浓度分布明显受到人为活动输入的影响。
[Abstract]:The main chemical compositions and sources of atmospheric aerosols in the continental shelf sea of Eastern China are very complex due to the combined effects of land and ocean terrain. Not only can the atmospheric aerosols affect the atmospheric radiation balance through direct and indirect radiation, but also affect the global environment. Atmospheric samples were collected in the Yellow Sea and Bohai Sea in the autumn and autumn of 2011, winter, summer and autumn of 2012. Concentrations of major water-soluble ions, some trace metal elements and low molecular weight organic acids were analyzed, and their distribution and sources were discussed.
(1) Total Suspended Particulates (TSP) in the Yellow Sea and Bohai Sea in spring and autumn were (0.18.04) g and (0.05.03) g, respectively. The total concentrations of major water-soluble ions were (23.3 (10.7) UG The average concentrations of the ions were NO3-nss-SO42-NH4+Cl-Na+nss-K+nss-Ca2+Mg2+, NO3-nss-SO42-NH4+Cl-Na+nss-K+nss-Ca2+Mg2+, and NO3-nss-SO42-NH4+Cl-Na+nss-K+nss-Ca2+Mg2+. The concentrations of trace metal ions in autumn were slightly higher than those in spring, and the concentrations of Al and Fe were the highest among all the metal ions, namely, in spring, Fe Al-ZnPbV-Cud, and in autumn, F-ZnPbV-Cd. EAlZnPbCuVCd. The mean concentrations of methanesulfonic acid (MSA) in the atmospheric aerosols of the Yellow Sea and Bohai Sea in spring were (22.0 6550 The bisection is (74.9 + 47.2) ng? M-3, (55.6 + 39.5) ng? M-3.
(2) The mass of TSP collected during the East China Sea summer voyage was (0.012.003) g and the total concentration of water-soluble ions was (12.3 The total concentration of water-soluble ions was (21.3 6550 The concentrations of trace metals in the East China Sea voyages were lower than those in the Yellow and Bohai Seas. The average concentrations of metals in summer were FeAlZn Pb V CuCd and in autumn were FeAl Zn Pb Cu VCd. The concentrations of organic acids in the East China Sea voyages were lower than those in the Yellow and Bohai Seas, and the concentrations of MSA in autumn were the highest. The average concentrations of CH3COOH and HCOOH in summer voyages were (43.6+37.0), (16.0+9.1) ng.m-3 and (50.8+45.0), (66.8+56.2) ng.m-3, respectively.
(3) The contribution of total water-soluble ions to TSP quality is the highest in summer, the second in autumn, and the lowest in spring. The enrichment factors of secondary ions NH4 +, nss-SO42 - and NO3 - are very large relative to crustal sources, and their correlation is significant, mainly from human sources, Mg2+ mainly from marine sources, and K + and Ca2+ mainly from crustal sources. The contributions of anthropogenic sources and crustal sources to trace metal elements are estimated respectively. The results show that the contribution of anthropogenic sources to metal elements is generally higher in the Yellow Sea and Bohai Sea than in the East China Sea. The contribution of anthropogenic sources to Cd, Zn and Pb is the greatest, while that of Fe and V is the joint contribution of natural and human sources.
(4) According to the mass ratio of nss-SO42-/MSA, the contribution rates of SO42-bio to nss-SO42-were calculated. The results showed that the contribution rates of SO42-bio to nss-SO42-in spring and autumn were close to 5.5% and 5.6%, respectively. The contribution rates of SO42-bio to nss-SO42-in summer, autumn and winter were 2.2%, 2.8% and 0.8% respectively. Source sulphates are relatively high, but the composition and concentration distribution of atmospheric aerosols in the coastal waters of Eastern China are obviously affected by anthropogenic input.
【学位授予单位】：中国海洋大学
【学位级别】：硕士
【学位授予年份】：2014
【分类号】：P732;X513
本文编号：2248280
[Abstract]:The main chemical compositions and sources of atmospheric aerosols in the continental shelf sea of Eastern China are very complex due to the combined effects of land and ocean terrain. Not only can the atmospheric aerosols affect the atmospheric radiation balance through direct and indirect radiation, but also affect the global environment. Atmospheric samples were collected in the Yellow Sea and Bohai Sea in the autumn and autumn of 2011, winter, summer and autumn of 2012. Concentrations of major water-soluble ions, some trace metal elements and low molecular weight organic acids were analyzed, and their distribution and sources were discussed.
(1) Total Suspended Particulates (TSP) in the Yellow Sea and Bohai Sea in spring and autumn were (0.18.04) g and (0.05.03) g, respectively. The total concentrations of major water-soluble ions were (23.3 (10.7) UG The average concentrations of the ions were NO3-nss-SO42-NH4+Cl-Na+nss-K+nss-Ca2+Mg2+, NO3-nss-SO42-NH4+Cl-Na+nss-K+nss-Ca2+Mg2+, and NO3-nss-SO42-NH4+Cl-Na+nss-K+nss-Ca2+Mg2+. The concentrations of trace metal ions in autumn were slightly higher than those in spring, and the concentrations of Al and Fe were the highest among all the metal ions, namely, in spring, Fe Al-ZnPbV-Cud, and in autumn, F-ZnPbV-Cd. EAlZnPbCuVCd. The mean concentrations of methanesulfonic acid (MSA) in the atmospheric aerosols of the Yellow Sea and Bohai Sea in spring were (22.0 6550 The bisection is (74.9 + 47.2) ng? M-3, (55.6 + 39.5) ng? M-3.
(2) The mass of TSP collected during the East China Sea summer voyage was (0.012.003) g and the total concentration of water-soluble ions was (12.3 The total concentration of water-soluble ions was (21.3 6550 The concentrations of trace metals in the East China Sea voyages were lower than those in the Yellow and Bohai Seas. The average concentrations of metals in summer were FeAlZn Pb V CuCd and in autumn were FeAl Zn Pb Cu VCd. The concentrations of organic acids in the East China Sea voyages were lower than those in the Yellow and Bohai Seas, and the concentrations of MSA in autumn were the highest. The average concentrations of CH3COOH and HCOOH in summer voyages were (43.6+37.0), (16.0+9.1) ng.m-3 and (50.8+45.0), (66.8+56.2) ng.m-3, respectively.
(3) The contribution of total water-soluble ions to TSP quality is the highest in summer, the second in autumn, and the lowest in spring. The enrichment factors of secondary ions NH4 +, nss-SO42 - and NO3 - are very large relative to crustal sources, and their correlation is significant, mainly from human sources, Mg2+ mainly from marine sources, and K + and Ca2+ mainly from crustal sources. The contributions of anthropogenic sources and crustal sources to trace metal elements are estimated respectively. The results show that the contribution of anthropogenic sources to metal elements is generally higher in the Yellow Sea and Bohai Sea than in the East China Sea. The contribution of anthropogenic sources to Cd, Zn and Pb is the greatest, while that of Fe and V is the joint contribution of natural and human sources.
(4) According to the mass ratio of nss-SO42-/MSA, the contribution rates of SO42-bio to nss-SO42-were calculated. The results showed that the contribution rates of SO42-bio to nss-SO42-in spring and autumn were close to 5.5% and 5.6%, respectively. The contribution rates of SO42-bio to nss-SO42-in summer, autumn and winter were 2.2%, 2.8% and 0.8% respectively. Source sulphates are relatively high, but the composition and concentration distribution of atmospheric aerosols in the coastal waters of Eastern China are obviously affected by anthropogenic input.
【学位授予单位】：中国海洋大学
【学位级别】：硕士
【学位授予年份】：2014
【分类号】：P732;X513
【参考文献】
相关期刊论文 前4条
1 陈兴茂,冯丽娟,李先国,祁建华,张曼平;青岛地区大气气溶胶中微量金属的时空分布[J];环境化学;2004年03期
2 江伟;李心清;曾勇;黄荣生;谭凌;徐刚;王兵;;贵州省遵义地区降水中低分子有机酸及其来源[J];环境科学;2008年09期
3 陈立奇,高鹏飞,杨绪林;环球海洋大气气溶胶化学研究 Ⅱ.来源示踪元素的特征[J];海洋与湖沼;1993年03期
4 张岩;张洪海;杨桂朋;;秋季渤海、北黄海大气气溶胶中水溶性离子组成特性与来源分析[J];环境科学;2013年11期
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